FUEL
·
2024
·
IF 6.7
Yuzhou Xia,Jilong Xiao,Jiacheng Zhang,Renkun Huang,Xiaohui Huang,Guiyang Yan,Liuping Zheng
The construction of step-scheme (S-scheme) heterojunction has become an effective strategy for enhancing photocatalytic CO 2 reduction. In this study, a sunflower-like S-scheme WO 3 /ZnIn 2 S 4 heterostructure is fabricated through the in-situ growth of ZnIn 2 S 4 nanosheets on WO 3 hollow sphere, aimed at improving selective CO 2 reduction. The constructed embedding configuration, featuring a WO 3 hollow sphere core and an outer layer of ZnIn 2 S 4 nanosheet, increases the contact interface and establishes a significant built-in electric field, thereby promoting the migration and separation of photogenerated carriers. The confined internal cavity of the three-dimensional (3D) sunflower-like architecture aids in limiting the free diffusion of CO 2 , and enriching CO 2 molecules at the surface of the photocatalyst, consequently enhancing reaction kinetics. Moreover, S vacancies on ZnIn 2 S 4 nanosheets promote the chemisorption and activation of CO 2 . As a result, the optimized evolution rates for CH 4 and CO of 58.7μmol g –1 h −1 and 51.3μmol g –1 h −1 , respectively, are achieved for WO 3 /ZnIn 2 S 4 heterojunction. The corresponding electron selectivity for CH 4 reaches 82.1 %, which is 13 and 1.5 times higher than those of bare WO 3 and ZnIn 2 S 4 , respectively. This provides valuable insights into the design of muti-functionalized S-scheme heterojunction photocatalysts.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Tingting Hou,Nengchao Luo,Yi-Tao Cui,Jianmin Lu,Lei Li,Katherine E. MacArthur,Marc Heggen,Ruotian Chen,Fengtao Fan,Wenming Tian,Shengye Jin,Feng Wang
Engineering the electronic properties of heterogeneous catalysts is an important strategy to enhance their activity towards CO 2 reduction. Herein, we prepared partially sulfurized cerium oxide (CeO x -S) nanoclusters with the size less than 2 nm on the surface of ZnIn 2 S 4 layers. Surface electronic properties of CeO x -S nanoclusters are facilely modulated by cerium coordination to sulfur, inducing the emergence of abundant Ce 3+ and oxygen vacancies. For the photoreduction of CO 2 , CeO x -S/ZnIn 2 S 4 hybrid catalysts exhibited a CO productivity of 1.8 mmol g −1 with a rate of 0.18 mmol g −1 h −1 , which was twice as higher as that of ZnIn 2 S 4 catalyst using triethylamine as a sacrificial electron donor. Further mechanistic studies reveal that the photogenerated electrons are trapped by oxygen vacancies on CeO x -S/ZnIn 2 S 4 catalysts and subsequently transfer to CO 2 , benefiting the activation of CO 2 . Moreover, the extremely high selectivity of CO is derived from the weak adsorption of CO on the surface of CeO x -S/ZnIn 2 S 4 catalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Sijia Liu,Xifei Zhou,Changqing Yang,Chaohai Wei,Yun Hu
The extensive use of sacrificial agents and the low carrier separation and utilization efficiency remain important factors limiting the development of photocatalytic hydrogen production . We report a three-layered, dual-functional photocatalysts of Cu atomics@UiO-66-NH 2 (U6N)/ZnIn 2 S 4 nanosheets (ZIS), for the simultaneous production of photocatalytic hydrogen and degradation of organic pollutants . When common and highly toxic organic pollutants (phenolic compounds and antibiotics) were substituted for the sacrificial agents, Cu@U6N/ZIS exhibited superior sustained hydrogen production, approximately 28 times greater than that of pure ZIS. The experimental results suggested that the window size of U6N (< organic pollutants molecular size) separates the reaction sites of organic pollutants oxidation and reduction of hydrogen ions (H + ), thereby achieving spatial separation of redox sites. Besides, the structure of Cu@U6N/ZIS, which was anchored Cu within U6N and encapsulated by ZIS nanosheets, forming Z-type heterojunctions, achieved the control of the directional transfer of photogenerated electrons. And the coupled system can effectively enhance water quality by reducing the biological toxicity of the wastewater. This study suggests new avenues for environmental restoration and non-fossil fuel production.
