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学者姓名：肖方兴
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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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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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With the advancement of science and technology, traditional energy sources such as oil and coal have been extensively depleted, leading to the emission of greenhouse gases like CO2. Consequently, issues such as energy scarcity and drastic environmental changes have emerged as pressing concerns that threaten human survival and development. Photocatalysis offers a promising solution by harnessing solar energy for chemical energy conversion, yielding clean and sustainable products. It is widely regarded as an emerging approach to address the energy crisis and environmental challenges. To achieve high-efficiency photocatalytic reactions, the selection of appropriate catalysts and co-catalysts plays a pivotal role. However, conventional photocatalysts such as TiO2, CdS, and g-C3N4 suffer from inherent limitations, including high charge recombination rates, low light utilization efficiency, poor stability, and sluggish charge transfer kinetics, which hinder the enhancement of photocatalytic efficiency. In this context, two-dimensional (2D) materials known as MXenes have gained prominence. These materials exhibit unique structural flexibility, diverse elemental compositions, superior conductivity, excellent carrier mobility, and abundant active sites, making them valuable co-catalysts in photocatalysis. MXenes accelerate interfacial charge transfer kinetics and mitigate charge recombination, enhancing the overall photocatalytic performance. This review provides a comprehensive overview of various methods employed to prepare high-quality MXenes under different conditions, such as water solution etching, water-free etching, and other physical methods. It also explores diverse strategies for constructing MXene-based composite photocatalytic systems, including in situ growth synthesis, in situ oxidation synthesis, and electrostatic self-assembly. Additionally, the review discusses various MXenes-based photosystems, such as MXene/TiO2, MXene/CdS, MXene/g-C3N4, MXene/WO3, and BiOBr/MXene/MMTex, and their applications in photocatalytic processes, including hydrogen production, CO2 reduction, environmental remediation, nitrogen fixation, and sterilization. The critical role of MXenes as reduction co-catalysts in these photoredox catalysis reactions is thoroughly examined, along with an elucidation of the relationship between MXene electronic structure and charge transfer characteristics. Furthermore, the review addresses the challenges related to the stability of MXenes in photocatalytic reactions and offers insights into potential strategies to mitigate this issue. Finally, the development prospects and future challenges of MXene-based composites in the field of photocatalysis are presented, taking into consideration the inherent limitations of MXenes and the requirements for industrialization. It is expected that this review will provide valuable insights into the physicochemical properties of MXenes and inspire innovative approaches to the rational design of diverse MXene-based photosystems for heterogeneous photocatalysis across various applications. © Editorial office of Acta Physico-Chimica Sinica.
Keyword ：
Charge transfer Charge transfer Interface configuration Interface configuration MXenes MXenes Photoredox catalysis Photoredox catalysis Two-dimensional Two-dimensional
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| GB/T 7714 | Cai, Y. , Xiao, F.-X. . Revisiting MXenes-based Photocatalysis Landscape: Progress, Challenges, and Future Perspectives [J]. | Acta Physico - Chimica Sinica , 2024 , 40 (8) . |
| MLA | Cai, Y. et al. "Revisiting MXenes-based Photocatalysis Landscape: Progress, Challenges, and Future Perspectives" . | Acta Physico - Chimica Sinica 40 . 8 (2024) . |
| APA | Cai, Y. , Xiao, F.-X. . Revisiting MXenes-based Photocatalysis Landscape: Progress, Challenges, and Future Perspectives . | Acta Physico - Chimica Sinica , 2024 , 40 (8) . |
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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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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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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 . |
| MLA | Su, Peng et al. "Precise Layer-by-Layer Assembly of Dual Quantum Dots Artificial Photosystems Enabling Solar Water Oxidation" . | SMALL (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 . |
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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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In the past few years, environmental and energy challenges arising from extensive burning of fossil fuels and CO2 emission have become the increasingly severe issue. One effective solution to address these problems is the reduction of CO2 into valuable solar fuels such as CO, CH4, and HCO2H through the semiconductor-based photocatalysis technology. Metal halide perovskites quantum dots (MHPs QDs) represent a new generation of photosensitizers that possess excellent photoelectric properties and have been attracting enormous attention in the field of photocatalytic CO2 reduction. This review provides a concise introduction on different types and preparation methods of MHPs QDs and discusses the specific applications especially photocatalytic CO2 reduction mechanism of MHPs QDs. Furthermore, future opportunities and challenges for constructing high-performance MHPs QDs-based photocatalysts are further elucidated. We anticipate that our review could provide enriched information on the photocatalytic application of MHPs QDs toward solar-to-fuel conversion.
