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学者姓名：沈少华
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Abstract ：
A variety of atomically dispersed transition-metal-anchored nitrogen-doped carbon (M-N-C) electrocatalysts have shown encouraging electrochemical CO2 reduction reaction (CO2RR) performance, with the underlying fundamentals of central transition-metal atom determined CO2RR activity and selectivity yet remaining unclear. Herein, a universal impregnation-acid leaching method was exploited to synthesize various M- N-C (M: Fe, Co, Ni, and Cu) single-atom catalysts (SACs), which revealed d-orbital electronic configuration-dependent activity and selectivity toward CO2RR for CO production. Notably, Ni-N-C exhibits a very high CO Faradaic efficiency (FE) of 97% at -0.65 V versus RHE and above 90% CO selectivity in the potential range from -0.5 to -0.9 V versus RHE, much superior to other M-N-C (M: Fe, Co, and Cu). With the d-orbital electronic configurations of central metals in M-N-C SACs well elucidated by crystal-field theory, Dewar-Chatt-Duncanson (DCD) and differential charge density analysis reveal that the vacant outermost d-orbital of Ni2+ in a Ni-N-C SAC would benefit the electron transfer from the C atoms in CO2 molecules to the Ni atoms and thus effectively activate the surface-adsorbed CO2 molecules. However, the outermost d-orbital of Fe3+, Co2+, and Cu2+ occupied by unpaired electrons would weaken the electron-transfer process and then impede CO2 activation. In situ spectral investigations demonstrate that the generation of *COOH intermediates is favored over Ni-N-C SAC at relatively low applied potentials, supporting its high CO2-to-CO conversion performance. Gibbs free energy difference analysis in the rate-limiting step in CO2RR and hydrogen evolution reaction (HER) reveals that CO2RR is thermodynamically favored for Ni-N-C SAC, explaining its superior CO2RR performance as compared to other SACs. This work presents a facile and general strategy to effectively modulate the CO2-to-CO selectivity from the perspective of electronic of central metals in M-N-C SACs.
Keyword ：
CO2 reduction reaction CO production crystal-field theory electronic configurations single-atom catalysts
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| GB/T 7714 | Wang, Jialin , Huang, Yu-Cheng , Wang, Yiqing et al. Atomically Dispersed Metal-Nitrogen-Carbon Catalysts with d-Orbital Electronic Configuration-Dependent Selectivity for Electrochemical CO2-to-CO Reduction [J]. | ACS CATALYSIS , 2023 . |
| MLA | Wang, Jialin et al. "Atomically Dispersed Metal-Nitrogen-Carbon Catalysts with d-Orbital Electronic Configuration-Dependent Selectivity for Electrochemical CO2-to-CO Reduction" . | ACS CATALYSIS (2023) . |
| APA | Wang, Jialin , Huang, Yu-Cheng , Wang, Yiqing , Deng, Hao , Shi, Yuchuan , Wei, Daixing et al. Atomically Dispersed Metal-Nitrogen-Carbon Catalysts with d-Orbital Electronic Configuration-Dependent Selectivity for Electrochemical CO2-to-CO Reduction . | ACS CATALYSIS , 2023 . |
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Abstract ：
Two iodide-derived copper (ID-Cu) electrocatalysts (E-ID-Cu and W-ID-Cu) are prepared by electrochemical/wet chemical iodination of Cu foil and subsequent in situ electrochemical reduction reaction. In comparison to electropolished Cu (EP-Cu), both E-ID-Cu and W-ID-Cu can produce multicarbon (C2+) products with much-improved selectivity, with Faradic efficiency (FE) reaching 64.39% for E-ID-Cu and 71.16% for W-ID-Cu at -1.1 V versus reversible hydrogen electrodes (RHE), which can be attributed to their localized geometry features with high defect density and high surface roughness. Given the well-determined FEs towards C2+ products, the partial current densities for C2+ production can be estimated to be 251.8 mA cm(-2) for E-ID-Cu and 290.0 mA cm(-2) for W-ID-Cu at -1.2 V versus RHE in a flow cell. In situ characterizations and theoretical calculations reveal that the high-density defects and high surface roughness can promote *CO adsorption by raising the d band center and then facilitate C-C coupling, contributing to the high selectivity of C2+ products for ID-Cu. Interestingly, the high surface roughness can increase the residence time of *C-H intermediates and decrease the formation energy of the *OCCO and*CH3CH2O intermediates, thus favoring C2+ production, with a unique C2H6 product observed over W-ID-Cu with FE of 10.14% at -0.7 V versus RHE.
