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学者姓名：徐艺军
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Abstract ：
Light-driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH4) into high value-added chemicals under ambient conditions. However, the high C−H bond dissociation energy of CH4 and the absence of well-defined C−H activation sites on catalysts significantly limit the highly efficient conversion of CH4 toward multicarbon (C2+) hydrocarbons, particularly ethylene (C2H4). Herein, we demonstrate a bimetallic design of Ag nanoparticles (NPs) and Pd single atoms (SAs) on ZnO for the cascade conversion of CH4 into C2H4 with the highest production rate compared with previous works. Mechanistic studies reveal that the synergistic effect of Ag NPs and Pd SAs, upon effecting key bond-breaking and -forming events, lowers the overall energy barrier of the activation process of both CH4 and the resulting C2H6, constituting a truly synergistic catalytic system to facilitate the C2H4 generation. This work offers a novel perspective on the advancement of photocatalytic directional CH4 conversion toward high value-added C2+ hydrocarbons through the subtle design of bimetallic cascade catalyst strategy. © 2024 Wiley-VCH GmbH.
Keyword ：
bimetallic sites bimetallic sites C−H activation C−H activation ethylene ethylene methane conversion methane conversion photocatalysis photocatalysis
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| GB/T 7714 | Wang, Y.-F. , Qi, M.-Y. , Conte, M. et al. Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane [J]. | Angewandte Chemie - International Edition , 2024 , 63 (34) . |
| MLA | Wang, Y.-F. et al. "Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane" . | Angewandte Chemie - International Edition 63 . 34 (2024) . |
| APA | Wang, Y.-F. , Qi, M.-Y. , Conte, M. , Tang, Z.-R. , Xu, Y.-J. . Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane . | Angewandte Chemie - International Edition , 2024 , 63 (34) . |
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Janus heterostructures consisting of multiple jointed components with distinct properties have gained growing interest in the photoredox catalytic field. Herein, we have developed a facile low-temperature method to gain anisotropic one-dimensional Au-tipped CdS (Au−CdS) nanorods (NRs), followed by assembling Ru molecular co-catalyst (RuN5) onto the surface of the NRs. The CdS NRs decorated with plasmonic Au nanoparticles (NPs) and RuN5 complex harness the virtues of metal-semiconductor and inorganic-organic interface, giving directional charge transfer channels, spatially separated reaction sites, and enhanced local electric field distribution. As a result, the Au−CdS−RuN5 can act as an efficient dual-function photocatalyst for simultaneous H2 evolution and valorization of biomass-derived alcohols. Benefiting from the interfacial charge decoupling and selective chemical bond activation, the optimal all-in-one Au−CdS−RuN5 heterostructure shows greatly enhanced photoactivity and selectivity as compared to bare CdS NRs, along with a remarkable apparent quantum yield of 40.2 % at 400 nm. The structural evolution and working mechanism of the heterostructures are systematically analyzed based on experimental and computational results. © 2024 Wiley-VCH GmbH.
Keyword ：
charge decoupling charge decoupling dual-function catalyst dual-function catalyst functional active site functional active site Janus structure Janus structure selective photoredox selective photoredox
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| GB/T 7714 | Han, C. , Zeng, Z. , Zhang, X. et al. All-in-One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis [J]. | Angewandte Chemie - International Edition , 2024 . |
| MLA | Han, C. et al. "All-in-One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis" . | Angewandte Chemie - International Edition (2024) . |
| APA | Han, C. , Zeng, Z. , Zhang, X. , Liang, Y. , Kundu, B.K. , Yuan, L. et al. All-in-One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis . | Angewandte Chemie - International Edition , 2024 . |
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Photocatalytic epoxide alcoholysis through C-O bond cleavage and formation has emerged as an alternative to synthesizing anti-tumoral pharmaceuticals and fine chemicals. However, the lack of crucial evidence to interpret the interaction between reactants and photocatalyst surface makes it challenging for photocatalytic epoxide alcoholysis with both high activity and regioselectivity. In this work, we report the hierarchical ZnIn2S4@CdS photocatalyst for epoxide alcoholysis with high regioselectivity nearly 100%. Mechanistic studies unveil that the precise activation switch on exposed Zn acid sites for C-O bond polarization and cleavage has a critical significance for achieving efficient photocatalytic performance. Furthermore, the establishment of Z-scheme heterojunction facilitates the interface charge separation and transfer. Remarkably, the underlying regioselective photocatalytic reaction pathway has been distinctly revealed.
