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学者姓名：刘尧
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Abstract ：
The large overpotential required for oxygen evolution reaction (OER) is one of the major factors limiting the efficiency of electrochemical water-electrolysis for hydrogen production. In this work, to decrease OER energy barrier and obtain low overpotential, amorphous-crystalline NiCo(OH)2 nanoplates are in-situ grown on nickel foam surface to form a catalyst-based electrode (ac-NiCo(OH)2/NF) for water-electrolysis application. As the inner amorphization of NiCo(OH)2 results in increased electron density of the metal sites, leading to the formation of tensile Ni-O bond, the coordinatively unsaturated Ni sites in the down-shift d-band centers toward Fermi level can lower the anti-bonding states. This can lead to optimized adsorption and desorption energies for oxygen-containing intermediates for OER. As expected, the prepared ac-NiCo(OH)2/NF electrode presents a low overpotential of 364 mV to deliver 1000 mA cm-2 toward OER with impressively high robust stability. When this electrocatalyst electrode serves as both the anode and cathode, the assembled anion exchange membrane (AEM) electrolyser only needs a cell voltage of 1.68 V to drive the overall water-electrolysis process at a current density of 10 mA cm-2.
Keyword ：
AEM electrolyser AEM electrolyser Amorphous-crystalline Amorphous-crystalline High current density High current density Oxygen evolution Oxygen evolution Unsaturated atoms Unsaturated atoms
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| GB/T 7714 | Ju, Shang , Liu, Yao , Pei, Maojun et al. Amorphization-induced abundant coordinatively unsaturated Ni active sites in NiCo(OH)2 for boosting catalytic OER and HER activities at high current densities for water-electrolysis [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 653 : 1704-1714 . |
| MLA | Ju, Shang et al. "Amorphization-induced abundant coordinatively unsaturated Ni active sites in NiCo(OH)2 for boosting catalytic OER and HER activities at high current densities for water-electrolysis" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 653 (2024) : 1704-1714 . |
| APA | Ju, Shang , Liu, Yao , Pei, Maojun , Shuai, Yankang , Zhai, Zibo , Yan, Wei et al. Amorphization-induced abundant coordinatively unsaturated Ni active sites in NiCo(OH)2 for boosting catalytic OER and HER activities at high current densities for water-electrolysis . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 653 , 1704-1714 . |
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The oxygen evolution reaction (OER) performance of NiCo LDH electrocatalysts can be improved through fluorine doping. The roles of Ni and Co active sites in such catalysts remain ambiguous and controversial. In addressing the issue, this study draws upon the molecular orbital theory and proposes the active center competitive mechanism between Ni and Co. The doped F-atoms can directly impact the valence state of metal atoms or exert an indirect influence through the dehydrogenation, thereby modulating the active center. As the F-atoms are progressively aggregate, the e(g) orbitals of Ni and Co transition from e(g)(2) to e(g)(1), and subsequently to e(g)(0). The corresponding valence state elevates from +2 to +3, and then to +4, signifying an initial increase followed by a subsequent decrease in the electrocatalytic performance. Furthermore, a series of F-NiCo LDH catalysts are synthesized to verify the e(g) orbital occupancy analysis, and the catalytic OER overpotentials are 303, 243, 240, and 246 mV at the current density of 10 mA cm(-2), respectively, which coincides well with the theoretical prediction. This investigation not only provides novel mechanistic insights into the transition and competition of Ni and Co in F-NiCo LDH catalysts but also establishes a foundation for the design of high-performance catalysts.
