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Preparation and morphological studies of tin sulfide nanoparticles and use as efficient photocatalysts for the degradation of rhodamine B and phenol

  • Abimbola E. Oluwalana and Peter A. Ajibade EMAIL logo
Published/Copyright: February 17, 2022
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Nanotechnology Reviews
From the journal Nanotechnology Reviews Volume 11 Issue 1

Abstract

Tin sulfide nanoparticles were prepared from tin(ii) dithiocarbamate complexes: bis(benzylmethyl dithiocarbamate)tin(ii) (SnS1), bis(dibenzyl dithiocarbamato)tin(ii) (SnS2), and bis(imidazolyldithiocarbamato)tin(ii) (SnS3) single-source precursors. Powder X-ray diffraction patterns of the as-prepared tin sulfide nanoparticles confirmed orthorhombic crystalline phase irrespective of the tin(ii) dithiocarbamate precursors used to prepare the tin sulfide nanoparticles. Transmission electron microscopic images showed SnS nanoparticles with average particle size of 1.35 ± 0.04 nm for SnS1, 2.63 ± 0.65 nm for SnS2, and 1.55 ± 0.15 nm for SnS3. The energy bandgap of the SnS nanoparticles obtained from Tauc plots are in the range 3.80–4.37 eV. The as-prepared SnS nanoparticles were used as photocatalysts for the degradation of rhodamine B with efficiency of 90.97, 61.53, and 80.26% for SnS1, SnS2, and SnS3, respectively, while for phenol degradation efficiency was 96.45, 75.13, and 90.69% after 180 min. The results indicate that the as-prepared SnS nanoparticle are efficient photocatalyst for rhodamine B and phenol degradation. The photocatalytic degradation of rhodamine B and phenol follows pseudo-first-order reaction kinetics model from which the photodegradation rate could be obtained. Scavenger studies show that electrons (e−), hydroxy radicals (˙OH), and holes (h+) play significant role in the photodegradation of rhodamine B and phenol by the SnS nanoparticles. Recyclability studies show the SnS photocatalyst could be reused for four cycles without losing its photodegradation ability.

Keywords: tin(ii) dithiocarbamate; single-source precursor; tin sulfide; nanoparticles; photocatalysis; recyclability

1 Introduction

In recent years, coordination chemistry of dithiocarbamate has received considerable attention because of its ability to coordinate metal ions in different oxidation states to give complexes in different structural motifs [1]. Interest in tin(ii) dithiocarbamate is due to its structural diversity [2], wide range of applications in agriculture, catalysis, biology, and as single-source precursors for the preparation of metal sulfide nanoparticles [1,3,4]. Over the years, IV–VI semiconductors’ nanoparticles are being studied due to their optical properties and small bandgap which make them useful for various applications in optoelectronic devices. Among this class of compound, SnS nanoparticles are of particular interest because of its high absorption coefficient, and photoelectric conversion efficiency [5,6,7]. In addition, it is being used as supercapacitor [8], solar cell [9,10], sensor [11], photodetector [12], and photocatalyst [13].

The divalent and tetravalent oxidation states of tin are common in most of its compound. Thus, SnS nanoparticles exist in different crystalline phases, which include SnS (divalent), SnS2 (tetravalent) Sn2S3, and Sn3S4 (mixed valency) [7]. SnS is one of the promising semiconductor nanoparticles that are being explored as potential photocatalyst for dye degradation to address problems associated with environmental pollution due to its high stability, tunable optical properties, nontoxic, and low bandgap (1.3–1.5 eV) [13,14]. Due to interest in the potential applications of SnS and SnS2 nanoparticles, several methods such as coprecipitation [15], aerosol-assisted chemical vapor deposition [16], chemical spray pyrolysis [17], thermal evaporation [18], sputtering [19], microwave-assisted radiation [20], atomic layer deposition [21], and single-source precursors [22,23,24] have been used to prepare tin sulfur nanoparticles. Among these synthetic approaches, the use of single-source precursor in which the tin sulfur bond is already formed in the complexes could result in clean high-quality SnS nanoparticles [22]. The use of different single-source precursors could lead to tin sulfur nanoparticles with different size, shape, and optical properties. Hence, the use of three tin(ii) dithiocarbamate complexes as single-source precursors in this paper to prepare tin sulfur nanoparticles and study the effect of the different precursors on the morphology and photocatalytic properties of the as-prepared tin sulfur nanoparticles.

Photocatalytic process is based on the generation of electron–hole pair in the semiconductor on absorption of light energy. The generated electron–hole reacts with oxygen from the surrounding and the aqueous solution to give highly reactive oxygen species such as superoxide and hydroxide radicals [25]. These radicals are responsible for the degradation of organic contaminants through photocatalytic process. Das and Dutta [25] reported the use of SnS nanorods for the degradation of trypan blue in the presence of sunlight which was favorable due to the inhibition of electron–hole recombination on the surface of the nanorods. Kabouche et al. [13] reported the elimination of rhodamine B using SnS nanoparticles under sunlight at 88.46% after 4 h. Chen et al. [26] report the degradation of rhodamine B and phenol at 64.8 and 51.5% for pristine SnS2 nanosheets after 4 h. SnS negatively charged nature was reported to be responsible for its superior visible light photocatalytic performance of cationic dyes [27]. The degradation of organic dyes have been reported to be influenced by the shape, size, and recombination properties of SnS nanoparticles [28]. To the best of our knowledge, the photocatalytic activity of SnS on phenol is minimal compared to SnS2. In view of this, there is a need to investigate photocatalytic efficiency and reusability of tin sulfide nanoparticles for the degradation of colored and colorless organic contaminants as related to particle size and recombination effect of as-synthesized SnS nanoparticles. In this study, we report the synthesis and characterization of three tin(ii) dithiocarbamate complexes and their use as molecular precursor to prepare SnS nanoparticles via hot injection method. The as-prepared SnS nanoparticles were used as photocatalyst for the degradation of rhodamine B and phenol under visible light irradiation, the photodegradation kinetics, mechanism, and recyclability were also evaluated.

