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Generative Artificial Intelligence Navigated Development of Solvents for Next Generation High-Performance Magnesium Batteries SCIE
期刊论文 | 2025 | ADVANCED MATERIALS
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Abstract :

Traditional trial-and-error methods are inefficient and costly in discovering novel solvents for next-generation magnesium (Mg) metal-based batteries. Therefore, this work establishes a simple yet efficient screening criterion for solvents by integrating artificial intelligence techniques with a virtual molecular database, potentially revolutionizing the traditional solvent design pathway. A total of 823 solvents are generated using a self-developed algorithm, and LUMO, Delta LUMO, ESPmin, ESPmax , and Eb are identified to establish the screening criterion through the analysis with machine learning (ML) models. Eighteen candidate solvents are successfully identified, and two of which are subsequently selected and experimentally validated, i.e., C1COCOC1 and COCC(C)OC (abbreviated as "DOX" and "DMP"). Notably, neither of these solvents has been previously reported for use in Mg batteries. Experimental results indicate that the DOX solvent, when paired with the Mg boron-based salt, i.e., Mg[B(hfip)4]2, can significantly enhance the electrochemical performance. At a current density of 1.0 mAcm-2, the average coulombic efficiency for Mg plating/stripping reaches 99.54 % after 5200 cycles. Furthermore, the Mg//Cu cell achieves a cumulative capacity exceeding 2000 mAhcm-2, surpassing previously reported results. In summary, this work establishes a virtual molecular database and develops a streamlined screening methodology for Mg battery solvents based on their physicochemical properties, reducing the candidate pool from 823 to 18 and improving efficiency by nearly 50-fold. This research paradigm is not limited to the development of Mg batteries and can be readily extended to the exploration of other battery systems.

Keyword :

dox dox generative artificial intelligence generative artificial intelligence mg metal batteries mg metal batteries solvent screening solvent screening virtual molecular database virtual molecular database

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GB/T 7714 Gao, Xiang , Yang, Ao-Qi , Yu, Wen-Bei et al. Generative Artificial Intelligence Navigated Development of Solvents for Next Generation High-Performance Magnesium Batteries [J]. | ADVANCED MATERIALS , 2025 .
MLA Gao, Xiang et al. "Generative Artificial Intelligence Navigated Development of Solvents for Next Generation High-Performance Magnesium Batteries" . | ADVANCED MATERIALS (2025) .
APA Gao, Xiang , Yang, Ao-Qi , Yu, Wen-Bei , Zhou, Jia-Cong , Pei, Mao-Jun , Chen, Jia-Cheng et al. Generative Artificial Intelligence Navigated Development of Solvents for Next Generation High-Performance Magnesium Batteries . | ADVANCED MATERIALS , 2025 .
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Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials SCIE
期刊论文 | 2025 , 37 (8) | ADVANCED MATERIALS
WoS CC Cited Count: 25
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Abstract :

Nitrate electroreduction is promising for achieving effluent waste-water treatment and ammonia production with respect to the global nitrogen balance. However, due to the impeded hydrogenation process, high overpotentials need to be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy is developed to optimize the interfacial H2O behavior for accelerating the hydrogenation conversion of nitrate to ammonia at ultralow overpotentials. The well-designed Ru & horbar;Ni(OH)(2) electrocatalyst shows a remarkable energy efficiency of 44.6% at +0.1 V versus RHE and a nearly 100% Faradaic efficiency for NH3 synthesis at 0 V versus RHE. In situ characterizations and theoretical calculations indicate that Ni(OH)(2) can regulate the interfacial H2O structure with a promoted H2O dissociation process and contribute to the spontaneous hydrogen spillover process for boosting NO3 (-) electroreduction to NH3 at Ru sites. Furthermore, the assembled rechargeable Zn-NO3 (-)/ethanol battery system exhibits an outstanding long-term cycling stability during the charge-discharge tests with the production of high-value-added ammonium acetate, showing great potential for simultaneously achieving nitrate removal, energy conversion, and chemical synthesis. This work can not only provide a guidance for interfacial H2O regulation in extensive hydrogenation reactions but also inspire the design of a novel hybrid flow battery with multiple functions.

