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An overview of hydrogen production from Al-based materials

  • Liang Sun EMAIL logo , Xiongshuai Ji , Yong Zhou , Hang Li , Wenyan Zhai EMAIL logo , Biqiang Chen , Hui Dong , Yanmin Liu and Tengwei Wang
Published/Copyright: November 21, 2023
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Nanotechnology Reviews
From the journal Nanotechnology Reviews Volume 12 Issue 1

Abstract

A profound overview of the recent development for on-time, on-demand hydrogen production from light metal-based hydrolysis is presented. Hydrogen energy is one of the clean and renewable energy sources which has been recognized as an alternative to fossil fuels. In addition, aluminum is the most suitable light activity metal for hydrolysis materials attributed to its safety, environmental friendliness, high-energy density, inexpensive, and low density with high strength ratio. In general, dense oxide films formed act as a barrier on aluminum surfaces. Accordingly, effective removal of the oxide film is a key measure in solving the Al–water reaction. In this review, recent advances in addressing the main drawbacks including high-purity aluminum with acid–alkali solutions, nano-powders of aluminum or composite with acid–base solutions, ball-milled nano-powders, alloying blocks, and gas atomization powders are summarized. The characteristics of these three technologies and the current research progress are summarized in depth. Moreover, it is essential to promote low-cost aluminum-based materials based on effective hydrogen production efficiency and explore ways for practical large-scale applications.

Keywords: hydrogen energy; Al-based alloys; hydrolysis reaction; activation metals; ball milling

1 Introduction

Energy is considered a “strategic commodity,” while the volume of global energy trade has developed substantially over the past 30 years. For global countries, energy security is the cornerstone of national security and a primary consideration in energy trade strategies and policies [1,2]. Currently, more than 80% of human energy consumption is accounted for by fossil fuels (coal, oil, and natural gas). Nevertheless, renewable energy stands in contrast to traditional biomass, which is being used far more quickly than they are being replenished. Derse et al. [3] noted that “Hydrogen network management is one of the focal issues for a cleaner and sustainable world. The developed model is compatible with the real world issues by incorporating safety conditions. The sensitivity analysis indicates that distances are effective on the total cost.” An urgent demand for developing clean and renewable green energy sources has been evoked [4]. On the one hand, the main cause of global warming was fossil fuels with an increase in the atmospheric greenhouse gas levels [5,6]. On the other hand, uniformly distributed fossil fuels which are controlled by certain countries globally raise conflicts regarding the security of supply and distribution in developing countries. Ultimately, finite sources of energy will be eventually depleted, and global competition and price increase of these resources cannot be ruled out in the future [7]. In response to increasing energy demand and low carbon needs, green and renewable energy has become a political and economic focal point finally [8]. For instance, Europe has committed to reducing greenhouse gas emissions by 80–95% below the 1990 levels by 2050 [9]. Of course, widening the utilization of solar, wind, hydro, and tidal natural energy can significantly reduce greenhouse gas emissions; however, they cannot be regulated because of intermittent sources [10,11]. The grid requires a certain percentage of stationary energy as a base; thus, storing clean energy is critical during this transformation. In order to phase out fossil fuels and limit climate change, hydrogen energy is considered the most promising option [9,12]. Hydrogen energy is a clean and renewable energy source and several advantages are as follows:

  1. Abundant reserves. Mainly in the form of hydrocarbons and water, and hydrogen is one of the most readily available elements on earth [13].

  2. Excellent energy density (122 kJ/g). Approximately 2.75 times more than that of hydrocarbon fuels [14].

  3. Non-toxic and non-polluting. Water is the only combustion product [15,16].

  4. Wide range of applications. High heat capacity can be benefited from hydrogen combustion to produce mechanical work in a heat engine, or as an energy material for fuel cells to generate electricity directly [17,18,19].

Hydrogen is a key chain between hydrogen-consuming industries and several essential sectors such as the electricity grid, gas grid, transportation, residential, agriculture, and energy storage [20]. Therefore, hydrogen energy is the most promising clean energy source at this stage [21,22]. Currently, fossil fuel hydrogen production methods have occupied the largest proportion of industrial hydrogen production (to date, the total volume of hydrogen consumption was 48% from natural gas, 30% from heavy oils and naphtha, and 18% from coal) [23,24,25,26]. Clearly, it is not in line with the strategic requirements of sustainable development in the world [27].

Thus, alternative methods of hydrogen production are urgently needed [24,28,29,30,31,32]. As shown in Figure 1, the production, application, and storage of hydrogen play a key role, yet it is always a challenge. As the density of hydrogen is only 7.14% of air density [33] and the ignition energy is only 0.02 mJ [14,34,35], special attention should be paid to safety issues during transportation. Metal hydrolysis behaves as a feature of convenient storage and transportation in hydrogen technology [36], which can provide on-time and on-demand hydrogen production. On the one hand, the replacement of large volumes, large weights, high-pressure resistant, or adiabatic hydrogen storage bottles can effectively avoid the safety problems during high-pressure gaseous hydrogen storage applications and low-temperature liquid hydrogen storage. On the other hand, infrastructure construction is suitable for gas applications in various special scenarios such as disaster area rescue, emergency power supply, field detection, single-armed combat, etc.

Figure 1 Importance of hydrogen in integrating different energy sectors.
Figure 1

Importance of hydrogen in integrating different energy sectors.

The theoretical hydrogen release content of aluminum (Al) is 11.1%, which is higher than that of Na (4.34%), Mg (8.3%), and Fe (3.57%) [37]. The production of hydrogen by hydrolysis reaction of hydrides (Mg and MgH2, NaBH4, LiAlH4, Al, etc.) recently attracted increased attention because of its safety and its amenability to mild reaction conditions. For example, in recent years, more and more attention has been paid to hydrogen generation by hydrolysis of metals, metal hydrides, or formic acid for their high theoretical hydrogen yield [38,39,40,41]. Generally, the energy efficiencies of the MgH2, H–Mg3La, and H–La2Mg17 hydrolysis cycles were 45.3, 40.1, and 41.1%, respectively, for half of the energy released by the exothermic reaction from this cycle was collected for recycling. However, the maximum energy efficiency (49.91%) indicates that the reaction of MgH2 with NaBO2 to form NaBH4 during ball milling is feasible [42,43]. Additionally, aluminum is the most abundant metal in the earth’s crust with a low density of 2,700 kg/m3. Likewise, it is of low cost and has high gravimetric and volumetric energy density and high energy efficiency (31.1 MJ/kg and 83.8 MJ/L) [44]. The Al–water reactions are as follows:

(1) 2 Al + 6 H 2 O → 2 Al ( OH ) 3 + 3 H 2 ,

(2) 2 Al + 4 H 2 O → 2 Al O ( OH ) + 3 H 2 .

According to reactions (1) and (2), 1 mol Al can produce 1.5 mol H2. Under theoretically standard conditions, 1,245 mL of hydrogen can be generated from 1 g of aluminum. The end-products of Al–water reaction (Al(OH)3, AlO(OH)) are non-toxic, non-polluting, and easy to collect and store. Other advantages include wide applications in flame retardants[45,46], adsorbents [47], etc. Therefore, the Al–water reaction can provide safe, environmentally friendly, and portable hydrogen energy. Furthermore, regeneration is a potential method for reducing the cost, and a one-step approach for hydrogen production, storage, and transportation is a new method via Li(Na)BH4 regeneration using Mg-based alloys and as the new topics for hydrogen-energy process chain and hydrogen economics [48,49,50].