Keyword ：
competitive mechanism competitive mechanism dehydrogenation dehydrogenation e(g) orbital occupancy e(g) orbital occupancy F-NiCo LDH electrocatalyst F-NiCo LDH electrocatalyst valence state valence state
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| GB/T 7714 | Pei, Mao-Jun , Shuai, Yan-Kang , Gao, Xiang et al. Ni and Co Active Site Transition and Competition in Fluorine-Doped NiCo(OH)2 LDH Electrocatalysts for Oxygen Evolution Reaction [J]. | SMALL , 2024 , 20 (31) . |
| MLA | Pei, Mao-Jun et al. "Ni and Co Active Site Transition and Competition in Fluorine-Doped NiCo(OH)2 LDH Electrocatalysts for Oxygen Evolution Reaction" . | SMALL 20 . 31 (2024) . |
| APA | Pei, Mao-Jun , Shuai, Yan-Kang , Gao, Xiang , Chen, Jia-Cheng , Liu, Yao , Yan, Wei et al. Ni and Co Active Site Transition and Competition in Fluorine-Doped NiCo(OH)2 LDH Electrocatalysts for Oxygen Evolution Reaction . | SMALL , 2024 , 20 (31) . |
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Spinel cobalt oxide (Co3O4), consisting of tetrahedral Co2+ (CoTd) and octahedral Co3+ (CoOh), is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction (CER). Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost CER. Herein, combining density functional theory calculations and experiment results assisted with operando analysis, we found that the CoOh site acts as the main active site for CER in spinel Co3O4, which shows better Cl- adsorption and more moderate intermediate adsorption toward CER than CoTd site, and does not undergo redox transition under CER condition at applied potentials. Guided by above findings, the oxygen vacancies were further introduced into the Co3O4 to precisely manipulate the electronic configuration of CoOh to boost Cl- adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity significantly. Our work figures out the importance of geometric configuration dependent CER activity, shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level. (c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press
Keyword ：
Active chlorine Active chlorine Chlorine evolution reaction Chlorine evolution reaction Electronic configuration optimization Electronic configuration optimization Geometry effects Geometry effects Spinel oxides Spinel oxides
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| GB/T 7714 | Cai, Linke , Liu, Yao , Zhang, Jingfang et al. Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction [J]. | JOURNAL OF ENERGY CHEMISTRY , 2024 , 92 : 95-103 . |
| MLA | Cai, Linke et al. "Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction" . | JOURNAL OF ENERGY CHEMISTRY 92 (2024) : 95-103 . |
| APA | Cai, Linke , Liu, Yao , Zhang, Jingfang , Jia, Qiqi , Guan, Jiacheng , Sun, Hongwei et al. Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction . | JOURNAL OF ENERGY CHEMISTRY , 2024 , 92 , 95-103 . |
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CO and H 2 S poisoning of Pt -based catalysts for hydrogen oxidation reaction (HOR) stands as one of the longstanding hindrances to the widespread commercialization of proton exchange membrane fuel cells. In this paper, a Ru/Ti 4 O 7 catalyst is successfully synthesized by the microwave -thermal method. This Ru/Ti 4 O 7 catalyst shows a much higher noble metal mass activity than those of commercial PtRu/C and conventional Ru/C catalysts. The performance of the Ru/Ti 4 O 7 catalyst under the exist of CO or H 2 S shows insignificant current decay, which is far superior to commercial PtRu/C and Pt/C catalysts. In this Ru/Ti 4 O 7 catalyst, the electron transfer between Ru and Ti to form d -p orbital hybridization is considered to be responsible for the favorable catalytic HOR performance and the corresponding CO and H 2 S tolerance. The interaction mechanism formed by electron transfer may open a promising way for the subsequent development of anti -poisoning catalysts for PEM fuel cell hydrogen oxidation reaction.
