Surfaces and Interfaces
·
2024
·
IF 5.7
Ziqi Zhang,Hui Yi,Jinyuan Cai,Weiguang Han,Fangyuan Zhang,Sheng-Qi Guo
Defect engineering is considered an effective means to improve the photocatalytic performance of semiconductors. However, current research on defects mainly focuses on single atom vacancies, lacking research on atomic vacancy pairs. In this work, we used SnS 2 as the research model and constructed SnS 2 nanostructures with rich S vacancies and dual S vacancy pairs, respectively. By comparing the photocatalytic activation O 2 performance of SnS 2 under different defect effects, it was found that dual S vacancy pairs have better performance optimization characteristics than S vacancies. Combining experiments and theoretical calculations, it is confirmed that dual S vacancy pairs have significant advantages over S vacancies in regulating the band structure, improving the separation efficiency of photogenerated charges and the migration rate of charge carriers, as well as activating the interface reaction of O 2 . In addition, when the catalyst is used for the removal of organic matter in water, it can be found that the optimization effect of dual defects on performance has good sustainability. This work contributes to a deeper understanding of the application scope of defect engineering and provides new ideas for the development of highly active photocatalysts.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Juan Du,Tianfeng Cai,Qiao Han,Hongda Wu,Qing Zhao,Lufan Zheng,Shuo Liu,Zhanxu Yang
The hydrogen spillover is considered a powerful strategy for improving the kinetics of hydrogen evolution reaction (HER) due to the decoupling of hydrogen adsorption and desorption. However, the hydrogen spillover rate strongly depends on the metal-support interfaces, and the Fermi levels (E f ) difference between metal and support hinders the occurrence of hydrogen spillover. Here, we prepared platinum (Pt) doped on molybdenum disulfide (MoS 2 ) with sulfur vacancies (Sv) catalyst (Pt/Sv-MoS 2 ) and investigated the internal relationship between metal-support interfaces and hydrogen spillover mechanism. The experimental and theoretical results show that sulfur (S) vacancies reduce the work function (ΔΦ) at the metal-support interface, thus accelerating the migration rate of hydrogen from Pt to Sv-MoS 2 . Meanwhile, the introduction of S vacancies promotes the high dispersion of Pt nanoparticles (Pt NPs) and weakens the electron supply from Pt to MoS 2 , facilitating active hydrogen (*H) adsorption step and thus increasing the hydrogen coverage on the Pt sites. Consequently, the prepared Pt/Sv-MoS 2 catalyst exhibited significantly enhanced HER activity, achieving an overpotential of 26 mV at 10 mA·cm −2 and a Tafel slope of only 28 mV·dec −1 , which is superior to commercial 20 % Pt/C.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Changming Zhang,Zhihao Liu,Yongjin Zou,Fen Xu,Lixian Sun,Zhicong Hu,Sensen Yu,Cuili Xiang
Spinel-type materials are attracting great attention as potential electrocatalysts for the hydrogen- and oxygen-evolution reactions. However, their inherent catalytic activities are not on par with those of precious-metal catalysts, and their poor stabilities continue to constrain their rapid development. In this study, we fabricated Zr-CuCo 2 S 4 nanowires and Co(OH) 2 nanosheet–nanowires using electrochemical methods, resulting in lattice defects, sulfur vacancies, and more exposed active sites that catalyze the hydrogen- and oxygen-evolution reactions. DFT calculations revealed that sulfur vacancies enhance intrinsic activity, while Zr doping reduces the energy barrier for H*–OH* adsorption, promotes the formation of additional sulfur vacancies, and modulates active-site Cu/Co valence states, which greatly enhances water-dissociation and H*-adsorption kinetics. Consequently, Zr-CuCo 2 S 4 /Co(OH) 2 requires low overpotentials of 88 and 208 mV, respectively, to support highly stable alkaline hydrogen- and oxygen-evolution reactions at 10 mA cm −2 . This study provides a rational strategy for designing low-cost spinels for green and clean energy.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Ruixue Liu,Xinli Li,Zhendi Jia,Yiyun Wang,Yanli Peng,Congming Tang,Zhi Chen,Lin Dong
The hydrodeoxygenation of lactic acid (LA) to propionic acid (PA) is of great significance for the conversion of biomass to valuable products; however, it remains a great challenge because of the trade-off between LA conversion and PA selectivity. Here, we prepared ultrathin MoS2 nanosheets containing rich sulfur vacancies by lithium exfoliation. With the increase of the lithium exfoliation time, sulfur vacancy in MoS2 is accordingly increased and LA adsorption and activation on sulfur vacancy is enhanced. Increasing sulfur vacancy lowered the valence band simultaneously and enhanced the dissociation of the H2 molecule. Density functional theory (DFT) calculations showed that the sulfur vacancy efficiently adsorbed α-C–OH of the LA molecule, weakened the C–O bond, and achieved selective conversion of LA to PA. At 215 °C, 92.4% of LA conversion and 95.8% PA selectivity were achieved over the sulfur vacancy-rich MoS2 nanosheets, which broke the activity–selectivity trade-off on hydrodeoxygenation of LA, and notably surpassed those of previously reported catalysts. More importantly, the activity of the catalyst remained almost unchanged after 8 cycles of reaction.
