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Cobalt-embedded few-layered carbon nanosheets toward enhanced hydrogen evolution:Rational design and insight into structure-performance correlation

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Journal of Energy Chemistry 2021年第7期30卷 156-161页

作者： Liwen Xing Hongyi Gao Dandan Jia Xiao Chen Mengyi Han Junjun Lv Ang Li Ge Wang Xingtian Shu Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology Beijing30 Xueyuan RoadBeijing 100083China Research Institute of Petroleum Processing SINOPECBeijing 100083China Institute of Advanced Materials Beijing Normal UniversityBeijing 100875China School of Chemistry Biology and Materials Engineering Suzhou University of Science and TechnologySuzhou 215009JiangsuChina Shunde Graduate School University of Science and Technology BeijingFoshan 528399GuangdongChina

Over the past decades, the energy and concomitant environment issues, such as energy shortage, air pollution and global warming, have been becoming increasingly striking world-wide challenges [1,2]. Such a dilemma in ... 详细信息

关键词： Electrocatalyst Metal-organic frameworks Carbon nanosheets Hydrogen evolution reaction structure-performance correlation

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Leveraging Dual-Atom Catalysts for Electrocatalysis Revitalization: Exploring the structure-performance correlation

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ADVANCED ENERGY MATERIALS 2024年第18期14卷 2303281-2303281页

作者： Wong, Man-Kei Foo, Joel Jie Loh, Jian Yiing Ong, Wee-Jun Xiamen Univ Malaysia Sch Energy & Chem Engn Sepang 43900 Selangor Darul Malaysia Xiamen Univ Malaysia Ctr Excellence NaNo Energy & Catalysis Technol CON Sepang 43900 Selangor Darul Malaysia Xiamen Univ Coll Chem & Chem Engn State Key Lab Phys Chem Solid Surfaces Xiamen 361005 Peoples R China Xiamen Univ Gulei Innovat Inst Zhangzhou 363200 Peoples R China Xiamen Univ Shenzhen Res Inst Shenzhen 518057 Peoples R China

In light of the profound shift toward renewable fuels, dual-atom catalysts (DACs) are impressively prospected as auspicious catalysts for electrocatalysis revitalization, toward accomplishing environmental remediation and sustainable global energy security. Leveraging appealing attributes such as inspiring synergistic effect, additional adjacent adsorption sites, and ultrahigh atom utilization, DACs are endowed with unprecedented stability, activity, and selectivity in multifarious energy-related applications. By virtue of addressing time and technological prominence to review this ground-breaking atomic electrocatalyst, this review first encompasses a correlation elucidation between the substrate, dual-atoms, and facile synthetic approaches with intriguing modification strategies. Furthermore, the state-of-the-art characterization techniques specially employed for DACs are spotlighted, alongside rigorously unveiling the novel mechanistic insights' milestone gained from both theoretical modeling and experimental research in multitudes of environmentally benign electrocatalytic applications, including O2 reduction, CO2 reduction, H2 evolution, O2 evolution, N2 reduction, and other fundamental reactions. As a final note, this review presents a brief conclusion highlighting current challenges and outlining prospects for this frontier. Importantly, this review deciphers the structure-performance correlation while excavating the advancement gained in DACs, thus is anticipated to shed light for the catalysis community on bolstering an intense evolution of DACs while triggering sapient inspiration for more robust next-generation catalysts. The central "golden" water droplet symbolizes the transformative impact of dual-atom catalysts (DACs) in electrocatalysis. This review unravels the intricate correlation between substrate selection, dual atoms, and sophisticated fabrication techniques for DACs. The review delves into state-of-the-art characterization methods, and shines

关键词： dual-atom catalysts electrocatalysis structure-performance correlation theoretical exploration

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In Situ Investigation on Life-Time Dynamic structure-performance correlation Toward Electrocatalyst Service Behavior in Water Splitting

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ADVANCED FUNCTIONAL MATERIALS 2022年第18期32卷 2111777-2111777页

作者： Xie, Yong Sun, Yu Tao, Huibing Wang, Xin Wu, Jing Ma, Kaikai Wang, Li Kang, Zhuo Zhang, Yue Univ Sci & Technol Beijing Sch Energy & Environm Engn Acad Adv Interdisciplinary Sci & Technol Beijing 100083 Peoples R China Univ Sci & Technol Beijing Sch Mat Sci & Engn State Key Lab Adv Met & Mat Beijing 100083 Peoples R China