This overview briefly introduced various hydrogen production technologies for aluminum-based materials, compared the development trends of each technology, and provided an outlook on the future advanced methods for aluminum-based materials. Theoretically, since the Gibbs free energy ∆G < 0 for the Al–water reaction, it means the reaction direction can conduct spontaneously with water. However, a dense alumina film is formed on the Al-based material surface for its activity, which prevents the Al–water reaction from proceeding [51,52]. Hence, eliminating the oxide layer is a key point to the problem of Al–water reaction.

2 Reaction with acid or alkali solution

Al2O3 is the main component of the dense film on the surface of aluminum which can react with both acid and alkali solutions at room temperature. The reaction mechanism among HCl is displayed as follows:

(3) Al 2 O 3 + 6 HCl → 2 Al Cl 3 + 3 H 2 O ,

(4) 2 Al + 6 HCl → 2 Al Cl 3 + 3 H 2 .

The acid solution reacts with Al2O3 first to destroy the outer oxide layer and then contacts the inner pure aluminum matrix, as evident from reactions (3) and (4). This reaction can evoke hydrogen generation directly. However, the H+ concentration decreases and the pH increases during the reaction. The hydrogen generation rate is bound to decrease whenever the acid supplementation is stopped. However, aluminum reacts differently with alkali solutions, and the surface aluminum passivation layer dissolved more easily than in acidic solutions. The reaction equations are given as follows [53,54,55]:

(5) Al 2 O 3 + 2 NaOH → 2 NaAl O 2 + H 2 O ,

(6) 2 Al + 6 H 2 O + 2 N a OH → 2 NaAl ( OH ) 4 + 3 H 2 ,

(7) NaAl ( OH ) 4 → NaOH + Al ( OH ) 3 .

First, the Al2O3 layer begins to dissolve in NaOH solution at the outer oxide layer. In other words, aluminum starts to lose its protective film and NaOH in the solution is consumed by the oxide layer and NaAl(OH)4 is produced, which in turn decomposes into NaOH again. Finally, aluminum directly reacts with water. During this whole process, NaOH does not participate in the Al–water reaction and only plays a role as a catalyst. Hiraki et al. [56] described the reaction of aluminum with sodium hydroxide solution which is shown in Figure 2. The schematic diagram of the experimental apparatus is shown in Figure 2(a), while the hydrogen generation and rate were detected with a flow meter. As shown in Figure 2(b), the content of H2 increases with time and the hydrogen generation rate starts to decrease after a certain time. When H2 is produced, the solution temperature increases rapidly. In addition, the pH of the solution decreases in the first period and then increases. The consumption of NaOH is mainly due to the formation of Al(OH)4 − first, and then Al(OH)4 − decomposes to Al(OH)3 and OH−. This reaction continues and moves in circles. Additionally, NaOH promotes the Al–water reaction more efficiently than KOH and Ca(OH)2 [57], while the reaction rate can be further increased by the temperature and the surface area of aluminum increased. In addition, the reaction rate is also strongly influenced by the concentration of the base solution. The consistency of CO2 in the air decreases the concentration gradient of free hydroxides in aqueous solutions and the reaction rate [58,59].

Figure 2 (a) Schematic diagram of the experimental apparatus (b) Time evolution of the temperature and pH of the NaOH aqueous solution, the accumulated volume and the generation rate of hydrogen [56].
Figure 2

(a) Schematic diagram of the experimental apparatus (b) Time evolution of the temperature and pH of the NaOH aqueous solution, the accumulated volume and the generation rate of hydrogen [56].

Although this kind of reaction provides a compact source of hydrogen, it is not suitable for practical use because highly concentrated acid and alkali solutions can corrode the equipment, and strict control of the pH of the solution is required to achieve good hydrolysis results.

3 Hydrolysis reactions of ball-milled aluminum matrix composites

A powerful means of activating aluminum is mechanical ball milling [60] which crushes the powder into particles by strongly impacting, grinding, and stirring the aluminum powder through mechanical alloying and milling [61,62]. In milling, large particles of metal are ground into small particles, and ball milling builds on this by converting small particles into nano-powder and forming new compounds between different metals; therefore, ball milling is a combination of mechanical alloying and milling. Generally, powders are susceptible to agglomeration during ball milling, which can deeply affect the hydrolysis reaction. Therefore, mixing aluminum with grinding aids (such as salts, metal oxides, or metal hydrides) for ball milling can effectively improve the hydrolytic activity of aluminum. During the ball milling process, the physical interaction occurs between the grinding aid and pores, cracks, and even fractures in the microstructure of the aluminum-based material, which not only deeply expands the specific surface area but also the distortion of the lattice structure and leads to elevated energy in the imperfections or defects of the metal matrix.

In this process, many active reaction sites are formed to promote the Al–water reaction [63,64]. The details of different grinding aids are discussed below.

3.1 Salt additives

Generally, NaCl is a common grinding aid in aluminum ball milling due to its low cost, safety, non-toxicity, good solubility, and environmentally friendly. NaCl addition in ball milling directly continuously chops or destroys the aluminum oxide layer of the aluminum powder and prevents the agglomeration of the powder. After activation of aluminum by mechanical treatment, NaCl particles embedded on the aluminum surface and a large number of pits on the aluminum surface emerged after dissolving in water, which increases the contact area of the Al–water reaction and promotes the reaction rate. Yolcular and Karaoglu [65] analyzed the relationship between the NaCl content and ball milling time for the aluminum powder during hydrogen production. It can be seen that without NaCl, as the ball milling time increases, the aluminum powder grows into spherical particles of 1–2 mm diameter due to agglomeration. If the NaCl content is increased from 5 to 20%, the diameter of the composite powder further decreased and the hydrogen generation rate reached 1,300 mL/(g min), as shown in Figure 3. The mixture with the addition of NaCl has a laminar structure and can exhibit better hydrolytic properties.

Figure 3 SEM images of the Al-NaCl powder mixtures milled for 12 h. (a) 0% NaCl, (b) 5% NaCl, (c) 10% NaCl, (d) 20% NaCl [65] (e) NaCl ball milling Al mechanism diagram; (f) Hydrogen generation rate in the reaction of water with the Al-X wt.% NaCl (X = 0, 5, 10, and 20%) powder mixture with 12 h milling time at 70°C.
Figure 3

SEM images of the Al-NaCl powder mixtures milled for 12 h. (a) 0% NaCl, (b) 5% NaCl, (c) 10% NaCl, (d) 20% NaCl [65] (e) NaCl ball milling Al mechanism diagram; (f) Hydrogen generation rate in the reaction of water with the Al-X wt.% NaCl (X = 0, 5, 10, and 20%) powder mixture with 12 h milling time at 70°C.

Irankhah et al. [66] explored the promotion of Al–water reaction by NaCl, KCl, and BaCl2. In comparison with NaCl, KCl and BaCl2 could cover the surface of Al effectively. As a result, BaCl2 could significantly reduce the induction time of the reaction, while the alloy powders of hydrogen yield with BaCl2 adjunction was considerably lower than that of NaCl and KCl. The hydrogen generation curve with different salt additives is shown in Figure 4. Chai et al. [61] investigated the effect of CoCl2 and NiCl2 on the Al–water reaction and found that the highest hydrogen yield was reached when the CoCl2 concentration was increased from 0.5 to 1 M. Nevertheless, the hydrogen yield diminished significantly when the CoCl2 concentration was further raised to 2 M. The effect of CoCl2 and NiCl2 concentrations on the hydrogen yield also showed similar trends. The reason was the formation of Co/Al and Ni/Al galvanic cells, which cause Co or Ni to aggregate on the surface, resulting in a decline in the specific surface area and consequently a decrease in the hydrogen yield. It is worth mentioning that the by-products of Co or Ni can be easily separated by their magnetic properties and reused in the subsequent hydrogen production cycle.

