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学者姓名：唐紫蓉
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Abstract ：
Cooperatively integrating CO2 reduction half-reaction with selective organic oxidation half-reaction presents an attractive opportunity to simultaneously utilize photogenerated holes and electrons to realize carbon neutrality and the production of value-added chemicals. Herein, we report the cooperative photoredox catalysis of tunable and efficient CO2 reduction to syngas paired with 4-methoxythiophenol (4-MTP) oxidation to bis(4methoxyphenyl) disulfide (4-MPD) over hybrid CdSe/CdS quantum dots (QDs). The strategy of constructing CdSe/CdS composites not only facilitates the efficiency of photoinduced carrier separation and transfer, improving the photoredox activity of two half-reactions, but also enhances CO2 activation, modulating the syngas CO/H2 ratio varying from 1:4-5:4. Mechanistic studies have revealed that 4-MTP is oxidized by holes located in CdS to generate hydrogen protons and sulfur-centered radicals, and then these radicals pair with each other to form 4-MPD with high selectivity, while the electrons in CdSe interact with protons and CO2 for syngas production. Furthermore, the feasibility of applying CdSe/CdS QDs to the cooperative photoredox catalysis of thiols with different substituents integrated with CO2 into corresponding disulfides and syngas has been demonstrated. This work envisages the development of QDs-based heterostructure catalysts for highly efficient photocatalytic co-production of syngas and value-added organic chemicals.
Keyword ：
CdSe/CdS QDs CdSe/CdS QDs CO 2 reduction CO 2 reduction Disulfides Disulfides Syngas Syngas Thiols oxidation Thiols oxidation
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| GB/T 7714 | Zhang, Yi , Gao, Long-Hui , Qi, Ming-Yu et al. Cooperative photoredox coupling of CO2 reduction with thiols oxidation by hybrid CdSe/CdS semiconductor quantum dots [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 367 . |
| MLA | Zhang, Yi et al. "Cooperative photoredox coupling of CO2 reduction with thiols oxidation by hybrid CdSe/CdS semiconductor quantum dots" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 367 (2025) . |
| APA | Zhang, Yi , Gao, Long-Hui , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Cooperative photoredox coupling of CO2 reduction with thiols oxidation by hybrid CdSe/CdS semiconductor quantum dots . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 367 . |
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Reducing the size of metal nanoparticle (NP) cocatalyst down to single-atom level to improve photocatalytic efficiency is inevitably accompanied by the changes of its coordination environment, geometric configuration, electronic structure and active site. Thus, the construction of single metal atom (SA) photocatalyst is not necessarily a panacea for activity improvement toward target catalytic reactions. Herein, we report a critical and benchmark comparison in a reasonable framework of ZnIn2S4/Pt NP (ZIS/Pt NP) and ZnIn2S4/Pt SA (ZIS/Pt SA) towards photocatalytic hydrogen (H2) evolution, aiming to demonstrate which is better between Pt NP and Pt SA as cocatalyst in boosting photoredox catalysis. Mechanism study proves that the higher charge separation/transfer and weaker H* adsorption strength over ZIS/Pt NP than ZIS/Pt SA promote the more effective reduction of protons to H2, leading to the higher activity of ZIS/Pt NP than ZIS/Pt SA. Our work is expected to timely inspire the critical and rational thinking on the function and intrinsic mechanism of SA and NP cocatalysts in enhancing the photoredox catalysis performance. © 2024 Elsevier B.V.
