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学者姓名：肖方兴
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Abstract ：
Atomically precise alloy nanoclusters (NCs) represent an emerging sector of metal nanomaterials as a new generation of photosensitizers for light harvesting and conversion, owing to their distinctive atom-stacking pattern, quantum confinement effect, and enriched active sites. Despite the sporadic progress made in the past few years in constructing alloy NCs photosystems, photoinduced charge transfer characteristics and photocatalytic mechanisms of alloy NCs still remain elusive. In this work, we conceptually demonstrate the rational design of alloy NC (Au1-xAgx, Au1-xPtx, and Au1-xCux)/transition metal chalcogenide (TMCs) heterostructure photosystems via a ligand-triggered self-assembly strategy. The results signify that electrons photoexcited in alloy NCs can smoothly transport to the TMC substrate with the aid of an intermediate ultrathin organic molecule layer, while holes migrate in the opposite direction, promoting the charge separation and prolonging the charge lifetime. Benefitting from the advantageous charge migration, the self-assembled alloy NC/TMC heterostructures exhibit significantly enhanced photoactivity towards selective photoredox organic transformation including selective reduction of aromatic nitro compounds to amino derivatives and selective oxidation of aromatic alcohols to aldehydes under visible light. The predominant active species during the photoredox catalysis are determined, through which alloy NC-dominated photoredox mechanisms are elucidated. Our work provides new insights into the smart construction of atomically precise alloy NC hybrid photosystems, and more importantly, paves the way for regulating the spatially vectorial charge transfer over alloy NCs to achieve solar-to-chemical energy conversion.
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| GB/T 7714 | Zheng, Bing-Xiong , Yuan, Jiao-Nan , Su, Peng et al. Alloy nanocluster artificial photosystems steering photoredox organic transformation [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (7) : 4908-4920 . |
| MLA | Zheng, Bing-Xiong et al. "Alloy nanocluster artificial photosystems steering photoredox organic transformation" . | JOURNAL OF MATERIALS CHEMISTRY A 13 . 7 (2025) : 4908-4920 . |
| APA | Zheng, Bing-Xiong , Yuan, Jiao-Nan , Su, Peng , Yan, Xian , Chen, Qing , Yuan, Meng et al. Alloy nanocluster artificial photosystems steering photoredox organic transformation . | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (7) , 4908-4920 . |
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Solar-driven CO2 conversion to high-value-added chemical fuels has been deemed as an emerging way of alleviating deteriorating energy depletion and greenhouse effect. Nevertheless, precise modulation of spatial vectorial charge migration/separation in CO2 artificial photosystem remains challenging due predominantly to the ultrashort charge lifetime, sluggish charge transfer kinetics, and ultra-stable symmetry of CO2 molecules, rendering stimulation of CO2 adsorption, activation and reduction a grand challenge. Herein, we conceptually demonstrate the design of a novel semiconductor-insulator-cocatalyst charge tunneling photosystem via a layer-by-layer (LbL) assembly strategy, which involves progressive intercalation of dual ultrathin insulating polymer layers in-between layered double hydroxides (LDHs) and transition metal chalcogenide (TMC). It is demonstrated for the first time unleash that electron-hole pairs photoexcited over TMC can simultaneously tunnel through the insulating polymer interim layers, followed by holes trapping by terminal LDHs and directional electrons migration to the CO2 molecules absorbing on the polymers surface, synergistically boosting the charge separation and reinforcing the solar CO2 reduction. This work would open a shining frontier to strategically craft novel charge-tunneling artificial photosystems and benefit the fundamental understanding on the CO2 photoreduction technology toward solar energy conversion.
