DataVXAdvanced Functional MaterialsPaper
journal article·2025-05

Surface‐Nanocurvation‐Induced Microenvironment Regulation Capable of Controlling the Activity of Single‐Atom Electrocatalysts

Xianghui Yu, Yunhui Xie, Xiaoxiao Dong, Dengchao Wang, Tong Sun, Qi Sun, Shuang Cao, Fanlu Meng, Ruqiang Zou, Chi Zhang, Qiang Xu, Chun‐Chao Hou

Advanced Functional Materials· Volume 35· Issue 22
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Source abstract

Abstract

Abstract Tuning the interfacial microenvironment of single‐atom catalysts with defined electronic structures and favorable electric fields is essential to overcome sluggish kinetics and thus boosts electrocatalytic oxygen reduction reaction (ORR) activity. However, the relationship between microenvironment regulation and catalyst properties remains poorly understood. Herein, enriched single‐atom Fe−N4 sites on nano‐curved carbon surfaces (cc‐Fe) are designed to investigate the influence of the interface microenvironment on catalyst behaviors. Density functional theory calculations, together with in situ spectro‐electrochemical experiments, indicate that curving the surface can effectively modulate the adsorbate binding energies on cc‐Fe, thereby promoting the protonation of O2*. Finite element method simulations demonstrate that surface nanocurvation‐induced strong local electrostatic fields can facilitate mass transfer, enhancing the kinetics of the proton‐coupled electron transfer process. The designed cc‐Fe catalyst exhibits superior ORR activity (E1/2 = 0.866 V, comparable to commercial Pt/C, E1/2 = 0.867 V) and outstanding stability (after 50 000 cycles, E1/2 decreases by only 9 mV), exceeding those of planar Fe−N4 and Pt/C. When assembled in a Zn–air battery, it also exhibits superior performance over a benchmark Pt/C air cathode. This study clarified the advantageous impacts of microenvironment regulation via curved configurations and paved the way for the development of high‐performance electrocatalysts.
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Research context

Energy storageNanomaterialsCatalysis & surfaces

OpenAlex topics: Electrocatalysts for Energy Conversion · CO2 Reduction Techniques and Catalysts · Advanced battery technologies research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

College of Chemistry and Chemical Engineering College of Materials Science and Engineering Institute for Sustainable Energy and Resources Qingdao University Qingdao Shandong 266071 P. R. China

College of Materials Science and Engineering Ocean University of China Qingdao Shandong 266100 P. R. China

University of Chinese Academy of Science Beijing 100049 P. R. China

School of Materials Science and Engineering Peking University Beijing 100871 P. R. China

School of Chemical Science and Engineering Tongji University Shanghai 200092 P. R. China

Shenzhen Key Laboratory of Micro/Nano‐Porous Functional Materials (SKLPM) SUSTech‐Kyoto University Advanced Energy Materials Joint Innovation Laboratory (SKAEM‐JIL) Key University Laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of Guangdong Department of Chemistry and Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 P. R. China

Funding

National Natural Science Foundation of China · Natural Science Foundation of Shandong Province · Fundamental Research Funds for the Central Universities · Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China

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