研究领域:
环境科学
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能源科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2023
·
IF 8.7
Shengjun Liu,Dianjun Chi,Rong Chen,Yan Ma,Huixue Fang,Kui Zhang,Bo Liu
Inspired by natural photosynthesis, the design of novel Z-scheme photocatalytic systems holds great promise for improving photocatalytic hydrogen production performance. Here, we constructed a Z-scheme heterojunction to effectively improve the charge separation of TiO 2 /ZnIn 2 S 4 , with the N-doped C layer acting as an electron bridge. The T@NC-A/ZIS-72 heterojunctions demonstrated hydrogen production activity approximately 12.1 and 97.9 times higher than those of ZnIn 2 S 4 and TiO 2 @NC-A, respectively. The excellent electron migration ability of the carbon layer accelerated the photocatalytic hydrogen production performance. Our design introduces a component to provide a dedicated charge transport pathway, overcoming the inherent properties of the material and providing a new perspective for enhancing photocatalytic performance.
研究领域:
材料科学
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光化学
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催化
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 28
·2201668
·
IF 15.153
Lin Zhao,Bixia Yang,Guoxin Zhuang,Yonglin Wen,Tingshi Zhang,Mingxiong Lin,Zanyong Zhuang,Yan Yu
Exploitation of atomic-level principles to optimize the charge transfer on ultrathin 2D heterostructures is an emerging frontier in relieving the energy and environmental crisis. Herein, a facile “topological-atom-extraction” protocol is disclosed, i.e., selective extraction of Zn from ultrathin half-unit-cell ZnIn 2 S 4 (HZIS) can embed thin In 2 O 3 domain into 1.60 nm thick HZIS layer to create an atomically thin in-plane In 2 O 3 /HZIS heterostructure. Thanks to the optimal distance and capability of charge separation, the in-plane In 2 O 3 /HZIS heterostructure is among the best ZnIn 2 S 4 -based CO 2 reduction reaction (CRR) photocatalysts, and indeed demonstrates a significant increase (from 6.8- to 128-fold) in CO production rate compared with those of out-plane ZIS@In 2 O 3 and out-plane In 2 O 3 -HZIS calcined heterostructures. Density Functional Theory simulation reveals that whereas the out-plane heterostructure has a much smaller ∆q of 0.2–0.25 e, the in-plane heterostructure with “zero distance contact” has an optimal ∆q of 1.05 e between In 2 O 3 and HZIS that induces remarkable charge redistribution on the in-plane heterojunction interface and creates local electric field confined within the ultrathin layer. The charge redistribution efficiently directs the charge-carrier separation in S-scheme photocatalytic system and endows long-lifetime carrier to CRR active HZIS. The findings demonstrate the strong versatility of engineering atomic-level heterojunctions for efficient catalysts design.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
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IF 13.1
Jianghua Zhao,Yifan Wang,Huai Liu,Rui Zhang,Wenlong Jia,Junhua Zhang,Yong Sun,Lincai Peng
Defect engineering is an effective strategy to enhance the photocatalytic performance of ZnIn2S4 (ZIS), but it remains a formidable challenge to manipulate the cationic defects in the catalyst because of their high formation energies. Herein, dual Zn and In defects have been successfully created in the ZnIn2S4 (ZIS-5) with a facile cetyltrimethylammonium chloride (CTAC)-assisted hydrothermal method. The resulting ZIS-5, rich in cation vacancies, achieved a 3.6-fold higher 2,5-diformylfuran (DFF) yield (92.0%) than the pristine ZIS (25.8%) for the visible-light-driven photocatalytic air-oxidation of 5-hydroxymethylfurfural (HMF). Especially, ZIS-5 delivers a high DFF productivity of 1600 μmol g–1 h–1, significantly surpassing the previously reported catalysts (75–953 μmol g–1 h–1) for the photocatalytic oxidation of HMF to DFF in air. Density functional theory (DFT) simulations revealed that the presence of dual Zn and In defects endows the catalyst with defect states that intersect the Fermi level and lower work function. These enhance the migration and separation of photogenerated carriers in ZIS-5, significantly promoting O2 activation and resulting in the generation of more reactive oxygen species (·O2– and 1O2) for the catalytic oxidation of HMF. This study offers valuable insights for guiding the design of photoredox reaction systems through cationic-defect-engineering strategies, enabling the efficient valorization of biomass-derived platform chemicals.
