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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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Switchable divergent organic transformations represent a straightforward but challenging method to synthesize structurally varied compounds starting from the same set of raw materials. Herein, we report the divergent dehydrocoupling of thiols into tunable disulfides/thioethers and H2 in response to the visible or ultraviolet (UV) light, over CdS quantum dots. Regulating the irradiation wavelength allows disulfides and thioethers to be synthesized in moderate to high yields with good functional group tolerance. Mechanistic studies reveal that thiols are oxidized to produce sulfur-centered radicals by photogenerated holes under visible light irradiation, which then undergo S-S coupling to form disulfides. While under UV light irradiation, the cleavage of C-S bonds in thiols occurs readily to afford aryl radicals, which interact with sulfur-centered radicals, undergoing C-S coupling to obtain thioethers. This work is expected to open an avenue of light-controlled switch to maneuver a radical conversion route for divergent synthesis of value-added fine chemicals.
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| GB/T 7714 | Qi, Ming-Yu , Shao, Xin-Ni , Tang, Zi-Rong et al. Light-Controlled Switch for Divergent Coupling of Thiols to Disulfides/Thioethers over CdS Quantum Dots [J]. | ACS MATERIALS LETTERS , 2025 , 7 (4) : 1533-1539 . |
| MLA | Qi, Ming-Yu et al. "Light-Controlled Switch for Divergent Coupling of Thiols to Disulfides/Thioethers over CdS Quantum Dots" . | ACS MATERIALS LETTERS 7 . 4 (2025) : 1533-1539 . |
| APA | Qi, Ming-Yu , Shao, Xin-Ni , Tang, Zi-Rong , Xu, Yi-Jun . Light-Controlled Switch for Divergent Coupling of Thiols to Disulfides/Thioethers over CdS Quantum Dots . | ACS MATERIALS LETTERS , 2025 , 7 (4) , 1533-1539 . |
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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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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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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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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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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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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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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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Photo-driven cross-coupling of o-arylenediamines and alcohols has emerged as an alternative for the synthesis of bio-active benzimidazoles. However, tackling the key problem related to efficient adsorption and activation of both coupling partners over photocatalysts towards activity enhancement remains a challenge. Here, we demonstrate an efficient interface synergy strategy by coupling exposed oxygen vacancies (VO) and Pd Lewis acid sites for benzimidazole and hydrogen (H2) coproduction over Pd-loaded TiO2 nanospheres with the highest photoredox activity compared to previous works so far. The results show that the introduction of VO optimizes the energy band structure and supplies coordinatively unsaturated sites for adsorbing and activating ethanol molecules, affording acetaldehyde active intermediates. Pd acts as a Lewis acid site, enhancing the adsorption of alkaline amine molecules via Lewis acid-base pair interactions and driving the condensation process. Furthermore, VO and Pd synergistically promote interfacial charge transfer and separation. This work offers new insightful guidance for the rational design of semiconductor-based photocatalysts with interface synergy at the molecular level towards the high-performance coproduction of renewable fuels and value-added feedstocks. We propose a highly efficient interface synergy strategy that integrates exposed VO sites with surface Pd Lewis acid sites to ensure effective adsorption and activation of both coupling partners, o-arylenediamines and alcohols, with the synergistic interaction between VO and Pd enhancing interfacial charge transfer, thereby achieving the highest performance so far in the field of photoredox mediated benzimidazole synthesis. image
Keyword ：
benzimidazoles synthesis benzimidazoles synthesis defect defect hydrogen evolution hydrogen evolution interface synergy interface synergy photoredox catalysis photoredox catalysis
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| GB/T 7714 | Huang, Zhi-Sang , Wang, Yin-Feng , Qi, Ming-Yu et al. Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (47) . |
| MLA | Huang, Zhi-Sang et al. "Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 47 (2024) . |
| APA | Huang, Zhi-Sang , Wang, Yin-Feng , Qi, Ming-Yu , Conte, Marco , Tang, Zi-Rong , Xu, Yi-Jun . Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (47) . |
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