Keyword :

ammonia synthesis ammonia synthesis hydrogen spillover hydrogen spillover interfacial H2O regulation interfacial H2O regulation nitrate electroreduction nitrate electroreduction rechargeable hybrid flow battery rechargeable hybrid flow battery ultralow overpotentials ultralow overpotentials

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GB/T 7714 Wan, Yuchi , Pei, Maojun , Tang, Yixiang et al. Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials [J]. | ADVANCED MATERIALS , 2025 , 37 (8) .
MLA Wan, Yuchi et al. "Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials" . | ADVANCED MATERIALS 37 . 8 (2025) .
APA Wan, Yuchi , Pei, Maojun , Tang, Yixiang , Liu, Yao , Yan, Wei , Zhang, Jiujun et al. Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials . | ADVANCED MATERIALS , 2025 , 37 (8) .
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Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials Scopus
期刊论文 | 2025 , 37 (8) | Advanced Materials
Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials EI
期刊论文 | 2025 , 37 (8) | Advanced Materials
Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes SCIE
期刊论文 | 2025 , 64 (23) | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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Abstract :

Passivation of magnesium (Mg) anode in the chloride-free magnesium bis(trifluoromethanesulfonyl)imide (Mg(TFSI)(2)) electrolyte is a key challenge for Mg metal batteries. Tailoring solvation structure and solid electrolyte interphase (SEI) has been considered an effective strategy. Herein, a series of imidazole co-solvents with different branched-chain structures (methyl, ethyl, and propyl) are introduced into the Mg(TFSI)(2)-ether electrolyte to address the passivation issue. The ion-solvent interaction, interfacial adsorption effect, and SEI formation are comprehensively studied by theoretical calculations and experimental characterizations. Through molecular structure analysis, the long-chain 1-propylimidazole (PrIm) exhibits a strong coordination ability to Mg2+ and a favorable parallel adsorption configuration on the Mg surface. As a result, PrIm co-solvent can not only restructure the solvation sheath of Mg2+, but also act as a dynamic protective shield to repel a part of TFSI- and 1,2-dimethoxyethane (DME) away from the Mg surface. Benefiting from the synergistic regulation effect of interfacial chemistry and ion-solvent interactions, the chloride-free Mg(TFSI)(2)-DME + PrIm electrolyte ensures minimal interface passivation and achieves highly reversible Mg plating/stripping. This work provides a guiding strategy for solvation structure regulation and interface engineering for rechargeable Mg metal batteries.

Keyword :

Adsorption Adsorption Imidazole co-solvent Imidazole co-solvent Magnesium metal battery Magnesium metal battery Mg(TFSI)(2) electrolyte Mg(TFSI)(2) electrolyte Solvation structure Solvation structure

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GB/T 7714 Yang, Aoqi , Gao, Xiang , Pei, Maojun et al. Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (23) .
MLA Yang, Aoqi et al. "Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 23 (2025) .
APA Yang, Aoqi , Gao, Xiang , Pei, Maojun , Zhou, Jiacong , Wang, Honggang , Liao, Can et al. Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (23) .
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Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes EI
期刊论文 | 2025 , 64 (23) | Angewandte Chemie - International Edition
Synergistic Effects of Interfacial Chemistry and Ion-Solvent Interactions to Enable Reversible Magnesium Metal Anode in Chloride-Free Mg(TFSI)2 Electrolytes Scopus
期刊论文 | 2025 , 64 (23) | Angewandte Chemie - International Edition
Modulating π - d Conjugated Coordination in Bionic Cu/Cu2O Heterojunctions for Efficient Photodegradation of Organic Contaminants SCIE
期刊论文 | 2025 , 10 (13) | ADVANCED MATERIALS TECHNOLOGIES
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Abstract :

In situ grown copper (Cu) metal is commonly integrated with Cu2O to enhance charge separation and improve photocatalytic degradation of azo dyes, such as Orange II and Methyl orange (MO). However, limited solvent diffusion remains a critical challenge for effective pollutant removal. Inspired by the dandelion structure, this work synthesizes a Cu/Cu2O composite with an interconnected nanotube structure and hollow nanosphere, facilitating solvent transport and increasing active surface area. The optimized Cu/Cu2O-S3 catalyst achieves 93 % photodegradation efficiency of Orange II and maintains 98 % stability over five cycles at a concentration of 100 mgL-1, significantly outperforming MO. While previous studies have attributed this performance to the dihedral angle and planarity of Orange II, the role of photogenerated electron transport at the catalyst-dye interface is largely overlooked. Here, this work reveals that electron transfer from the 3d orbitals of Cu transfer to the 2p energy levels of N, C, O atoms, enhancing carrier mobility and binding interactions. Moreover, the extra alpha-OH group in Orange II promotes uniform electronic distribution and planar pi-bond formation, further improving photocatalytic performance. These insights provide a deeper understanding of photocatalytic mechanisms and offer valuable strategies for designing more efficient catalysts.