Keyword ：
defect density electrochemical CO2 reduction flow cells iodide derived copper surface roughness
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| GB/T 7714 | Shi, Yuchuan , Wang, Yiqing , Dong, Chung-Li et al. Localized Geometry Determined Selectivity of Iodide-Derived Copper for Electrochemical CO2 Reduction [J]. | ADVANCED ENERGY MATERIALS , 2023 . |
| MLA | Shi, Yuchuan et al. "Localized Geometry Determined Selectivity of Iodide-Derived Copper for Electrochemical CO2 Reduction" . | ADVANCED ENERGY MATERIALS (2023) . |
| APA | Shi, Yuchuan , Wang, Yiqing , Dong, Chung-Li , Nga, Ta Thi Thuy , Wei, Daixing , Wang, Jialin et al. Localized Geometry Determined Selectivity of Iodide-Derived Copper for Electrochemical CO2 Reduction . | ADVANCED ENERGY MATERIALS , 2023 . |
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Abstract ：
Particle-fluid and particle-particle interactions can be widely seen in lots of natural and industrial processes. In order to understand these interactions, two-dimensional fluid flowing around and through nine porous particles was studied in this paper based on the lattice Boltzmann method due to its simplicity. Uniform spatial distribution and random spatial distribution were considered and the effects of Reynold number (Re), Darcy number (Da), and the distance between the particles (dx and dy) on the flow characteristics were analyzed in detail. The investigated ranges of the parameters were 10 <= Re <= 40, 10(-6) <= Da <= 10(-2), D <= dx <= 4D and D <= dy <= 4D (D is the diameter of the particles). For uniform spatial distribution, it is observed that when dx(dy) increases, the interactions between the particles become weak and the fluid can flow into the spacing between the particles. Besides, the average drag coefficient (C-Dave) increases with dx(dy) increasing at Re = 20 and the increase rate gradually slows down. Furthermore, the distance change in the direction vertical to inflow direction has more obvious impact on the average drag coefficient. For example, for Re = 20 and Da = 10(-4), when dx equals D and dy increases from 2D to 3D, C-Dave increases by 5.79%; when dy equals D and dx increases from 2D to 3D, C-Dave increases by 2.61%.
Keyword ：
Drag coefficient Flow pattern Lattice Boltzmann method Multiple porous particles Uniform and random spatial distribution
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| GB/T 7714 | Zhang, Mingyue , Jin, Hui , Shen, Shaohua . Numerical simulation of the flow characteristics around and through multiple porous particles [J]. | COMPUTATIONAL PARTICLE MECHANICS , 2022 . |
| MLA | Zhang, Mingyue et al. "Numerical simulation of the flow characteristics around and through multiple porous particles" . | COMPUTATIONAL PARTICLE MECHANICS (2022) . |
| APA | Zhang, Mingyue , Jin, Hui , Shen, Shaohua . Numerical simulation of the flow characteristics around and through multiple porous particles . | COMPUTATIONAL PARTICLE MECHANICS , 2022 . |
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Abstract ：
Herein, a novel strategy of interface charge modulation for manipulating interface built-in electric fields (IEFs) and boosting spatial charge separation is introduced to alleviate charge recombination in the bulk and at the surface of hematite photoanodes. Hydrothermally grown Ti-doped hematite (Hem) nanorods are decorated with graphitic carbon nitride (g-C3N4) species and small molybdenum oxide (MoO3) clusters using a facile two-step dip-coating process. Compared with the pristine Hem, the obtained Hem/C3N4/MoO3 exhibits increased photoelectrochemical water splitting performance with its photoanodic current density remarkably increased from 0.3 to 1.6 mA cm(-2) at 1.23 V versus reversible hydrogen electrode (RHE) and incident photon-to-current conversion efficiency reaching 18.4% at 1.23 V versus RHE at 300 nm. The IEFs are introduced in the Hem/C3N4/MoO3 heterojunction by modulating the interfacial charge property via a type II band alignment at the Hem/C3N4 interface and an enhanced band bending at the surface of the photoanode, which substantially promote the spatial charge separation. By relieving the bottleneck of charge carrier transfer dynamics, this work in interfacial charge modulation provides a facile and effective strategy to boost the spatial charge separation in Hem-based photoanodes and other semiconducting devices for efficient solar energy conversion.