2 Experimental

2.1 Materials

Tin(ii) chloride dihydrate, tri-n-octyl phosphine (TOP), hexadecylamine (HDA), methanol, rhodamine B, phenol, silver nitrate (SN), isopropanol (IPA), ammonium oxalate (AO), and acrylamide (AC) were purchased from Sigma-Aldrich and used without further purification. Potassium salt of benzyl methyl dithiocarbamate (L1), dibenzyl dithiocarbamate (L2), and imidazolyl dithiocarbamate (L3) were prepared using modified literature methods [29,30,31].

2.2 Characterization techniques

Infrared spectra data were obtained from Agilent Technologies Cary 630 FTIR spectrometer in the frequency region of 4,000–650 cm−1. The 1H and 13C NMR spectra of the complexes were measured using Bruker Avance III 400 MHz NMR spectrometer. Elemental analysis was carried out using ThermoScientific Flash 2000. The crystalline phases of the synthesized nanoparticles were identified using a powder X-ray diffraction (XRD) pattern obtained from Philips PW1830 diffraction spectrometer operated at 40 kV and 40 mA equipped with Co anode of Kα = 1.79290 Å. The size, shape, lattice fringes, and selected area electron diffraction (SAED) patterns of the nanoparticles were investigated using a JEOL JEM-2100 high-resolution transmission electron microscope (HRTEM). Image J analysis software was used to measure the particle size distribution based on 150–250 nanoparticles. Perkin Elmer 25 UV-Vis spectrophotometer and LS 45 fluorescence were used for optical absorption and emission measurement, respectively.

2.3 Synthesis of tin(ii) dithiocarbamate complexes

Tin chloride dihydrate (2.5 mmol, 0.5641 g) was dissolved in 20 mL ethanol and added dropwise to 5 mmol ethanolic solution of ligands (benzyl methyl dithiocarbamate (L1), dibenzyl dithiocarbamate (L2), and imidazolyl dithiocarbamate (L3) (0.9800 g, 0.9225 g and 1.0965 g)). The reaction was stirred at room temperature for 3 h (Scheme 1). The resulting precipitate was washed severally with ethanol and dried under vacuum.

Scheme 1 Preparation of the tin(ii) dithiocarbamate complexes.
Scheme 1

Preparation of the tin(ii) dithiocarbamate complexes.

2.3.1 [Sn(L1)2]

Yield: 69%, 1.0399 g; melting point: 132.3–134.3℃. ESI-MS+ (m/z) [M + DMSO] 591, anal. calcd for C18H22N2SnS4 (%), C: 42.28, H: 3.94, N: 5.48; found. C: 41.97, H: 4.01, N: 5.56. 1H-NMR: (DMSO-d 6): δ 2.55 (s, 6H –CH3), 5.32 (s, 4H –CH2), 7.31–7.50 (m, 10H –C6H5), 13C-NMR: (CDCl3) ẟ 39.4 (CH3), 56.3 (CH2), 127.9 –129.1 (C6H5), 190.3 (CS2) Selected FTIR bands (cm−1): 1,250 υ(C–N), 1,498 υ(N–CS2), 960 υ(C–S).

2.3.2 [Sn(L2)2]

Yield: 73%, 1.4314 g; melting point: 102.4–103.6℃. ESI-MS+ (m/z) [M + DMSO] 745, anal. calcd for C30H30N2SnS4 (%), C: 54.31, H: 4.25, N: 4.22; found. C: 54.34, H: 4.25, N: 4.22. 1H-NMR: (DMSO-d 6) δ 5.07 (s, 8H CH2), 7.31–7.48 (m, 20H C6H5). 13C-NMR: (DMSO-d 6) δ 59.7 (N–CH2), 127.9–129.9 (C6H5), 190.4 (CS2). Selected FTIR bands (cm−1): 1,214 (C–N), 970 (C–S), 1,490 (N–CS2).

2.3.3 [Sn(L3)2]

Yield: 52%, 0.6205 g; melting point: decomposes at 250℃. Selected FTIR bands (cm−1): 1,276 υ(C–N), 1,447 υ(N–CS2), 997 υ(C–S).

2.4 Preparation of HDA-capped SnS nanoparticles

Around 0.4 g of each tin(ii) dithiocarbamate complex was dissolved in 5 mL of TOP before introducing into 4 g of hot HDA at 120℃ under nitrogen and stirred for 1 h. Afterward, the mixture was cooled to 70℃, followed by the addition of cold methanol. The product was separated by centrifugation. Tin sulfide synthesized from [Sn(L1)2], [Sn(L2)2], and [Sn(L3)2] was labeled SnS1, SnS2, and SnS3, respectively.

