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学者姓名：徐艺军
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Abstract ：
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 , 63 (38) . |
| MLA | Han, C. et al. "All-in-One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis" . | Angewandte Chemie - International Edition 63 . 38 (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 , 63 (38) . |
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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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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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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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Simultaneously utilizing photoinduced electrons and holes to direct splitting of thiols into value-added disulfides and clean hydrogen (H2) fuels conforms the development standards of green chemistry. Herein, a cobalt phos-phate (Co-Pi) and reduced graphene oxide (GR) modified CdS photocatalyst is synthesized and utilized for photocatalytic selective conversion of 4-methoxythiophenol (4-MTP) to bis(4-methoxyphenyl) disulfide (4-MPD) coupled with H2 evolution. In this dual-cocatalyst system, Co-Pi effectively captures and releases the holes from CdS through the chemical state change of Co to accelerate the surface thiols oxidation reaction, while GR is used as an electron collector and an active site for the proton reduction to H2. Consequently, the bifunctional GR-CdS-(Co-Pi) photocatalyst demonstrates significantly higher photoactivity than blank CdS. This work affords a new paradigm of incorporating dual-cocatalysts with semiconductor photocatalysts to efficiently take advantage of the photoinduced electrons and holes for photoredox-catalyzed cooperative coupling of organic transformation and H2 evolution.
Keyword ：
CdS CdS Cobalt phosphate Cobalt phosphate Coupling photoredox reaction Coupling photoredox reaction Disulfide Disulfide Hydrogen Hydrogen Reduced graphene oxide Reduced graphene oxide
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| GB/T 7714 | Sun, Ming -Hui , Qi, Ming -Yu , Tang, Zi-Rong et al. Dual cocatalysts decorated CdS nanoparticles for efficient dehydrocoupling of thiols into disulfides [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 321 . |
| MLA | Sun, Ming -Hui et al. "Dual cocatalysts decorated CdS nanoparticles for efficient dehydrocoupling of thiols into disulfides" . | APPLIED CATALYSIS B-ENVIRONMENTAL 321 (2023) . |
| APA | Sun, Ming -Hui , Qi, Ming -Yu , Tang, Zi-Rong , Xu, Yi-Jun . Dual cocatalysts decorated CdS nanoparticles for efficient dehydrocoupling of thiols into disulfides . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 321 . |
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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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Plastic waste pollution is becoming one of the most pressing environmental crises due to the large-scale production without satisfactory recycling schemes, especially with the outbreak of the COVID-19 pandemic in recent years. Upcycling of plastic waste into valuable chemicals powered by solar energy presents a substantially untapped opportunity to turn waste into treasure. In this review, the fundamental principles from plastic nonselective degradation to selective synthesis are first clarified. Then, we aim to outline the representative recent advances in photoredox-based catalytic plastic waste conversion. Particular emphasis is placed on the valorization of plastic waste regarding nonselective degradation versus selective synthesis. Finally, we present challenges and individual insights for further exploration of the plastic waste conversion domain. It is anticipated that this timely and critical review would provide an instructive direction and foresight on the selective conversion of plastics to valueadded chemical feedstocks, thus stimulating the development of a circular and sustainable plastic economy in the coming decades.
Keyword ：
nonselective degradation nonselective degradation photocatalysis photocatalysis plastic waste conversion plastic waste conversion selective synthesis selective synthesis upcycling value-added chemicals upcycling value-added chemicals
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| GB/T 7714 | Zhang, Yi , Qi, Ming-Yu , Tang, Zi-Rong et al. Photoredox-Catalyzed Plastic Waste Conversion: Nonselective Degradation versus Selective Synthesis [J]. | ACS CATALYSIS , 2023 , 13 (6) : 3575-3590 . |
| MLA | Zhang, Yi et al. "Photoredox-Catalyzed Plastic Waste Conversion: Nonselective Degradation versus Selective Synthesis" . | ACS CATALYSIS 13 . 6 (2023) : 3575-3590 . |
| APA | Zhang, Yi , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Photoredox-Catalyzed Plastic Waste Conversion: Nonselective Degradation versus Selective Synthesis . | ACS CATALYSIS , 2023 , 13 (6) , 3575-3590 . |
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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 ubiquity of solid-liquid interfaces in nature and the significant role of their atomic-scale structure in determining interfacial properties have led to intensive research. Particularly in electrocatalysis, however, a molecular-level picture that clearly describes the dynamic interfacial structures and organizations with their correlation to preferred reaction pathways in electrochemical reactions remains poorly understood. In this review, CO2 electroreduction reaction (CO2RR) is spatially and temporally understood as a result of intricate interactions at the interface, in which the interfacial features are highly relevant. We start with the discussion of current understandings and model development associated with the charged electrochemical interface as well as its dynamic landscape. We further highlight the interactive dynamics from the interfacial field, catalyst surface charges and various gradients in electrolyte and interfacial water structures at interfaces under CO2RR working conditions, with emphasis on the interfacial-structure dependence of catalytic reactivity/selectivity. Significantly, a probing energy-dependent "in situ characterization map" for dynamic interfaces based on various complementary in situ/operando techniques is proposed, aiming to present a comprehensive picture of interfacial electrocatalysis and to provide a more unified research framework. Moreover, recent milestones in both experimental and theoretical aspects to establish the correct profile of electrochemical interfaces are stressed. Finally, we present key scientific challenges with related perspectives toward future opportunities for this exciting frontier.