Keyword ：
band bending built-in electric field hematite nanorods heterojunction photoelectrochemical water splitting
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| GB/T 7714 | Mao, Lianlian , Deng, Hao , Li, Mingtao et al. Manipulating interface built-in electric fields for efficient spatial charge separation in hematite-based photoanodes [J]. | SCIENCE CHINA-MATERIALS , 2022 , 66 (2) : 603-613 . |
| MLA | Mao, Lianlian et al. "Manipulating interface built-in electric fields for efficient spatial charge separation in hematite-based photoanodes" . | SCIENCE CHINA-MATERIALS 66 . 2 (2022) : 603-613 . |
| APA | Mao, Lianlian , Deng, Hao , Li, Mingtao , Shen, Shaohua . Manipulating interface built-in electric fields for efficient spatial charge separation in hematite-based photoanodes . | SCIENCE CHINA-MATERIALS , 2022 , 66 (2) , 603-613 . |
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Abstract ：
Photocatalytic technology has been considered as a promising and sustainable technology to convert solar energy to storable chemical energy. With active sites (single metal atoms and clusters) atomically dispersed on the semiconductor, the mass and charge transfer in photocatalysis can be significantly promoted, and the photocatalytic performance can be remarkably improved. However, it is still controversial whether clusters or single-atoms are the real active sites in catalysts. In this review, the recent advances in single-atom photocatalysis are briefly introduced, with the competition and synergy of single-atoms and clusters analyzed and discussed. Then, the state-of-the-art technologies in the identification and characterization of single-atoms and clusters as photocatalytic active sites are presented. Finally, the future development of single-atoms/clusters synergistic photocatalysis in solar-chemical energy conversions such as water splitting and CO2 reduction is prospected.
Keyword ：
Cluster Photocatalysis Single-atom catalyst
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| GB/T 7714 | Lin Zhi , Peng Zhiming , He Weiqing et al. Single-atom and Cluster Photocatalysis:Competition and Cooperation [J]. | CHEMICAL JOURNAL OF CHINESE UNIVERSITIES-CHINESE , 2022 , 43 (9) . |
| MLA | Lin Zhi et al. "Single-atom and Cluster Photocatalysis:Competition and Cooperation" . | CHEMICAL JOURNAL OF CHINESE UNIVERSITIES-CHINESE 43 . 9 (2022) . |
| APA | Lin Zhi , Peng Zhiming , He Weiqing , Shen Shaohua . Single-atom and Cluster Photocatalysis:Competition and Cooperation . | CHEMICAL JOURNAL OF CHINESE UNIVERSITIES-CHINESE , 2022 , 43 (9) . |
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Abstract ：
Limited by the retarded charge carrier migration and the sluggish four-electron reaction kinetics, it is still a great challenge for polymeric semiconductors to achieve efficient photocatalytic water oxidation. Herein, single Co atoms and ultra-small CoOx clusters are simultaneously introduced into polymeric perylene diimide (PDI) through a facile impregnation-calcination two-step method. The obtained Co-PDI exhibits excellent photocatalytic water oxidation activity under visible-light irradiation, with an oxygen evolution rate reaching as high as 5.53 mmol h(-1) g(-1) (lambda > 420 nm). The apparent quantum yield for oxygen evolution is determined to be 8.17% at 450 nm, and remains 0.77% at even longer visible light wavelength of 700 nm without redundant co-catalysts, indicating that Co-PDI may serve as an excellent oxygen evolution photocatalyst for water splitting. Theoretical calculations and experimental results demonstrate that single Co atoms act as the electron mediators connecting adjacent PDI layers to build directional channels for rapid charge transfer, while ultra-small CoOx clusters as hole collectors and reaction sites to accelerate oxygen evolution reaction kinetics. The study presents a facile and reliable strategy to effectively activate polymeric semiconductors for efficient photocatalysis by rationally modulating atomic structures and active sites for promoted charge carrier transfer and surface reaction kinetics.