Electrocatalytic water splitting is recognized as quite a promising protocol for the renewable hydrogen energy production, and significant effort has been devoted to the design of high-performance electrocatalysts that can efficiently alleviate the critical issue of fossil fuel scarcity. However, the vast majority of traditional design strategies restrictedly focus on the pristine electrocatalyst structure and ultimate performance results, which may lead to the incorrect or even opposite understanding of catalytic structure-performance correlations. With the burgeoning development of in situ techniques, the dynamic service behaviors of electrocatalysts during water splitting have been growingly investigated from enriched perspectives, only by which can the life-time dynamic structure-performance correlations be established. Herein, to shed new light on the next-stage development of in situ investigations for water splitting electrocatalysts, a series of dynamic service behavior that existed in water splitting process and highlight their key role for understanding the life-time dynamic structure-performance correlations is comprehensively summarized. Besides, a wide variety of in situ techniques are systematically dissected in terms of their functional features, advantages, and limitations. Critical challenges and prospects are also discussed for establishing the life-time dynamic structure-performance correlations of water splitting electrocatalysts.

关键词： in situ techniques service behavior structure-performance correlation water splitting electrocatalysts

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Investigating the structural descriptor of perfluorosulfonic acid membranes for enhanced fuel cell performance and durability

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 2025年 126卷 459-467页

作者： Lee, Seung Hyun Lim, Jinhyuk Park, Jiyoung Kim, Myounghwan Goo, Youngmo Shin, Dongyoon Korea Automot Technol Inst Hydrogen Fuel Cell Technol R&D Dept 86 Gongdan ro474 beon gil Chang Won 51577 Gyungsangnamdo South Korea Korea Automot Technol Inst Future Powertrain Technol Res Lab 303 Pungse Ro Cheonan Si 31214 Chungnam South Korea

Enhancing the performance and durability of polymer electrolyte membranes (PEMs) in electrochemical energy systems continues to be a critical challenge. In this study, we propose a structural descriptor that clarifies the relationship between nanostructural features and membrane performance. Solvent vapor annealing (SVA) was employed as a low-temperature post-treatment to effectively modulate the internal morphology of the membrane without altering its chemical structure or physical form. Consequently, the SVA R-membrane exhibited a 64.2 % increase in proton conductivity and significant improvements in both chemical and mechanical durability. These enhancements are attributed to improved ion channel continuity, facilitated by optimized phase separation and alignment of hydrophilic and hydrophobic domains. Furthermore, a non-linear correlation between d-spacing and proton conductivity was identified. This finding underscores the importance of balancing ionic channel architecture and the ratio of crystalline domains to enhance membrane performance. Overall, these findings provide a practical and scalable strategy for the rational design of high-performance and durable PEMs.

关键词： Polymer electrolyte membrane structure descriptor structure-performance correlation Nanostructural design optimization Solvent vapor annealing Phase separation

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Recent Advances in Perovskite Oxides for Oxygen Evolution Reaction: structures, Mechanisms, and Strategies for performance Enhancement

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ADVANCED FUNCTIONAL MATERIALS 2025年第10期35卷

作者： Sun, Xiong Yuan, Ying Liu, Shuzhi Zhao, Hongqing Yao, Suqiang Sun, Yuying Zhang, Mingyue Liu, Yijiang Lin, Zhiqun Xiangtan Univ Coll Chem Xiangtan 411105 Hunan Peoples R China Xiangtan Univ Minist Educ Key Lab Environmentally Friendly Chem & Applicat Xiangtan 411105 Hunan Peoples R China Natl Univ Singapore Dept Chem & Biomol Engn Singapore 117585 Singapore

Perovskite-type oxides are widely employed as oxygen evolution reaction (OER) electrocatalysts due to their tunable composition, diverse structure, abundant natural reserves, remarkable stability, and low cost. The intrinsic OER electrocatalytic activity of these perovskite oxides is generally enhanced by improving conductivity, increasing specific surface area, and optimizing the adsorption of oxygen-containing intermediates. This is achieved through rationally designed strategies, including compositional engineering, defect engineering, hybridization, and surface regulation. In this review, recent advances in perovskite oxides for OER are summarized, with a focus on exploring structure-performance relationships. This review provides a brief introduction to the application of perovskite oxides in OER, followed by the classification and characteristics of these perovskite oxides. The primary OER catalytic mechanisms, and well-established activity descriptors are discussed. The key strategies are concentrated for enhancing OER activity, including composition engineering, defect engineering, hybridization, and surface reconstruction. Finally, the challenges and opportunities in developing high-performance perovskite oxides as OER electrocatalysts are presented.