Keyword ：
Charge transfer Charge transfer Photoredox catalysis Photoredox catalysis Proton adsorption Proton adsorption Pt nanoparticle Pt nanoparticle Pt single atom Pt single atom
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| GB/T 7714 | Li, Y.-H. , Huang, Z.-S. , Qi, M.-Y. et al. Benchmark comparison study on metal single atom versus metal nanoparticle in photoredox catalysis: Which is better? [J]. | Molecular Catalysis , 2024 , 567 . |
| MLA | Li, Y.-H. et al. "Benchmark comparison study on metal single atom versus metal nanoparticle in photoredox catalysis: Which is better?" . | Molecular Catalysis 567 (2024) . |
| APA | Li, Y.-H. , Huang, Z.-S. , Qi, M.-Y. , Tang, Z.-R. . Benchmark comparison study on metal single atom versus metal nanoparticle in photoredox catalysis: Which is better? . | Molecular Catalysis , 2024 , 567 . |
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Utilizing semiconductor quantum dots (QDs) to construct a bifunctional reaction system of coupling CO2 reduction with biomass valorization represents an appealing approach for the production of useable fuels and value-added chemicals. Herein, we present an efficient cooperative photocatalytic process for simultaneously achieving the reduction of CO2 to syngas and the oxidation of biomass-derived furfuryl alcohol to furfural and hydrofuroin over SiO2-supported CdSe/CdS QDs (CdSe/CdS-SiO2). The type-II band alignment in CdSe/CdS core/shell heterostructures enables effective charge separation and interfacial charge migration concurrently. By further assembly onto a spherical SiO2 support, the optimized CdSe/CdS-SiO2 composite exhibits remarkably enhanced activities for syngas and furfural/hydrofuroin production, which are 2.3 and 3.5 times higher than those of binary CdSe/CdS core/shell QDs, and 90.4 and 18.5 times higher than those of bare CdSe QDs, along with good stability. In particular, by altering the thickness of the CdS shell, the syngas CO/H2 ratio can be precisely modulated within a wide range (1.6 to 7.1), which serves as crucial feedstock for the production of liquid fuels. This work is expected to develop core/shell QD-based photocatalysts for versatile and available photoredox-catalyzed reaction systems that integrate CO2 valorization with biomass upgrading. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Zhang, L.-X. , Tang, Z.-R. , Qi, M.-Y. et al. Engineering semiconductor quantum dots for co-upcycling of CO2 and biomass-derived alcohol [J]. | Journal of Materials Chemistry A , 2024 , 12 (30) : 19029-19038 . |
| MLA | Zhang, L.-X. et al. "Engineering semiconductor quantum dots for co-upcycling of CO2 and biomass-derived alcohol" . | Journal of Materials Chemistry A 12 . 30 (2024) : 19029-19038 . |
| APA | Zhang, L.-X. , Tang, Z.-R. , Qi, M.-Y. , Xu, Y.-J. . Engineering semiconductor quantum dots for co-upcycling of CO2 and biomass-derived alcohol . | Journal of Materials Chemistry A , 2024 , 12 (30) , 19029-19038 . |
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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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Abstract ：
Reducing the size of metal nanoparticle (NP) cocatalyst down to single-atom level to improve photocatalytic efficiency is inevitably accompanied by the changes of its coordination environment, geometric configuration, electronic structure and active site. Thus, the construction of single metal atom (SA) photocatalyst is not necessarily a panacea for activity improvement toward target catalytic reactions. Herein, we report a critical and benchmark comparison in a reasonable framework of ZnIn2S4/Pt 2 S 4 /Pt NP (ZIS/Pt NP) and ZnIn2S4/Pt 2 S 4 /Pt SA (ZIS/Pt SA) towards photocatalytic hydrogen (H2) 2 ) evolution, aiming to demonstrate which is better between Pt NP and Pt SA as cocatalyst in boosting photoredox catalysis. Mechanism study proves that the higher charge separation/ transfer and weaker H* adsorption strength over ZIS/Pt NP than ZIS/Pt SA promote the more effective reduction of protons to H2, 2 , leading to the higher activity of ZIS/Pt NP than ZIS/Pt SA. Our work is expected to timely inspire the critical and rational thinking on the function and intrinsic mechanism of SA and NP cocatalysts in enhancing the photoredox catalysis performance.
Keyword ：
Charge transfer Charge transfer Photoredox catalysis Photoredox catalysis Proton adsorption Proton adsorption Pt nanoparticle Pt nanoparticle Pt single atom Pt single atom
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| GB/T 7714 | Li, Yue-Hua , Huang, Zhi-Sang , Qi, Ming-Yu et al. Benchmark comparison study on metal single atom versus metal nanoparticle in photoredox catalysis: Which is better? [J]. | MOLECULAR CATALYSIS , 2024 , 567 . |
| MLA | Li, Yue-Hua et al. "Benchmark comparison study on metal single atom versus metal nanoparticle in photoredox catalysis: Which is better?" . | MOLECULAR CATALYSIS 567 (2024) . |
| APA | Li, Yue-Hua , Huang, Zhi-Sang , Qi, Ming-Yu , Tang, Zi-Rong . Benchmark comparison study on metal single atom versus metal nanoparticle in photoredox catalysis: Which is better? . | MOLECULAR CATALYSIS , 2024 , 567 . |
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Photocatalytic selective organic transformations coupled with hydrogen (H2) generation under anaerobic conditions is a promising alternative to tackle the challenges of global energy scarcity and green synthesis. In this work, we report the synthesis and application of Ni doped Mn0.25Cd0.75S (MCS-Ni) composites for efficient selective dehydrocoupling of amines into imines and H2. The optimal MCS-Ni composite displays markedly enhanced activities for imines and H2 generation, which are 7.9 and 11.5 times as high as those of pristine MCS, respectively. The Ni doping modulates the electronic structure of MCS, which improves the light-harvesting abilities and inhibits the recombination of photo-generated electron-hole pairs, thereby remarkably improving the photocatalytic performance of the MCS-Ni composite. Furthermore, the electron paramagnetic resonance (EPR) technique reveals that carbon centered radicals are the critical intermediates in the amine oxidation reaction. This work is promising to provide inspiration towards the rational construction of metal doped semiconductor composite photocatalysts with effective utilization of photo-generated electrons and holes for the coproduction of clean H2 fuel and high-value added chemicals in a collaborative photoredox reaction.