Keyword ：
charge tunneling charge tunneling insulating polymers insulating polymers layered double hydroxides layered double hydroxides photocatalytic CO2 reduction photocatalytic CO2 reduction transition metal chalcogenide transition metal chalcogenide
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| GB/T 7714 | Chen, Qing , Chen, Yi-Han , Zhu, Jun-Rong et al. Customizing Synchronous Charge Tunneling Photosystems Toward Solar CO2 Conversion [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (13) . |
| MLA | Chen, Qing et al. "Customizing Synchronous Charge Tunneling Photosystems Toward Solar CO2 Conversion" . | ADVANCED FUNCTIONAL MATERIALS 35 . 13 (2025) . |
| APA | Chen, Qing , Chen, Yi-Han , Zhu, Jun-Rong , Li, Zhuang-Yan , Xiao, Fang-Xing . Customizing Synchronous Charge Tunneling Photosystems Toward Solar CO2 Conversion . | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (13) . |
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Abstract ：
Atomically precise metal nanoclusters (NCs) emerge as a novel class of photosensitizers, distinguished by their discrete energy band structures and abundance of catalytically active sites; however, their broader adoption in heterogeneous photocatalysis remains hindered by the challenges of ultrashort carrier lifetimes, limited stability, and the complexity of charge transport regulation. In this work, we conceptually design the metal NCs photosensitized and graphene (GR)-encapsulated transition metal chalcogenide (TMC) (GR/metal NCs/TMCs) heterostructure via a cascade electrostatic self-assembly strategy. In this multilayer ternary heterostructure, metal NCs are integrated between TMCs and GR nanosheets, which act as photosensitizers for enhancing the light absorption of TMCs and meanwhile increase the carrier density of composite photosystem. The favorable interfacial charge transport between metal NCs and TMCs along with the advantageous electron-withdrawing capability of GR simultaneously boosts charge separation over metal NCs. Benefiting from such peculiar carrier transport characteristics, the self-assembled GR/metal NCs/TMCs heterostructure demonstrates remarkably boosted and stable photoactivities toward selective photoredox organic transformation, including photocatalytic anaerobic reduction of aromatic nitro compounds to amino derivatives and photocatalytic oxidation of aromatic alcohols to aldehydes under visible light. Furthermore, the mechanisms underlying the photocatalytic processes are elucidated with clarity. Our work affords a quintessential paradigm for customizing atomically precise metal NCs in engineered photosystems aimed at converting solar energy into chemical energy.
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| GB/T 7714 | Yan, Xian , Zheng, Bing-Xiong , Zhu, Jun-Rong et al. Spatially Confining Atomically Precise Metal Nanoclusters Steers Photoredox Organic Transformation [J]. | INORGANIC CHEMISTRY , 2025 , 64 (7) : 3572-3581 . |
| MLA | Yan, Xian et al. "Spatially Confining Atomically Precise Metal Nanoclusters Steers Photoredox Organic Transformation" . | INORGANIC CHEMISTRY 64 . 7 (2025) : 3572-3581 . |
| APA | Yan, Xian , Zheng, Bing-Xiong , Zhu, Jun-Rong , Li, Yu-Bing , Xiao, Fang-Xing . Spatially Confining Atomically Precise Metal Nanoclusters Steers Photoredox Organic Transformation . | INORGANIC CHEMISTRY , 2025 , 64 (7) , 3572-3581 . |
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Photocatalysis represents an emerging technology for solving the deteriorating energy crisis and environmental problems by directly harvesting green, renewable, and sustainable solar energy. Due to the maximum atomic utilization efficiency, tunable electronic structures and outstanding catalytic activities, single-atom catalysts (SACs) have emerged as promising candidates for photocatalysis. Although many reviews on single-atom photocatalysis have been reported in the past few years, a comprehensive review devoted to specifically elucidating the generic characteristics of SACs in heterogeneous photocatalysis has so far not yet appeared. In this review, we summarize the latest progress in SACs mediated photocatalysis paired with diverse photocatalytic mechanisms from a fresh insight. Firstly, we elucidate the various synthetic strategies for SACs with a focus on the advantages and disadvantages of each approach. Subsequently, state-of-the-art characterization methods utilized for unleashing the fine structures of single-atom photocatalysts have been concisely overviewed. Furthermore, widespread applications of SACs in diverse photocatalytic redox reactions are comprehensively introduced. Finally, the remaining challenges and future opportunities in this booming research field are outlooked for guiding the rational design of robust, stable, and high-performance SACs. Our review could inspire sparkling ideas on how to smartly utilize single atoms for crafting high-efficiency artificial photosystems towards solar energy conversion.