关键词： composition engineering defect engineering OER electrocatalysts pervoskite oxides structure-performance correlation

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"Cu-N x " Site-Driven Selectivity Switch for Electrocatalytic CO2 Reduction

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ACS APPLIED MATERIALS & INTERFACES 2025年第4期17卷 6326-6336页

作者： Ma, Xinyue Shao, Jie Mao, Baoguang Ye, Fenghui Wang, Zichun Mao, Junjie Chen, Aibing Wang, Dan Zhang, Lipeng Dong, Hui Lin, Husitu Li, Ning Hu, Chuangang Beijing Univ Chem Technol State Key Lab Organ Inorgan Composites Beijing 100029 Peoples R China Beijing Univ Chem Technol Beijing Adv Innovat Ctr Soft Matter Sci & Engn Beijing 100029 Peoples R China Anhui Normal Univ Coll Chem & Mat Sci Minist Educ Key Lab Funct Mol Solids Wuhu 241002 Peoples R China Hebei Univ Sci & Technol Sch Chem & Pharmaceut Engn Shijiazhuang 050018 Peoples R China

The comprehensive understanding of the effect of the chemical environment surrounding active sites on the pathway for the electrochemical carbon dioxide reduction reaction (eCO(2)RR) is essential for the development of advanced catalysts for large-scale applications. Based on a series of model catalysts engineered by the coordination of copper ions with various isomers of phenylenediamine [i.e., o-phenylenediamine (oPD), m-phenylenediamine (mPD), and p-phenylenediamine (pPD)] featuring two amino groups in ortho-, meta-, and para-positions, the steric effects could significantly govern the selectivity of the "Cu-N" sites for eCO(2)RR. It was found the steric distance between adjacent copper and nitrogen active sites in Cu-oPD enhanced the C-C coupling of the *COOH intermediate, thereby resulting in increased selectivity for C2H4 production. In contrast, the weak van der Waals interactions arising from steric electrostatic effects surrounding the *CHO intermediate on Cu-pPD facilitated subsequent hydrogenation, leading to the preferential synthesis of CH4. However, Cu-mPD exhibited diminished eCO(2)RR activity due to a higher free energy associated with the rate-determining step, which primarily led to the formation of H-2. This study underscores the significant role of a steric effect-driven selectivity switch for eCO(2)RR.

关键词： steric effect electrocatalytic CO2 reductionreaction structure-performance correlation tunable selectivity catalytic mechanism

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Multi-scale structure engineering of covalent organic framework for electrochemical charge storage

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SusMat 2024年第1期4卷 4-33页

作者： Xiaofang Zhang Fangling Li Shuangqiao Yang Baiqi Song Richu Luo Rui Xiong Weilin Xu State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile UniversityWuhanChina State Key Laboratory of Polymer Materials Engineering Polymer Research Institute at Sichuan UniversityChengduChina

Covalent organic frameworks(COFs),which are constructed by linking organic building blocks via dynamic covalent bonds,are newly emerged and burgeoning crystalline porous copolymers with features including programmable topological architecture,pre-designable periodic skeleton,well-defined micro-/meso-pore,large specific surface area,and customizable electroactive *** benefits make COFs as promising candidates for advanced electrochemical energy ***,for now,structure engineering of COFs from multiscale aspects has been conducted to enable optimal overall electrochemical performance in terms of structure durability,electrical conductivity,redox activity,and charge *** this review,we give a fundamental and insightful study on the correlations between multi-scale structure engineering and eventual electrochemical properties of COFs,started with introducing their basic chemistries and charge storage *** careful discussion on the significant achievements in structure engineering of COFs from linkages,redox sites,polygon skeleton,crystal nanostructures,and composite microstructures,and further their effects on the electrochemical behavior of COFs are ***,the timely cutting-edge perspectives and in-depth insights into COFbased electrodematerials to rationally screen their electrochemical behaviors for addressing future challenges and implementing electrochemical energy storage applications are proposed.

关键词： covalent organic frameworks electrochemical energy storage multi-scale structure engineering structure-performance correlation

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Reversible Adsorption and Light-Driven Release of CO2 Using Hollow Carbon Sphere-Based Adsorbents with Photothermal Conversion Feature

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ACS SUSTAINABLE CHEMISTRY & ENGINEERING 2025年第20期13卷 7418-7429页

作者： Li, Kaining Shimomura, Hanami Kuwahara, Yasutaka Yoshii, Takeharu Nishihara, Hirotomo Yamashita, Hiromi Osaka Univ Grad Sch Engn Div Mat & Mfg Sci 2-1 Yamada Oka Suita Osaka 5650871 Japan Osaka Univ Inst Open & Transdisciplinary Res Initiat OTRI Innovat Catalysis Sci Div 2-1 Yamadaoka Suita Osaka 5650871 Japan Tohoku Univ Inst Multidisciplinary Res Adv Mat 2-1-1 Katahira Aoba ku Sendai Miyagi 9808577 Japan Tohoku Univ Adv Inst Mat Res WPI AIMR 2-1-1 KatahiraAoba Ku Sendai Miyagi 9808577 Japan