Keyword ：
Hydrogen evolution Hydrogen evolution Imines synthesis Imines synthesis Mn0.25Cd0.75S Mn0.25Cd0.75S Ni doping Ni doping Photoredox reaction Photoredox reaction
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| GB/T 7714 | Li, Xiao-Juan , Wan, Hai-Tao , Qi, Ming-Yu et al. Photocatalytic imines synthesis integrated with H2 evolution over Ni doped Mn0.25Cd0.75S catalyst [J]. | MOLECULAR CATALYSIS , 2024 , 564 . |
| MLA | Li, Xiao-Juan et al. "Photocatalytic imines synthesis integrated with H2 evolution over Ni doped Mn0.25Cd0.75S catalyst" . | MOLECULAR CATALYSIS 564 (2024) . |
| APA | Li, Xiao-Juan , Wan, Hai-Tao , Qi, Ming-Yu , Tan, Chang-Long , Tang, Zi-Rong . Photocatalytic imines synthesis integrated with H2 evolution over Ni doped Mn0.25Cd0.75S catalyst . | MOLECULAR CATALYSIS , 2024 , 564 . |
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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. We present a bimetallic design of Ag nanoparticles (NPs) and Pd single atoms (SAs) on ZnO for the cascade photocatalytic CH4 conversion toward C2H4 with the highest production rate compared with previous works. The synergistic effect of Ag NPs and Pd SAs 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. image
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, Yin-Feng , Qi, Ming-Yu , Conte, Marco 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, Yin-Feng 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, Yin-Feng , Qi, Ming-Yu , Conte, Marco , Tang, Zi-Rong , Xu, Yi-Jun . 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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Integrating selective organic transformation and hydrogen (H2) evolution in one photoredox reaction system is one of the most sustainable and promising approaches to efficiently produce solar fuels and chemicals by simultaneously utilizing photogenerated electrons and holes. Herein, through the cation-exchange engineering method, the nanoleaf-like Pd/CdS composites are gingerly fabricated for visible-light-driven receptor-free dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to 3,4-dihydroisoquinoline (DHIQ) and H2 under ambient conditions. The optimized electronic structure endows Pd/CdS with a narrow band gap and suitable energy band positions, thus facilitating the light harvesting as well as the separation and transfer of photoexcited charge carriers. Consequently, the Pd/CdS exhibits significantly improved photoredox activity compared to bare CdS. In-situ Fourier-transform infrared spectroscopy and electron paramagnetic resonance spectroscopy track the progression of reaction intermediates during such a dual-functional photoredox-catalyzed system, revealing that the carbon-centered radical is the key reaction intermediate in this reaction process. It is anticipated that this work would guide the rational utilization of CdS-based materials to enable simultaneous photochemical coupling of organic transformation and H2 evolution.