Keyword ：
photocatalytic oxygen evolution polymeric perylene diimide single metal atoms ultra-small clusters
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| GB/T 7714 | Lin, Zhi , Wang, Yiqing , Peng, Zhiming et al. Single-Metal Atoms and Ultra-Small Clusters Manipulating Charge Carrier Migration in Polymeric Perylene Diimide for Efficient Photocatalytic Oxygen Production [J]. | ADVANCED ENERGY MATERIALS , 2022 , 12 (26) . |
| MLA | Lin, Zhi et al. "Single-Metal Atoms and Ultra-Small Clusters Manipulating Charge Carrier Migration in Polymeric Perylene Diimide for Efficient Photocatalytic Oxygen Production" . | ADVANCED ENERGY MATERIALS 12 . 26 (2022) . |
| APA | Lin, Zhi , Wang, Yiqing , Peng, Zhiming , Huang, Yu-Cheng , Meng, Fanqi , Chen, Jeng-Lung et al. Single-Metal Atoms and Ultra-Small Clusters Manipulating Charge Carrier Migration in Polymeric Perylene Diimide for Efficient Photocatalytic Oxygen Production . | ADVANCED ENERGY MATERIALS , 2022 , 12 (26) . |
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Abstract ：
Polymeric carbon nitride(PCN) has emerged as a promising candidate for photocatalytic hydrogen evolution, but its dependence on scarce and high-cost noble metal co-catalysts severely limits its extensive application. It will be of great promise to develop non-noble metal single-atom co-catalysts with low-cost and high atom utilization to improve the photocatalytic performance over PCN. Herein, single Ni atoms are successfully anchored onto carbon-vacant PCN nanosheets(CCN-SANi) via a two-step ammonia thermal treatment and photo-deposition process. Theoretical calculations and experimental results demonstrate that the optical absorption property and the charge transfer ability of CCN-SANi have been significantly improved with the introduction of single Ni atoms to form Ni-N-3 sites. In comparison to carbon-vacant PCN(CCN) loaded with Ni clusters, the obtained CCN-SANi exhibits 11.4 times increased photocatalytic performance, with the highest hydrogen evolution rate reaching 511 mu mol/(g.h), which is even 1.7 times higher than that of CCN loaded with Pt clusters. This research proposes an inspiring and reliable strategy to design novel single-atom semiconducting polymers with electronic structures manipulated for efficient photocatalysis.
Keyword ：
Photocatalytic hydgogen evolution Polymeric carbon nitride Single metal atom
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| GB/T 7714 | Lin Zhi , Zhang Zhengqi , Wang Yiqing et al. Anchoring Single Nickel Atoms on Carbon-vacant Carbon Nitride Nanosheets for Efficient Photocatalytic Hydrogen Evolution [J]. | CHEMICAL RESEARCH IN CHINESE UNIVERSITIES , 2022 , 38 (5) : 1243-1250 . |
| MLA | Lin Zhi et al. "Anchoring Single Nickel Atoms on Carbon-vacant Carbon Nitride Nanosheets for Efficient Photocatalytic Hydrogen Evolution" . | CHEMICAL RESEARCH IN CHINESE UNIVERSITIES 38 . 5 (2022) : 1243-1250 . |
| APA | Lin Zhi , Zhang Zhengqi , Wang Yiqing , Peng Zhiming , Wang Xinxin , Wang Ruizhe et al. Anchoring Single Nickel Atoms on Carbon-vacant Carbon Nitride Nanosheets for Efficient Photocatalytic Hydrogen Evolution . | CHEMICAL RESEARCH IN CHINESE UNIVERSITIES , 2022 , 38 (5) , 1243-1250 . |
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Abstract ：
Surficial redox reactions play an essential role in photocatalytic water splitting, and are closely related to the surface properties of a specific photocatalyst. In this work, using monoclinic BiVO4 decahedral single crystals as a model photocatalyst, we report on the interrelationship between the photocatalytic activity and the surficial reaction sites for charge-carrier consumption. By controlled hydrothermal synthesis, the ratio of {010} to {110} facets on BiVO4, which respectively serve as reductive and oxidative sites, is carefully tailored. Our results show that superior photocatalytic water oxidation could be obtained on BiVO4 decahedrons with a medium ratio of reductive/oxidative sites and that efficient overall water splitting could be achieved via further modification of appropriate cocatalysts in Z-scheme system. The excellent photocatalytic performance is attributed to the accelerated selective redox reactions by realizing balanced charge-carrier consumption, which provides insightful guidance for prospering photocatalytic reactions in energy conversion.
