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学者姓名：吴悦
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Abstract ：
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 等. "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) 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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Unravelling the influence of strain and geometric effects on the electrochemical reduction of carbon dioxide (CO2RR) on Cu-based (or Pd-based) alloys remains challenging due to complex local microenvironment variables. Herein, we employ two PdCu alloys (nanoparticles and nanodendrites) to demonstrate how CO2RR selectivity can shift from CO to HCOO-. Despite sharing consistent phases, exposed crystal facets, and overall oxidative states, these alloys exhibit different local strain profiles due to their distinct geometries. By integrating experimental data, in-situ spectroscopy, and density functional theory calculations, we revealed that CO2 prefers adsorption on tensile-strained areas with carbon-side geometry, following a *COOH-to-CO pathway. Conversely, on some compressive-strained regions induced by the dendrite-like morphology, CO2 adopts an oxygen-side geometry, favoring an *OCHO-to-HCOO pathway due to the downshift of the d-band center. Notably, our findings elucidate a dominant *OCHO-to-HCOO- pathway in catalysts when featuring both adsorption geometries. This research provides a comprehensive model for local environment of bimetallic alloys, and establishes a clear relationship between the CO2RR pathway shift and variation in local strain environments of PdCu alloys.
Keyword ：
CO2 electroreduction CO2 electroreduction local strain local strain pathway shift pathway shift PdCu alloys PdCu alloys
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| GB/T 7714 | Liu, Chuhao , Bu, Yifan , Xu, Yifei et al. Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift [J]. | NATIONAL SCIENCE REVIEW , 2024 , 11 (12) . |
| MLA | Liu, Chuhao et al. "Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift" . | NATIONAL SCIENCE REVIEW 11 . 12 (2024) . |
| APA | Liu, Chuhao , Bu, Yifan , Xu, Yifei , Mahmood, Azhar , Xie, Jisheng , Fu, Yifan et al. Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift . | NATIONAL SCIENCE REVIEW , 2024 , 11 (12) . |
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Cocatalyst is of paramount significance to provide fruitful active sites for suppressing the spatial charge recombination toward boosted photocatalysis. Up to date, exploration of robust and stable cocatalysts is remained challenging. Inspired by the intrinsic merits of single-atom catalysts (SACs), such as distinctive electronic structure and high atomic utilization efficiency, single-atom/transition metal chalcogenides (TMCs) is utilized as a model to synthesize CdS-Pd single-atom catalyst (CdS-PdSA) heterostructures. This demonstrates the precise anchoring of isolated metal single-atom catalysts (SACs) onto TMCs through a simple yet effective wet-chemical strategy. The resulting heterostructures exhibit significantly enhanced and stable photocatalytic activity for selective anaerobic organic transformations and hydrogen production under visible light. This enhancement is primarily inferred due to the role of Pd SACs as electron pumps, which directionally trap the electrons photoexcited over CdS, accelerating the spatial charge separation and prolonging the carrier lifespan. The charge transport route and photocatalytic mechanism are elucidated. This work underscores the potential of SACs as cocatalysts in heterogeneous photocatalysis, offering valuable insights for the rational design of atomic-level cocatalysts for solar-to-chemical energy conversion and beyond. Metal single atoms act as electron pumps to expedite the unidirectional electron transfer from the TMCs matrix to the metal single atoms, contributing to the markedly augmented organic transformation and hydrogen generation activities. image
Keyword ：
charge transfer charge transfer electron pump electron pump photoreduction catalysis photoreduction catalysis single atoms single atoms TMC TMC
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| GB/T 7714 | Chen, Jia-Qi , Cai, Yu-Shan , Yan, Xian et al. Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis [J]. | SMALL , 2024 , 20 (51) . |
| MLA | Chen, Jia-Qi et al. "Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis" . | SMALL 20 . 51 (2024) . |
| APA | Chen, Jia-Qi , Cai, Yu-Shan , Yan, Xian , Mo, Qiao-Ling , Yuan, Jiao-Nan , Liu, Chu-Hao et al. Single-Atom Electron Pumps Over Transition Metal Chalcogenides Boosting Photocatalysis . | SMALL , 2024 , 20 (51) . |
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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 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.
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| GB/T 7714 | Cai, Yu-Shan , Chen, Jia-Qi , Su, Peng et al. Atomically precise metal nanoclusters combine with MXene towards solar CO2 conversion [J]. | CHEMICAL SCIENCE , 2024 , 15 (33) : 13495-13505 . |
| MLA | Cai, Yu-Shan et al. "Atomically precise metal nanoclusters combine with MXene towards solar CO2 conversion" . | CHEMICAL SCIENCE 15 . 33 (2024) : 13495-13505 . |
| APA | Cai, Yu-Shan , Chen, Jia-Qi , Su, Peng , Yan, Xian , Chen, Qing , Wu, Yue et al. Atomically precise metal nanoclusters combine with MXene towards solar CO2 conversion . | CHEMICAL SCIENCE , 2024 , 15 (33) , 13495-13505 . |
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Unravelling the influence of strain and geometric effects on the electrochemical reduction of carbon dioxide(CO2RR)on Cu-based(or Pd-based)alloys remains challenging due to complex local microenvironment variables.Herein,we employ two PdCu alloys(nanoparticles and nanodendrites)to demonstrate how CO2RR selectivity can shift from CO to HCOO-.Despite sharing consistent phases,exposed crystal facets,and overall oxidative states,these alloys exhibit different local strain profiles due to their distinct geometries.By integrating experimental data,in-situ spectroscopy,and density functional theory calculations,we revealed that CO2 prefers adsorption on tensile-strained areas with carbon-side geometry,following a*COOH-to-CO pathway.Conversely,on some compressive-strained regions induced by the dendrite-like morphology,CO2 adopts an oxygen-side geometry,favoring an *OCHO-to-HCOO pathway due to the downshift of the d-band center.Notably,our findings elucidate a dominant *OCHO-to-HCOO-pathway in catalysts when featuring both adsorption geometries.This research provides a comprehensive model for local environment of bimetallic alloys,and establishes a clear relationship between the CO2RR pathway shift and variation in local strain environments of PdCu alloys.
