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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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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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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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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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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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Metal nanoclusters (NCs), characterized by the merits of unique stacking structure, quantum confinement effect, and abundant active centers, have garnered enormous attention in photocatalysis. However, inherent instability, fast carrier recombination, and complex interfacial charge transport mechanism of metal NCs remain the core challenges, thereby refraining their wide-spread applications in heterogeneous photocatalysis. In this work, tailor-made L-glutathione reduced (GSH) protected Au22(GSH)18 NCs are anchored on the transition metal chalcogenide (CdS) for constructing CdS/Au22(GSH)18 heterostructure artificial photosystems by a self-assembly approach. The CdS/Au22(GSH)18 nanocomposite exhibits the improved visible-light-driven photoactivity for reduction of aromatic nitro compounds compared with single counterpart. This is mainly attributed to the pivotal role of Au22(GSH)18 NCs as visible-light-absorbing antennas and the suitable energy level alignment between Au22(GSH)18 NCs and CdS, considerably improving the charge migration and separation efficiency and thereby enhancing the photocatalytic performances. Our investigation provides enriched information on the charge transport mechanism of metal NCs in photoredox organic transformation.
Keyword ：
CdS CdS Charge transport Charge transport Metal nanoclusters Metal nanoclusters Nanocomposite Nanocomposite Selective reduction Selective reduction
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| GB/T 7714 | Xie, Huawei , Zhang, Junyi , Xiao, Guangcan et al. Photosensitization of transition metal chalcogenide with metal nanoclusters for boosted photocatalysis [J]. | MOLECULAR CATALYSIS , 2025 , 581 . |
| MLA | Xie, Huawei et al. "Photosensitization of transition metal chalcogenide with metal nanoclusters for boosted photocatalysis" . | MOLECULAR CATALYSIS 581 (2025) . |
| APA | Xie, Huawei , Zhang, Junyi , Xiao, Guangcan , Xiao, Fang-Xing . Photosensitization of transition metal chalcogenide with metal nanoclusters for boosted photocatalysis . | MOLECULAR CATALYSIS , 2025 , 581 . |
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The core factors dictating the photocatalysis efficiency are predominantly centered on controllable modulation of anisotropic spatial charge transfer/separation and regulating vectorial charge transport pathways. Nonetheless, the sluggish charge transport kinetics and incapacity of precisely tuning interfacial charge flow at the nanoscale level are still the primary dilemma. Herein, we conceptually demonstrate the elaborate design of a cascade charge transport chain over transition metal chalcogenide-insulating polymer-cocatalyst (TIC) photosystems via a progressive self-assembly strategy. The intermediate ultrathin non-conjugated insulating polymer layer, i.e., poly(diallyl-dimethylammonium chloride) (PDDA), functions as the interfacial electron relay medium, and simultaneously, outermost co-catalysts serve as the terminal "electron reservoirs", synergistically contributing to the charge transport cascade pathway and substantially boosting the interfacial charge separation. We found that the insulating polymer mediated unidirectional charge transfer cascade is universal for a large variety of metal or non-metal reducing co-catalysts (Au, Ag, Pt, Ni, Co, Cu, NiSe2, CoSe2, and CuSe). More intriguingly, such peculiar charge flow characteristics endow the self-assembled TIC photosystems with versatile visible-light-driven photoredox catalysis towards photocatalytic hydrogen generation, anaerobic selective organic transformation, and CO2-to-fuel conversion. Our work would provide new inspiration for smartly mediating spatial vectorial charge transport towards emerging solar energy conversion. The core factors dictating the photocatalysis efficiency are predominantly centered on controllable modulation of anisotropic spatial charge transfer/separation and regulating vectorial charge transport pathways.