Keyword ：
Characterization Characterization Photocatalysis Photocatalysis Single-atom Single-atom Solar energy conversion Solar energy conversion Synthesis Synthesis
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| GB/T 7714 | Chen, Jia-Qi , Wu, Yue , Xiao, Fang-Xing . Single-atom photocatalysis: A new frontier toward solar energy conversion [J]. | MOLECULAR CATALYSIS , 2025 , 575 . |
| MLA | Chen, Jia-Qi et al. "Single-atom photocatalysis: A new frontier toward solar energy conversion" . | MOLECULAR CATALYSIS 575 (2025) . |
| APA | Chen, Jia-Qi , Wu, Yue , Xiao, Fang-Xing . Single-atom photocatalysis: A new frontier toward solar energy conversion . | MOLECULAR CATALYSIS , 2025 , 575 . |
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Abstract ：
Atomically precise metal nanoclusters (NCs) stand out within metal nanomaterials due to the distinctive atomic stacking configuration, discrete energy band, quantum confinement effect, and enriched catalytic centers, positioning them as promising substitutes for conventional photosensitizers in solar energy absorption and utilization. However, the light-induced poor stability and ultrashort carrier lifetime of metal NCs as well as the difficulties in modulating charge migration collectively constrain their potential applications in photoredox catalysis. In this work, we conceptually construct the metal NC artificial photosystems by electrostatically self-assembling l-glutathione (GSH)-capped Au-25(GSH)(18) NCs onto transition metal chalcogenide (TMC) substrates (CdS, Zn0.5Cd0.5S, and ZnIn2S4) at ambient conditions. Benefiting from the advantageous photosensitization effect of Au-25@(GSH)(18) NCs, these self-assembled TMCs/Au-25@(GSH)(18) NC heterostructures exhibit significantly enhanced photocatalytic hydrogen production performance (lambda > 420 nm). This universal photoactivity enhancement is predominantly attributed to the suitable energy level alignment between Au-25@(GSH)(18) NCs and TMCs, which considerably enhances the interfacial charge transfer and effectively extends the carrier lifetime. In addition, the photocatalytic mechanism is determined. This work would spark continued interest in crafting diverse atomically precise metal NC photocatalytic systems toward solar-to-hydrogen energy conversion.
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| GB/T 7714 | Li, Yu-Bing , Xiao, Fang-Xing . Atomically Precise Metal Nanocluster-Mediated Solar Hydrogen Production [J]. | INORGANIC CHEMISTRY , 2025 , 64 (7) : 3608-3615 . |
| MLA | Li, Yu-Bing et al. "Atomically Precise Metal Nanocluster-Mediated Solar Hydrogen Production" . | INORGANIC CHEMISTRY 64 . 7 (2025) : 3608-3615 . |
| APA | Li, Yu-Bing , Xiao, Fang-Xing . Atomically Precise Metal Nanocluster-Mediated Solar Hydrogen Production . | INORGANIC CHEMISTRY , 2025 , 64 (7) , 3608-3615 . |
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Magic-sized nanoclusters (MSCs) have been attracting enduring interest by virtue of the quantum confinement effect, discrete energy band structure, and enriched catalytic active sites. Nevertheless, up to date, exploration of MSCs artificial photosystems and fine-tuning of spatial vectorial charge transfer in photoredox catalysis have so far been scarcely reported. Hence, we employed a facile and easily accessible layer-by-layer (LbL) assembly strategy to highly ordered, alternately, and periodically deposit oppositely charged tailor-made transition metal chalcogenides (TMCs) MSCs and non-conjugated polymer (NCP) building blocks on the MO substrate, resulting in the MO/(NCP-TMCs MSCs)n multilayer heterostructures. It is affirmed that the ultra-thin NCP uniformly intercalated at the interface of every TMCs MSCs layer fosters the unidirectional electron flow from TMCs MSCs to MO substrate with the assistance of NCP, and moreover the multilayered interface configuration benefits the establishment of cascade tandem charge transfer route, synergistically giving rise to the significantly enhanced charge separation and boosted solar water oxidation performances of MO/(TMCs MSCs-NCP)n heterostructure under simulated solar light irradiation. Our work elucidates the specific roles of NCP and MSCs as charge relay mediators and photosensitizers, affording a quintessential paradigm to rationally regulate the photocarrier transport and separation over MSCs for solar energy conversion.