Keyword ：
BiVO4 photocatalytic reactive site water splitting
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| GB/T 7714 | Guan, Xiangjiu , Tian, Li , Zhang, Yazhou et al. Photocatalytic water splitting on BiVO4: Balanced charge-carrier consumption and selective redox reaction [J]. | NANO RESEARCH , 2022 . |
| MLA | Guan, Xiangjiu et al. "Photocatalytic water splitting on BiVO4: Balanced charge-carrier consumption and selective redox reaction" . | NANO RESEARCH (2022) . |
| APA | Guan, Xiangjiu , Tian, Li , Zhang, Yazhou , Shi, Jinwen , Shen, Shaohua . Photocatalytic water splitting on BiVO4: Balanced charge-carrier consumption and selective redox reaction . | NANO RESEARCH , 2022 . |
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Abstract ：
Photo(electro)catalysis is a promising route to utilizing solar energy to produce valuable chemical fuels. In recent years, lead halide perovskites (LHPs) as a class of high-performance semiconductor materials have been extensively used in photo(electro)catalytic solar fuel production because of their excellent photophysical properties. However, instability issues make it arduous for LHPs to achieve their full potential in photo(electro)catalysis. This Perspective discusses the instability issues and summarizes the stabilization strategies employed for prolonging the stability or durability of LHPs in photo(electro)catalytic solar fuel production. The strategies for particulate photocatalytic systems (including composition engineering, surface passivation, core- shell structures construction, and solvent selection) and for thin-film PEC systems (including physical protective coating, A site cation additive, and surface/interface passivation) are introduced. Finally, some challenges and opportunities regarding the development of stable and efficient LHPs for photo(electro)catalysis are proposed.
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| GB/T 7714 | Chen, Jie , Hong, Xin , Wang, Yiqing et al. Instability Issues and Stabilization Strategies of Lead Halide Perovskites for Photo(electro)catalytic Solar Fuel Production [J]. | JOURNAL OF PHYSICAL CHEMISTRY LETTERS , 2022 , 13 (7) : 1806-1824 . |
| MLA | Chen, Jie et al. "Instability Issues and Stabilization Strategies of Lead Halide Perovskites for Photo(electro)catalytic Solar Fuel Production" . | JOURNAL OF PHYSICAL CHEMISTRY LETTERS 13 . 7 (2022) : 1806-1824 . |
| APA | Chen, Jie , Hong, Xin , Wang, Yiqing , Guan, Xiangjiu , Wang, Ruizhe , Wang, Yiduo et al. Instability Issues and Stabilization Strategies of Lead Halide Perovskites for Photo(electro)catalytic Solar Fuel Production . | JOURNAL OF PHYSICAL CHEMISTRY LETTERS , 2022 , 13 (7) , 1806-1824 . |
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Abstract ：
Despite of suitable band structures for harvesting solar light and driving water redox reactions, polymeric carbon nitride (PCN) has suffered from poor charge transfer ability and sluggish surface reaction kinetics, which limit its photocatalytic activity for water splitting. Herein, atomically dispersed Zn-coordinated three-dimensional (3D) sponge-like PCN (Zn-PCN) is synthesized through a novel intermediate coordination strategy. Advanced characterizations and theoretical calculations well evidence that Zn single atoms are coordinated and stabilized on PCN in the form of Zn-N-6 configuration featured with an electron-deficient state. Such an electronic configuration has been demonstrated contributive to promoted electron excitation, accelerated charge separation and transfer as well as reduced water redox barriers. Further benefited from the abundant surface active sites derived from the 3D porous structure, Zn-PCN realizes visible-light photocatalysis for overall water splitting with H-2 and O-2 simultaneously evolved at a stoichiometric ratio of 2:1. This work brings new insights into the design of novel single-atom photocatalysts by deepening the understanding of electronic configurations and reactive sites favorable to excellent photocatalysis for water splitting and related solar energy conversion reactions.
Keyword ：
Overall water splitting Photocatalysis Polymeric carbon nitride Zn single atoms
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| GB/T 7714 | Zhao, Daming , Wang, Yiqing , Dong, Chung-Li et al. Electron-Deficient Zn-N-6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting [J]. | NANO-MICRO LETTERS , 2022 , 14 (1) . |
| MLA | Zhao, Daming et al. "Electron-Deficient Zn-N-6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting" . | NANO-MICRO LETTERS 14 . 1 (2022) . |
| APA | Zhao, Daming , Wang, Yiqing , Dong, Chung-Li , Meng, Fanqi , Huang, Yu-Cheng , Zhang, Qinghua et al. Electron-Deficient Zn-N-6 Configuration Enabling Polymeric Carbon Nitride for Visible-Light Photocatalytic Overall Water Splitting . | NANO-MICRO LETTERS , 2022 , 14 (1) . |
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