Keyword ：
Epoxide Alcoholysis Epoxide Alcoholysis Hierarchical Structure Hierarchical Structure Photocatalysis Photocatalysis Regioselectivity Regioselectivity Vacancy Regulation Vacancy Regulation
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| GB/T 7714 | Li, Jing-Yu , Tan, Chang-Long , Qi, Ming-Yu et al. Exposed Zinc Sites on Hybrid ZnIn2S4@CdS Nanocages for Efficient Regioselective Photocatalytic Epoxide Alcoholysis [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
| MLA | Li, Jing-Yu et al. "Exposed Zinc Sites on Hybrid ZnIn2S4@CdS Nanocages for Efficient Regioselective Photocatalytic Epoxide Alcoholysis" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 22 (2023) . |
| APA | Li, Jing-Yu , Tan, Chang-Long , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Exposed Zinc Sites on Hybrid ZnIn2S4@CdS Nanocages for Efficient Regioselective Photocatalytic Epoxide Alcoholysis . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
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二硫化物及其衍生物是生物、医药和工业合成的重要中间体,不仅在蛋白质功能化和药物传递系统中发挥着重要作用,而且在橡胶硫化剂、农药和抗氧化剂的生产中广泛应用.在传统合成策略中,有毒或昂贵的试剂通常被用于硫醇的偶联,且该过程存在反应条件苛刻、选择性低和反应时间长等问题.相比之下,光催化技术能够通过S-S偶联,将硫醇选择性地转化为二硫化物同时产氢,构建一种由光催化析氢和选择性有机合成相结合的光氧化还原体系.该双功能光催化反应体系能够充分利用光生电子和空穴的能量,同时获得绿色的清洁燃料和高价值的精细化学品,从而满足经济和社会可持续发展的目标.本文采用简便的水热法和原位沉积法成功合成了PdS助催化剂修饰的ZnIn_2S_4复合光催化剂.在可见光照射下,二元PdS-ZnIn_2S_4复合材料可以高效地催化硫醇进行选择性脱氢偶联,充分利用高能电子和空穴,同时获得清洁的氢能源以及增值的二硫化物.研究表明, PdS作为一种高效的氧化型助催化剂,不仅可以有效地从ZnIn_2S_4半导体中捕获光生空穴,促进光生载流子的分离和转移,而且能作为硫醇氧化的活性反应位点,从而显著提高ZnIn_2S_4的光催化性能.3%PdS-ZnIn_2S_4复合材料具备最佳的光催化活性,其双(4-甲氧基苯基)二硫化物和氢气的产量分别是ZnIn_2S_4的8.4和10.7倍.此外,二硫化物在该光催化反应过程中表现出优异的选择性(>99.0%).循环活性实验以及催化反应前后的X射线光电子能谱结果表明,二元PdS-ZnIn_2S_4复合材料具有良好的光催化稳定性.PdS-ZnIn_2S_4可以有效地催化多种具有不同取代基的硫醇的脱氢偶联,生成相应的S-S目标产物,说明了二元PdS-ZnIn_2S_4复合材料在光催化硫醇转化中的普适性.此外,原位傅里叶变换红外光谱揭示了反应物在催化剂表面的动态变化.通过电子顺磁共振光谱技术对反应过程中的自由基中间体进行原位监测,确认了硫中心自由基是硫醇氧化偶联过程中关键的自由基中间体.综上,本文为以绿色可持续的方式同时获得清洁太阳能燃料和具有高附加值的化学品提供了参考.