2.5 Evaluation of the photocatalytic degradation of rhodamine B by the HDA-capped SnS nanoparticles

The photocatalytic activity of the synthesized SnS nanoparticles was evaluated by measuring the degradation of aqueous rhodamine B and phenol solution (3 × 10−5 M). Typically, 40 mg of the catalyst (SnS) was dispersed into 40 mL of the organic pollutants. The reaction solution was stirred for 30 min in the dark to attain adsorption and desorption equilibrium between the pollutant and the catalyst (SnS) prior to visible-light irradiation. The solution was placed 10 cm away from 80 W high-pressure mercury lamp. Around 4 mL of solution was taken at regular intervals (30 min) for 180 min. The degradation process was monitored using UV-Vis spectrophotometer at 553 and 270 nm wavelength for rhodamine B and phenol, respectively.

3 Results and discussion

3.1 Spectroscopic studies

The mode of coordination of the dithiocarbamate ligands to the tin(ii) ion is determined by the υ (C–S) vibrational mode (Figures S1–S3). A single band in the range 960–997 cm−1 appeared in the complexes for υ (C–S) vibration, which indicate the dithiocarbamato anions coordinate to the tin(ii) ion in bidentate chelating mode [32,33] through the two sulfur atoms. Also, an intermediate band between single and double bond C–N appeared in the range 1,447–1,498 cm−1, which can be attributed to the delocalization of the electron density within the N–CS2 bonds of the dithiocarbamate to the tin(ii) center [34].

The 1H-NMR spectrum of [Sn(L1)2] in Figure S4 displayed a singlet peak of six protons at 2.55 ppm which is assigned to the methyl protons, the methylene protons resonated as a singlet at 5.32 ppm with four protons, while the dithiocarbamate aromatic ring protons appeared as a multiplet in the region of 7.31–7.80 ppm. In [Sn(L2)2] the methylene proton has a singlet peak at 5.02 ppm with eight protons, while the aromatic ring resonated as multiplet in the range 7.31–7.48 ppm with 20 protons (Figure S5). The –CH2 proton peaks appeared at the same region in [Sn(L1)2] and [Sn(L2)2] due to the alkyl derivative attached to the nitrogen atom [25].

13C-NMR of [Sn(L1)2] and [Sn(L2)2] showed a signal at 190.3 and 190.4 ppm, respectively, due to CS2, the peak shifted downfield due to significant contribution from the N–C π-electrons of the dithiocarbamate moiety. The nitrogen atom experiences a ẟ + surplus charge localization while –CS2M metallochelate a ẟ − delocalization. The aromatic carbon resonated around 127.9–129.9 ppm, the methylene proton resonated at 56.3 and 59.7 ppm for [Sn(L1)2] and [Sn(L2)2], respectively, while in [Sn(L1)2] methyl carbon resonated at 39.4 ppm.

3.2 Morphological studies of the SnS nanoparticles

3.2.1 XRD analysis

The XRD patterns of the SnS nanoparticles are presented in Figure 1. The 2θ peaks at 22.8°, 24.5°, 27.6°, 39.2°, 42.8°, 44.1°, 47.0°, 48.1°, 49.9°, 52.0°, 53.4°, 56.6°, 58.1°, 60.8°, and 69.5° are indexed to (110), (120), (021), (131), (141), (102), (002), (211), (112), (511), (122), (061), (420), (103), and (081) planes of SnS orthorhombic (o-SnS) phase (JCPDS 39-0354; herzenbergite) [1]. The calculated lattice parameter a = 0.4328 nm, b = 0.1119 nm, and c = 0.3978 nm are consistent with standard values. In the XRD patterns, SnS2, Sn2S3, and Sn3S4 characteristic peaks were not observed indicating the formation of pure SnS phase irrespective of the tin(ii) dithiocarbamate precursor used to prepare the nanoparticles.

Figure 1 Powder X-ray diffraction pattern of SnS1 (a) SnS2 (b) and SnS3 (c) nanoparticles.
Figure 1

Powder X-ray diffraction pattern of SnS1 (a) SnS2 (b) and SnS3 (c) nanoparticles.

3.2.2 HRTEM and SEM analysis of the SnS nanoparticles

The HRTEM images, lattice fringes, SAED patterns, and the particle size distribution graph of the as-synthesized SnS nanoparticles are presented in Figure 2. SnS1 obtained from [Sn(L1)2] is spherically shaped and well dispersed with average particle size of 1.35 ± 0.04 nm. Monodispersed nanoparticles were obtained for SnS2 prepared from [Sn(L2)2] with average particle size of 2.63 ± 0.65 nm while SnS3 obtained from [Sn(L3)2] is monodispersed with a size distribution of 1.55 ± 0.15 nm. The results indicate that the as-synthesized SnS nanoparticles are quantum dots due to their size being less than 10 nm. The results indicate that the precursors have an effect on the size of the nanoparticles obtained, as a result of the different binding strength of the dithiocarbamate moiety to the tin(ii) metal center, which leads to different rate of decomposition of the precursor during thermolysis [35,36]. An interplanar lattice fringe d-spacing of 0.34 nm that is visible in the HRTEM images for SnS1 and SnS3 corresponds to the d-spacing of (222) plane of o-SnS [37], while 0.27 and 0.32 nm was obtained in SnS2 that corresponds to (011) and (200) planes, respectively, of o-SnS [38]. The SAED patterns of SnS1 and SnS2 show bright spots in the diffraction rings, which indicates that the as-synthesized SnS nanoparticles are crystalline in nature [39]. In addition, the clear spots indicate that the as-synthesized SnS composed of a single crystalline structure [40] as confirmed by XRD. SnS3 is amorphous in nature as evidence by the SAED patterns as there is no diffraction ring or spot [41].