Figure 4 SEM images of 5 h ball milled Al powder with (a, b) 2 wt.% NaCl; (c, d) 2 wt.% KCl; (e, f) 2 wt.%BaCl2; (g) Effect of type of salt on the hydrogen generation yield after ball milling for 5 h [66].
Figure 4

SEM images of 5 h ball milled Al powder with (a, b) 2 wt.% NaCl; (c, d) 2 wt.% KCl; (e, f) 2 wt.%BaCl2; (g) Effect of type of salt on the hydrogen generation yield after ball milling for 5 h [66].

3.2 Oxide additives

The addition of oxide in the ball milling also directly makes close contact between aluminum powder and oxide powder and reduces the generation of the oxide film, so that the modified aluminum powder can react with water to generate hydrogen continuously.

Deng et al. [67] investigated the effect of different oxides (γ-Al2O3, α-Al2O3, TiO2) on the hydrogen production rate of the Al–water reaction. After the oxide was added, the surface of the aluminum particles was covered with fine oxide particles, which were not as smooth as the original aluminum particles, as shown by the SEM and TEM micrographs in Figure 5(a–h); the hydrogen production curve is shown in Figure 5(i). Due to the low nucleation and conversion potential, the density of the oxide film of the ball-milled Al is lower than before. Consequently, the new particles can readily react with water for hydrogen production. Dupiano et al. [68] explored the effect of the addition of five different metal powders (MoO3, Bi2O3, CuO, MgO, Al2O3) on the hydrogen production of the Al–water reaction. The surface structure of oxide powder additions detected by SEM is shown in Figure 5(j–n) and the hydrolysis reactions at 80°C are shown in Figure 5(o). It is obvious that Al–Bi2O3 has the fastest reaction rate and the highest hydrogen yield. In addition, an interesting phenomenon was found during the reaction of Bi2O3. The reaction would stop when the experimental temperature was lowered to room temperature, and the generation rate returned to the original when the temperature was 80°C.

Figure 5 SEM micrographs of (a) pure Al powder and those modified by (b) g-Al2O3, (c) a-Al2O3 and (d) TiO2 grains (e–h) TEM micrographs of the composition of 70 vol% Al+30 vol% oxide(e) pure Al powder (f) γ-Al2O3, (g) α-Al2O3 (h) TiO2 (i) Hydrogen production curve of 70 vol% Al+ 30 vol% oxide at 22°C [67] (j–n) SEM images of different oxide additions; (o) Hydrogen production for different composites reacting with water at 80°C [68].
Figure 5

SEM micrographs of (a) pure Al powder and those modified by (b) g-Al2O3, (c) a-Al2O3 and (d) TiO2 grains (e–h) TEM micrographs of the composition of 70 vol% Al+30 vol% oxide(e) pure Al powder (f) γ-Al2O3, (g) α-Al2O3 (h) TiO2 (i) Hydrogen production curve of 70 vol% Al+ 30 vol% oxide at 22°C [67] (j–n) SEM images of different oxide additions; (o) Hydrogen production for different composites reacting with water at 80°C [68].

3.3 Addition of low melting point metals

The advantages of adding the low melting point metals to ball-milled aluminum are as follows: (1) discontinuous oxide film on the aluminum surface; (2) higher energy potential of the melting point metal than that of aluminum, and galvanic cell corrosions occur in water; and (3) prohibition of the production of Al(OH)3 on the aluminum surface.

3.3.1 Binary Al composites

From Table 1, it is evident that Bi and Sn worked as active metals for binary Al composites. Nevertheless, the hydrogen yield from binary Al composites is low (85%) and the amount of active metal added is comparably high with large consumption.

Table 1

A summary of ball-milled binary Al composites

Composite (wt%) Reaction temperature (°C) Hydrogen yield (%) Ref.
Al–10 wt% In 90 <15 [69]
Al–23 wt% Bi Room temperature ∼80 [70]
Al–10 wt% Bi 35 81 [71]
Al–10 wt% Sn 35 74 [71]

3.3.2 Ternary Al composites

By the hydrolysis performance of Bi and Sn in binary composites, researchers started to investigate different ratios of Al–Bi–Sn alloys. Table 2 shows some of the recent articles on ternary composites. The hydrogen yield of Al–Bi–Sn alloys with a 5 wt% (Bi + Sn) content is close to the theoretical values at room temperature. Even with the same composition of the material, different ball milling procedures (ball milling time, ball-to-powder ratio) displayed different hydrogen production performances. Microstructures show that Bi and Sn promote structural disruption of Al during the mechanochemical treatment, which easily reduces the size of Al particles. Bi and Sn are relatively uniformly distributed throughout the Al particles promoting the galvanic cell reaction between the Al and Bi/Sn during the Al–water reaction.

Table 2

A summary of ball-milled ternary Al composites

Activation metals Composite (wt%) Reaction temperature (°C) Hydrogen yield (%) Ref.
Bi–Sn Al–9Bi–1Sn Room temperature 99 [72]
Al–7.5Bi–2.5Sn Room temperature 99 [72]
Al–5Bi–5Sn Room temperature 99 [72]
Al–2.5Bi–7.5Sn Room temperature 38.5 [72]
Al–4.5Bi–0.5Sn Room temperature 99 [72]
Al–3.75Bi–1.25Sn Room temperature 98 [72]
Al–2.5Bi–2.5Sn Room temperature 99 [72]
Al–7.5Bi–2.5Sn 35 86 [71]
Al–5Bi–5Sn 35 84 [71]
Bi-In Al–8.38Bi–4.71In Room temperature 95 [73]
Al–9.38Bi–0.62In Room temperature 81.5 [74]
Al–8.76Bi–1.26In Room temperature 82.5 [74]
Al–7.5Bi–2.5In Room temperature 95.5 [74]
Al–5Bi–5In Room temperature 93 [74]
Al–3.74Bi–6.26In Room temperature 77 [74]
Al–2.5Bi–7.5In Room temperature 93 [74]
Al–1.26Bi–8.76In Room temperature ∼65 [74]
Al–0.62Bi–9.38In Room temperature 0 [74]
In-Sn Al–2.54In–10.55Sn Room temperature 93 [73]
Al–9.82In–3.27Sn Room temperature 93 [73]
Al–1In–3Sn 60 11.91 [75]
Al–3In–3Sn Room temperature 15 [76]
Al–3In–5Sn Room temperature 16 [76]
Al–3In–7Sn Room temperature 18 [76]
Al–3In–10Sn Room temperature 19 [76]
Al–0.5In–9.5Sn Room temperature 25 [77]
Al–2In–8Sn Room temperature 97 [77]
Al–3.5In–6.5Sn Room temperature 96 [77]
Al–5In–5Sn Room temperature 99 [77]
Al–6.5In–3.5Sn Room temperature 97 [77]
Al–8In–2Sn Room temperature 91 [77]
Al–9.5In–0.5Sn Room temperature 0 [77]
Al–1In–4Sn Room temperature 63 [77]
Al–1.75In–3.25Sn Room temperature 75 [77]
Al–2.5In–2.5Sn Room temperature 83 [77]
Al–3.25In–1.75Sn Room temperature 71 [77]

In addition, researchers also investigated the effect of ball milling on Al–Bi–In and Al–In–Sn powders. As shown in Table 1, the Al–In mixture is essentially non-hydrolytic with water. However, Al–In–Sn powders show good hydrolysis after the gradual replacement of a portion of In with Sn. The hydrogen yield of Al–7.5Bi–2.5In powders is close to the theoretical values. Hence, Bi and In were completely dispersed on the aluminum surface, destroying the protective layer on the aluminum surface which is different from Bi–Sn. Unlike the previous two composites, Al–In–Sn formed new phases during ball milling – In3Sn and InSn4. Nearly 100% hydrogen yield was achieved with Al–5In–5Sn.