Keyword ：
二硫化物合成 二硫化物合成 光氧化还原反应 光氧化还原反应 析氢 析氢 氧化型助催化剂 氧化型助催化剂 硫铟锌 硫铟锌
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| GB/T 7714 | 李晓娟 , 祁明雨 , 李婧宇 et al. PdS修饰的ZnIn_2S_4复合材料用于可见光催化硫醇偶联制备二硫化物同时产氢（英文） [J]. | Chinese Journal of Catalysis , 2023 , 51 (08) : 55-65 . |
| MLA | 李晓娟 et al. "PdS修饰的ZnIn_2S_4复合材料用于可见光催化硫醇偶联制备二硫化物同时产氢（英文）" . | Chinese Journal of Catalysis 51 . 08 (2023) : 55-65 . |
| APA | 李晓娟 , 祁明雨 , 李婧宇 , 谭昌龙 , 唐紫蓉 , 徐艺军 . PdS修饰的ZnIn_2S_4复合材料用于可见光催化硫醇偶联制备二硫化物同时产氢（英文） . | Chinese Journal of Catalysis , 2023 , 51 (08) , 55-65 . |
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Abstract ：
Photocatalytic epoxide alcoholysis through C-O bond cleavage and formation has emerged as an alternative to synthesizing anti-tumoral pharmaceuticals and fine chemicals. However, the lack of crucial evidence to interpret the interaction between reactants and photocatalyst surface makes it challenging for photocatalytic epoxide alcoholysis with both high activity and regioselectivity. In this work, we report the hierarchical ZnIn2S4@CdS photocatalyst for epoxide alcoholysis with high regioselectivity nearly 100 %. Mechanistic studies unveil that the precise activation switch on exposed Zn acid sites for C-O bond polarization and cleavage has a critical significance for achieving efficient photocatalytic performance. Furthermore, the establishment of Z-scheme heterojunction facilitates the interface charge separation and transfer. Remarkably, the underlying regioselective photocatalytic reaction pathway has been distinctly revealed.
Keyword ：
Epoxide Alcoholysis Epoxide Alcoholysis Hierarchical Structure Hierarchical Structure Photocatalysis Photocatalysis Regioselectivity Regioselectivity Vacancy Regulation Vacancy Regulation
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| GB/T 7714 | Li, Jing-Yu , Tan, Chang-Long , Qi, Ming-Yu et al. Exposed Zinc Sites on Hybrid ZnIn2S4@CdS Nanocages for Efficient Regioselective Photocatalytic Epoxide Alcoholysis [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
| MLA | Li, Jing-Yu et al. "Exposed Zinc Sites on Hybrid ZnIn2S4@CdS Nanocages for Efficient Regioselective Photocatalytic Epoxide Alcoholysis" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 22 (2023) . |
| APA | Li, Jing-Yu , Tan, Chang-Long , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Exposed Zinc Sites on Hybrid ZnIn2S4@CdS Nanocages for Efficient Regioselective Photocatalytic Epoxide Alcoholysis . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (22) . |
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Ternary composites of reduced graphene oxide (GR)-CdS-Pd have been successfully synthesized via solvothermal and photodeposition methods for photocatalytic selective conversion of benzyl alcohol (BA) coupled with hydrogen (H 2 ) production, which exhibit significantly improved photoactivity and selectivity than bare CdS. Mechanistic studies unveil that the cooperative effect of the close interface contact and matched energy level alignment between electrical conducting GR nanosheets (NSs) and CdS nanoparticles (NPs) in GR-CdS-Pd composite not only benefits the separation and transfer of photogenerated carriers but also improves the photocorrosion resistance of CdS. The photodeposited Pd NPs further promote the photogenerated charge separation and accelerate the formation of intermediate products ( alpha-hydroxybenzyl radicals), thereby contributing to enhanced conversion of BA. This work would facilitate the rational design of GR as cocatalyst to construct an efficient and stable CdS-based composite photocatalyst for cooperative coupling of fine chemical synthesis and H 2 evolution. (c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Keyword ：
Alcohol oxidation Alcohol oxidation Coupling photoredox reaction Coupling photoredox reaction Hydrogen Hydrogen Pd Pd Reduced graphene oxide Reduced graphene oxide