Figure 2 HRTEM images: (a) SAED patterns; (b) lattice fringes; (c) corresponding size distribution graph (insert) of SnS nanoparticles.
Figure 2

HRTEM images: (a) SAED patterns; (b) lattice fringes; (c) corresponding size distribution graph (insert) of SnS nanoparticles.

The SEM images of the SnS nanoparticles in Figure S6 have powdery morphology due to high surface energy and the small particle size [42]. The elemental mapping of the samples was done and the EDX spectrum (Figure S7) confirms the formation of SnS nanoparticles through the detection of Sn and S peaks in the atomic ratio of 1:1 in agreement with the expected value. The carbon (C) and oxygen peaks could be ascribed to the capping agents while gold (Au) peak detected is attributed to coating of samples using gold.

3.3 Optical studies of the SnS nanoparticles

The UV-Vis absorption spectra and Tauc plot of the as-synthesized SnS nanoparticles are presented in Figure 3a and b. The nanoparticle absorption band edges were observed at 320, 285, and 307 nm for SnS1, SnS2, and SnS3, respectively. On extrapolation of (αhv)2 vs hv plots straight-line portion to the x-axis using direct allowed transition, the bandgap energy values were found to be 3.80 eV for SnS1, 4.37 for SnS2, and 4.07 eV for SnS3, which are blue-shifted in comparison to the bulk SnS (1.51 eV) which can be ascribed to quantum confinement effect enhancement due to the size of the nanoparticles, defects, and grain boundary disorder [43,44]. It has been shown that the bandgap energy values are beneficial for photocatalytic activity; hence the decreased bandgap of SnS1 toward the visible region shows that high energy is needed for the recombination of electron–hole pair occurrence [45]. The emission spectra (Figure 3c) were used to study electron–hole pair separation and recombination effect of HDA-capped SnS nanoparticles via the emission intensity. The emission peaks were observed at 394, 400, and 403 nm for SnS1, SnS2, and SnS3, respectively, which could be attributed to excitons of SnS radiative recombination [44,46]. However, the intensity was noticed to follow the order SnS2 > SnS3 > SnS1, which suggests that SnS1 has the longest separation time for the electron–hole pair generated while SnS2 has fast separation efficiency of photoinduced charge carriers [47]. The lower recombination rate of the electron–hole pair observed in SnS1 and SnS3 will make these nanoparticles show higher photocatalytic efficiency (Figures 4a and 5a). Overall, the result shows that the dithiocarbamate moiety bonded to tin(ii) metal center played a significant role in the decomposition which affected the optical properties of the as-synthesized SnS nanoparticles.

Figure 3 (a) SnS nanoparticles absorption spectra; (b) Tauc plots; and (c) emission spectra.
Figure 3

(a) SnS nanoparticles absorption spectra; (b) Tauc plots; and (c) emission spectra.

Figure 4 (a) Degradation bar chart; (b) plot of C t /C 0 versus time; (c) kinetic studies; (d–f) recycling runs using SnS as photocatalyst for rhodamine B degradation.
Figure 4

(a) Degradation bar chart; (b) plot of C t /C 0 versus time; (c) kinetic studies; (d–f) recycling runs using SnS as photocatalyst for rhodamine B degradation.

Figure 5 (a) Degradation bar chart; (b) plot of C t /C 0 versus time; (c) kinetic studies; (d–f) recycling runs using SnS as photocatalyst for phenol degradation.
Figure 5

(a) Degradation bar chart; (b) plot of C t /C 0 versus time; (c) kinetic studies; (d–f) recycling runs using SnS as photocatalyst for phenol degradation.

3.4 Photocatalytic activity and stability of SnS nanoparticles

The degradation of rhodamine B and phenol by SnS nanoparticles under mercury light irradiation is observed by absorption spectra. Rhodamine B and phenol absorption maxima at 553 and 270 nm was observed to decrease with time, which indicates the degradation of the organic contaminants (Figures S7 and S8). The photodegradation of rhodamine B was 90.97, 61.53, and 80.26% by SnS1, SnS2, and SnS3, respectively, while against phenol it was 96.45, 75.13, and 90.69% after 180 min as shown in Figures 4a and 5a. The low degradation efficiency observed by SnS2 for the degradation of rhodamine B and phenol could be attributed to the fast recombination of photogenerated electron–hole pair as detected in the photoluminescence spectra (Figure 3c). In addition, the particle size of the as-prepared SnS nanoparticles influences the photocatalytic properties as the large particle size resulted in lower degradation efficiency [48]. The as-prepared SnS nanoparticles showed better degradation of rhodamine B and phenol compared to previous studies in the literature as presented in Table 1.