研究领域:
材料科学
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2023
·Vol. 20
·期 20
·2307386
·
IF 13.3
Shiting Wu,Xiaohui Li,Jiaqi Liu,Hanfeng Wu,Hanshuai Xu,Wangfeng Bai,Liang Mao,Xiaowei Shi
Selective photocatalytic production of high-value acetaldehyde concurrently with H 2 from bioethanol is an appealing approach to meet the urgent environment and energy issues. However, the difficult ethanol dehydrogenation and insufficient active sites for proton reduction within the catalysts, and the long spatial distance between these two sites always restrict their catalytic activity. Here, guided by the strong metal-substrate interaction effect, an atomic-level catalyst design strategy to construct Pt-S 3 single atom on ZnIn 2 S 4 nanosheets (Pt SA -ZIS) is demonstrated. As active center with optimized H adsorption energy to facilitate H 2 evolution reaction, the unique Pt single atom also donates electrons to its neighboring S atoms with electron-enriched sites formed to activate the O─H bond in * CH 3 CHOH and promote the desorption of * CH 3 CHO. Thus, the synergy between Pt single atom and ZIS together will reduce the energy barrier for the ethanol oxidization to acetaldehyde, and also narrow the spatial distance for proton mass transfer. These features enable Pt SA -ZIS photocatalyst to produce acetaldehyde with a selectivity of ≈100%, which will spontaneously transform into 1,1-diethoxyethane via acetalization to avoid volatilization. Meanwhile, a remarkable H 2 evolution rate (184.4 µmol h −1 ) is achieved with a high apparent quantum efficiency of 10.50% at 400 nm.
研究领域:
材料科学
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催化化学
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能源转化
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Hong Yao,Guozhe Sui,Jinlong Li,Dongxuan Guo,Jiaqi Wang,Yuanzhi Yue,Bing Jia,Xuan Xuan,Jing Tang
The construction of efficient Z-scheme heterojunctions is considered as a promising approach to improve the transfer and separation of photogenerated carries in the field of photocatalytic hydrogen evolution from water splitting. Herein, a novel ZnIn 2 S 4 /P-Ni-MOF-74 with Z-scheme heterostructure is successfully fabricated from rhombic P-Ni-MOF-74 derived from Ni-MOF-74 through phosphorization treatment and ZnIn 2 S 4 flakes via a hydrothermal method . The Z-scheme ZnIn 2 S 4 /P-Ni-MOF-74 heterojunctions can provide abundant active centers, broaden the response range to visible light region, accelerate the transfer of interfacial charges, and suppress the recombination rate of photogenerated electron-hole pairs. As a result, ZnIn 2 S 4 /P-Ni-MOF-74 (20 wt% P-Ni-MOF-74) acquires a hydrogen production rate of 7865.31 μmol g −1 h −1 , which is 4.46 times higher than that of ZnIn 2 S 4 . An apparent quantum yield is 7.84% at 420 nm wavelength. Overall, this work may provide a new pathway for the rational design of efficient Z-scheme heterojunctions with photocatalytic hydrogen evolution.
研究领域:
材料科学
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能源科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Hongmei Zhao,Tingting Zhang,Dongyu Shan,Ying Zhu,Ge Gao,Ye Liu,Jing Liu,Meiying Liu,Wansheng You
An intervening barrier for photocatalytic water decomposition and pollutant degradation is the frustratingly quick recombination of e − - h + pairs. Delicate design of heterojunction photocatalysts by coupling the semiconductors at nanoscale with well-matched geometrical and electronic alignments is an effective strategy to ameliorate the charge separation. Here a facile and environment-friendly l -cysteine-assisted hydrothermal process under weakly alkaline conditions is demonstrated for the first time to fabricate ZnIn 2 S 4 /In(OH) 3 hollow microspheres with intimate contact, which are verified by XRD, SEM, (HR)TEM, XPS , N 2 adsorption-desorption, UV–Vis DRS and photoluminescence spectra. ZnIn 2 S 4 /In(OH) 3 heterostructure (L-cys/Zn 2+ = 4, molar ratio) with a band-gap of 2.50 eV, demonstrates the best photocatalytic performance for water reduction and MB degradation under visible light, outperforming its counterparts (In(OH) 3 and ZnIn 2 S 4 ). The excellent activity of ZnIn 2 S 4 /In(OH) 3 heterostructure arises from the intercrossed band-edge positions as well as the unique hollow structure with large surface area and wide pore-size distribution, which are beneficial for the efficient charge migration from bulk to surface as well as at the interface between ZnIn 2 S 4 and In(OH) 3 . This work provides an efficient and eco-friendly strategy for one-pot synthesis of heterostructured composites with intimate contact for photocatalytic application.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yutong Chen,Rong Wu,Jianyong Yue,Dezheng Kong,Chen Zhang,Shunhang Wei
