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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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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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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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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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Atomically precise metal nanoclusters (NCs) have been deemed as a new generation of metal nanomaterials because of their characteristic atomic stacking fashion, quantum confinement effect, and multitude of active sites. The discrete molecular-like energy band structure of metal NCs endows them with photosensitization capability for light harvesting and conversion. However, applications of metal NCs in photoelectrocatalysis are limited by the ultrafast charge recombination and unfavorable stability, impeding the construction of metal NC-based photosystems. In this work, we elaborately crafted multilayered metal oxide (MO)/(metal NCs/insulating polymer)(n) photoanodes by a facile layer-by-layer (LbL) assembly technique. In these well-defined heterostructured photoanodes, glutathione (GSH)-wrapped metal NCs (Ag-x@GSH, Ag-9@GSH(6), Ag-16@GSH(9), and Ag-31@GSH(19)) and an insulating poly(allylamine hydrochloride) (PAH) layer are alternately deposited on the MO substrate in a highly ordered integration mode. We found that photoelectrons of metal NCs can be tunneled into the MO substrate via the intermediate ultrathin insulating polymer layer by stimulating the tandem charge transfer route, thus facilitating charge separation and boosting photoelectrochemical water oxidation performances. Our work would open a new frontier for judiciously regulating directional charge transport over atomically precise metal NCs for solar-to-hydrogen conversion.
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| GB/T 7714 | Chen, Qing , Xiao, Yang , Xiao, Fang-Xing . Crafting Insulating Polymer Mediated and Atomically Precise Metal Nanoclusters Photosensitized Photosystems Towards Solar Water Oxidization [J]. | INORGANIC CHEMISTRY , 2024 , 63 (2) : 1471-1479 . |
| MLA | Chen, Qing et al. "Crafting Insulating Polymer Mediated and Atomically Precise Metal Nanoclusters Photosensitized Photosystems Towards Solar Water Oxidization" . | INORGANIC CHEMISTRY 63 . 2 (2024) : 1471-1479 . |
| APA | Chen, Qing , Xiao, Yang , Xiao, Fang-Xing . Crafting Insulating Polymer Mediated and Atomically Precise Metal Nanoclusters Photosensitized Photosystems Towards Solar Water Oxidization . | INORGANIC CHEMISTRY , 2024 , 63 (2) , 1471-1479 . |
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Quantum dots (QDs) colloidal nanocrystals are attracting enduring interest by scientific communities for solar energy conversion due to generic physicochemical merits including substantial light absorption coefficient, quantum confinement effect, enriched catalytically active sites, and tunable electronic structure. However, photo-induced charge carriers of QDs suffer from ultra-short charge lifespan and poor stability, rendering controllable vectorial charge modulation and customizing robust and stable QDs artificial photosystems challenging. Herein, tailor-made oppositely charged transition metal chalcogenides quantum dots (TMCs QDs) and MXene quantum dots (MQDs) are judiciously harnessed as the building blocks for electrostatic layer-by-layer assembly buildup on the metal oxides (MOs) framework. In these exquisitely designed LbL assembles MOs/(TMCs QDs/MQDs)n heterostructured photoanodes, TMCs QDs layer acts as light-harvesting antennas, and MQDs layer serves as electron-capturing mediator to relay cascade electrons from TMCs QDs to the MOs substrate, thereby yielding the spatially ordered tandem charge transport chain and contributing to the significantly boosted charge separation over TMCs QDs and solar water oxidation efficiency of MOs/(TMCs QDs/MQDs)n photoanodes. The relationship between interface configuration and charge transfer characteristics is unambiguously unlocked, by which photoelectrochemical mechanism is elucidated. This work would provide inspiring ideas for precisely mediating interfacial charge transfer pathways over QDs toward solar energy conversion. Cascade charge transfer channel is elaborately designed over transition metal chalcogenides quantum dots via a facile layer-by-layer assembly strategy for significantly boosted solar water oxidation. image