Table 1

Rhodamine B and phenol photodegradation by SnS nanoparticles

Irradiation time (min) Light source Organic pollutant Degradation (%) Ref.
210 350 W xenon arc lamp Rhodamine B 67.21 [49]
240 Solar light (90 mW cm−2) Rhodamine B 38 [50]
90 500 W xenon lamp Rhodamine B 11 [51]
180 100 W incandescent lamp Rhodamine B 58.3 [52]
90 Xenon lamp (XQ350W) Rhodamine B 20 [53]
120 300 W xenon arc lamp Rhodamine B 61 [54]
120 500 W xenon arc lamp Rhodamine B 64.8 [26]
120 Solar-simulator Rhodamine B 77 [55]
240 500 W xenon lamp Phenol 63.1 [56]
60 300 W xenon lamp Phenol 1.7 [27]
60 300 W Xe lamp Phenol 15.6 [57]
240 500 W xenon arc lamp Phenol 51.5 [26]
180 80 W mercury lamp Rhodamine B 90.97 This work
180 80 W mercury lamp Phenol 96.45 This work

The concentration curves of rhodamine B and phenol residual in the presence of the as-prepared SnS nanoparticles are presented in Figures 4b and 5b. A blank test of the rhodamine B and phenol without catalyst shows that the organic contaminants are stable under visible light irradiation. The absence of degradation by the organic contaminants indicates that the degradation process is not by photolysis but by the presence of the catalyst [27]. The photocatalytic degradation kinetics of rhodamine B and phenol evaluated was using the pseudo-first-order model [26].

ln C t C 0 = − k t ,

where k is the rate constant (min−1), C t and C 0 are the concentration at time t and initial concentration of rhodamine B, respectively. The photodegradation rate constant was calculated to be 0.3926, 0.1517, and 0.2642 min−1 for SnS1, SnS2, and SnS3, respectively, from the slope of the fitted line in Figure 4c for rhodamine B, with a correlation coefficient >0.98. Phenol rate constant of degradation was calculated to be 0.51, 0.2295, and 0.3777 min−1 for SnS1, SnS2, and SnS3, respectively, with correlation coefficient >0.99 from the fitted line shown in Figure 5c.

The stability and recyclability of catalyst are an important factor in practical application. Hence, the stability of the as-synthesized SnS nanoparticles was investigated for stability by performing the photodegradation of rhodamine B and phenol using the same catalyst four times. The results (Figure 4d–f) clearly show that as-synthesized SnS nanophotocatalyst showed slight degradation efficiency after four cycles and this indicates that the catalysts are stable and can be reused for the photodegradation of rhodamine B. In phenol, the same process was followed and about 6.01, 8.23, and 7.56% degradation efficiency reduction were observed for SnS1, SnS2, and SnS3, respectively, as shown in Figure 5d–f. The reduction in efficiency observed could be attributed to reaction of byproducts on the catalyst active site, or deposition of the organic contaminants on the catalyst surface or loss of catalyst during the process of washing and collection [57].

3.4.1 Effect of scavengers on the photocatalytic degradation of rhodamine B

Photodegradation process is controlled by the migration of electron–hole pair photogenerated to the surface of the catalyst [58,59]. Consequently, it is important to know the effect of superoxide radical (˙O2 −), holes (h+), electrons (e−), and hydroxyl radical (˙OH) on the photodegradation of rhodamine B by HDA-capped SnS nanoparticles. Hence, scavengers such as SN were used for e−, AC for ˙O2 −, AO for h+, and IPA for ˙OH were introduced to the photocatalytic system [60,61].

Photodegradation efficiency of rhodamine B decreases significantly after the addition of SN, AO, and IPA from 90.97% to 4.19, 18.86 and 11.71%, respectively (Figure 6a), while the addition of AC reduced the efficiency to 47.15%. This shows that e−, h+, and ˙OH are the main active species in the degradation of rhodamine B using SnS1 nanoparticles with O2 − serving as a secondary oxidant species [62]. The use of SnS2 as photocatalyst, SN, AO, and IPA inhibited the photodegradation of rhodamine B significantly indicating that e−, h+, and ˙OH are the main active species involve, while ˙O2 − plays minor role in the degradation process. Also, SnS3 followed the same trend as observed in SnS1 and SnS2. The addition of SN, IPA, and AO (e−, ˙OH, and h+ scavengers) leads to a decrease in the degradation efficiency, which indicate that the photogenerated electron–hole pairs are important in the photodegradation process which is confirm by the degradation process involving the ˙O2 − and ˙OH radicals. From the results obtained, the order of reactive oxidative species responsible for photocatalytic degradation by the SnS nanoparticles is e− > ˙OH > h + > ˙O2 −.

Figure 6 (a) Effect of scavengers on the photodegradation of rhodamine B and (b) phenol, by SnS nanoparticles.
Figure 6

(a) Effect of scavengers on the photodegradation of rhodamine B and (b) phenol, by SnS nanoparticles.

In the presence of a mercury lamp (visible light), irradiation of the SnS nanoparticles causes the excitation of the valence band electrons to the conduction band. Electron–hole pairs are generated, which migrate to the SnS surface, where they undergo redox reaction with rhodamine B on the SnS surface. The electrons generated react with oxygen to give superoxide and hydroxyl radicals through reduction, which degrades rhodamine B into CO2, H2O, NH4 +, NO3 −, and Cl− [61].