Photocatalytic overall water splitting (POWS) is an efficient technology that converts solar energy into H 2 energy, holding significant importance in the realms of energy and the environment. As a visible-light photocatalyst, ZnIn 2 S 4 , despite being an ideal low-dimensional semiconductor for photocatalytic overall water splitting, has its performance therein affected by poor charge separation. The present study reports the successful synthesis of a novel Bi 4 NbO 8 Cl/ZnIn 2 S 4 :Mo Z-scheme heterojunction via a hydrothermal method. Under AM 1.5G irradiation, the POWS H 2 evolution rate was measured at 84.8 μmol g −1 h −1 , while the O 2 evolution rate was determined to be 47.0 μmol g −1 h −1 . Under simulated solar light irradiation, Bi 4 NbO 8 Cl/ZnIn 2 S 4 :Mo heterojunction exhibits an apparent quantum efficiency (AQE) of 0.22 % at 420 ± 20 nm and a solar-to-hydrogen (STH) conversion efficiency of 0.026 %. UV–Vis–NIR spectroscopic analysis unequivocally demonstrated a significant enhancement in the utilization efficiency of the Bi 4 NbO 8 Cl/ZnIn 2 S 4 :Mo Z-scheme heterojunction in the near-infrared light region compared to the pristine ZnIn 2 S 4 and Bi 4 NbO 8 Cl. This improvement extends the spectral absorption boundary of the photocatalyst, allowing efficient capture of a considerable proportion of low-energy photons in sunlight. Unique charge transfer mechanism of Z-scheme heterojunction was revealed by in-situ XPS and EPR tests. Z-scheme heterojunction effectively promoted the respective enrichment of electrons and holes generated by photo-excitation in ZnIn 2 S 4 :Mo and Bi 4 NbO 8 Cl, thereby improving the performance of POWS. This study not only establishes an experimental foundation for the design and construction of Z-scheme heterojunctions but also explores a new approach to augment the utilization efficiency of the near-infrared solar spectrum.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Qianqian Nie,Linfeng Liu,Jiayou Liu,Mingwei Shen,Xiaoxiang Huang,Zhongchao Tan,Hesheng Yu
Bi2Fe4O9/ZnIn2S4 (BFO/ZIS) composites are synthesized by using a facile impregnation method and tested for the photocatalytic degradation of xanthate for the first time. The effects of multiple parameters, including catalyst dosage and the pH value of solution, on xanthate photodegradation are investigated systematically. Furthermore, the photocatalytic mechanisms of BFO/ZIS are proposed based on various characterizations and density functional theory calculations. Results show that the degradation efficiency of 30BFO/ZIS is 98.25% during 90 min of visible light irradiation, which is 2.63 and 2.89 times higher than that of pure ZIS and BFO, respectively. This is mainly because the type II heterojunction formed between BFO and ZIS improves the separation of photogenerated carriers. Furthermore, the xanthate photodegradation efficiency of 30BFO/ZIS decreases slightly from 98.25 to 92.86% after four cycles, indicating its excellent durability and stability. Finally, the chemical oxygen demand (COD) removal efficiency of 30BFO/ZIS is up to 81.06%, exhibiting a high degree of mineralization.
研究领域:
材料科学
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环境科学
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化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Qin Li,Yang Xia,Chao Yang,Kangle Lv,Ming Lei,Mei Li
Facing the requirement of modern industrial development, selective reduction of 4-nitroaniline (4-NA) into p-phenylenediamine (PPD) via a facile, economic and eco-friendly photocatalysis technique has attracted more and more attention in recent years. In this study, ZnIn 2 S 4 (ZIS) nanosheets grew in-situ on the surface of TiO 2 hollowspheres through a hydrothermal method and formed a direct Z-scheme heterojunction composite, which exhibited exceedingly better photocatalytic 4-NA reduction performance than bare ZIS and TiO 2 . Such enhancement was mainly attributed to the dissimilar dimensionalities, intimate contact, and matchable band edge positions between ZIS and TiO 2 semiconductors. Moreover, the substantial mechanism for the photocatalytic reaction in the ZIS/TiO 2 system was reasonably proposed. Inspired by recent applications of the Z-scheme heterostructured materials in solar energy conversion and artificial photosynthesis, this work would arouse an increasing interest in designing more Z-scheme photocatalyst systems with high efficiency and extensive applications.
研究领域:
材料科学
·
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）