Keyword :

cycling stability cycling stability orbital modulation orbital modulation photocatalytic degradation photocatalytic degradation pi - d conjugation pi - d conjugation

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GB/T 7714 Fu, Huan-Huan , Chen, Yu-Long , Xu, Bao-Ming et al. Modulating π - d Conjugated Coordination in Bionic Cu/Cu2O Heterojunctions for Efficient Photodegradation of Organic Contaminants [J]. | ADVANCED MATERIALS TECHNOLOGIES , 2025 , 10 (13) .
MLA Fu, Huan-Huan et al. "Modulating π - d Conjugated Coordination in Bionic Cu/Cu2O Heterojunctions for Efficient Photodegradation of Organic Contaminants" . | ADVANCED MATERIALS TECHNOLOGIES 10 . 13 (2025) .
APA Fu, Huan-Huan , Chen, Yu-Long , Xu, Bao-Ming , Liu, Yao , Yu, Wen-Bei , Li, Yu et al. Modulating π - d Conjugated Coordination in Bionic Cu/Cu2O Heterojunctions for Efficient Photodegradation of Organic Contaminants . | ADVANCED MATERIALS TECHNOLOGIES , 2025 , 10 (13) .
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Modulating π − d Conjugated Coordination in Bionic Cu/Cu2O Heterojunctions for Efficient Photodegradation of Organic Contaminants EI
期刊论文 | 2025 , 10 (13) | Advanced Materials Technologies
Modulating π − d Conjugated Coordination in Bionic Cu/Cu2O Heterojunctions for Efficient Photodegradation of Organic Contaminants Scopus
期刊论文 | 2025 , 10 (13) | Advanced Materials Technologies
A fluorinated artificial protection layer for wide temperature range and ultra-long cycle-life dendrite-free sodium metal battery SCIE
期刊论文 | 2025 , 517 | CHEMICAL ENGINEERING JOURNAL
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Abstract :

Sodium metal as the anodes for sodium metal batteries (SMBs) possess several advantages, including high theoretical capacity, high abundance and low-cost, which make SMBs formidable contenders for constructing alternative batteries to lithium-based ones. However, the presence of an undesirable solid electrolyte interface (SEI) between Na metal and liquid electrolyte can result in sluggish Na ion transfer kinetics, substantial consumption of electrolyte, and dendrite growth issues, particularly at ultra-low temperatures. To address these challenges, a three-dimensional (3D) artificial protection layer composed of Na3Bi and NaF (NBF) on the Na anode surface is successfully fabricated through a simple in-situ reaction. Both theoretical and experimental findings demonstrate that this artificial protection layer exhibits strong sodiophilicity, enhanced ionic conductivity, excellent and electronic insulation property, which can effectively suppress the continuous electrolyte decomposition. As a result, at low operating temperatures (-30 degrees C), such an NBF symmetric cell achieves a long cycle life of over 1400 h (0.1 mA cm-2@ 0.1 mAh cm-2). And the electrochemical performance of NBF is exceptional when it is utilized as the anodes in symmetric cells, demonstrating a cycle-life exceeding 2390 h at 0.5 mA cm-2@0.5 mAh cm-2, and also in sodium metal full cells at 5C, exhibiting over 2000 cycles. Therefore, the results provide support for the possibility of utilizing the artificial protection layer in developing a safeguarding coating for sodium metal anodes.

Keyword :

Artificial protection layer Artificial protection layer Dendrite growth Dendrite growth Electrolyte decomposition Electrolyte decomposition Long cycle-life Long cycle-life Sodium metal battery Sodium metal battery Wide temperature range Wide temperature range

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GB/T 7714 Qi, Jing , Liu, Yao , Pei, Maojun et al. A fluorinated artificial protection layer for wide temperature range and ultra-long cycle-life dendrite-free sodium metal battery [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 517 .
MLA Qi, Jing et al. "A fluorinated artificial protection layer for wide temperature range and ultra-long cycle-life dendrite-free sodium metal battery" . | CHEMICAL ENGINEERING JOURNAL 517 (2025) .
APA Qi, Jing , Liu, Yao , Pei, Maojun , Jiang, Yidong , Luo, Yiyuan , Ma, Dakai et al. A fluorinated artificial protection layer for wide temperature range and ultra-long cycle-life dendrite-free sodium metal battery . | CHEMICAL ENGINEERING JOURNAL , 2025 , 517 .
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A fluorinated artificial protection layer for wide temperature range and ultra-long cycle-life dendrite-free sodium metal battery EI
期刊论文 | 2025 , 517 | Chemical Engineering Journal
A fluorinated artificial protection layer for wide temperature range and ultra-long cycle-life dendrite-free sodium metal battery Scopus
期刊论文 | 2025 , 517 | Chemical Engineering Journal
Machine Learning-Assisted Molecular Orbital Insights into OER Activity Descriptors of Component Gradient Ni-Based LDH Electrocatalysts SCIE
期刊论文 | 2025 , 21 (32) | SMALL
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Abstract :