Keyword ：
CdSe quantum dots CdSe quantum dots charge transfer charge transfer metal oxide metal oxide MXene quantum dots MXene quantum dots photoelectrochemical water oxidation photoelectrochemical water oxidation
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| GB/T 7714 | Su, Peng , Li, Shen , Xiao, Fang-Xing . Precise Layer-by-Layer Assembly of Dual Quantum Dots Artificial Photosystems Enabling Solar Water Oxidation [J]. | SMALL , 2024 , 20 (35) . |
| MLA | Su, Peng et al. "Precise Layer-by-Layer Assembly of Dual Quantum Dots Artificial Photosystems Enabling Solar Water Oxidation" . | SMALL 20 . 35 (2024) . |
| APA | Su, Peng , Li, Shen , Xiao, Fang-Xing . Precise Layer-by-Layer Assembly of Dual Quantum Dots Artificial Photosystems Enabling Solar Water Oxidation . | SMALL , 2024 , 20 (35) . |
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Wholly distinct from conjugated polymers which are featured by generic charge transfer capability stemming from a conjugated molecular structure, solid nonconjugated polymers mediated charge transport has long been deemed as theoretically impossible because of the deficiency of pi electrons along the molecular skeleton, thereby retarding their widespread applications in solar energy conversion. Herein, we first conceptually unveil that intact encapsulation of metal oxides (e.g., TiO2, WO3, Fe2O3, and ZnO) with an ultrathin nonconjugated polyelectrolyte of branched polyethylenimine (BPEI) can unexpectedly accelerate the unidirectional charge transfer to the active sites and foster the defect generation, which contributes to the boosted charge separation and prolonged charge lifetime, ultimately resulting in considerably improved photoelectrochemical (PEC) water oxidation activities. The interfacial charge transport origins endowed by BPEI adornment are elucidated, which include acting as a hole-withdrawing mediator, promoting vacancy generation, and stimulating the directional charge flow route. We additionally ascertain that such charge transport characteristics of BPEI are universal. This work would unlock the charge transfer capability of nonconjugated polymers for solar water oxidation. The nonconjugated insulating polymer was utilized as a charge transport mediator for boosting charge migration and separation over metal oxides toward solar water oxidation.
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| GB/T 7714 | Hou, Shuo , Xie, Huawei , Xiao, Fang-Xing . Nonconjugated Polymers Enabled Solar Water Oxidation [J]. | INORGANIC CHEMISTRY , 2024 , 63 (19) : 8970-8976 . |
| MLA | Hou, Shuo et al. "Nonconjugated Polymers Enabled Solar Water Oxidation" . | INORGANIC CHEMISTRY 63 . 19 (2024) : 8970-8976 . |
| APA | Hou, Shuo , Xie, Huawei , Xiao, Fang-Xing . Nonconjugated Polymers Enabled Solar Water Oxidation . | INORGANIC CHEMISTRY , 2024 , 63 (19) , 8970-8976 . |
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固态非共轭聚合物由于缺乏沿分子链框架的离域π电子,长期以来被视为不具备转移能力的绝缘聚合物.因此,利用这类固态绝缘聚合物作为载体介质来刺激电荷转移或光氧化还原催化,在传统观念中被认为是不可行的.在异相光催化中,为了提升催化效率,常采用煅烧法去除非共轭绝缘聚合物,以暴露更多的活性位点,增强界面接触,从而减少界面电荷传输阻力并加速电荷转移.然而,由于聚合物的结构多样性和易获取性,深入探索非共轭绝缘聚合物在光催化中的电荷传输机制具有重要意义. 本文采用静电自组装策略,在常温下,将表面带负电荷的ZnIn2S4(ZIS)纳米片分散在带正电荷的固态绝缘支化聚乙烯亚胺(bPEI)的溶液中,通过两者间的静电作用力,制得具有高活性的、Zn空位调控的bPEI/ZIS光催化剂.X射线粉末衍射、拉曼光谱和紫外-可见漫反射光谱结果表明,bPEI的包覆并未改变ZIS的晶体结构和光学性质.高分辨透射电镜、原子力显微镜、X射线光电子能谱、傅里叶变换红外光谱和热重分析等结果证明了bPEI的成功包覆及显著的电子相互作用.采用瞬态吸收光谱、光致发光光谱、时间分辨光致发光光谱、光电流强度曲线和电化学阻抗曲线等光电化学测试,研究了催化剂的电荷传输路径和分离效率.电子顺磁共振谱和同步辐射吸收谱结果表明,采用15 mg mL-1的bPEI溶液包裹的ZIS(简称15bPEI/ZIS)中的Zn空位浓度显著高于ZIS,有利于延长载流子寿命.结合理论计算结果,推断bPEI的包裹可以优化Zn空位浓度,促进H2O和4-硝基苯胺的吸附.研究了析氧反应(OER)每步所需的自由能,结果表明,bPEI的存在有利于光生电子的转移.光催化还原硝基化合物性能评价结果表明,与ZIS相比,15bPEI/ZIS表现出更好的光催化活性和稳定性.在可见光下还原4-硝基苯胺体系中,15bPEI/ZIS的转化率可达91.58％,显著优于纯ZIS的16.33％.通过在体系中混合ZIS和bPEI制得15bPEI+ZIS,发现其光催化活性不如15bPEI/ZIS.同时,在惰性气氛下煅烧15bPEI/ZIS制得15bPEI/ZIS-200 ℃,相较于15bPEI/ZIS,15bPEI/ZIS-200 ℃的光催化性能没有显著提升,证明15bPEI/ZIS样品中ZIS和bPEI间界面结合紧密,存在强电子相互作用,有利于提升界面电荷传输效率.此外,在ZIS表面包裹多种含胺基的有机分子和聚合物催化剂,以及在ZIS和bPEI层间生长/刻蚀构建不同绝缘SiO2厚度的催化剂,通过光催化实验证实胺基官能团参与了界面电荷传输过程,并在光催化反应中抑制电荷复合并提供大量活性位点. 综上,本文从异相光催化的角度揭示了固态非共轭绝缘聚合物的电荷传输能力,并探讨了绝缘聚合物中单体片段对光催化性能的贡献作用.这种由绝缘聚合物包覆引起的协同缺陷工程、丰富的表面活性位点和加速的电荷流动动力学,共同显著提升了光催化活性.这一发现为利用固态绝缘聚合物操控电荷转移以实现太阳能转换提供新思路.