Taking into account the costs of the raw material, ternary Al–Bi–Sn powder is a particularly suitable choice, and with a suitable ball milling process, excellent hydrogen production can be achieved for practical applications in future.

3.3.3 Quaternary and multiple Al composites

The progress of hydrogen production performance of quaternary Al composites is summarized in Table 3. It can be seen that the hydrogen production performance of the quaternary Al composite is excellent, whereas it has no obvious advantage over the ternary Al composites, and it is more difficult to recover the fourth-series Al composites due to their complexity.

Table 3

A summary of quaternary and quinary ball milled Al composites

Activation metals Composite (wt%) Reaction temperature (°C) Hydrogen yield (%) Ref.
Ga–In–Sn Al–3Ga–3In–3Sn Room temperature 88 [76]
Al–3Ga–3In–5Sn Room temperature 99 [76]
Al–3Ga–3In–7Sn Room temperature 68 [76]
Al–3Ga–3In–10Sn Room temperature 68 [76]
Al–1Ga–1In–2Sn 60 14.71 [75]
Bi–In–Sn Al–3.93Bi–3.93In–5.24Sn Room temperature 91.2 [73]
Al–6.54Bi–3.93In–2.62Sn Room temperature Approximately 93 [73]
Al–3.93Bi–6.54In–2.26Sn Room temperature 98 [73]
Al–3.93Bi–2.62In–6.54Sn Room temperature Approximately 95 [73]
Bi–Ga–Zn Al–10Bi–8Ga–2Zn Room temperature 47 [78]
Al–10Bi-2Ga–8Zn Room temperature 66 [78]
Al–10Bi–5Ga–5Zn Room temperature 80 [78]
Al–8Bi–2Ga–10Zn Room temperature 76 [78]
Al–2Bi–8Ga–10Zn Room temperature 0 [78]
Al–5Bi–5Ga–10Zn Room temperature 68 [78]
Al–2Bi–10Ga–8Zn Room temperature 0 [78]
Al–8Bi–10Ga–2Zn Room temperature 16 [78]
Al–5Bi–10Ga–5Zn Room temperature 86 [78]

3.4 Other additives

The effects of additions of different mixtures on the hydrolysis effect of the composite have been analyzed. Wu et al. [79] prepared Al–10 mol% CaH2–10 mol% NiCl2 and it gave a hydrogen yield of 92.1% at 75°C with a maximum hydrogen generation rate of 1566.3 mL/(g min) after 3 h ball milling. The hydrolysis process leads to the formation of a new compound Ca2Al(OH)6Cl( H2O)2, which stimulates to remove the dense by-product layer. Liu et al. [80] developed a mixture of Al and Li3AlH6 which gave 92.8% of hydrogen yield at room temperature. Chen et al. [81] added 5 wt% NaCl during ball milling of Al–10 wt% Bi(OH)3, and the hydrogen generation rate elevated to 1,000 mL/(g min) at 30°C. Liao et al. [82] prepared Al–5wt%Bi@C and achieved 36% hydrogen yield at 60°C; the SEM micrographs are shown in Figure 6(a) and (b). On the contrary, when sintered in a plasma discharge sintering furnace, the product of blocks gave 100% theoretical hydrogen yield, as shown in Figure 6(c). Also, the sintered material reflects excellent oxidation resistance and still displays a 75.5% hydrogen yield after being exposed to air for 30 days. The main reason is that the number of carbon defects and cracks increased by the sintering process on the surface of the block. The effect of different processing methods on the surface microstructure of the Al–Bi@C material is shown in Figure 6(d and e). As shown in Figure 6(f), the intensity ratio of the D band to the G band (ID/IG) is 0.948 for Al–Bi@C milled and 0.952 for Al–Bi@C SPS. This indicates that ball milling increases the carbon defects and the SPS process further enhances carbon defects, which helps to improve the reactivity of the block. In particular, the sintering process not only increases the hydrogen generation rate of Al composites but also improves its oxidation resistance. Therefore, this method is expected to have practical uses in the field of hydrogen supply.

Figure 6 SEM-EDS (a) and TEM (b) images of Bi@C; SEM-EDS images of (c) Al-Bi@C milled and (d) Al-Bi@C SPS; (e)Raman spectra of Al–Bi@C SPS and Al–Bi@C milled; (f) Hydrogen generation curves for Al-5 wt.% Bi@C milled and Al-5 wt.% Bi@C SPS [82].
Figure 6

SEM-EDS (a) and TEM (b) images of Bi@C; SEM-EDS images of (c) Al-Bi@C milled and (d) Al-Bi@C SPS; (e)Raman spectra of Al–Bi@C SPS and Al–Bi@C milled; (f) Hydrogen generation curves for Al-5 wt.% Bi@C milled and Al-5 wt.% Bi@C SPS [82].

Generally, aluminum powder composites prepared by ball milling had the advantages of high hydrogen yield, high hydrogen generation rate, and short reaction induction time. The higher the activity, the higher the requirements for preparation, transportation, and storage. However, its short storage time is an obvious disadvantage. Furthermore, the high cost and time-consuming ball milling procedure is another obstacle not suitable for large-scale processing. Nonetheless, it cannot be overlooked that the high activity provided by the ball-milled aluminum powder can provide a large amount of hydrogen swiftly in an emergency and has a wide range of prospects for commercial application.

4 Low melting point metal-activated aluminum alloys

4.1 Block alloys

When hydrargyrum is dropped on the aluminum plate where the oxide film has just been removed, tall blocks will gradually grow on the aluminum plate. As shown in Figure 7(a–c), it was found that hydrargyrum can help the hydrolysis reaction to produce hydrogen from aluminum that has just been removed from the oxide film at 65°C [83]. The main reason is hydrargyrum stops the regeneration of the aluminum oxide film. The reaction is shown in Figure 7(d). Similarly, Woodall et al. [84] first prepared different compositions of Al–Ga liquid alloys which can react with water and produce hydrogen at room temperature. After the dissolution of low melting point metals, the Al2O3 layer become discontinuous and porous, which indeed improved the activities of the Al matrix. Thus, the effects of other low melting point metals (Li, Bi, In, Sn, Mg, etc.) on the hydrogen production from the Al–water reaction were investigated below.

Figure 7 Proposed aluminum hydrolysis model induced by mercury [83].
Figure 7

Proposed aluminum hydrolysis model induced by mercury [83].