The conventional theories to predict the oxygen evolution reaction (OER) performance in electrochemical water-electrolysis, including the d-band center and the e(g) orbital occupancy, encounter limitations under specific conditions. The d-band center serves as a partial descriptor of adsorption energy, leading to inconsistencies, and the e(g) orbital occupancy theory underestimates the contributions of other orbitals. Here, a machine learning-assisted molecular orbital investigation is conducted to explore 3d orbitals characteristics. To account for the crystal field effect and mitigate partition errors arising from orbital degeneracy, 3d orbitals are categorized into e(g) and t(2g). The proposed descriptors are designed not only to predict performance but also to aid in elucidating the underlying determinants of performance. It elucidates nuanced performance determinants that are context-dependent and can be categorized into two distinct types: electron-deficient, e.g., Fe (3d(6)) and Co (3d(7)), and electron-rich, e.g., Cu (3d(9)) and Zn (3d(10)). For electron-deficient metals, the orbitals are unoccupied, with the electrons populating the t(2g) orbital preferentially released as the valence state increases, thereby influencing performance, and vice versa. In summary, this work establishes a complex correlation between molecular orbitals and catalytic activity via ML, offering a novel perspective for advancing the design and elucidating the mechanisms of high-performance OER electrocatalysts.

Keyword :

e(g)/t(2g) e(g)/t(2g) electron-rich/electron-deficient electron-rich/electron-deficient LDH LDH machine learning machine learning molecular orbital molecular orbital

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GB/T 7714 Pei, Mao-Jun , Gao, Xiang , Shuai, Yan-Kang et al. Machine Learning-Assisted Molecular Orbital Insights into OER Activity Descriptors of Component Gradient Ni-Based LDH Electrocatalysts [J]. | SMALL , 2025 , 21 (32) .
MLA Pei, Mao-Jun et al. "Machine Learning-Assisted Molecular Orbital Insights into OER Activity Descriptors of Component Gradient Ni-Based LDH Electrocatalysts" . | SMALL 21 . 32 (2025) .
APA Pei, Mao-Jun , Gao, Xiang , Shuai, Yan-Kang , Xu, Jia-Ming , Chen, Jia-Cheng , Zeng, Qing et al. Machine Learning-Assisted Molecular Orbital Insights into OER Activity Descriptors of Component Gradient Ni-Based LDH Electrocatalysts . | SMALL , 2025 , 21 (32) .
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Machine Learning-Assisted Molecular Orbital Insights into OER Activity Descriptors of Component Gradient Ni-Based LDH Electrocatalysts EI
期刊论文 | 2025 , 21 (32) | Small
Machine Learning-Assisted Molecular Orbital Insights into OER Activity Descriptors of Component Gradient Ni-Based LDH Electrocatalysts Scopus
期刊论文 | 2025 | Small
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 SCIE
期刊论文 | 2024 , 653 , 1704-1714 | JOURNAL OF COLLOID AND INTERFACE SCIENCE
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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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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 Scopus
期刊论文 | 2024 , 653 , 1704-1714 | Journal of Colloid and Interface Science
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 EI
期刊论文 | 2024 , 653 , 1704-1714 | Journal of Colloid and Interface Science
Advanced Ru/Ti 4 O 7 catalyst for Tolerating CO and H 2 S poisoning to hydrogen oxidation reaction SCIE
期刊论文 | 2024 , 65 , 205-214 | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
WoS CC Cited Count: 2
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Abstract :

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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Advanced Ru/Ti4O7 catalyst for Tolerating CO and H2S poisoning to hydrogen oxidation reaction Scopus
期刊论文 | 2024 , 65 , 205-214 | International Journal of Hydrogen Energy
Advanced Ru/Ti4O7 catalyst for Tolerating CO and H2S poisoning to hydrogen oxidation reaction EI
期刊论文 | 2024 , 65 , 205-214 | International Journal of Hydrogen Energy
Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction SCIE CSCD
期刊论文 | 2024 , 92 , 95-103 | JOURNAL OF ENERGY CHEMISTRY
WoS CC Cited Count: 10
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Abstract :

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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Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction Scopus CSCD
期刊论文 | 2024 , 92 , 95-103 | Journal of Energy Chemistry
Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction
期刊论文 | 2024 , 92 (5) , 95-103 | 能源化学
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Abstract :

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 cat-alytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely mod-ulate 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 inter-mediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condi-tion 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 opti-mize the reaction path of CER and thus to enhance the intrinsic CER activity significantly.Our work fig-ures 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.

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GB/T 7714 Linke Cai , Yao Liu , Jingfang Zhang et al. Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction [J]. | 能源化学 , 2024 , 92 (5) : 95-103 .
MLA Linke Cai et al. "Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction" . | 能源化学 92 . 5 (2024) : 95-103 .
APA Linke Cai , Yao Liu , Jingfang Zhang , Qiqi Jia , Jiacheng Guan , Hongwei Sun et al. Unveiling the geometric site dependent activity of spinel Co3O4 for electrocatalytic chlorine evolution reaction . | 能源化学 , 2024 , 92 (5) , 95-103 .
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