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学者姓名：唐紫蓉
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Abstract ：
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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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. © 2024 Elsevier B.V.
Keyword ：
Amines Amines Electronic structure Electronic structure Electron spin resonance spectroscopy Electron spin resonance spectroscopy Image enhancement Image enhancement Manganese compounds Manganese compounds Nickel Nickel Paramagnetic resonance Paramagnetic resonance Reaction intermediates Reaction intermediates Semiconductor alloys Semiconductor alloys Semiconductor doping Semiconductor doping
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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. © 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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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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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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Simultaneous utilization of photogenerated electrons and holes within a photoredox system enables effective hydrogen (H2) production and organic synthesis, aligning with eco-friendly chemistry principles and current energy challenges. Here, we report the preparation and application of cocatalyst MoS2 decorated CdS (MoS2-CdS) composites for the photoredox-mediated C-N coupling of amines to imines and H2 generation under visible light illumination. The H2 and N-benzylidenebenzylamine yields for the optimal MoS2-CdS are 28.9 and 15.0 times higher than those of bare CdS, respectively. Mechanism studies reveal that the enhanced photocatalytic activity results from the MoS2 acting as an electron sink, which accelerates the separation and migration of photogenerated charge carriers. Additionally, the pH(center dot CH)NH2 intermediates are found to play a pivotal role in the dehydrogenative coupling of benzylamine. Furthermore, the MoS2-CdS composites exhibit universal applicability in the conversion of various aromatic amines into corresponding imines integrated with H2 evolution.
Keyword ：
Amines oxidation Amines oxidation Hydrogen production Hydrogen production MoS 2 cocatalyst MoS 2 cocatalyst Photoredox dual reaction Photoredox dual reaction
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| GB/T 7714 | Shao, Xin-Ni , Wang, Yin-Feng , Qi, Ming-Yu et al. MoS2 decorated CdS composite catalyst for photoredox-mediated C-N coupling of amines to imines and hydrogen production [J]. | MOLECULAR CATALYSIS , 2024 , 557 . |
| MLA | Shao, Xin-Ni et al. "MoS2 decorated CdS composite catalyst for photoredox-mediated C-N coupling of amines to imines and hydrogen production" . | MOLECULAR CATALYSIS 557 (2024) . |
| APA | Shao, Xin-Ni , Wang, Yin-Feng , Qi, Ming-Yu , Tang, Zi-Rong . MoS2 decorated CdS composite catalyst for photoredox-mediated C-N coupling of amines to imines and hydrogen production . | MOLECULAR CATALYSIS , 2024 , 557 . |
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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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Solar-driven carbon dioxide (CO2) reduction integrated with selective organic synthesis proposes a sustainable paradigm to achieve carbon neutrality concomitantly with value-added fuels and chemicals production. Here, we report the synergistic coupling reaction of CO2 reduction and amines oxidation to syngas and secondary amines over Cu doped CdS quantum dots (Cu:CdS QDs) under visible light. This system is compatible with various amines to afford the corresponding secondary amines with outstanding selectivity. Notably, the syngas CO/H2 ratio can be obtained in a window from 1:2 to 2:1 by altering the Cu doping content. Mechanistic studies unveil that doped Cu not only improves the charge separation efficiency, but also serves as active sites for the adsorption/activation of CO2, thus adjusting the syngas ratio. This work is envisaged to enable a viable strategy for the rational design of transition metal-doped semiconductor QDs toward the co-production of syngas and high-value chemicals in one photoredox cycle.
Keyword ：
C-N coupling C-N coupling CO2 reduction CO2 reduction Cu doping Cu doping Redox photocatalysis Redox photocatalysis Syngas production Syngas production
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| GB/T 7714 | Gao, Long-Hui , Xiao, Wei-Yun , Qi, Ming-Yu et al. Photoredox-catalyzed coupling of CO2 reduction and amines oxidation by Cu doped CdS quantum dots [J]. | MOLECULAR CATALYSIS , 2024 , 554 . |
| MLA | Gao, Long-Hui et al. "Photoredox-catalyzed coupling of CO2 reduction and amines oxidation by Cu doped CdS quantum dots" . | MOLECULAR CATALYSIS 554 (2024) . |
| APA | Gao, Long-Hui , Xiao, Wei-Yun , Qi, Ming-Yu , Li, Jing-Yu , Tan, Chang-Long , Tang, Zi-Rong . Photoredox-catalyzed coupling of CO2 reduction and amines oxidation by Cu doped CdS quantum dots . | MOLECULAR CATALYSIS , 2024 , 554 . |
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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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