3.4.2 Effect of scavengers on the photocatalytic degradation of phenol

To investigate the mechanism of phenol photodegradation over the as-synthesized SnS catalyst, scavengers such as SN, AC, AO, and IPA were used as trapping agents for e‒, ˙O2 −, h +, and ˙OH radicals [60,61]. h+, ˙O2 −, and ˙OH directly oxidize phenol to CO2 and H2O, while e‒ reduces the benzene ring structure followed by oxidation [63]. Hence it is important to investigate the radicals responsible for the degradation process of phenol over the as-synthesized SnS quantum dots. In Figure 6b, the addition of AO inhibited degradation efficiency from 96.45 to 10.87% (SnS1), 75.13 to 9.41% (SnS2), and 90.69 to 8.53% (SnS3). The reduction in efficiency is an indication that photogenerated holes (h+) are reactive species during the photodegradation process. Similarly, the addition of IPA reduced the performance of SnS1 (96.45–21.02%), SnS2 (75.13–12.87%), and SnS3 (90.69–11.88%), suggesting that ·OH also played an important role in the degradation of phenol in the catalyst. Phenol degradation was inhibited by e‒ trapping, which indicates that some phenols were degraded via reduction mechanism through the SnS catalyst [64]. Moreover, Figure 6b demonstrates that the presence of AC reduces the photodegradation efficiency to 39.57 32.83, and 42.53% for SnS1, SnS2, and SnS3, respectively. These results suggest that although e‒ was involved in the photodegradation process, ·O2 ‒ also played an active role [65]. This trend confirms that the reactive species follows the sequence of h+ > ˙OH > e‒ > ˙O2 ‒ which corresponds to what is in the literature [46,48,66].

4 Conclusion

In summary, we have synthesized tin(ii) complexes of benzyl methyl dithiocarbamate, dibenzyl dithiocarbamate, and imidazolyl dithiocarbamate and used them as molecular precursors to prepare SnS1, SnS2, and SnS3 nanoparticles, respectively, via solvothermal method at low temperature (120℃). Monodispersed spherical nanoparticles were obtained for SnS1 and SnS2 with average particle size of 1.35 ± 0.04 and 2.63 ± 0.65 nm, respectively, while SnS3 was agglomerated with average size of 1.55 ± 0.15 nm. Different bandgap energy was obtained for the as-prepared SnS nanoparticles 3.80 eV (SnS1), 4.37 eV (SnS2), and 4.07 eV (SnS3). The results indicate that the bandgap energy can be tuned using different dithiocarbamate complexes due to variation in the obtained nanoparticle size. The synthesized SnS nanoparticles were used as photocatalyst for rhodamine B degradation under visible light irradiation, degradation efficiency of 90.97, 61.55, and 80.26% was achieved for SnS1, SnS2, and SnS3, respectively, and their corresponding degradation in phenol was 96.45, 75.13, and 90.69%. The result obtained shows that the nanoparticle size has an influence on the photodegradation efficiency. Electrons (e−), holes (h+), and radicals (˙O2 − and ˙OH) were found to be active in rhodamine B and phenol degradation using SnS nanoparticles. Also, the nanoparticles were highly stable and reusable.

  1. Funding information: The authors acknowledge funding from the National Research Foundation (Grant Number 129275) and Sasol South Africa.

  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: 2021-09-28
Revised: 2021-11-14
Accepted: 2022-01-01
Published Online: 2022-02-17