研究领域:
催化化学
·
生物质转化
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Lian Yi,François Nkinahamira,Hongyi Jiang,Jingyuan Huang,Yueyong Ma,Rongshu Zhu
The development of photocatalyst is essential for achieving efficient photocatalytic water splitting for hydrogen production . Therefore, a novel Mo 2 N (MN) decorated ZnIn 2 S 4 (ZIS) with sulfur-rich vacancy (Sv-ZIS) photocatalyst was rationally constructed via a facile calcining-hydrothermal method for efficient photocatalytic H 2 production. The optimized photocatalyst exhibits an outstanding photocatalytic H 2 production rate of 10.28 mmol·g −1 ·h −1 , 7.52 and 3.11 times higher than that of bare ZIS and S V -ZnIn 2 S 4 (S V -ZIS), respectively. The characterizations reveal that the presence of MN and S-vacancies improves the light absorption capacity, and facilitates the separation and migration of photogenerated carriers. Density functional theory calculations (DFT) have confirmed that MN can optimize ΔG H* to approach 0, which is favorable for photocatalytic hydrogen production . Therefore, the combined effect of MN and S-vacancies facilitates efficient photocatalytic H 2 production of S V -ZIS/MN.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Aihua Yan,Tongyang Zhang,Fei Huang,Quande Wang,Shijian Lu,Wenxue Zhao,Ye Gao,Zigao Su,Huaqi Yuan
Multiplex modification is considered as one of attractive methods to achieve highly-efficient photocatalytic water splitting into hydrogen evolution performance. Herein, MoS 2 /S v -ZnIn 2 S 4 /ZnS (MS/S v -ZIS/ZS) composites were constructed by a facile in-situ engineering technique. The sulfur vacancy, Ohmic-type contact and I-type heterojunction were systematically integrated into the composites. The unique structure could not only facilitate a directional charge transfer and accelerate the charge extraction, but also enhance the charge utilization and improve the hydrogen reduction reaction dynamics. As a result, the composites exhibited a promoted hydrogen evolution rate of 9.5 mmol g −1 h −1 , which was about 3.8 times higher than that of pure ZIS. This work may extend the in-situ preparation strategy and motivate the intensive investigation of high-efficiency ZIS-based photocatalysts.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 14
·3334
·
IF 4.2
Aizhen Liao,Zhengchu Liu,Yiqing Wei,Qinghua Xie,Ting Kong,Maolin Zeng,Wenpeng Wang,Chao Yang,Linji Zhang,Yonggang Xu,Yong Zhou,Zhigang Zou
The synthesis of the accurate composition and morphological/structural design of multielement semiconductor materials is considered an effective strategy for obtaining high-performance hybrid photocatalysts. Herein, sulfur vacancy (Vs)-bearing In2S3/CuInS2microflower heterojunctions (denoted Vs-In2S3/CuInS2) were formed in situ using In2S3microsphere template-directed synthesis and a metal ion exchange-mediated growth strategy. Photocatalysts with flower-like microspheres can be obtained using hydrothermally synthesized In2S3microspheres as a template, followed by Ostwald ripening growth during the metal cation exchange of Cu+and In3+. The optimal heterostructured Vs-In2S3/CuInS2microflowers exhibited CO and CH4evolution rates of 80.3 and 11.8 μmol g−1h−1, respectively, under visible-light irradiation; these values are approximately 4 and 6.8 times higher than those reported for pristine In2S3, respectively. The enhanced photocatalytic performance of the Vs-In2S3/CuInS2catalysts could be attributed to the synergistic effects of the following factors: (i) the constructed heterojunctions accelerate charge-carrier separation; (ii) the flower-like microspheres exhibit highly uniform morphologies and compositions, which enhance electron transport and light harvesting; and (iii) the vs. may trap excited electrons and, thus, inhibit charge-carrier recombination. This study not only confirms the feasibility of the design of heterostructures on demand, but also presents a simple and efficient strategy to engineer metal sulfide photocatalysts with enhanced photocatalytic performance.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science Bulletin