Keyword ：
charge transport charge transport layer-by-layer assembly layer-by-layer assembly magic-sized nanoclusters magic-sized nanoclusters non-conjugated polymer non-conjugated polymer photoelectrochemical water splitting photoelectrochemical water splitting
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| GB/T 7714 | Li, Zhuang-Yan , Yuan, Meng , Xiao, Fang-Xing . Magic-Sized Nanoclusters-Induced Cascade Tandem Charge Transfer for Solar Water Oxidation [J]. | SMALL , 2025 , 21 (13) . |
| MLA | Li, Zhuang-Yan et al. "Magic-Sized Nanoclusters-Induced Cascade Tandem Charge Transfer for Solar Water Oxidation" . | SMALL 21 . 13 (2025) . |
| APA | Li, Zhuang-Yan , Yuan, Meng , Xiao, Fang-Xing . Magic-Sized Nanoclusters-Induced Cascade Tandem Charge Transfer for Solar Water Oxidation . | SMALL , 2025 , 21 (13) . |
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Atomically precise metal nanoclusters (NCs) have been deemed a new generation of photosensitizers for light harvesting on account of their quantum confinement effect, peculiar atom-stacking mode, and enriched catalytic active sites. Nonetheless, to date, precise charge modulation over metal NCs has still been challenging considering their ultra-short carrier lifetime and poor stability. In this work, we conceptually demonstrate the integration of metal NCs with MXene in transition metal chalcogenide (TMC) photosystems via a progressive, exquisite, and elegant interface design to trigger tunable, precise and high-efficiency charge motion over metal NCs, stimulating a directional carrier transport pathway. In this customized ternary heterostructured photosystem, metal NCs function as light-harvesting antennas, MXene serves as a terminal electron reservoir, and the TMC substrate provides suitable energy level alignment for retracting photocarriers of metal NCs, giving rise to a spatial cascade charge transport route and markedly boosting charge separation efficiency. The interface configuration and energy level alignment engineering synergistically contribute to the considerably enhanced visible-light-driven photocatalytic CO2-to-CO reduction performance of the metal NCs/TMCs/MXene heterostructure. The intermediate active species during the photocatalytic CO2 reduction are unambiguously determined, based on which the photocatalytic mechanism is elucidated. Our work will provide an inspiring idea to bridge the gap between atomically precise metal NCs and MXene in terms of controllable charge migration for solar-to-fuel conversion. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Cai, Y.-S. , Chen, J.-Q. , Su, P. et al. Atomically precise metal nanoclusters combine with MXene towards solar CO2 conversion [J]. | Chemical Science , 2024 , 15 (33) : 13495-13505 . |
| MLA | Cai, Y.-S. et al. "Atomically precise metal nanoclusters combine with MXene towards solar CO2 conversion" . | Chemical Science 15 . 33 (2024) : 13495-13505 . |
| APA | Cai, Y.-S. , Chen, J.-Q. , Su, P. , Yan, X. , Chen, Q. , Wu, Y. et al. Atomically precise metal nanoclusters combine with MXene towards solar CO2 conversion . | Chemical Science , 2024 , 15 (33) , 13495-13505 . |
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Abstract ：
Atomically precise metal nanoclusters (NCs), distinguished by their unique electronic structures, quantum confinement effects, and enriched active sites, have been considered highly promising photosensitizers for light harvesting and conversion. However, the ultra-short carrier lifetime and poor stability of metal NCs remarkably retard their widespread applications in photocatalysis. In this study, we achieved the modulation of carrier separation over metal NCs via heterostructure engineering by smartly integrating atomically precise silver NCs [Ag16(GSH)9] with transition metal chalcogenides (TMCs). The favorable energy level alignment between metal NCs and TMCs facilitates the electron transfer from the metal NCs to the TMCs, leading to a significantly prolonged charge lifetime and considerably enhanced photoactivity toward the selective reduction of nitro compounds to amino derivatives under visible light. The photocatalytic mechanism of these composite photosystems is elucidated herein. This work advances our fundamental understanding of charge transfer mechanisms over atomically precise metal NCs for solar energy conversion. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Zhang, J. , Zhan, L. , Ning, B. et al. Photoredox catalysis enabled by atomically precise metal nanoclusters [J]. | Inorganic Chemistry Frontiers , 2024 , 11 (20) : 6970-6980 . |
| MLA | Zhang, J. et al. "Photoredox catalysis enabled by atomically precise metal nanoclusters" . | Inorganic Chemistry Frontiers 11 . 20 (2024) : 6970-6980 . |
| APA | Zhang, J. , Zhan, L. , Ning, B. , He, Y. , Xiao, G. , Chen, Z. et al. Photoredox catalysis enabled by atomically precise metal nanoclusters . | Inorganic Chemistry Frontiers , 2024 , 11 (20) , 6970-6980 . |
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Magic-sized nanoclusters (MSCs) have recently deemed as a novel and crucial sector of nanomaterials on account of their large absorption coefficient for light harvesting, peculiar quantum confinement effect, and abundant active. Nevertheless, precise control of photoinduced charge carriers over MSCs has so far not yet been reported because of the ultra-short carrier lifetime and intrinsic instability of MSCs, which renders the complexity of MSCs photosystems with photoredox mechanism remaining blank. Herein, we for the first time conceptually demonstrate the grafting of amino-containing organic molecular onto the L-cysteine (L-Cys) ligand of CdSe@L-Cys MSCs as charge transport mediator, and the amino functional group acts as an efficient electron-withdrawing trap, which markedly boosts the charge separation and prolongs the charge lifetime of CdSe@L-Cys MSCs, resulting in the significantly improved photocatalytic hydrogen generation performances under visible light irradiation along with favorable stability. Our work will provide sparking ideas for fine tuning of photoinduced charge separation and transfer over transition metal chalcogenides MSCs photosystems for solar-to-hydrogen energy conversion. © 2024 Elsevier Inc.