Keyword ：
Charge transfer Charge transfer Metal halide perovskites Metal halide perovskites Photocatalytic CO 2 reduction Photocatalytic CO 2 reduction Quantum dots Quantum dots
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| GB/T 7714 | Xu, Shu-Ran , Xiao, Fang-Xing . Metal halide perovskites quantum dots: Synthesis and modification strategies for solar CO2 conversion [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 42 (12) . |
| MLA | Xu, Shu-Ran et al. "Metal halide perovskites quantum dots: Synthesis and modification strategies for solar CO2 conversion" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 42 . 12 (2024) . |
| APA | Xu, Shu-Ran , Xiao, Fang-Xing . Metal halide perovskites quantum dots: Synthesis and modification strategies for solar CO2 conversion . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 42 (12) . |
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Wastewater pollutants are a major threat to natural resources, with antibiotics and heavy metals being common water contaminants. By harnessing clean, renewable solar energy, photocatalysis facilitates the synergistic removal of heavy metals and antibiotics. In this paper, MXene was both a template and raw material, and MXene-derived oxide (TiO2) and SnIn4S8 Z-scheme composite materials were synthesized and characterized. The synergistic mode of photocatalytic reduction and oxidation leads to the enhanced utilization of e(-)/h(+) pairs. The TiO2/SnIn4S8 exhibited a higher photocatalytic capacity for the simultaneous removal of tetracycline (TC) (20 mg center dot L-1) and Cr(VI) (15 mg center dot L-1). The main active substances of TC degradation and Cr(VI) reduction were identified via free radical scavengers and electron paramagnetic resonance (EPR). Additionally, the potential photocatalytic degradation route of TC was thoroughly elucidated through liquid chromatography-mass spectrometry (LC-MS).
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| GB/T 7714 | Ning, Boyuan , Chen, Zhixin , Cai, Yanqing et al. Simultaneous Photocatalytic Tetracycline Oxidation and Cr(VI) Reduction by Z-Scheme Multiple Layer TiO2/SnIn4S8 [J]. | LANGMUIR , 2024 . |
| MLA | Ning, Boyuan et al. "Simultaneous Photocatalytic Tetracycline Oxidation and Cr(VI) Reduction by Z-Scheme Multiple Layer TiO2/SnIn4S8" . | LANGMUIR (2024) . |
| APA | Ning, Boyuan , Chen, Zhixin , Cai, Yanqing , Xiao, Fang-Xing , Xu, Pingfan , Xiao, Guangcan et al. Simultaneous Photocatalytic Tetracycline Oxidation and Cr(VI) Reduction by Z-Scheme Multiple Layer TiO2/SnIn4S8 . | LANGMUIR , 2024 . |
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Fe -N -doped carbon materials (Fe -N -C) are promising candidates for oxygen reduction reaction (ORR) relative to Pt -based catalysts in proton exchange membrane fuel cells (PEMFCs). However, the intrinsic contributions of Fe -N4 moiety with different chemical/spin states (e.g. D1, D2, D3) to ORR are unclear since various states coexist inevitably. In the present work, Fe -N -C core-shell nanocatalyst with single lowspin Fe(II)-N4 species (D1) is synthesized and identified with ex -situ ultralow temperature M & ouml;ssbauer spectroscopy (T = 1.6 K) that could essentially differentiate various Fe -N4 states and invisible Fe -O species. By quantifying with CO -pulse chemisorption, site density and turnover frequency of Fe -N -C catalysts reach 2.4 x 1019 site g-1 and 23 e site -1 s-1 during the ORR, respectively. Half -wave potential (0.915 VRHE) of the Fe -N -C catalyst is more positive (approximately 54 mV) than that of Pt/C. Moreover, we observe that the performance of PEMFCs on Fe -N -C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm -2 combined with the peak power density of 0.685 W cm -2, suggesting the critical role of Fe(II)-N4 site (D1). After 500 h of running, PEMFCs still deliver a power density of 1.26 W cm -2 at 1.0 bar H2 -O2. An unexpected rate -determining step is figured out by isotopic labelling experiment and theoretical calculation. This work not only offers valuable insights regarding the intrinsic contribution of Fe -N4 with a single spin state to alkaline/acidic ORR, but also provides great opportunities for developing high-performance stable PEMFCs. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
Keyword ：
Active site Active site Fuel cells Fuel cells Isotopic labelling Isotopic labelling Non-platinum group metals (PGMs) Non-platinum group metals (PGMs) Oxygen reduction reaction Oxygen reduction reaction TOF TOF
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| GB/T 7714 | Wan, Yan , Yu, Linhui , Yang, Bingxin et al. Fe-N-C core-shell catalysts with single low-spin Fe(II)-N4 species for oxygen reduction reaction and high-performance proton exchange membrane fuel cells [J]. | JOURNAL OF ENERGY CHEMISTRY , 2024 , 93 : 538-546 . |
| MLA | Wan, Yan et al. "Fe-N-C core-shell catalysts with single low-spin Fe(II)-N4 species for oxygen reduction reaction and high-performance proton exchange membrane fuel cells" . | JOURNAL OF ENERGY CHEMISTRY 93 (2024) : 538-546 . |
| APA | Wan, Yan , Yu, Linhui , Yang, Bingxin , Li, Caihong , Fang, Chen , Guo, Wei et al. Fe-N-C core-shell catalysts with single low-spin Fe(II)-N4 species for oxygen reduction reaction and high-performance proton exchange membrane fuel cells . | JOURNAL OF ENERGY CHEMISTRY , 2024 , 93 , 538-546 . |
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