·
2024
·
IF 18.8
Guanshun Xie,Le Liao,Jie Wang,Peng Zhang,Benhua Xu,Xiuqiang Xie,Chi Chen,Babak Anasori,Nan Zhang
Selective CO 2 -to-CO photoreduction is under intensive research and requires photocatalysts with tuned microstructures to accelerate the reaction kinetics. Here, we report CuInS 2 nanosheet arrays with sulfur vacancies (V S ) grown on the two-dimensional (2D) support of Ti 3 C 2 T x MXene for CO 2 -to-CO photoreduction. Our results reveal that the use of Ti 3 C 2 T x induces strong support effect, which causes the hierarchical nanosheet arrays growth of CuInS 2 and simultaneously leads to charge transfer from CuInS 2 to Ti 3 C 2 T x support, resulting in V S formed in CuInS 2 . The strong support effect based on Ti 3 C 2 T x is proven to be applicable to prepare a series of different metal indium sulfide arrays with V S . CuInS 2 nanosheet arrays with V S supported on Ti 3 C 2 T x benefit the photocatalytic selective reduction of CO 2 to CO, manifesting a remarkable over 14.8-fold activity enhancement compared with pure CuInS 2 . The experimental and computational investigations pinpoint that V S of CuInS 2 resulting from the support effect of Ti 3 C 2 T x lowers the barrier of the rate-limiting step of *COOH → *OH + *CO, which is the key to the photoactivity enhancement. This work demonstrates MXene support effects and offers an effective approach to regulate the atomic microstructure of metal sulfides toward enhancing photocatalytic performance.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Benteng Sun,Zhangqian Liang,Yeye Qian,Xuesong Xu,Ye Han,Jian Tian
Here, we reported that sulfur vacancy-rich O-doped 1T-MoS2 nanosheets (denoted as SV-1T-MoS2) can surpass the activity of Pt as cocatalysts to assist in the photocatalytic nitrogen fixation of CdS nanorods. SV-1T-MoS2 cocatalysts exhibit sulfur vacancies, O-doping, more metallic 1T phase, and high electronic conductivity, thus leading to the exposure of more active edge sites, high Brunauer–Emmett–Teller surface area, enhanced visible light absorption, and improved electron separation and transfer, which are beneficial for photocatalytic nitrogen fixation. Consequently, the optimized 30 wt % SV-1T-MoS2-/CdS composites exhibit an outstanding nitrogen fixation rate of 8220.83 μmol L–1 h–1 g–1 and long-term stability under simulated solar light irradiation, significantly higher than pure CdS nanorods, CdS–Pt (0.1 wt %), and 30 wt % 1T-MoS2/CdS composites. The catalytic mechanism of photocatalytic nitrogen fixation on SV-1T-MoS2 is discussed by density functional theory calculations.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Wenxue Zhao,Aihua Yan,Zigao Su,Fei Huang,Jixu Zhang,Ye Gao,Huaqi Yuan,Bolei Hui,Heng Wang
