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学者姓名：肖方兴
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Abstract ：
Black phosphorus (BP), a promising two-dimensional (2D) layered semiconductor material, has gained enormous attention due to its impressive properties over the past several years. Although plenty of methods have been developed to synthesize high-quality BP, most of the currently available BP materials still suffer from unsatisfactory crystallization, purity, and stability in air, hindering their practical application. A facile approach to synthesizing ultrahigh-quality single-crystal BP is of significance to shed light on the nature of 2D semiconductor materials and their massive application. In this work, we present the facile and efficient circulating vapor growth approach to growing bulk single-crystal BP. The as-grown BP material features high crystallinity and ultrahigh purity (higher than 99.999 at %), exceeding those of all the previously reported and some commercially available BP crystals. It also maintains excellent stability in air and water after 15 consecutive days of test. Moreover, the as-synthesized BP material features good thermal stability, oxidation resistance, and excellent electrical properties, as well. This study provides a new approach for the fabrication of ultrahigh-quality BP material and thus promotes its application.
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| GB/T 7714 | Lu, Shao-Jun , Tang, Ling , Xiao, Zechen et al. Synthesis of High-Quality Bulk Single-Crystal Black Phosphorus by the Circulating Vapor Growth Approach [J]. | INORGANIC CHEMISTRY , 2024 , 63 (24) : 11092-11101 . |
| MLA | Lu, Shao-Jun et al. "Synthesis of High-Quality Bulk Single-Crystal Black Phosphorus by the Circulating Vapor Growth Approach" . | INORGANIC CHEMISTRY 63 . 24 (2024) : 11092-11101 . |
| APA | Lu, Shao-Jun , Tang, Ling , Xiao, Zechen , Zhang, Mo , Guo, Wei , Tan, Mingwu et al. Synthesis of High-Quality Bulk Single-Crystal Black Phosphorus by the Circulating Vapor Growth Approach . | INORGANIC CHEMISTRY , 2024 , 63 (24) , 11092-11101 . |
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Solar CO2 reduction to renewable hydrocarbon fuels offers a promising pathway to carbon neutrality, but it is retarded by tough CO2 activation, complicated mechanisms, sluggish charge transport kinetics, and a scarcity of strategies for precise tuning of charge transport pathways. Herein, we first conceptually design a novel insulating polymer-mediated electron-tunneling artificial photosystem via progressive interface configuration regulation, wherein tailor-made Ag@citrate nanocrystals (NCs) are controllably self-assembled on transition metal chalcogenides (TMCs) assisted by an ultrathin insulating polymer interim layer, i.e., poly(allylamine hydrochloride) (PAH). In this multilayered nano-architecture, a solid ultra-thin insulating PAH interim layer serves as an unexpected charge tunneling mediator to stimulate smooth electron transfer from the TMC substrate to the terminal electron reservoirs of Ag@citrate NCs, engendering the tandem charge transfer route and significantly boosting the visible-light-driven photocatalytic CO2-to-syngas conversion performances. Furthermore, we have ascertained that such TMC-insulating polymer-metal NC tunneling photosystems are universal. This study would spark new inspiration for unleashing the long-term neglected charge tunneling capability of insulating polymers and diversifying non-conjugated polymer-based artificial photosystems for solar-to-fuel energy conversion.
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| GB/T 7714 | Yan, Xian , Yuan, Meng , Yuan, Ya-Long et al. Photocarrier tunneling triggering CO2 photocatalysis [J]. | CHEMICAL SCIENCE , 2024 , 15 (27) : 10625-10637 . |
| MLA | Yan, Xian et al. "Photocarrier tunneling triggering CO2 photocatalysis" . | CHEMICAL SCIENCE 15 . 27 (2024) : 10625-10637 . |
| APA | Yan, Xian , Yuan, Meng , Yuan, Ya-Long , Su, Peng , Chen, Qing , Xiao, Fang-Xing . Photocarrier tunneling triggering CO2 photocatalysis . | CHEMICAL SCIENCE , 2024 , 15 (27) , 10625-10637 . |
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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 , 40 (17) : 9144-9154 . |
| MLA | Ning, Boyuan et al. "Simultaneous Photocatalytic Tetracycline Oxidation and Cr(VI) Reduction by Z-Scheme Multiple Layer TiO2/SnIn4S8" . | LANGMUIR 40 . 17 (2024) : 9144-9154 . |
| 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 , 40 (17) , 9144-9154 . |
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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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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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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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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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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 , 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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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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