© 2022 Abimbola E. Oluwalana and Peter A. Ajibade, published by De Gruyter

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

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  102. Effect of micron-scale pores increased by nano-SiO2 sol modification on the strength of cement mortar
  103. Fractional simulations for thermal flow of hybrid nanofluid with aluminum oxide and titanium oxide nanoparticles with water and blood base fluids
  104. The effect of graphene nano-powder on the viscosity of water: An experimental study and artificial neural network modeling
  105. Development of a novel heat- and shear-resistant nano-silica gelling agent
  106. Characterization, biocompatibility and in vivo of nominal MnO2-containing wollastonite glass-ceramic
  107. Entropy production simulation of second-grade magnetic nanomaterials flowing across an expanding surface with viscidness dissipative flux
  108. Enhancement in structural, morphological, and optical properties of copper oxide for optoelectronic device applications
  109. Aptamer-functionalized chitosan-coated gold nanoparticle complex as a suitable targeted drug carrier for improved breast cancer treatment
  110. Performance and overall evaluation of nano-alumina-modified asphalt mixture
  111. Analysis of pure nanofluid (GO/engine oil) and hybrid nanofluid (GO–Fe3O4/engine oil): Novel thermal and magnetic features
  112. Synthesis of Ag@AgCl modified anatase/rutile/brookite mixed phase TiO2 and their photocatalytic property
  113. Mechanisms and influential variables on the abrasion resistance hydraulic concrete
  114. Synergistic reinforcement mechanism of basalt fiber/cellulose nanocrystals/polypropylene composites
  115. Achieving excellent oxidation resistance and mechanical properties of TiB2–B4C/carbon aerogel composites by quick-gelation and mechanical mixing
  116. Microwave-assisted sol–gel template-free synthesis and characterization of silica nanoparticles obtained from South African coal fly ash
  117. Pulsed laser-assisted synthesis of nano nickel(ii) oxide-anchored graphitic carbon nitride: Characterizations and their potential antibacterial/anti-biofilm applications
  118. Effects of nano-ZrSi2 on thermal stability of phenolic resin and thermal reusability of quartz–phenolic composites
  119. Benzaldehyde derivatives on tin electroplating as corrosion resistance for fabricating copper circuit
  120. Mechanical and heat transfer properties of 4D-printed shape memory graphene oxide/epoxy acrylate composites
  121. Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
  122. Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
  123. Gray correlation analysis of factors influencing compressive strength and durability of nano-SiO2 and PVA fiber reinforced geopolymer mortar
  124. Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
  125. Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
  126. Mechanisms of the improved stiffness of flexible polymers under impact loading
  127. Anticancer potential of gold nanoparticles (AuNPs) using a battery of in vitro tests
  128. Review Articles
  129. Proposed approaches for coronaviruses elimination from wastewater: Membrane techniques and nanotechnology solutions
  130. Application of Pickering emulsion in oil drilling and production
  131. The contribution of microfluidics to the fight against tuberculosis
  132. Graphene-based biosensors for disease theranostics: Development, applications, and recent advancements
  133. Synthesis and encapsulation of iron oxide nanorods for application in magnetic hyperthermia and photothermal therapy
  134. Contemporary nano-architectured drugs and leads for ανβ3 integrin-based chemotherapy: Rationale and retrospect
  135. State-of-the-art review of fabrication, application, and mechanical properties of functionally graded porous nanocomposite materials
  136. Insights on magnetic spinel ferrites for targeted drug delivery and hyperthermia applications
  137. A review on heterogeneous oxidation of acetaminophen based on micro and nanoparticles catalyzed by different activators
  138. Early diagnosis of lung cancer using magnetic nanoparticles-integrated systems
  139. Advances in ZnO: Manipulation of defects for enhancing their technological potentials
  140. Efficacious nanomedicine track toward combating COVID-19
  141. A review of the design, processes, and properties of Mg-based composites
  142. Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
  143. Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
  144. Recent progress and challenges in plasmonic nanomaterials
  145. Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
  146. Electronic noses based on metal oxide nanowires: A review
  147. Framework materials for supercapacitors
  148. An overview on the reproductive toxicity of graphene derivatives: Highlighting the importance
  149. Antibacterial nanomaterials: Upcoming hope to overcome antibiotic resistance crisis
  150. Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
  151. A review of atomic layer deposition modelling and simulation methodologies: Density functional theory and molecular dynamics
  152. Recent advances in the preparation of PVDF-based piezoelectric materials
  153. Recent developments in tensile properties of friction welding of carbon fiber-reinforced composite: A review
  154. Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
  155. Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
  156. Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
  157. Nanotechnology application on bamboo materials: A review
  158. Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
  159. Nanostructured lipid carrier system: A compendium of their formulation development approaches, optimization strategies by quality by design, and recent applications in drug delivery
  160. 3D printing customized design of human bone tissue implant and its application
  161. Design, preparation, and functionalization of nanobiomaterials for enhanced efficacy in current and future biomedical applications
  162. A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
  163. Nanotechnology interventions as a putative tool for the treatment of dental afflictions
  164. Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
  165. A focused review of short electrospun nanofiber preparation techniques for composite reinforcement
  166. Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
  167. Latest developments in the upconversion nanotechnology for the rapid detection of food safety: A review
  168. Strategic applications of nano-fertilizers for sustainable agriculture: Benefits and bottlenecks
  169. Molecular dynamics application of cocrystal energetic materials: A review
  170. Synthesis and application of nanometer hydroxyapatite in biomedicine
  171. Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
  172. Biological applications of ternary quantum dots: A review
  173. Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
  174. Application of antibacterial nanoparticles in orthodontic materials
  175. Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
  176. Nanozymes – A route to overcome microbial resistance: A viewpoint
  177. Recent developments and applications of smart nanoparticles in biomedicine
  178. Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
  179. Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
  180. Diamond-like carbon films for tribological modification of rubber
  181. Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
  182. Recent research progress and advanced applications of silica/polymer nanocomposites
  183. Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
  184. Recent advances in perovskites-based optoelectronics
  185. Biogenic synthesis of palladium nanoparticles: New production methods and applications
  186. A comprehensive review of nanofluids with fractional derivatives: Modeling and application
  187. Electrospinning of marine polysaccharides: Processing and chemical aspects, challenges, and future prospects
  188. Electrohydrodynamic printing for demanding devices: A review of processing and applications
  189. Rapid Communications
  190. Structural material with designed thermal twist for a simple actuation
  191. Recent advances in photothermal materials for solar-driven crude oil adsorption
https://doi.org/10.1515/ntrev-2022-0054
Keywords for this article
tin(ii) dithiocarbamate; single-source precursor; tin sulfide; nanoparticles; photocatalysis; recyclability