4.1.1 Binary and ternary Al alloys

Woodall et al. [85] found that Al–72 wt% Ga and Al–50 wt% Ga show hydrolysis at 26–27°C, which is clearly due to the melting point of the Al (Ga) solid solution (about 26.6°C). Along with the hydrolysis reaction process and temperature, Ga dissolves in the Al matrix which does not participate in the reaction and only acts as an active component similar to a catalyst. Nevertheless, the hydrogen yield of Al–Ga alloys is deficient, which cannot satisfy the practical requirements. The emergence of binary alloys provides us with the possibility of hydrogen generation from the Al–water reaction but the hydrogen yield is low and the amount of a single precious metal is too large to be suitable for general applications. Otherwise, Al–Ga alloys not only display lower hydrogen production efficiency but also exhibit mechanical brittleness. In particular, Zhou et al. [86,87] verified this conclusion by first-principles calculations and found that the solid solution of Ga significantly reduces the strong toughness of the aluminum matrix. Al–Ga alloys are observed to produce H2 at a reaction temperature of about 26°C which is close to the melting point of Al–Ga eutectic. Therefore, lowering the melting point of the low melting point phase in the alloy to reduce the initial reaction temperature is an important idea. He et al. [88] investigated the reactivity of Al–Ga–In and Al–Ga–Sn alloys with water. The heat absorption peaks of Al–Ga–In and Al–Ga–Sn appear at 15°C and 19°C, respectively, as shown by DSC, which basically coincide with the melting points of Al–Ga–In and Al–Ga–Sn eutectics of 15.3 and 20.5°C, respectively. It was found that the Al–Ga–In alloys showed reactivity at about 10°C and the Al–Ga–Sn alloys started to show reactivity at 20°C. The reason for this is that the aluminum–water reaction is exothermic, so the reaction temperature is slightly below the melting point. The 15 wt% (Ga + In) Al–Ga-In alloys have a hydrogen yield of more than 90% in water at 20°C. In comparison, the hydrogen yield of the 15 wt% (Ga + Sn) Al–Ga–Sn is only 12%. Although the hydrogen yield of the Al–Ga–In alloys is much higher than that of Al–Ga–Sn alloys, the hydrogen generation rate is lower than Al–Ga–Sn alloys. In general, the low melting point phase determines the starting temperature of the hydrolysis reaction, and the initial temperature at which the reaction point begins to occur follows the melting point Al–Ga–In < Al–Ga–Sn < Al–Ga, and the different compositions seriously affect the H2 generation rate and H2 yield. In addition, there is micro-galvanic cell corrosion in the aluminum–water reaction of the alloys, which means that the difference between Ga, In, and Sn and Al also affects the hydrogen generation rate. Consequently, further research is needed to develop alloys that combine hydrogen generation rates, hydrogen yields, and lower reaction temperatures.

4.1.2 Quaternary and multi-alloys

Wang et al. [89] observed the Al–Ga–In–Sn alloys showed a heat absorption peak at 11.2°C by the DSC test, slightly above the melting point of 10.7°C for Ga–In–Sn eutectic. When the mass ratio of In/Sn is equal to 1.5:0.7, the In3Sn phase appears, and when the mass ratio is equal to 1:1, not only the In3Sn phase but also the InSn4 phase appears in the alloys. du Preez and Bessarabov [77] further observed that the formation of In and Sn intermetallic phases is determined by the molar ratio of In/Sn and In3Sn was the dominant In–Sn phase in composites with an In/Sn ratio of <0.97.

The principle of hydrogen production in Al–Ga–In–Sn alloys is mainly based on the fact that the addition of low melting point metals generates eutectic phases with very low melting points (In3Sn, InSn4), and even though most Ga dissolves in Al, trace amounts of Ga dissolve in the InSn eutectic phase, forming a Ga–In–Sn eutectic phase (named GIS phase). The GIS phase also dissolves a certain amount of Al atoms, completely surrounding these Al atoms. Al atoms react preferentially with water, even if the Al atoms in the eutectic phase have completed reacting. They will be supplemented by Al atoms with increased activity due to the solid solution of Ga and continue to undergo hydrolysis reactions. The low melting point phase not only protects the solid-solution Al atoms from oxidation but also provides a channel for the Al atoms to diffuse to the reaction sites [91]; these lower melting point “channels” allow the alloys to react with water at lower temperatures. The reaction mechanisms of the alloys are shown in Figure 8. In order to produce larger amounts of H2, it is necessary to maintain a suitable number of “channels” and the eutectic phase must be small and uniformly distributed [92,93]. If the channels are too small, the activation energy will be reduced, thereby slowing down the hydrolysis reaction and reducing the hydrogen generation rate. If the channels are too large, at the same time, the content of rare and precious metals will increase, which will increase the cost. Only when the low melting point eutectic phase is uniformly and finely distributed on the surface of the aluminum substrate can all the aluminum be activated to the maximum.

Figure 8 Diagram of hydrolysis reaction mechanism of hydrolysis Al-Ga-In-Sn alloys (a); (b) [90].
Figure 8

Diagram of hydrolysis reaction mechanism of hydrolysis Al-Ga-In-Sn alloys (a); (b) [90].

Al–Ga–In–Sn alloys have excellent hydrogen production properties, and researchers added other metals (Bi, Zn, Cu, Mg, Li) or compounds (Al2O3, Al–5Ti–B) to achieve one or more goals of cost reduction, reaction rate modulation. and strength increase. Ga and In are expensive, so the proportion of their use needs to be kept as low as possible. Huang et al. [94] added Bi to 80 wt% Al–Ga–In–Sn alloys to replace In, compared with the Al–Ga–In–Sn alloys, the hydrogen generation rate was smooth and controllable, and the hydrogen yield could reach the theoretical value. An et al. [95] increased the Al content to 90 wt% on this basis, and the hydrogen yield at 40°C was already close to 100%, with a maximum hydrogen generation rate of 780 mL/(g min). Wei et al. [96] explored the effect of partial substitution of InSn4 with Cu on the hydrogen production effect and found that the hydrogen yield and hydrogen generation rate of Al–Ga–InSn4–Cu alloy ingots with 3 wt% Cu content were better than Al–Ga–InSn4 alloys.

Along with an increase in the hydrogen yield, the hydrogen generation rate in the alloys needs to be regulated. Wei et al. [97] replaced Al in the Al–Ga–In3Sn alloys with Al2O3 and found that 1 wt% Al2O3 contributed to the raised hydrogen generation rate of the alloys but had no effect on the hydrogen yield. Grain refinement is an important method to enhance the hydrogen generation rate. Du et al. [98] added 0.12 wt% Al–5Ti–B to Al–Ga–In–Sn alloys; the grain size was reduced from 129 to 57 μm, as shown in Figure 9, and the alloys achieved 87% H2 yield at 30°C. Wei et al. [97] found that replacing In and Sn with Al2O3 can slow down the hydrogen generation rate of the alloys but has little effect on the hydrogen yield. He et al. [99] prepared Al–Ga–In–Sn–Li alloys with different Li contents. On increasing the Li content, the hydrogen generation rate of the alloys decreased significantly, while the hydrogen yield decreased slightly. Liu et al. [100] investigated the effect of Zn by replacing some of In3Sn on the hydrogen production properties of the Al–Ga–In3Sn alloys and realized that at 2 wt% Zn content, the hydrogen generation rate of the alloys decreased significantly compared to the hydrogen generation rate of the alloys without Zn. While the presence of Zn in the alloys is similar to that of Ga, mainly in the form of Al–Zn solid solution, it can retard the peak hydrogen generation rate mainly due to the formation of an Al–Zn micro-galvanic cell. In addition, Cu and Mg can effectively slow down the hydrogen generation rate but have less effect on the hydrogen yield [101,102,103,104].

