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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 ：
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 ：
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 ：
Carbon nitride-based photocatalysts hold an enormous potential in producing hydrogen. A strategy to simultaneously create isotype heterojunctions and active sites in highly-crystallized carbon nitride is anticipated to significantly boost the photocatalytic activity, but is yet to be realized. Herein, we find that cobalt salt added in the ionothermal synthesis can promote the phase transition of heptazine-based crystalline carbon nitride (CCN) to triazine-based poly(triazine imide) (PTI), rendering the creation of single-atom cobalt coordinated isotype CCN/PTI heterojunction. Co-CCN/PTI exhibits an appreciable apparent quantum yield of 20.88% at 425 nm for photocatalytic hydrogen production with a rate achieving 3538 mu mol h(-1) g(-1) (lambda & nbsp;> 420 nm), which is 4.8 times that of CCN and 27.6 times that of PTI. The high photocatalytic activity is attributed to the Type II isotype highly-crystallized CCN/PTI heterojunction for promoting charge carrier migration, and the single-atom Co sites for accelerating surface oxidation reaction. (C)& nbsp;2021 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
Keyword ：
Crystalline carbon nitride Isotype heterojunctions Photocatalytic hydrogen production Poly(triazine imide) Single-atom cobalt
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| GB/T 7714 | Shen, Shaohua , Chen, Jie , Wang, Yiqing et al. Boosting photocatalytic hydrogen production by creating isotype heterojunctions and single-atom active sites in highly-crystallized carbon nitride [J]. | SCIENCE BULLETIN , 2022 , 67 (5) : 520-528 . |
| MLA | Shen, Shaohua et al. "Boosting photocatalytic hydrogen production by creating isotype heterojunctions and single-atom active sites in highly-crystallized carbon nitride" . | SCIENCE BULLETIN 67 . 5 (2022) : 520-528 . |
| APA | Shen, Shaohua , Chen, Jie , Wang, Yiqing , Dong, Chung-Li , Meng, Fanqi , Zhang, Qinghua et al. Boosting photocatalytic hydrogen production by creating isotype heterojunctions and single-atom active sites in highly-crystallized carbon nitride . | SCIENCE BULLETIN , 2022 , 67 (5) , 520-528 . |
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Abstract ：
To solve surface carrier recombination and sluggish water oxidation kinetics of hematite (alpha-Fe2O3) photoanodes, herein, an attractive surface modification strategy is developed to successively deposit ultrathin CoOx overlayer and Ni single atoms on titanium (Ti)-doped alpha-Fe2O3 (Ti:Fe2O3) nanorods through a two-step atomic layer deposition (ALD) and photodeposition process. The collaborative decoration of ultrathin CoOx overlayer and Ni single atoms can trigger a big boost in photo-electrochemical (PEC) performance for water splitting over the obtained Ti:Fe2O3/CoOx/Ni photoanode, with the photocurrent density reaching 1.05 mA cm(-2) at 1.23 V vs. reversible hydrogen electrode (RHE), more than three times that of Ti:Fe2O3 (0.326 mA cm(-2)). Electrochemical and electronic investigations reveal that the surface passivation effect of ultrathin CoOx overlayer can reduce surface carrier recombination, while the catalysis effect of Ni single atoms can accelerate water oxidation kinetics. Moreover, theoretical calculations evidence that the synergy of ultrathin CoOx overlayer and Ni single atoms can lower the adsorption free energy of OH* intermediates and relieve the potential-determining step (PDS) for oxygen evolution reaction (OER). This work provides an exemplary modification through rational engineering of surface electrochemical and electronic properties for the improved PEC performances, which can be applied in other metal oxide semiconductors as well.
Keyword ：
hematite nanorods photo-electrochemical water splitting single-atom catalysts surface modification ultrathin overlayers
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| GB/T 7714 | Mao, Lianlian , Huang, Yu-Cheng , Deng, Hao et al. Synergy of Ultrathin CoOx Overlayer and Nickel Single Atoms on Hematite Nanorods for Efficient Photo-Electrochemical Water Splitting [J]. | SMALL , 2022 . |
| MLA | Mao, Lianlian et al. "Synergy of Ultrathin CoOx Overlayer and Nickel Single Atoms on Hematite Nanorods for Efficient Photo-Electrochemical Water Splitting" . | SMALL (2022) . |
| APA | Mao, Lianlian , Huang, Yu-Cheng , Deng, Hao , Meng, Fanqi , Fu, Yanming , Wang, Yiqing et al. Synergy of Ultrathin CoOx Overlayer and Nickel Single Atoms on Hematite Nanorods for Efficient Photo-Electrochemical Water Splitting . | SMALL , 2022 . |
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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 ：
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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