Keyword ：
光氧化还原催化 光氧化还原催化 电荷转移 电荷转移 绝缘聚合物 绝缘聚合物 聚电解质 聚电解质 自组装 自组装
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| GB/T 7714 | 莫乔铃 , 熊锐 , 董俊豪 et al. 绝缘聚合物调控光氧化还原催化的起源研究 [J]. | 催化学报 , 2024 , 63 (8) : 109-123 . |
| MLA | 莫乔铃 et al. "绝缘聚合物调控光氧化还原催化的起源研究" . | 催化学报 63 . 8 (2024) : 109-123 . |
| APA | 莫乔铃 , 熊锐 , 董俊豪 , 萨百晟 , 郑晶莹 , 陈青 et al. 绝缘聚合物调控光氧化还原催化的起源研究 . | 催化学报 , 2024 , 63 (8) , 109-123 . |
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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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Surface charge transfer doping (SCTD) has been established as an efficient strategy to achieve strong electronic coupling interactions between semiconductors and dopants, which lead to highly efficient electron transport over semiconductors. Herein, we report a facile, easily accessible, and effective SCTD strategy to exquisitely modulate the interfacial charge transfer over transition metal chalcogenides (TMCs: CdS, Zn0.5Cd0.5S, CdIn2S4, and ZnIn2S4) through surface modification with a nonconjugated polymer, poly(dimethyldiallylammonium chloride) (PDDA). We provide evidence that PDDA, as a surface electron transfer acceptor, can be used to enable rapid, directional, and tunable charge transfer along with an optimal charge lifetime over TMCs in photoredox catalysis because of the high-efficiency electron-trapping property of quaternary ammonium functional groups in the molecular structure of PDDA. The thus-assembled PDDA-encapsulated TMC composite artificial photosystems demonstrate significantly enhanced and versatile photoredox catalytic activities toward visible-light-responsive photocatalytic reduction of aromatic nitro compounds, photocatalytic oxidation of aromatic alcohols, and photocatalytic H2 production, wherein the ultrathin PDDA layer accelerates the interfacial charge transport and separation rate over TMC substrates. Moreover, it was evidenced that such an interface engineering strategy is general for a collection of TMCs. Our work will provide conceptual insights into nonconjugated polymer-based artificial photosystems for optimizing solar energy utilization.
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| GB/T 7714 | Cai, Lifeng , Chen, Qing , Xu, Ruijie et al. Transition Metal Chalcogenides/Nonconjugated Polymer Artificial Photosystems for Photoredox Catalysis [J]. | INORGANIC CHEMISTRY , 2024 , 63 (51) : 24382-24391 . |
| MLA | Cai, Lifeng et al. "Transition Metal Chalcogenides/Nonconjugated Polymer Artificial Photosystems for Photoredox Catalysis" . | INORGANIC CHEMISTRY 63 . 51 (2024) : 24382-24391 . |
| APA | Cai, Lifeng , Chen, Qing , Xu, Ruijie , Li, Tao , Liang, Jie , Xiao, Fang-Xing . Transition Metal Chalcogenides/Nonconjugated Polymer Artificial Photosystems for Photoredox Catalysis . | INORGANIC CHEMISTRY , 2024 , 63 (51) , 24382-24391 . |
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