Keyword ：
CO poisoning CO poisoning H2 H2 Hydrogen oxidation reaction Hydrogen oxidation reaction PEM fuel cell PEM fuel cell
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| GB/T 7714 | Xie, Yujie , Lian, Bianyong , Deng, Shuqi et al. Advanced Ru/Ti 4 O 7 catalyst for Tolerating CO and H 2 S poisoning to hydrogen oxidation reaction [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2024 , 65 : 205-214 . |
| MLA | Xie, Yujie et al. "Advanced Ru/Ti 4 O 7 catalyst for Tolerating CO and H 2 S poisoning to hydrogen oxidation reaction" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 65 (2024) : 205-214 . |
| APA | Xie, Yujie , Lian, Bianyong , Deng, Shuqi , Lin, Qingqu , Wang, Kaili , Zheng, Yun et al. Advanced Ru/Ti 4 O 7 catalyst for Tolerating CO and H 2 S poisoning to hydrogen oxidation reaction . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2024 , 65 , 205-214 . |
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The low utilization of photogenerated carriers and the limited diffusion of solvents are the major bottlenecks of Cu2O-based photocatalysts for organic pollutant removal. In the effort to overcome these issues, this work, based on the DFT calculations and inspired by the dandelion structure, successfully synthesized nanostructured Cu/Cu2O photocatalysts with effective solvent diffusion channels and high carrier utilization. These catalysts with interconnected nanotube structure (the "stem") and hollow nanosphere morphology containing active facets (the "fruit") not only show increased reaction sites, but also contain the Cu/Cu2O heterojunction for facilitating the transfer and separation of photogenerated carriers at the interface. Consequently, the as-prepared Cu/Cu2O-4 nanocatalyst delivers excellent photocatalytic performance, that is, the removal efficiency of high-concentration Orange II (100 mg L-1) reaches 90% within 10 min and can be maintained at 90.4% after four cycles. This work provides a promising route for the construction of high-performance catalysts, as well as the mechanism for study of organic pollutant removal.
Keyword ：
carrier utilization carrier utilization Cu2O Cu2O dandelion design dandelion design diffusion channel diffusion channel heterojunction heterojunction nanostructured Cu nanostructured Cu photocatalytic degradation photocatalytic degradation
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| GB/T 7714 | Yu, Wen-Bei , Yi, Ming , Fu, Huan-Huan et al. Dandelion-Like Nanostructured Cu/Cu2O Heterojunctions with Fast Diffusion Channels Enabling Rapid Photocatalytic Pollutant Removal [J]. | ACS APPLIED NANO MATERIALS , 2023 , 6 (4) : 2928-2941 . |
| MLA | Yu, Wen-Bei et al. "Dandelion-Like Nanostructured Cu/Cu2O Heterojunctions with Fast Diffusion Channels Enabling Rapid Photocatalytic Pollutant Removal" . | ACS APPLIED NANO MATERIALS 6 . 4 (2023) : 2928-2941 . |
| APA | Yu, Wen-Bei , Yi, Ming , Fu, Huan-Huan , Pei, Mao-Jun , Liu, Yao , Xu, Bao-Ming et al. Dandelion-Like Nanostructured Cu/Cu2O Heterojunctions with Fast Diffusion Channels Enabling Rapid Photocatalytic Pollutant Removal . | ACS APPLIED NANO MATERIALS , 2023 , 6 (4) , 2928-2941 . |
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Layered double hydroxide (LDH) catalysts provide promising OER activity which can be employed in overall water splitting for hydrogen production. However, their weak surface hydrogen adsorption (H-ad) and high water dissociation energy can result in the inferior hydrogen evolution reactions (HER) activity. In this paper, a highly efficient HER catalyst of F-doped NiCoMo LDH is successfully designed and synthesized through in situ growing on nickel foam (F-NiCoMo LDH/NF) for overall water splitting. DFT calculations demonstrate that the introduction of Mo and F atoms in NiCo LDH can induce the generation of anisotropic lattice strain, resulting in the generation of high-energy active interface and shifting the d-band centers. Therefore, the adsorption energy of H-ad is optimized and the water dissociation energy barrier is decreased. As a result, this F-NiCoMo LDH/NF catalyst electrode displays a low overpotential of 107.5 mV at 10 mA cm(-2) and a small Tafel slope of 67.2 mV dec(-1) for HER. The assembled electrolyzer by employing this catalyst electrode requires only 1.83 V to deliver 300 mA cm(-2) and operates stably for 100 h.