Figure 9 The fracture surfaces of 6 wt.% Al-Ga-In-Sn alloys with different Ti contents and relations of Al grain size with Ti contents: (a) Ti free, (b) Ti 0.03 wt.%, (c) Ti 0.06 wt.%, (d) Ti 0.09 wt.%, (e) Ti 0.12 wt.%, (f) Ti 0.15 wt.%, (g) Ti 0.18 wt.%, (h) Ti 0.24 wt.%, (i) relations of Al grain size with Ti contents [98].
Figure 9

The fracture surfaces of 6 wt.% Al-Ga-In-Sn alloys with different Ti contents and relations of Al grain size with Ti contents: (a) Ti free, (b) Ti 0.03 wt.%, (c) Ti 0.06 wt.%, (d) Ti 0.09 wt.%, (e) Ti 0.12 wt.%, (f) Ti 0.15 wt.%, (g) Ti 0.18 wt.%, (h) Ti 0.24 wt.%, (i) relations of Al grain size with Ti contents [98].

Soluble materials are critical in horizontal well fracturing technology for unconventional oil and gas field development. The water-soluble nature of the alloys allows them to be used as a downhole soluble fracturing material, subject to compressive performance requirements. With the addition of Cu and Mg, the Al grain size becomes significantly finer and the strength of the Al–Ga–In–Sn alloys increases [101,102,103]. The functions of the different materials are summarized in Table 4.

Table 4

Effect of adding different materials to Al–Ga–In–Sn alloys

Materials Refining grain Slows down the generation rate Increase yields
Bi √
Zn √
Cu √ √ √
Mg √ √
Li √
Al2O3 √ √
Al–5Ti–B √ √

4.2 Gas-atomized alloys

The gas atomization process is a widely used powder manufacturing process that offers good uniformity and the possibility of mass production. It is a process in which a high-speed, high-pressure media flow is generated by an atomizing nozzle to crush the molten metal into fine droplets, which are subsequently spherified, cooled, and solidified into a metal powder. In addition, gas atomization is more suitable for mass production than ball milling [105].

As previously mentioned, ball-milled Al–Bi–Sn composites reflected high H2 yield and H2 generation rates, yet this composite cannot be prepared by melting because it is a difficult miscible alloy that can easily cause solid–liquid separation. Wang et al. [106] prepared Al–10wt%Bi–10wt%Sn powder by gas atomization and the powder showed outstanding hydrogen generation performance, with 80.4% H2 yield at 0°C for 88 min and 91.3% at 30°C for 16 min with water. Liu et al. [108] prepared Al–20wt%Bi powder with a core–shell structure, as shown in Figure 10(a–g). The powder reacted at room temperature and reached 100% theoretical H2 yield, as shown in Figure 10(h).

Figure 10 (a–c) SEM images of the 80Al-10Bi-10Sn wt. % powders: (a, b) surfaces, (c) cross-section; (d–g) EPMA element mappings of the cross section of the powders: (d) BSE, (e) Al, (f) Bi, and (g) Sn. (h) Hydrogen generation curves of the 80Al-10Bi-10Sn wt.% powders in distilled water [106] (i) A typical gas atomization device [107].
Figure 10

(a–c) SEM images of the 80Al-10Bi-10Sn wt. % powders: (a, b) surfaces, (c) cross-section; (d–g) EPMA element mappings of the cross section of the powders: (d) BSE, (e) Al, (f) Bi, and (g) Sn. (h) Hydrogen generation curves of the 80Al-10Bi-10Sn wt.% powders in distilled water [106] (i) A typical gas atomization device [107].

The composite powder prepared by gas atomization has a significant H2 generation rate at low temperatures and the process is simpler than ball milling. However, the disadvantages are similar to ball milling, which can lead to unsafe storage and short storage times.

5 Conclusions

Hydrogen, with its high calorific value, low density, and only water as a combustion product is a promising renewable energy source. Nevertheless, there are safety risks in storage and transport, so there is a need to develop a safe, environmentally friendly, and portable hydrogen energy application. Hydrolysis of aluminum-based materials can improve this role. Surface passivation of aluminum in air remains a major obstacle to the reaction of aluminum with water and this study provides a detailed review of the main methods for removing Al2O3 or destroying it from aluminum surfaces:

  1. The reaction of aluminum with acid–alkali solutions is the simplest principle of hydrogen production and has high requirements for experimental equipment.

  2. Ball milling of aluminum powder can produce hydrogen quickly and is suitable for rapid hydrogen production under emergency conditions, but extra attention should be paid to the safety hazards and short storage time of aluminum powder as well as the time and cost of ball milling.

  3. The melting and casting have the advantages of a simple process, low cost, high efficiency, and easy factory mechanization that are difficult to replace. Although the hydrogen yield and the hydrogen generation rate are lower than ball milling, it has the additional advantage of long storage times under dry conditions.

  4. The gas materialization adds a process to turn the solute into a powder when casting. The properties of the powder are close to powder prepared by ball milling, and advantages are similar to those of the ball milling, with poorer safety and shorter storage times.

In brief, Al-based materials have been successfully used in mobile hydrogen production equipment, hydrogen fuel cells, and other fields, and it has wide application prospects in many fields. For Al-based materials to have a better commercial future, there are still some issues that need continued attention:

  1. As the alloys are water-soluble and can be strengthened by adding reinforcing metals, other scenarios have been developed for use and for developing applications for a wider range of use environments.

  2. In order to improve energy efficiency and reduce raw material costs, the use of high-purity aluminum is gradually being replaced by scrap aluminum or industrial pure aluminum.

  3. For cost and environmental considerations, the focus should be on scientific research and analysis in terms of by-product analysis, collection, and reuse.

# These authors contributed equally to this work and should be considered first co-authors.

  1. Funding information: This work was supported by the Key Research and Development Program of Shaanxi (Program No. 2022QCY-LL-58), the Natural Science Basic Research Plan in Shaanxi Province of China (2023-JC-YB-458), Science and Technology Project of Huaneng Group Co, Ltd. (HNKJ 20-H41), and the Graduate Student Innovation and Practical Ability Training Program of Xi’an Shiyou University (YCS20212116).

  2. Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  3. Conflict of interest: The authors state no conflict of interest.

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Received: 2021-12-31
Revised: 2023-01-25
Accepted: 2023-02-09
Published Online: 2023-11-21

© 2023 the author(s), published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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https://doi.org/10.1515/ntrev-2022-0521
Keywords for this article
hydrogen energy; Al-based alloys; hydrolysis reaction; activation metals; ball milling
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BY 4.0