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| GB/T 7714 | Yan, Xian , Dong, Jun-Hao , Zheng, Jing-Ying et al. Customizing precise, tunable, and universal cascade charge transfer chains towards versatile photoredox catalysis [J]. | CHEMICAL SCIENCE , 2024 , 15 (8) : 2898-2913 . |
| MLA | Yan, Xian et al. "Customizing precise, tunable, and universal cascade charge transfer chains towards versatile photoredox catalysis" . | CHEMICAL SCIENCE 15 . 8 (2024) : 2898-2913 . |
| APA | Yan, Xian , Dong, Jun-Hao , Zheng, Jing-Ying , Wu, Yue , Xiao, Fang-Xing . Customizing precise, tunable, and universal cascade charge transfer chains towards versatile photoredox catalysis . | CHEMICAL SCIENCE , 2024 , 15 (8) , 2898-2913 . |
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Benefiting from their excellent light-capturing ability, suitable energy band structure and abundant active sites, transition metal chalcogenides (TMCs) have been attracting widespread attention in heterogeneous photocatalysis. Nonetheless, TMCs still suffer from sluggish charge transfer kinetics, a rapid charge recombination rate and poor stability, rendering the construction of high-performance artificial photosystems challenging. Here, a ternary dumbbell-shaped CdS/MoS2/CuS heterostructure with spatially separated catalytically active sites has been elaborately designed. In such a heterostructured nanoarchitecture, MoS2 clusters, selectively grown on both ends of the CdS nanowires (NWs), act as terminal electron collectors, while CuS nanolayers, coated on the sidewalls of CdS NWs through ion exchange, form a P-N heterojunction with the CdS NW framework, which accelerates the migration of holes from CdS to CuS, effectively suppressing the oxidation of sulfide ions and improving the stability of CdS NWs. The well-defined dumbbell-shaped CdS/MoS2/CuS ternary heterostructure provides a structural basis for spatially precise regulation of the charge migration pathway, where photogenerated electrons and holes directionally migrate to the MoS2 and CuS catalytic sites, respectively, ultimately achieving efficient carrier separation and significantly enhancing photoactivity for both photocatalytic hydrogen generation and selective organic transformation under visible light. Moreover, we have also ascertained that such ion exchange and interface configuration engineering strategies are universal. Our work features a simple yet efficient strategy for smartly designing multi-component heterostructures to precisely modulate spatially vectorial charge separation at the nanoscale for solar-to-hydrogen conversion. Dumbbell-shaped heterostructures are constructed through a progressive targeted modification strategy, and a charge transfer channel is carefully designed to enhance photocatalytic selective organic transformation.
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| GB/T 7714 | Su, Peng , Yan, Xian , Xiao, Fang-Xing . Customizing dumbbell-shaped heterostructured artificial photosystems steering versatile photoredox catalysis [J]. | CHEMICAL SCIENCE , 2024 , 15 (36) : 14778-14790 . |
| MLA | Su, Peng et al. "Customizing dumbbell-shaped heterostructured artificial photosystems steering versatile photoredox catalysis" . | CHEMICAL SCIENCE 15 . 36 (2024) : 14778-14790 . |
| APA | Su, Peng , Yan, Xian , Xiao, Fang-Xing . Customizing dumbbell-shaped heterostructured artificial photosystems steering versatile photoredox catalysis . | CHEMICAL SCIENCE , 2024 , 15 (36) , 14778-14790 . |
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Atomically precise metal nanoclusters (NCs) have garnered significant interest due to their unique atomic stacking structures, the effect of quantum confinement, and enriched active sites but suffer from thermal- or light-induced poor instability and self-aggregation, together with in situ self-conversion to conventional metal nanoparticles (NPs). How to effectively harness the generic detrimental self-transformation property of metal NCs has so far not garnered immense attention within the realm of catalysis. In this work, we develop a layer-by-layer assembly technology to accurately anchor metal NCs to the metal oxide matrix. Then, the anchoring of metal NCs to metal NPs is triggered by a simple thermal treatment that enables precise control over the interface structure, resulting in a hollow core-shell heterostructure with a metal core (Au, Ag) encapsulated by a metal oxide (CeO2, Fe2O3, SnO2) shell. Benefiting from the synergistic interplay between metal NPs and the metal oxide substrate, such self-assembled metal NPs@metal oxide heterostructures display excellent catalytic activities and stability in the reduction of aromatic nitro compounds. The detailed catalytic mechanism is elucidated. Our work offers fresh impetus for the judicious utilization of the inherent instability of metal NCs for catalytic selective organic transformation.
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| GB/T 7714 | Ning, Boyuan , He, Suhua , Lin, Xin et al. Interface Engineering: Enhanced Catalysis Through Precise Control of Metal Nanocluster Transformation [J]. | INORGANIC CHEMISTRY , 2024 , 63 (50) : 23742-23748 . |
| MLA | Ning, Boyuan et al. "Interface Engineering: Enhanced Catalysis Through Precise Control of Metal Nanocluster Transformation" . | INORGANIC CHEMISTRY 63 . 50 (2024) : 23742-23748 . |
| APA | Ning, Boyuan , He, Suhua , Lin, Xin , Xiao, Fang-Xing . Interface Engineering: Enhanced Catalysis Through Precise Control of Metal Nanocluster Transformation . | INORGANIC CHEMISTRY , 2024 , 63 (50) , 23742-23748 . |
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