CO2 capture and storage (CCS), an important negative CO2 emissions technology, offers a promising solution for alleviating the greenhouse effect and achieving the carbon neutrality target set by the Paris Climate Accord. However, current strategies using amine-based adsorbents suffer from the issues of energy-intensive adsorbent regeneration and the heating requirement to release CO2 for storage and utilization. Here, we report a novel photothermal adsorbent, hollow carbon spheres encapsulating poly(ethylenimine) (PEI@HCS), which features efficient CO2 capture and photocontrolled desorption capabilities. Upon light irradiation, the surface temperature of PEI@HCS rises to approximately 120 degrees C due to the photothermal properties of HCS, enabling the release of 0.96 mmol-CO2 g-adsorbent(-1) (91% of the captured CO2). In contrast, the traditional SiO2-supported PEI adsorbent (PEI/SiO2) achieves only 65 degrees C with no CO2 desorption. PEI@HCS also exhibits excellent reusability over multiple dark-light cycles, which is associated with the protective effect of HCS. Furthermore, a correlation study reveals that both mesoporous pore volume and specific surface area show a positive correlation with CO2 adsorption performance, which can be modulated by varying the PEI content and the calcination temperature of HCS preparation. This work is anticipated to offer new inspiration for the development of green and energy-saving carbon capture and storage technologies.

关键词： CO2 capture and storage (CCS) photothermalCO(2) release hollow carbon sphere aminopolymer porous material structure-performance correlation

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Impact of Hydrotalcite's Basic Sites on the Catalyst Stability and the Branching Selectivity in α-Hydroxyketone Aldolization

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ACS CATALYSIS 2023年第24期13卷 15811-15823页

作者： Rammal, Fatima Matthijssen, Joost Khalil, Ibrahim Calderon-Ardila, Sergio Makshina, Ekaterina Sels, Bert F. Katholieke Univ Leuven Ctr Sustainable Catalysis & Engn B-3001 Leuven Belgium

Reconstructed hydrotalcites serve as powerful catalysts for the aldolization of alpha-hydroxyketones, exemplified here by the glycerol-derived dihydroxyacetone (DHA), toward the formation of branched hexoses (dendroketoses). Due to the multichemical functionality of these hydroxyketones, various competitive reactions such as keto-aldehyde isomerization (e.g., dihydroxyacetone (DHA)/glyceraldehyde (GLA) equilibrium) are possible, reducing the branching selectivity of the aldolization reaction. This study reveals that the nature of the basic sites (as determined via CDCl3 probe FT-IR and CO2-TPD experiments) strongly affects the branching selectivity of the condensation reaction as well as the stability of the hydrotalcite catalyst. For instance, strong basic sites not only allow the undesired keto-aldehyde isomerization but also promote the Cannizzaro reactions toward the formation of organic carboxylic acids leading to the catalyst leaching and waste generation. Thus, subsequent chemical transformations of branched sugars cannot occur without prior purification. For instance, the hydrogenation toward biobased branched polyol, which is the industrial target in casu base condensation of DHA. Tuning the basic properties of the reconstructed hydrotalcite based on this knowledge ultimately led to an active, selective, and stable catalyst with improved regeneration possibility.

关键词： reconstructed hydrotalcite dihydroxyacetone dendroketose aldolization branched sugars active basic sites structure-performance correlation catalyst stability

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Highly active sites of low spin Fe^(Ⅱ)N_(4)species:The identification and the ORR performance

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Nano Research 2021年第1期14卷 122-130页

作者： Huizhu Cai Bingbing Chen Xiao Zhang Yuchen Deng Dequan Xiao Ding Ma Chuan Shi State Key Laboratory of Fine Chemicals College of Chemical EngineeringDalian University of TechnologyDalian 116024China College of Chemistry and Molecular Engineering and College of Engineering Peking UniversityBeijing 100871China Center for Integrative Materials Discovery Department of Chemistry and Chemical EngineeringUniversity of New HavenCT 06516USA

Over recent years,catalytic materials of Fe-N-C species have been recognized being active for oxygen reduction reaction(ORR).However,the identification of active site remains challenging as it generally involves a pyrolysis process and mixed components being *** Fe_(3)C/C and Fe_(2)N/C samples were synthesized by temperature programmed reduction of Fe precursors in 15%CH_(4)/H_(2)and pure NH_(3),*** acid leaching of Fe_(2)N/C sample,only single sites of FeN_(4)species were presented,providing an ideal model for identification of catalytic functions of the single sites of FeN_(4)in ORR.A correlation was conducted between the concentration of Fe^(Ⅱ)N_(4)in low spin state by Mossbauer spectra and the kinetic current density at 0.8 V in alkaline media,and such a structure-performance correlation assures the catalytic roles of low spin Fe^(Ⅱ)N_(4) species as highly active sites for the ORR.

关键词： single sites of FeN_(4) oxygen reduction reaction structure-performance correlation electrocatalysis

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