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| GB/T 7714 | Sun, Ming -Hui , Qi, Ming-Yu , Tan, Chang-Long et al. Interfacial engineering of CdS for efficient coupling photoredox [J]. | CHINESE CHEMICAL LETTERS , 2023 , 34 (7) . |
| MLA | Sun, Ming -Hui et al. "Interfacial engineering of CdS for efficient coupling photoredox" . | CHINESE CHEMICAL LETTERS 34 . 7 (2023) . |
| APA | Sun, Ming -Hui , Qi, Ming-Yu , Tan, Chang-Long , Tang, Zi-Rong , Xu, Yi-Jun . Interfacial engineering of CdS for efficient coupling photoredox . | CHINESE CHEMICAL LETTERS , 2023 , 34 (7) . |
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Semiconductor quantum dots have been emerging as one of the most ideal materials for artificial photosynthesis. Here, we report the assembled ZnS-CdS hybrid heterostructure for efficient coupling cooperative redox catalysis toward the oxidation of 1-phenylethanol to acetophenone/2,3-diphenyl-2,3butanediol (pinacol) integrated with the reduction of protons to H2. The strong interaction and typical type-I band-position alignment between CdS quantum dots and ZnS quantum dots result in efficient separation and transfer of electron-hole pairs, thus distinctly enhancing the coupled photocatalyzed-redox activity and stability. The optimal ZnS-CdS hybrid also delivers a superior performance for various aromatic alcohol coupling photoredox reaction, and the ratio of electrons and holes consumed in such redox reaction is close to 1.0, indicating a high atom economy of cooperative coupling catalysis. In addition, by recycling the scattered light in the near field of a SiO2 sphere, the SiOzsupported ZnS-CdS (denoted as ZnS-CdS/SiO2) catalyst can further achieve a 3.5-fold higher yield than ZnS-CdS hybrid. Mechanistic research clarifies that the oxidation of 1-phenylethanol proceeds through the pivotal radical intermediates of center dot C(CH3)(OH)Ph. This work is expected to promote the rational design of semiconductor quantum dots-based heterostructured catalysts for coupling photoredox catalysis in organic synthesis and clean fuels production.
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| GB/T 7714 | Zhang, Lin-Xing , Qi, Ming-Yu , Tang, Zi-Rong et al. Heterostructure-Engineered Semiconductor Quantum Dots toward Photocatalyzed-Redox Cooperative Coupling Reaction [J]. | RESEARCH , 2023 , 6 . |
| MLA | Zhang, Lin-Xing et al. "Heterostructure-Engineered Semiconductor Quantum Dots toward Photocatalyzed-Redox Cooperative Coupling Reaction" . | RESEARCH 6 (2023) . |
| APA | Zhang, Lin-Xing , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Heterostructure-Engineered Semiconductor Quantum Dots toward Photocatalyzed-Redox Cooperative Coupling Reaction . | RESEARCH , 2023 , 6 . |
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The precise design of the charge carrier relay channel and active sites of semiconductor-based photocatalysts is highly crucial for target selective photoredox synthesis. In this context, we report an atomic-level catalyst design strategy based on depositing Pt single atoms (SAs) onto Cu-doped ultrathin cadmium sulfide nanosheets (CdS/Cu/Pt) to enable an optimized band structure, a directional charge transfer channel, and favorable catalytic sites for efficient and selective dehydrocoupling of amines to imines and hydrogen (H2). The Cu dopant acts as a unique electron bridge to construct a directional Cu-Pt electron transfer channel with the assistance of atomically dispersed Pt sites, thereby promoting charge separation and transfer kinetics. The introduction of Pt SAs not only facilitates the H2 generation by decreasing the overpotential of proton reduction but also improves the selectivity of imines synthesis because the weak adsorption of imines on Pt SAs prevents further hydrogenation of imines to secondary amines. This work is anticipated to inspire a further rational design of semiconductor-based photocatalysts with atomic precision for the coproduction of renewable fuels and value-added fine chemicals.