Keyword ：
CdSe MSCs CdSe MSCs Charge transport Charge transport Organic molecular Organic molecular Photocatalytic hydrogen generation Photocatalytic hydrogen generation
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| GB/T 7714 | Yuan, M. , Yan, X. , Yuan, J.-N. et al. Maneuvering magic-sized transition metal chalcogenides nanoclusters for Solar-to-Hydrogen conversion [J]. | Journal of Catalysis , 2024 , 437 . |
| MLA | Yuan, M. et al. "Maneuvering magic-sized transition metal chalcogenides nanoclusters for Solar-to-Hydrogen conversion" . | Journal of Catalysis 437 (2024) . |
| APA | Yuan, M. , Yan, X. , Yuan, J.-N. , Su, P. , Chen, Q. , Xiao, F.-X. . Maneuvering magic-sized transition metal chalcogenides nanoclusters for Solar-to-Hydrogen conversion . | Journal of Catalysis , 2024 , 437 . |
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Solar-driven syngas generation by CO2 reduction provides a sustainable strategy to produce renewable fossil fuels. Nevertheless, this promising approach often suffers from tough CO2 activation, sluggish reaction kinetics and complex selectivity. Herein, we exquisitely constructed spatially directional charge transport channel over two-dimensional transition metal chalcogenide (TMC)-based heterostructure via a facile and universal electrostatic self-assembly method. Tailor-made positively charged non-conjugated insulating polymer of poly(diallyl-dimethyl-ammonium chloride) (PDDA) and negatively charged graphene oxide (GO) precursor as building blocks are controllably anchored on the TMC substrate, by which ultrathin PDDA layer is intercalated at the interface of GO and TMC. We ascertain that, in this customized sandwiched heterostructures, PDDA interim layer functions as an electron-relaying mediator, whilst graphene (GR) obtained from in-situ GO reduction during the photocatalytic reaction serves as a terminal electron-trapping reservoir, synergistically facilitating the spatially vectorial charge separation/migration over TMC, thus endowing the TMC/PDDA/GR heterostructures with conspicuously enhanced visible-light-driven photoactivity toward CO2-to-syngas conversion. Our work would inspire judicious ideas for finely modulating charge transfer over polymer-mediated photosystems and benefit our fundamental understanding of solar CO2 conversion. © 2024 Elsevier B.V.
Keyword ：
Charge transfer Charge transfer Co-catalyst Co-catalyst Non-conjugated polymer Non-conjugated polymer Photocatalytic CO2-to-syngas reduction Photocatalytic CO2-to-syngas reduction Transition metal chalcogenide Transition metal chalcogenide
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| GB/T 7714 | Chen, Q. , Li, J.-L. , Mo, Q.-L. et al. Photocarrier relay modulating solar CO2-to-syngas conversion [J]. | Chemical Engineering Journal , 2024 , 497 . |
| MLA | Chen, Q. et al. "Photocarrier relay modulating solar CO2-to-syngas conversion" . | Chemical Engineering Journal 497 (2024) . |
| APA | Chen, Q. , Li, J.-L. , Mo, Q.-L. , Xiao, F.-X. . Photocarrier relay modulating solar CO2-to-syngas conversion . | Chemical Engineering Journal , 2024 , 497 . |
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