Articles in the same Issue

  1. Research Articles
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  11. Thermohydraulic performance of thermal system integrated with twisted turbulator inserts using ternary hybrid nanofluids
  12. Study of mechanical properties of epoxy/graphene and epoxy/halloysite nanocomposites
  13. Effects of CaO addition on the CuW composite containing micro- and nano-sized tungsten particles synthesized via aluminothermic coupling with silicothermic reduction
  14. Cu and Al2O3-based hybrid nanofluid flow through a porous cavity
  15. Design of functional vancomycin-embedded bio-derived extracellular matrix hydrogels for repairing infectious bone defects
  16. Study on nanocrystalline coating prepared by electro-spraying 316L metal wire and its corrosion performance
  17. Axial compression performance of CFST columns reinforced by ultra-high-performance nano-concrete under long-term loading
  18. Tungsten trioxide nanocomposite for conventional soliton and noise-like pulse generation in anomalous dispersion laser cavity
  19. Microstructure and electrical contact behavior of the nano-yttria-modified Cu-Al2O3/30Mo/3SiC composite
  20. Melting rheology in thermally stratified graphene-mineral oil reservoir (third-grade nanofluid) with slip condition
  21. Re-examination of nonlinear vibration and nonlinear bending of porous sandwich cylindrical panels reinforced by graphene platelets
  22. Parametric simulation of hybrid nanofluid flow consisting of cobalt ferrite nanoparticles with second-order slip and variable viscosity over an extending surface
  23. Chitosan-capped silver nanoparticles with potent and selective intrinsic activity against the breast cancer cells
  24. Multi-core/shell SiO2@Al2O3 nanostructures deposited on Ti3AlC2 to enhance high-temperature stability and microwave absorption properties
  25. Solution-processed Bi2S3/BiVO4/TiO2 ternary heterojunction photoanode with enhanced photoelectrochemical performance
  26. Electroporation effect of ZnO nanoarrays under low voltage for water disinfection
  27. NIR-II window absorbing graphene oxide-coated gold nanorods and graphene quantum dot-coupled gold nanorods for photothermal cancer therapy
  28. Nonlinear three-dimensional stability characteristics of geometrically imperfect nanoshells under axial compression and surface residual stress
  29. Investigation of different nanoparticles properties on the thermal conductivity and viscosity of nanofluids by molecular dynamics simulation
  30. Optimized Cu2O-{100} facet for generation of different reactive oxidative species via peroxymonosulfate activation at specific pH values to efficient acetaminophen removal
  31. Brownian and thermal diffusivity impact due to the Maxwell nanofluid (graphene/engine oil) flow with motile microorganisms and Joule heating
  32. Appraising the dielectric properties and the effectiveness of electromagnetic shielding of graphene reinforced silicone rubber nanocomposite
  33. Synthesis of Ag and Cu nanoparticles by plasma discharge in inorganic salt solutions
  34. Low-cost and large-scale preparation of ultrafine TiO2@C hybrids for high-performance degradation of methyl orange and formaldehyde under visible light
  35. Utilization of waste glass with natural pozzolan in the production of self-glazed glass-ceramic materials
  36. Mechanical performance of date palm fiber-reinforced concrete modified with nano-activated carbon
  37. Melting point of dried gold nanoparticles prepared with ultrasonic spray pyrolysis and lyophilisation
  38. Graphene nanofibers: A modern approach towards tailored gypsum composites
  39. Role of localized magnetic field in vortex generation in tri-hybrid nanofluid flow: A numerical approach
  40. Intelligent computing for the double-diffusive peristaltic rheology of magneto couple stress nanomaterials
  41. Bioconvection transport of upper convected Maxwell nanoliquid with gyrotactic microorganism, nonlinear thermal radiation, and chemical reaction
  42. 3D printing of porous Ti6Al4V bone tissue engineering scaffold and surface anodization preparation of nanotubes to enhance its biological property
  43. Bioinspired ferromagnetic CoFe2O4 nanoparticles: Potential pharmaceutical and medical applications
  44. Significance of gyrotactic microorganisms on the MHD tangent hyperbolic nanofluid flow across an elastic slender surface: Numerical analysis
  45. Performance of polycarboxylate superplasticisers in seawater-blended cement: Effect from chemical structure and nano modification
  46. Entropy minimization of GO–Ag/KO cross-hybrid nanofluid over a convectively heated surface
  47. Oxygen plasma assisted room temperature bonding for manufacturing SU-8 polymer micro/nanoscale nozzle
  48. Performance and mechanism of CO2 reduction by DBD-coupled mesoporous SiO2
  49. Polyarylene ether nitrile dielectric films modified by HNTs@PDA hybrids for high-temperature resistant organic electronics field
  50. Exploration of generalized two-phase free convection magnetohydrodynamic flow of dusty tetra-hybrid Casson nanofluid between parallel microplates
  51. Hygrothermal bending analysis of sandwich nanoplates with FG porous core and piezomagnetic faces via nonlocal strain gradient theory
  52. Design and optimization of a TiO2/RGO-supported epoxy multilayer microwave absorber by the modified local best particle swarm optimization algorithm
  53. Mechanical properties and frost resistance of recycled brick aggregate concrete modified by nano-SiO2
  54. Self-template synthesis of hollow flower-like NiCo2O4 nanoparticles as an efficient bifunctional catalyst for oxygen reduction and oxygen evolution in alkaline media
  55. High-performance wearable flexible strain sensors based on an AgNWs/rGO/TPU electrospun nanofiber film for monitoring human activities
  56. High-performance lithium–selenium batteries enabled by nitrogen-doped porous carbon from peanut meal
  57. Investigating effects of Lorentz forces and convective heating on ternary hybrid nanofluid flow over a curved surface using homotopy analysis method
  58. Exploring the potential of biogenic magnesium oxide nanoparticles for cytotoxicity: In vitro and in silico studies on HCT116 and HT29 cells and DPPH radical scavenging
  59. Enhanced visible-light-driven photocatalytic degradation of azo dyes by heteroatom-doped nickel tungstate nanoparticles
  60. A facile method to synthesize nZVI-doped polypyrrole-based carbon nanotube for Ag(i) removal
  61. Improved osseointegration of dental titanium implants by TiO2 nanotube arrays with self-assembled recombinant IGF-1 in type 2 diabetes mellitus rat model
  62. Functionalized SWCNTs@Ag–TiO2 nanocomposites induce ROS-mediated apoptosis and autophagy in liver cancer cells
  63. Triboelectric nanogenerator based on a water droplet spring with a concave spherical surface for harvesting wave energy and detecting pressure
  64. A mathematical approach for modeling the blood flow containing nanoparticles by employing the Buongiorno’s model
  65. Molecular dynamics study on dynamic interlayer friction of graphene and its strain effect
  66. Induction of apoptosis and autophagy via regulation of AKT and JNK mitogen-activated protein kinase pathways in breast cancer cell lines exposed to gold nanoparticles loaded with TNF-α and combined with doxorubicin
  67. Effect of PVA fibers on durability of nano-SiO2-reinforced cement-based composites subjected to wet-thermal and chloride salt-coupled environment
  68. Effect of polyvinyl alcohol fibers on mechanical properties of nano-SiO2-reinforced geopolymer composites under a complex environment
  69. In vitro studies of titanium dioxide nanoparticles modified with glutathione as a potential drug delivery system
  70. Comparative investigations of Ag/H2O nanofluid and Ag-CuO/H2O hybrid nanofluid with Darcy-Forchheimer flow over a curved surface
  71. Study on deformation characteristics of multi-pass continuous drawing of micro copper wire based on crystal plasticity finite element method
  72. Properties of ultra-high-performance self-compacting fiber-reinforced concrete modified with nanomaterials
  73. Prediction of lap shear strength of GNP and TiO2/epoxy nanocomposite adhesives
  74. A novel exploration of how localized magnetic field affects vortex generation of trihybrid nanofluids
  75. Fabrication and physicochemical characterization of copper oxide–pyrrhotite nanocomposites for the cytotoxic effects on HepG2 cells and the mechanism
  76. Thermal radiative flow of cross nanofluid due to a stretched cylinder containing microorganisms
