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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 , 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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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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Visible light induced oxidative C-C and C-N coupling provides a milder alternative to the current synthetic strategies. However, the photochemical C-C coupling of benzylamine and chromoselective C-C/C-N conversion are not widely reported. Herein, we demonstrate that the introduction of indium vacancies in ZnIn2S4 improves the catalytic activity for C-C coupling of benzylamine and imparts a strong chromoselectivity for C-C or C-N coupled products. A high C-C selectivity of ∼80% is achieved with a benzylamine conversion of ∼80%. Mechanistic studies unveil the switchable reaction routes between kinetically favored C-C coupling and thermodynamically favored C-N coupling under specific illumination conditions. © 2024 American Chemical Society.
Keyword ：
C−C bond formation C−C bond formation C−N bond formation C−N bond formation defect engineering defect engineering photocatalytic photocatalytic wavelength selective wavelength selective ZnIn2S4 ZnIn2S4
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| GB/T 7714 | Leng, X. , Zhou, X. , Ma, L. et al. Wavelength-Selective C-C and C-N Bond Formation via Defect-Engineered ZnIn2S4 [J]. | ACS Catalysis , 2024 , 14 (15) : 11554-11563 . |
| MLA | Leng, X. et al. "Wavelength-Selective C-C and C-N Bond Formation via Defect-Engineered ZnIn2S4" . | ACS Catalysis 14 . 15 (2024) : 11554-11563 . |
| APA | Leng, X. , Zhou, X. , Ma, L. , Du, Y. , Peng, O. , Chen, Z. et al. Wavelength-Selective C-C and C-N Bond Formation via Defect-Engineered ZnIn2S4 . | ACS Catalysis , 2024 , 14 (15) , 11554-11563 . |
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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 H2 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 H2 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 H2 evolution. © 2024 American Chemical Society.
Keyword ：
alcohols oxidation alcohols oxidation H2 production H2 production lactones synthesis lactones synthesis MXene MXene quantum dots quantum dots
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| GB/T 7714 | Qi, M.-Y. , Xiao, W.-Y. , Conte, M. 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, M.-Y. 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, M.-Y. , Xiao, W.-Y. , Conte, M. , Tang, Z.-R. , Xu, Y.-J. . 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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The scarcity of strategies to finely modulate the interface assembly between MXene and semiconductors often restricts their full potential for photocatalysis. Herein, resorting to the cetyltrimethylammonium bromide (CTAB) surfactant intercalation effect, we report the rational synthesis of hierarchical seaurchin-like CdS-Ti3C2T x MXene-CTAB (CdS-T-C) ensembles to modulate the interface and structure of MXene-semiconductor heterojunctions for significantly boosted photoredox coupling catalysis. The ternary CdS-T-C exhibits markedly enhanced activity toward visible light photoreforming of benzyl alcohol (BA) to benzaldehyde (BAD) and H2 cooperatively, as compared to bare CdS and conventional CdS-Ti3C2T x MXene (CdS-T) that suffer from serious MXene restacking with obvious electronic and optical property attenuation. Mechanistic studies reveal that the CTAB interfacial intercalation alleviates the restacking of Ti3C2T x , thus weakening the light shielding effect while promoting the charge transport and surface activity of MXene. This work demonstrates an appealing strategy to regulate the interfacial cross-coupling configuration of MXene-semiconductor composites for efficient solar-to-chemical conversion.
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| GB/T 7714 | Zhang, Hanbo , Si, Tingting , Yuan, Lan et al. Surfactant-Assisted Assembly of Hierarchical CdS-Ti3C2T x MXene toward Enhanced Cooperative Photoredox Catalysis [J]. | ACS MATERIALS LETTERS , 2024 , 7 (1) : 257-264 . |
| MLA | Zhang, Hanbo et al. "Surfactant-Assisted Assembly of Hierarchical CdS-Ti3C2T x MXene toward Enhanced Cooperative Photoredox Catalysis" . | ACS MATERIALS LETTERS 7 . 1 (2024) : 257-264 . |
| APA | Zhang, Hanbo , Si, Tingting , Yuan, Lan , Han, Chuang , Xu, Yi-Jun . Surfactant-Assisted Assembly of Hierarchical CdS-Ti3C2T x MXene toward Enhanced Cooperative Photoredox Catalysis . | ACS MATERIALS LETTERS , 2024 , 7 (1) , 257-264 . |
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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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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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