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| GB/T 7714 | Chuhao Liu , Yifan Bu , Yifei Xu et al. Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift [J]. | 国家科学评论（英文版） , 2024 , 11 (12) : 14-21 . |
| MLA | Chuhao Liu et al. "Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift" . | 国家科学评论（英文版） 11 . 12 (2024) : 14-21 . |
| APA | Chuhao Liu , Yifan Bu , Yifei Xu , Azhar Mahmood , Jisheng Xie , Yifan Fu et al. Local-strain-induced CO2 adsorption geometries and electrochemical reduction pathway shift . | 国家科学评论（英文版） , 2024 , 11 (12) , 14-21 . |
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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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Rational construction of high-efficiency photoelectrodes with optimized carrier migration to the ideal active sites, is crucial for enhancing solar water oxidation. However, complexity in precisely modulating interface configuration and directional charge transfer pathways retards the design of robust and stable artificial photosystems. Herein, a straightforward yet effective strategy is developed for compact encapsulation of metal oxides (MOs) with an ultrathin non-conjugated polymer layer to modulate interfacial charge migration and separation. By periodically coating highly ordered TiO2 nanoarrays with oppositely charged polyelectrolyte of poly(dimethyl diallyl ammonium chloride) (PDDA), MOs/polymer composite photoanodes are readily fabricated under ambient conditions. It is verified that electrons photogenerated from the MOs substrate can be efficiently extracted by the ultrathin solid insulating PDDA layer, significantly boosting the carrier transport kinetics and enhancing charge separation of MOs, and thus triggering a remarkable enhancement in the solar water oxidation performance. The origins of the unexpected electron-withdrawing capability of such non-conjugated insulating polymer are unambiguously uncovered, and the scenario occurring at the interface of hybrid photoelectrodes is elucidated. The work would reinforce the fundamental understanding on the origins of generic charge transport capability of insulating polymer and benefit potential wide-spread utilization of insulating polymers as co-catalysts for solar energy conversion. Uniform non-conjugated insulating polymer encapsulation on the metal oxides remarkably enhances the spatially directional electron transport, wherein the ultrathin insulating polymer functions as an electron trap to facilitate the charge separation in solar water splitting. image
Keyword ：
charge transport charge transport interface modulation interface modulation non-conjugated polymer non-conjugated polymer photoelectrochemical water splitting photoelectrochemical water splitting
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| GB/T 7714 | Liu, Jia-Liang , Yan, Xian , Yuan, Jiao-Nan et al. Identifying Root Origin of Insulating Polymer Mediated Solar Water Oxidation [J]. | SMALL , 2024 , 20 (48) . |
| MLA | Liu, Jia-Liang et al. "Identifying Root Origin of Insulating Polymer Mediated Solar Water Oxidation" . | SMALL 20 . 48 (2024) . |
| APA | Liu, Jia-Liang , Yan, Xian , Yuan, Jiao-Nan , Wu, Yue , Wang, Xin , Xiao, Fang-Xing . Identifying Root Origin of Insulating Polymer Mediated Solar Water Oxidation . | SMALL , 2024 , 20 (48) . |
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Solid non-conjugated polymers have long been regarded as insulators due to deficiency of delocalized Tr electrons along the molecular chain framework. Up to date, origin of insulating polymer regulated charge transfer has not yet been uncovered. In this work, we unleash the root origin of charge transport capability of insulating polymer in photocatalysis. We ascertain that insulating polymer plays crucial roles in fine tuning of electronic structure of transition metal chalcogenides (TMCs), which mainly include altering surface electron density of TMCs for accelerating charge transport kinetics, triggering the generation of defect over TMCs for prolonging carrier lifetime, and acting as hole-trapping mediator for retarding charge recombination. These synergistic roles contribute to the charge transfer of insulating polymer. Our work opens a new vista of utilizing solid insulating polymers for maneuvering charge transfer toward solar energy conversion.
Keyword ：
Charge transfer Charge transfer Insulating polymer Insulating polymer Photoredox catalysis Photoredox catalysis Polyelectrolyte Polyelectrolyte Self-assembly Self-assembly
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| GB/T 7714 | Mo, Qiao-Ling , Xiong, Rui , Dong, Jun-Hao et al. Identification of origin of insulating polymer maneuvered photoredox catalysis [J]. | CHINESE JOURNAL OF CATALYSIS , 2024 , 63 : 109-123 . |
| MLA | Mo, Qiao-Ling et al. "Identification of origin of insulating polymer maneuvered photoredox catalysis" . | CHINESE JOURNAL OF CATALYSIS 63 (2024) : 109-123 . |
| APA | Mo, Qiao-Ling , Xiong, Rui , Dong, Jun-Hao , Sa, Bai-Sheng , Zheng, Jing-Ying , Chen, Qing et al. Identification of origin of insulating polymer maneuvered photoredox catalysis . | CHINESE JOURNAL OF CATALYSIS , 2024 , 63 , 109-123 . |
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