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  43. Molecular dynamics study of deformation mechanism of interfacial microzone of Cu/Al2Cu/Al composites under tension
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  101. Preliminary trials of the gold nanoparticles conjugated chrysin: An assessment of anti-oxidant, anti-microbial, and in vitro cytotoxic activities of a nanoformulated flavonoid
  102. Effect of micron-scale pores increased by nano-SiO2 sol modification on the strength of cement mortar
  103. Fractional simulations for thermal flow of hybrid nanofluid with aluminum oxide and titanium oxide nanoparticles with water and blood base fluids
  104. The effect of graphene nano-powder on the viscosity of water: An experimental study and artificial neural network modeling
  105. Development of a novel heat- and shear-resistant nano-silica gelling agent
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  107. Entropy production simulation of second-grade magnetic nanomaterials flowing across an expanding surface with viscidness dissipative flux
  108. Enhancement in structural, morphological, and optical properties of copper oxide for optoelectronic device applications
  109. Aptamer-functionalized chitosan-coated gold nanoparticle complex as a suitable targeted drug carrier for improved breast cancer treatment
  110. Performance and overall evaluation of nano-alumina-modified asphalt mixture
  111. Analysis of pure nanofluid (GO/engine oil) and hybrid nanofluid (GO–Fe3O4/engine oil): Novel thermal and magnetic features
  112. Synthesis of Ag@AgCl modified anatase/rutile/brookite mixed phase TiO2 and their photocatalytic property
  113. Mechanisms and influential variables on the abrasion resistance hydraulic concrete
  114. Synergistic reinforcement mechanism of basalt fiber/cellulose nanocrystals/polypropylene composites
  115. Achieving excellent oxidation resistance and mechanical properties of TiB2–B4C/carbon aerogel composites by quick-gelation and mechanical mixing
  116. Microwave-assisted sol–gel template-free synthesis and characterization of silica nanoparticles obtained from South African coal fly ash
  117. Pulsed laser-assisted synthesis of nano nickel(ii) oxide-anchored graphitic carbon nitride: Characterizations and their potential antibacterial/anti-biofilm applications
  118. Effects of nano-ZrSi2 on thermal stability of phenolic resin and thermal reusability of quartz–phenolic composites
  119. Benzaldehyde derivatives on tin electroplating as corrosion resistance for fabricating copper circuit
  120. Mechanical and heat transfer properties of 4D-printed shape memory graphene oxide/epoxy acrylate composites
  121. Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
  122. Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
  123. Gray correlation analysis of factors influencing compressive strength and durability of nano-SiO2 and PVA fiber reinforced geopolymer mortar
  124. Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
  125. Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
  126. Mechanisms of the improved stiffness of flexible polymers under impact loading
  127. Anticancer potential of gold nanoparticles (AuNPs) using a battery of in vitro tests
  128. Review Articles
  129. Proposed approaches for coronaviruses elimination from wastewater: Membrane techniques and nanotechnology solutions
  130. Application of Pickering emulsion in oil drilling and production
  131. The contribution of microfluidics to the fight against tuberculosis
  132. Graphene-based biosensors for disease theranostics: Development, applications, and recent advancements
  133. Synthesis and encapsulation of iron oxide nanorods for application in magnetic hyperthermia and photothermal therapy
  134. Contemporary nano-architectured drugs and leads for ανβ3 integrin-based chemotherapy: Rationale and retrospect
  135. State-of-the-art review of fabrication, application, and mechanical properties of functionally graded porous nanocomposite materials
  136. Insights on magnetic spinel ferrites for targeted drug delivery and hyperthermia applications
  137. A review on heterogeneous oxidation of acetaminophen based on micro and nanoparticles catalyzed by different activators
  138. Early diagnosis of lung cancer using magnetic nanoparticles-integrated systems
  139. Advances in ZnO: Manipulation of defects for enhancing their technological potentials
  140. Efficacious nanomedicine track toward combating COVID-19
  141. A review of the design, processes, and properties of Mg-based composites
  142. Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
  143. Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
  144. Recent progress and challenges in plasmonic nanomaterials
  145. Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
  146. Electronic noses based on metal oxide nanowires: A review
  147. Framework materials for supercapacitors
  148. An overview on the reproductive toxicity of graphene derivatives: Highlighting the importance
  149. Antibacterial nanomaterials: Upcoming hope to overcome antibiotic resistance crisis
  150. Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
  151. A review of atomic layer deposition modelling and simulation methodologies: Density functional theory and molecular dynamics
  152. Recent advances in the preparation of PVDF-based piezoelectric materials
  153. Recent developments in tensile properties of friction welding of carbon fiber-reinforced composite: A review
  154. Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
  155. Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
  156. Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
  157. Nanotechnology application on bamboo materials: A review
  158. Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
  159. Nanostructured lipid carrier system: A compendium of their formulation development approaches, optimization strategies by quality by design, and recent applications in drug delivery
  160. 3D printing customized design of human bone tissue implant and its application
  161. Design, preparation, and functionalization of nanobiomaterials for enhanced efficacy in current and future biomedical applications
  162. A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
  163. Nanotechnology interventions as a putative tool for the treatment of dental afflictions
  164. Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
  165. A focused review of short electrospun nanofiber preparation techniques for composite reinforcement
  166. Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
  167. Latest developments in the upconversion nanotechnology for the rapid detection of food safety: A review
  168. Strategic applications of nano-fertilizers for sustainable agriculture: Benefits and bottlenecks
  169. Molecular dynamics application of cocrystal energetic materials: A review
  170. Synthesis and application of nanometer hydroxyapatite in biomedicine
  171. Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
  172. Biological applications of ternary quantum dots: A review
  173. Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
  174. Application of antibacterial nanoparticles in orthodontic materials
  175. Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
  176. Nanozymes – A route to overcome microbial resistance: A viewpoint
  177. Recent developments and applications of smart nanoparticles in biomedicine
  178. Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
  179. Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
  180. Diamond-like carbon films for tribological modification of rubber
  181. Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
  182. Recent research progress and advanced applications of silica/polymer nanocomposites
  183. Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
  184. Recent advances in perovskites-based optoelectronics
  185. Biogenic synthesis of palladium nanoparticles: New production methods and applications
  186. A comprehensive review of nanofluids with fractional derivatives: Modeling and application
  187. Electrospinning of marine polysaccharides: Processing and chemical aspects, challenges, and future prospects
  188. Electrohydrodynamic printing for demanding devices: A review of processing and applications
  189. Rapid Communications
  190. Structural material with designed thermal twist for a simple actuation
  191. Recent advances in photothermal materials for solar-driven crude oil adsorption
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