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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 ：
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 ：
ABSTRACT: Modulating the band alignment of semiconducting photoelectrodes is essential for efficient carrier transport and consequently optimized photoelectrochemical performances. Herein, a CdS/TiO2 bilayer is coated on a CdTe absorber via chemical bath deposition and magnetron sputtering, successively, to build directional interfacial charge transfer channels for efficient photoelectrochemical hydrogen evolution. The obtained multilayered CdTe/CdS/TiO2/Pt photocathode yields a dramatically increased photocurrent density of ???9.6 mA cm???2 at ???0.4 V vs reversible hydrogen electrode (RHE) under simulated sunlight (AM 1.5 G, 100 mW cm???2). It is well evidenced that, with the CdS/TiO2 bilayer coated onto CdTe, the CdTe/CdS/TiO2 heterojunction, with a well aligned band structure, generates favorable conduction band offset, energetically facilitating electron transfer from CdTe to CdS, and then to TiO2. Moreover, the CdTe/CdS/TiO2/Pt photocathode shows good stability for water reduction due to the TiO2 protective layer stabilizing against the photocorrosion of CdTe/CdS. This study provides referable guidance for designing multilayer photoelectrodes for stable and efficient solar water splitting from the viewpoint of interface energetics engineering.
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| GB/T 7714 | Chen, Xiangyan , Yin, Zhuocheng , Cao, Kun et al. Building Directional Charge Transport Channel in CdTe-Based Multilayered Photocathode for Efficient Photoelectrochemical Hydrogen Evolution [J]. | ACS MATERIALS LETTERS , 2022 , 4 (8) : 1381-1388 . |
| MLA | Chen, Xiangyan et al. "Building Directional Charge Transport Channel in CdTe-Based Multilayered Photocathode for Efficient Photoelectrochemical Hydrogen Evolution" . | ACS MATERIALS LETTERS 4 . 8 (2022) : 1381-1388 . |
| APA | Chen, Xiangyan , Yin, Zhuocheng , Cao, Kun , Shen, Shaohua . Building Directional Charge Transport Channel in CdTe-Based Multilayered Photocathode for Efficient Photoelectrochemical Hydrogen Evolution . | ACS MATERIALS LETTERS , 2022 , 4 (8) , 1381-1388 . |
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Abstract ：
n-Si, believed as a promising photoanode candidate, has suffered from sluggish oxygen evolution reaction (OER) kinetics and poor chemical stability when exposed to aqueous electrolyte. Herein, CoOx/Ni:CoOOH bilayers were successfully deposited on n-Si substrate by atomic layer-deposition (ALD) and photoassisted electrochemical deposition (PED) for stabilizing and catalyzing photoelectrochemical (PEC) water oxidation. In comparison to the n-Si/CoOx photoanode as reference, the prepared n-Si/CoOx/Ni:CoOOH photoanode upon the optimized PED process presents a much improved PEC performance for water splitting, with the onset potential cathodically shifted to similar to 1.03 V vs. reversible hydrogen electrode (RHE) and the photocurrent density much increased to 20 mA cm(-2) at 1.23 V vs. RHE. It is revealed that the introduction of Ni dopants increases the work functions of the deposited Ni:CoOOH overlayers, which gives rise to the upward band bending weakened at the n-Si/CoOx/Ni:CoOOH cascading interface while strengthened at the Ni:CoOOH/electrolyte interface (with the band bending shifted from downward to upward), contributing to the decreased and the increased driving forces for charge transfer at the interfaces, respectively. Then, the balanced driving forces at the interfaces would endow the n-Si/CoOx/Ni:CoOOH photoanode with the best PEC performance. Moreover, PED has been evidenced superior to ED to dope Ni into CoOOH with the formed overlayer effectively catalyzing and stabilizing PEC water splitting.
Keyword ：
n-Si photoanode photoelectrochemical water splitting work function
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| GB/T 7714 | Yin, Zhuocheng , Shi, Yuchuan , Shen, Shaohua . A n-Si/CoOx/Ni:CoOOH photoanode producing 600 mV photovoltage for efficient photoelectrochemical water splitting [J]. | SCIENCE CHINA-MATERIALS , 2022 , 65 (12) : 3442-3451 . |
| MLA | Yin, Zhuocheng et al. "A n-Si/CoOx/Ni:CoOOH photoanode producing 600 mV photovoltage for efficient photoelectrochemical water splitting" . | SCIENCE CHINA-MATERIALS 65 . 12 (2022) : 3442-3451 . |
| APA | Yin, Zhuocheng , Shi, Yuchuan , Shen, Shaohua . A n-Si/CoOx/Ni:CoOOH photoanode producing 600 mV photovoltage for efficient photoelectrochemical water splitting . | SCIENCE CHINA-MATERIALS , 2022 , 65 (12) , 3442-3451 . |
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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 ：
To improve the photocatalytic efficiency and realize the scaling up of photocatalytic hydrogen evolution reactions, the hydrodynamic distribution of particulate photocatalysts should be thoroughly understood through direct experimental observations and reasonable theoretical analysis. In this study, detailed investigations were conducted to reveal the shear-induced distribution of TiO2 photocatalyst suspensions dominated by laminar shear and gravity at different particle concentrations. Clusters with dense and compact structures were inevitably formed in an ultrasonication-pretreated TiO2 suspension without shear flow, owing to particle aggregation in the electrostatically controlled regime. Under the application of shear, with shear competing with the potential barrier, the particle aggregation would transition from a slow electrostatically controlled mode to a fast shear-controlled mode, with the formation of loose and fractal clusters, resulting in improved light absorption. Both the structure and size distributions of TiO2 clusters in suspensions could be determined by the applied shear via two effects, namely, cluster separation and restructuring, leading to reduced cluster sizes, and cluster collective settling, contributing to cluster growth. Considering these two rivalrous effects, the sizes of the formed clusters in suspensions initially increased and then decreased with the increasing shear rates. The applied shear could delay the cluster settling through a downward spiral trajectory, resulting in a long-term suspension of photocatalyst clusters for the prolonged solar illumination. Furthermore, at the increased particle concentrations, the cluster growth could be suppressed at relatively low shear rates, thus contributing to a homogeneous distribution of cluster sizes. This study deepens the understanding of particulate photocatalyst behaviors in hydrodynamic conditions and helps analyze potential strategies to optimize the solid-phase distribution in scaled-up photocatalytic water splitting systems.