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| GB/T 7714 | Wang, Jiali , Tan, Hui-Ying , Qi, Ming-Yu et al. Spatially and temporally understanding dynamic solid-electrolyte interfaces in carbon dioxide electroreduction [J]. | CHEMICAL SOCIETY REVIEWS , 2023 , 52 (15) : 5013-5050 . |
| MLA | Wang, Jiali et al. "Spatially and temporally understanding dynamic solid-electrolyte interfaces in carbon dioxide electroreduction" . | CHEMICAL SOCIETY REVIEWS 52 . 15 (2023) : 5013-5050 . |
| APA | Wang, Jiali , Tan, Hui-Ying , Qi, Ming-Yu , Li, Jing-Yu , Tang, Zi-Rong , Suen, Nian-Tzu et al. Spatially and temporally understanding dynamic solid-electrolyte interfaces in carbon dioxide electroreduction . | CHEMICAL SOCIETY REVIEWS , 2023 , 52 (15) , 5013-5050 . |
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Constructing highly active photocatalysts with rich reactivesitesfor photofixation of CO2 with organic compounds implementsan environmentally friendly route for CO2 valorizationand carbon neutralization. Herein, we report the isolated cobalt (Co)single-atom (SA)-decorated two-dimensional (2D) single-layer ZnIn2S4 (ZIS) nanosheet composites (Co-(s)ZIS)with dual active centers of Co and Zn for CO2 fixationwith epoxides under visible light. The unique ensemble of Co-(s)ZIS optimizes light harvesting, promotes charge carrier separation,and enriches the bifunctional active sites for the efficient adsorptionand activation of the reactants of epoxides and CO2. Consequently,the Co-(s)ZIS exhibits significantly improved CO2-epoxide cycloaddition performance compared to bulk ZIS. In addition,the synergetic photoredox manner of simultaneously exploiting photogeneratedelectrons and holes efficiently facilitates the activation of CO2 and epoxides, thereby further reducing the energy barrierof CO2 fixation. This work not only provides a paradigmof rationally interfacial engineered SA-onto-2D semiconductors forCO(2) valorization but also highlights the structure-activityrelationship by the well-defined active sites in this SA-based hybridplatform.
Keyword ：
carbon dioxide anion radical carbon dioxide anion radical carbon dioxidephotofixation carbon dioxidephotofixation carbon dioxide valorization carbon dioxide valorization monolayered ZnIn2S4 monolayered ZnIn2S4 single-atom catalysis single-atom catalysis
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| GB/T 7714 | Tan, Chang-Long , Qi, Ming-Yu , Tang, Zi-Rong et al. Isolated Single-Atom Cobalt in the ZnIn2S4 Monolayer with Exposed Zn Sites for CO2 Photofixation [J]. | ACS CATALYSIS , 2023 , 13 (12) : 8317-8329 . |
| MLA | Tan, Chang-Long et al. "Isolated Single-Atom Cobalt in the ZnIn2S4 Monolayer with Exposed Zn Sites for CO2 Photofixation" . | ACS CATALYSIS 13 . 12 (2023) : 8317-8329 . |
| APA | Tan, Chang-Long , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Isolated Single-Atom Cobalt in the ZnIn2S4 Monolayer with Exposed Zn Sites for CO2 Photofixation . | ACS CATALYSIS , 2023 , 13 (12) , 8317-8329 . |
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