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| GB/T 7714 | Zhai, Zibo , Li, Hongwei , Zhou, Chuang-an et al. Anisotropic Strain Boosted Hydrogen Evolution Reaction Activity of F-NiCoMo LDH for Overall Water Splitting [J]. | JOURNAL OF THE ELECTROCHEMICAL SOCIETY , 2023 , 170 (3) . |
| MLA | Zhai, Zibo et al. "Anisotropic Strain Boosted Hydrogen Evolution Reaction Activity of F-NiCoMo LDH for Overall Water Splitting" . | JOURNAL OF THE ELECTROCHEMICAL SOCIETY 170 . 3 (2023) . |
| APA | Zhai, Zibo , Li, Hongwei , Zhou, Chuang-an , Zheng, Hui , Liu, Yao , Yan, Wei et al. Anisotropic Strain Boosted Hydrogen Evolution Reaction Activity of F-NiCoMo LDH for Overall Water Splitting . | JOURNAL OF THE ELECTROCHEMICAL SOCIETY , 2023 , 170 (3) . |
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In this paper, carbon-matrix-embedded Mott-Schottky (MS) heterojunction of CoS2/NiS2 (CoS2/NiS2@C) is prepared. The obtained CoS2/NiS2@C offers superior sodium storage performance such as large specific capacity (861.0 mAh/g at 2 A/g), extraordinary rate capability (649.2 mAh/g at 10 A/g, 371.4 mAh/g at 40 A/g) and excellent cycling stability (380.5 mAh/g after 3000 cycles at 10 A/g, and 298.5 mAh/g after 2000 cycles at 40 A/ g). Electrochemical measurements and density functional theory (DFT) calculations as well as in/ex-situ characterization techniques are employed to reveal the underlying mechanisms. It is found that the outperforming sodium storage properties of CoS2/NiS2@C can be mainly attributed to the C-S bond and the MS heterojunction. The C-S bond formed at the interface between CoS2/NiS2 and the carbon matrix promotes the migration of the sodium ions in the carbon matrix to the embedded CoS2/NiS2, while the MS heterojunction accelerates the electrochemical reaction kinetics of CoS2/NiS2. Moreover, full-cell is assembled with CoS2/NiS2@C and Na3V2(PO4)3/C to validate the practical application of CoS2/NiS2@C. The full-cell achieves both high specific capacity and outstanding rate performance, demonstrating the great application potential of such CoS2/NiS2@C anode in high-performance sodium-ion batteries.
Keyword ：
Anode materials Anode materials C-S covalent bond C-S covalent bond Mott -Schottky heterojunction Mott -Schottky heterojunction Sodium-ion batteries Sodium-ion batteries Transition metal sulfides Transition metal sulfides
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| GB/T 7714 | Zheng, Hui , Pei, Maojun , Qiu, Ruoxue et al. High-Capacity and High-Rate sodium storage of CoS2/NiS2@C anode material enabled by interfacial C-S covalent bond and Mott-Schottky heterojunction [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 476 . |
| MLA | Zheng, Hui et al. "High-Capacity and High-Rate sodium storage of CoS2/NiS2@C anode material enabled by interfacial C-S covalent bond and Mott-Schottky heterojunction" . | CHEMICAL ENGINEERING JOURNAL 476 (2023) . |
| APA | Zheng, Hui , Pei, Maojun , Qiu, Ruoxue , Ma, Dakai , Deng, Shuqi , Jiao, Xuechao et al. High-Capacity and High-Rate sodium storage of CoS2/NiS2@C anode material enabled by interfacial C-S covalent bond and Mott-Schottky heterojunction . | CHEMICAL ENGINEERING JOURNAL , 2023 , 476 . |
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