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| GB/T 7714 | Hu, Xiaowei , Jiang, Heqing , Ma, Chenyu et al. Shear-Induced Aggregation and Distribution in Photocatalysis Suspension System for Hydrogen Production [J]. | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2022 , 61 (19) : 6722-6732 . |
| MLA | Hu, Xiaowei et al. "Shear-Induced Aggregation and Distribution in Photocatalysis Suspension System for Hydrogen Production" . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 61 . 19 (2022) : 6722-6732 . |
| APA | Hu, Xiaowei , Jiang, Heqing , Ma, Chenyu , Duan, Shuna , Wang, Yechun , Shi, Jinwen et al. Shear-Induced Aggregation and Distribution in Photocatalysis Suspension System for Hydrogen Production . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2022 , 61 (19) , 6722-6732 . |
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Abstract ：
In fabricating an artificial photosynthesis (AP) electrode for water oxidation, we have devised a semiconductor-mediator-catalyst structure that mimics photosystem II (PSII). It is based on a surface layer of vertically grown nanorods of Fe2O3 on fluorine doped tin oxide (FTO) electrodes with a carbazole mediator base and a Ru(II) carbene complex on a nanolayer of TiO2 as a water oxidation co-catalyst. The resulting hybrid assembly, FTO|Fe2O3|-carbazole|TiO2|-Ru(carbene), demonstrates an enhanced photoelectrochemical (PEC) water oxidation performance compared to an electrode without the added carbaozle base with an increase in photocurrent density of 2.2-fold at 0.95 V vs. NHE and a negatively shifted onset potential of 500 mV. The enhanced PEC performance is attributable to carbazole mediator accelerated interfacial hole transfer from Fe2O3 to the Ru(II) carbene co-catalyst, with an improved effective surface area for the water oxidation reaction and reduced charge transfer resistance.
Keyword ：
heterogeneous catalysis photocatalysis photoelectrochemistry water oxidation water splitting
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| GB/T 7714 | Niu, Fujun , Wang, Degao , Williams, Lenzi J. et al. A Semiconductor-Mediator-Catalyst Artificial Photosynthetic System for Photoelectrochemical Water Oxidation [J]. | CHEMISTRY-A EUROPEAN JOURNAL , 2022 , 28 (10) . |
| MLA | Niu, Fujun et al. "A Semiconductor-Mediator-Catalyst Artificial Photosynthetic System for Photoelectrochemical Water Oxidation" . | CHEMISTRY-A EUROPEAN JOURNAL 28 . 10 (2022) . |
| APA | Niu, Fujun , Wang, Degao , Williams, Lenzi J. , Nayak, Animesh , Li, Fei , Chen, Xiangyan et al. A Semiconductor-Mediator-Catalyst Artificial Photosynthetic System for Photoelectrochemical Water Oxidation . | CHEMISTRY-A EUROPEAN JOURNAL , 2022 , 28 (10) . |
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Abstract ：
Charge-carrier separation is regarded as one of the critical issues of photocatalytic water splitting and could be accelerated by constructing microscopic junctions in photocatalysts. Homojunction photocatalysts consisting of different forms of semiconductor with identical compositions could inherit the advantages of heterojunction-based photocatalysts in charge separation due to the built-in electric field, while omitting the potential drawbacks of interfacial lattice distortion by providing continuous band bonding. Therefore, homojunction-based photocatalysts have recently drawn growing attention in water splitting. In this review, the synthetic approaches to preparing photocatalysts with various homojunction structures including p-n junction, phase junction, and facet junction were introduced, together with a comprehensive analysis and discussion on the latest progress in the application of photocatalytic water splitting. This review work is expected to inspire more related work with promoted research on designing efficient homojunction-based photocatalytic systems for water splitting.
Keyword ：
charge separation homojunction photocatalytic water splitting
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| GB/T 7714 | Guan, Xiangjiu , Zong, Shichao , Shen, Shaohua . Homojunction photocatalysts for water splitting [J]. | NANO RESEARCH , 2022 , 15 (12) : 10171-10184 . |
| MLA | Guan, Xiangjiu et al. "Homojunction photocatalysts for water splitting" . | NANO RESEARCH 15 . 12 (2022) : 10171-10184 . |
| APA | Guan, Xiangjiu , Zong, Shichao , Shen, Shaohua . Homojunction photocatalysts for water splitting . | NANO RESEARCH , 2022 , 15 (12) , 10171-10184 . |
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