Keyword ：
4-Dihydroisoquinoline production 4-Dihydroisoquinoline production CdS-based materials CdS-based materials H 2 evolution H 2 evolution Pd doping Pd doping Redox coupling photocatalysis Redox coupling photocatalysis
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| GB/T 7714 | Chen, Yu , Qi, Ming-Yu , Tang, Zi-Rong . Photoredox-promoted co-production of 3,4-dihydroisoquinoline and H2 over Pd-doped leaf-like CdS catalyst [J]. | MOLECULAR CATALYSIS , 2024 , 561 . |
| MLA | Chen, Yu et al. "Photoredox-promoted co-production of 3,4-dihydroisoquinoline and H2 over Pd-doped leaf-like CdS catalyst" . | MOLECULAR CATALYSIS 561 (2024) . |
| APA | Chen, Yu , Qi, Ming-Yu , Tang, Zi-Rong . Photoredox-promoted co-production of 3,4-dihydroisoquinoline and H2 over Pd-doped leaf-like CdS catalyst . | MOLECULAR CATALYSIS , 2024 , 561 . |
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Semiconductor-based photocatalysis has evolved over the past decade into a prevalent approach for alcohol oxidation to afford the corresponding carbonyl compounds or C-C/C-O coupled products. Nonetheless, photocatalytic oxidative lactonization of diols to lactones still significantly lags behind, even though lactones represent a class of ring moieties with excellent biological activities. In this work, we present the high-performance visible-light-mediated lactonization of diols to lactones and H-2 over the Ti3C2Tx MXene-supported CdS quantum dots (QDs) with Ni decoration (Ni/CdS/Ti3C2Tx ). Ti3C2Tx acts as a two-dimensional platform for immobilizing CdS to promote the separation and migration of charge carriers, while concomitantly the Cd2+ confinement effect of Ti3C2Tx significantly retards the hole-induced photocorrosion of CdS. The unique modifications of atomically dispersed Ni species are either incorporated as Ni clusters in CdS to accelerate H-2 evolution, or anchored as a Ni single atom on Ti3C2Tx for the efficient adsorption and cyclization of diols. The optimized Ni/CdS/Ti3C2Tx exhibits remarkably enhanced activity for lactone synthesis, which is 80.4 times higher than that of blank CdS, along with excellent selectivity and high durability. This work brings a conceptual idea to overcome the well-known intrinsic drawback of photoinduced decomposition in semiconductor-based photocatalysts and offers a generic and robust strategy of utilizing atomically dispersed cocatalyst as active sites for efficient and robust photoredox lactones synthesis and H-2 evolution.
Keyword ：
alcohols oxidation alcohols oxidation H-2 production H-2 production lactones synthesis lactones synthesis MXene MXene quantum dots quantum dots
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| GB/T 7714 | Qi, Ming-Yu , Xiao, Wei-Yun , Conte, Marco et al. Interfacial Synergy of Ni Single Atom/Clusters and MXene Enabling Semiconductor Quantum Dots Based Superior Photoredox Catalysis [J]. | ACS CATALYSIS , 2024 , 15 (1) : 129-138 . |
| MLA | Qi, Ming-Yu et al. "Interfacial Synergy of Ni Single Atom/Clusters and MXene Enabling Semiconductor Quantum Dots Based Superior Photoredox Catalysis" . | ACS CATALYSIS 15 . 1 (2024) : 129-138 . |
| APA | Qi, Ming-Yu , Xiao, Wei-Yun , Conte, Marco , Tang, Zi-Rong , Xu, Yi-Jun . Interfacial Synergy of Ni Single Atom/Clusters and MXene Enabling Semiconductor Quantum Dots Based Superior Photoredox Catalysis . | ACS CATALYSIS , 2024 , 15 (1) , 129-138 . |
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Solar-driven CO2 reduction combined with plastic waste valorization presents a versatile approach to simultaneously reset misaligned hydrocarbon resources and achieve a carbon-neutral cycle. Herein, we demonstrate a co-upcycling heterogeneous photoredox catalysis for efficient CO2 reduction to tunable syngas, integrated with polyethylene terephthalate (PET) plastic conversion for accessing acetate, over the spherical band-gap-engineered Zn x Cd1-x S catalyst. The key to steering the syngas H2/CO rate is to modulate the conduction band bottom potentials of the Zn x Cd1-x S photocatalysts by altering the Zn/Cd ratio, which results in syngas H2/CO production over a wide range. Moreover, controlled variations in the molar ratio of Zn/Cd regulate the electron-hole separation capability, thereby endowing Zn0.8Cd0.2S with the optimum syngas and acetate production rates. The underlying mechanistic origin of such a redox reaction involving CO2-assisted PET plastic conversion has been systematically investigated. This win-win cooperative photoredox catalysis offers a tantalizing possibility for co-upcycling of CO2 and PET into value-added feedstocks.
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| GB/T 7714 | Zhang, Yi , Qi, Ming-Yu , Conte, Marco et al. Efficient Photoredox Co-Upcycling of CO2 and Plastic Waste by Band-Gap-Engineered Zn x Cd1-x S Catalyst [J]. | ACS MATERIALS LETTERS , 2024 , 7 (1) : 359-367 . |
| MLA | Zhang, Yi et al. "Efficient Photoredox Co-Upcycling of CO2 and Plastic Waste by Band-Gap-Engineered Zn x Cd1-x S Catalyst" . | ACS MATERIALS LETTERS 7 . 1 (2024) : 359-367 . |
| APA | Zhang, Yi , Qi, Ming-Yu , Conte, Marco , Tang, Zi-Rong , Xu, Yi-Jun . Efficient Photoredox Co-Upcycling of CO2 and Plastic Waste by Band-Gap-Engineered Zn x Cd1-x S Catalyst . | ACS MATERIALS LETTERS , 2024 , 7 (1) , 359-367 . |
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