ZnIn 2 S 4 is a promising and typical semiconductor for photocatalytic water splitting into hydrogen production. However, the low charge-carrier utilization restricts its hydrogen evolution performance and practical application. In this work, a synergistic strategy of sulfur vacancy (S v ), internal electric field (IEF) and Mo-S bond was utilized for improving the charge-carrier utilization of MoS 2 /S v -MnS/ZnIn 2 S 4 composites. In particular, Z-scheme S v -MnS/ZnIn 2 S 4 heterojunction not only tackled the charge-carrier recombination problem but also improved the redox capability. Meanwhile, Schottky-type MoS 2 /S v -MnS contact further promoted the charge transfer through Mo-S bond “bridge”, accelerated the surface hydrogen reduction reaction kinetics, and thus boosted the charge-carrier utilization. As a result, the optimal MoS 2 /S v -MnS/ZnIn 2 S 4 catalysts could expeditiously produce 1.75 mL of hydrogen production within 3 h, and achieve a photocatalytic hydrogen evolution rate of 13.02 mmol g -1 h -1 . This work provides an ingenious method to synthesize ZnIn 2 S 4 -based photocatalysts with highly-efficient charge-carrier utilization.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiang He,Zhongqing Yang,Ziqi Wang,Linlin Gu,Jiaqi Qiu,Jingyu Ran
The rapid recombination of photogenerated electron-hole pairs and the slow electron transfer rate at the catalyst-solution interface seriously limit hydrogen production from α-cellulose photoreforming. Herein, a sulfur-vacancy-enriched ZnIn 2 S 4 (S VH -ZIS) photocatalyst was prepared, and Pt nanoclusters were grown on its surface by in situ photodeposition. Sulfur vacancies coupling Pt nanoclusters optimize the electron transport channel and realize efficient electron migration from α-cellulose to H + through the photocatalyst. The construction of sulfur vacancies promoted the formation of ·OH and enhanced the adsorption and activation of glucose, which significantly improved the oxidation of α-cellulose and accelerated the oxidation kinetics of α-cellulose. Meanwhile, the sulfur vacancies promote the separation efficiency of photogenerated electron-hole pairs and broaden the absorption wavelength range of light. Pt clusters provide hydrogen evolution reaction sites and achieve spatial separation of oxidation and reduction reaction sites. As a result, the hydrogen yield of α-cellulose photoreforming catalyzed by 0.25 % Pt/S VH -ZIS reached 522.76 μmol/g/h, which was 6.02 times that of 0.25 % Pt/S VL -ZIS (sulfur-vacancy-poor ZIS) and significantly higher than that of most previously reported photocatalysts.
研究领域:
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 10
·103507
·
IF 4.316
Fuhua Chen,Hao Guo,Lili Zhao,Xin Guo,Shunchang Li,Ying Chu,Xueying Wang,Yongping Zhu
As a cathode material for thermal batteries, WS2 has high thermal decomposition temperature and large specific capacity, but it is an intermittent semiconductor, with relatively low conductivity. This low conductivity can prolong the activation time and reduce the discharge specific capacity of thermal batteries. Here, we prepared WS2 with sulfur vacancies through a simple high-temperature annealing method and used electron paramagnetic resonance spectroscopy and X-ray photoelectron spectroscopy to detect the presence of sulfur vacancies. The result shows that sulfur vacancies were successfully introduced in WS2, and the existence of sulfur vacancies can effectively improve the discharge performance of thermal batteries. While maintaining the nanostructure, the thermal decomposition temperature still exceeds 1000 °C, which is far beyond the traditional FeS2 (550 °C) and CoS2 (650 °C) cathodes. The Li-B/LiF-LiBr-LiCl/WS2 with sulfur vacancies (treated at 500 °C) couple has higher discharge specific capacity (when the cut-off voltage is 0.5 V, it is 380.58 mAh g−1, which is 14.85% higher than the original WS2) and lower total polarization (about 21% lower than original WS2). This work provides a beginning for further study of sulfur vacancies defect materials as the cathode of thermal batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）