  77. In vitro study of the biphasic calcium phosphate/chitosan hybrid biomaterial scaffold fabricated via solvent casting and evaporation technique for bone regeneration
  78. Insights into the thermal characteristics and dynamics of stagnant blood conveying titanium oxide, alumina, and silver nanoparticles subject to Lorentz force and internal heating over a curved surface
  79. Effects of nano-SiO2 additives on carbon fiber-reinforced fly ash–slag geopolymer composites performance: Workability, mechanical properties, and microstructure
  80. Energy bandgap and thermal characteristics of non-Darcian MHD rotating hybridity nanofluid thin film flow: Nanotechnology application
  81. Green synthesis and characterization of ginger-extract-based oxali-palladium nanoparticles for colorectal cancer: Downregulation of REG4 and apoptosis induction
  82. Abnormal evolution of resistivity and microstructure of annealed Ag nanoparticles/Ag–Mo films
  83. Preparation of water-based dextran-coated Fe3O4 magnetic fluid for magnetic hyperthermia
  84. Statistical investigations and morphological aspects of cross-rheological material suspended in transportation of alumina, silica, titanium, and ethylene glycol via the Galerkin algorithm
  85. Effect of CNT film interleaves on the flexural properties and strength after impact of CFRP composites
  86. Self-assembled nanoscale entities: Preparative process optimization, payload release, and enhanced bioavailability of thymoquinone natural product
  87. Structure–mechanical property relationships of 3D-printed porous polydimethylsiloxane films
  88. Nonlinear thermal radiation and the slip effect on a 3D bioconvection flow of the Casson nanofluid in a rotating frame via a homotopy analysis mechanism
  89. Residual mechanical properties of concrete incorporated with nano supplementary cementitious materials exposed to elevated temperature
  90. Time-independent three-dimensional flow of a water-based hybrid nanofluid past a Riga plate with slips and convective conditions: A homotopic solution
  91. Lightweight and high-strength polyarylene ether nitrile-based composites for efficient electromagnetic interference shielding
  92. Review Articles
  93. Recycling waste sources into nanocomposites of graphene materials: Overview from an energy-focused perspective
  94. Hybrid nanofiller reinforcement in thermoset and biothermoset applications: A review
  95. Current state-of-the-art review of nanotechnology-based therapeutics for viral pandemics: Special attention to COVID-19
  96. Solid lipid nanoparticles for targeted natural and synthetic drugs delivery in high-incidence cancers, and other diseases: Roles of preparation methods, lipid composition, transitional stability, and release profiles in nanocarriers’ development
  97. Critical review on experimental and theoretical studies of elastic properties of wurtzite-structured ZnO nanowires
  98. Polyurea micro-/nano-capsule applications in construction industry: A review
  99. A comprehensive review and clinical guide to molecular and serological diagnostic tests and future development: In vitro diagnostic testing for COVID-19
  100. Recent advances in electrocatalytic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid: Mechanism, catalyst, coupling system
  101. Research progress and prospect of silica-based polymer nanofluids in enhanced oil recovery
  102. Review of the pharmacokinetics of nanodrugs
  103. Engineered nanoflowers, nanotrees, nanostars, nanodendrites, and nanoleaves for biomedical applications
  104. Research progress of biopolymers combined with stem cells in the repair of intrauterine adhesions
  105. Progress in FEM modeling on mechanical and electromechanical properties of carbon nanotube cement-based composites
  106. Antifouling induced by surface wettability of poly(dimethyl siloxane) and its nanocomposites
  107. TiO2 aerogel composite high-efficiency photocatalysts for environmental treatment and hydrogen energy production
  108. Structural properties of alumina surfaces and their roles in the synthesis of environmentally persistent free radicals (EPFRs)
  109. Nanoparticles for the potential treatment of Alzheimer’s disease: A physiopathological approach
  110. Current status of synthesis and consolidation strategies for thermo-resistant nanoalloys and their general applications
  111. Recent research progress on the stimuli-responsive smart membrane: A review
  112. Dispersion of carbon nanotubes in aqueous cementitious materials: A review
  113. Applications of DNA tetrahedron nanostructure in cancer diagnosis and anticancer drugs delivery
  114. Magnetic nanoparticles in 3D-printed scaffolds for biomedical applications
  115. An overview of the synthesis of silicon carbide–boron carbide composite powders
  116. Organolead halide perovskites: Synthetic routes, structural features, and their potential in the development of photovoltaic
  117. Recent advancements in nanotechnology application on wood and bamboo materials: A review
  118. Application of aptamer-functionalized nanomaterials in molecular imaging of tumors
  119. Recent progress on corrosion mechanisms of graphene-reinforced metal matrix composites
  120. Research progress on preparation, modification, and application of phenolic aerogel
  121. Application of nanomaterials in early diagnosis of cancer
  122. Plant mediated-green synthesis of zinc oxide nanoparticles: An insight into biomedical applications
  123. Recent developments in terahertz quantum cascade lasers for practical applications
  124. Recent progress in dielectric/metal/dielectric electrodes for foldable light-emitting devices
  125. Nanocoatings for ballistic applications: A review
  126. A mini-review on MoS2 membrane for water desalination: Recent development and challenges
  127. Recent updates in nanotechnological advances for wound healing: A narrative review
  128. Recent advances in DNA nanomaterials for cancer diagnosis and treatment
  129. Electrochemical micro- and nanobiosensors for in vivo reactive oxygen/nitrogen species measurement in the brain
  130. Advances in organic–inorganic nanocomposites for cancer imaging and therapy
  131. Advancements in aluminum matrix composites reinforced with carbides and graphene: A comprehensive review
  132. Modification effects of nanosilica on asphalt binders: A review
  133. Decellularized extracellular matrix as a promising biomaterial for musculoskeletal tissue regeneration
  134. Review of the sol–gel method in preparing nano TiO2 for advanced oxidation process
  135. Micro/nano manufacturing aircraft surface with anti-icing and deicing performances: An overview
  136. Cell type-targeting nanoparticles in treating central nervous system diseases: Challenges and hopes
  137. An overview of hydrogen production from Al-based materials
  138. A review of application, modification, and prospect of melamine foam
  139. A review of the performance of fibre-reinforced composite laminates with carbon nanotubes
  140. Research on AFM tip-related nanofabrication of two-dimensional materials
  141. Advances in phase change building materials: An overview
  142. Development of graphene and graphene quantum dots toward biomedical engineering applications: A review
  143. Nanoremediation approaches for the mitigation of heavy metal contamination in vegetables: An overview
  144. Photodynamic therapy empowered by nanotechnology for oral and dental science: Progress and perspectives
  145. Biosynthesis of metal nanoparticles: Bioreduction and biomineralization
  146. Current diagnostic and therapeutic approaches for severe acute respiratory syndrome coronavirus-2 (SARS-COV-2) and the role of nanomaterial-based theragnosis in combating the pandemic
  147. Application of two-dimensional black phosphorus material in wound healing
  148. Special Issue on Advanced Nanomaterials and Composites for Energy Conversion and Storage - Part I
  149. Helical fluorinated carbon nanotubes/iron(iii) fluoride hybrid with multilevel transportation channels and rich active sites for lithium/fluorinated carbon primary battery
  150. The progress of cathode materials in aqueous zinc-ion batteries
  151. Special Issue on Advanced Nanomaterials for Carbon Capture, Environment and Utilization for Energy Sustainability - Part I
  152. Effect of polypropylene fiber and nano-silica on the compressive strength and frost resistance of recycled brick aggregate concrete
  153. Mechanochemical design of nanomaterials for catalytic applications with a benign-by-design focus
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