Keyword ：
atomic-level electrontransfer channel atomic-level electrontransfer channel Cu doping Cu doping H-2 evolution H-2 evolution Pt single atoms Pt single atoms selective imines synthesis selective imines synthesis
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| GB/T 7714 | Li, Yue-Hua , Wang, Yin-Feng , Li, Jing-Yu et al. Selective Imines Synthesis by Designing an Atomic-Level Cu-Pt Electron Transfer Channel over CdS Nanosheets [J]. | ACS CATALYSIS , 2023 , 14 (2) : 657-669 . |
| MLA | Li, Yue-Hua et al. "Selective Imines Synthesis by Designing an Atomic-Level Cu-Pt Electron Transfer Channel over CdS Nanosheets" . | ACS CATALYSIS 14 . 2 (2023) : 657-669 . |
| APA | Li, Yue-Hua , Wang, Yin-Feng , Li, Jing-Yu , Qi, Ming-Yu , Conte, Marco , Tang, Zi-Rong et al. Selective Imines Synthesis by Designing an Atomic-Level Cu-Pt Electron Transfer Channel over CdS Nanosheets . | ACS CATALYSIS , 2023 , 14 (2) , 657-669 . |
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Semiconductor-based artificial photoredox-catalyzed organic synthesis offers a promising and green opportunity to harness solar energy for green organic chemistry. However, the precise manipulation of product selectivity over semiconductor-based photocatalysts for selective organic synthesis remains challenging. In this work, we report the rational preparation and application of two kinds of cocatalyst, (RuS2 or Cu2S)-decorated monolayer ZnIn2S4, for the selective dehydrocoupling of aromatic amines into tunable C=N coupled imines or C-N coupled secondary amines, respectively, under visible light irradiation. The presence of the RuS2 or Cu2S cocatalyst not only facilitates the charge carrier separation and migration owing to the well-matched energy band structure, but also maneuvers the interfacial charge transfer routes for the selectivity switching between C=N and C-N product formation. This work would inspire the rational design of ingenious semiconductor-based composites toward selective modulation in heterogeneous photocatalytic organic synthesis.
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| GB/T 7714 | Zheng, Jian-Hui , Qi, Ming-Yu , Tang, Zi-Rong et al. Manipulating selective amine transformation pathways via cocatalyst-modified monolayer ZnIn2S4 photocatalysts [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2023 , 11 (8) : 4013-4019 . |
| MLA | Zheng, Jian-Hui et al. "Manipulating selective amine transformation pathways via cocatalyst-modified monolayer ZnIn2S4 photocatalysts" . | JOURNAL OF MATERIALS CHEMISTRY A 11 . 8 (2023) : 4013-4019 . |
| APA | Zheng, Jian-Hui , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Manipulating selective amine transformation pathways via cocatalyst-modified monolayer ZnIn2S4 photocatalysts . | JOURNAL OF MATERIALS CHEMISTRY A , 2023 , 11 (8) , 4013-4019 . |
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Semiconductor quantum dots (QDs), as a newfashioned light-absorbing material with great promise in artificial photosystems, generally exhibit attractive photoactivity and selectivity in organic photoredox transformation thanks to their tunable redox potential, high-efficiency light harvesting capability, and high extinction coefficient in the visible region. Utilizing QDs as a versatile platform to convert organic compounds into value-added feedstocks provides an effective way to alleviate energy and chemical feedstock supply problems. In this review, we concisely summarize the basic principles of photocatalytic organic conversions over semiconductor QDs and the effects of grain size, surface active sites and ligands on their catalytic performance. Then, we highlight the recent progress of QDs enabling multifarious photocatalytic organic transformations, including nitroaromatic reduction, selective alcohol oxidation, sulfide oxidation, C-H functionalization and so on. In the end, we discuss the current challenges and future prospects in further developing efficient semiconductor QD-based photocatalysts toward photoredox-catalyzed organic conversion.
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| GB/T 7714 | Wu, Hui-Li , Qi, Ming-Yu , Tang, Zi-Rong et al. Semiconductor quantum dots: a versatile platform for photoredox organic transformation [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2023 , 11 (7) : 3262-3280 . |
| MLA | Wu, Hui-Li et al. "Semiconductor quantum dots: a versatile platform for photoredox organic transformation" . | JOURNAL OF MATERIALS CHEMISTRY A 11 . 7 (2023) : 3262-3280 . |
| APA | Wu, Hui-Li , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Semiconductor quantum dots: a versatile platform for photoredox organic transformation . | JOURNAL OF MATERIALS CHEMISTRY A , 2023 , 11 (7) , 3262-3280 . |
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