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Improving C–N–FeOx Oxygen Evolution Electrocatalysts through Hydroxyl-Modulated Local Coordination Environment

  • Tianyun Jing
    Tianyun Jing
    School of Materials Science and Engineering, Jiangsu University, 212013 Zhenjiang, People’s Republic of China
    More by Tianyun Jing
  • Ning Zhang
    Ning Zhang
    Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, 999077 Kowloon, Hong Kong, People’s Republic of China
    More by Ning Zhang
  • Chaonan Zhang
    Chaonan Zhang
    School of Materials Science and Engineering, Jiangsu University, 212013 Zhenjiang, People’s Republic of China
  • Stefanos Mourdikoudis
    Stefanos Mourdikoudis
    Department of Inorganic Chemistry, University of Chemistry and Technology Prague, Technická 5, 16628 Prague 6, Czech Republic
  • Zdeněk Sofer*
    Zdeněk Sofer
    Department of Inorganic Chemistry, University of Chemistry and Technology Prague, Technická 5, 16628 Prague 6, Czech Republic
    *Email [email protected]
  • Wei Li
    Wei Li
    Institute of Surface Micro and Nano Materials, Xuchang University, Xuchang, Henan 461002, People’s Republic of China
    More by Wei Li
  • Pinjiang Li
    Pinjiang Li
    Institute of Surface Micro and Nano Materials, Xuchang University, Xuchang, Henan 461002, People’s Republic of China
    More by Pinjiang Li
  • Tingting Li
    Tingting Li
    Institute of Surface Micro and Nano Materials, Xuchang University, Xuchang, Henan 461002, People’s Republic of China
    More by Tingting Li
  • Yunpeng Zuo*
    Yunpeng Zuo
    Department of Inorganic Chemistry, University of Chemistry and Technology Prague, Technická 5, 16628 Prague 6, Czech Republic
    Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute, Palacký University, 77900 Olomouc, Czech Republic
    *Email: [email protected]
    More by Yunpeng Zuo
  • , and 
  • Dewei Rao*
    Dewei Rao
    School of Materials Science and Engineering, Jiangsu University, 212013 Zhenjiang, People’s Republic of China
    *Email: [email protected]
    More by Dewei Rao
Cite this: ACS Catal. 2022, 12, 12, 7443–7452
Publication Date (Web):June 8, 2022
https://doi.org/10.1021/acscatal.2c01153
Copyright © 2022 American Chemical Society

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    Abstract

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    Ultrafine FeOx in the sub-nanometric or atomic scale is one of the promising catalysts for boosted oxygen evolution reaction (OER) activity, although there is further potential for improvement in comparison to commercial catalysts. Recent studies show that hydroxyl modification on the surface of catalysts can ameliorate hydrophilicity and catalytic activity, thus helping to bring such catalysts closer to scale-up and commercialization stages. To deeply understand the effect of hydroxyl, atomic-level dispersed FeOx in porous carbon nitride (CN-FeOx) was proposed through a spatially confined approach, which involved an in situ coordination effect between resorcinol and Fe ions. After hydroxyl modification, the generated CN-FeOx-OH hybrid material displayed significantly enhanced mass activity compared to CN-FeOx and commercial RuO2 (0.16 A/mgmetal) under an overpotential of 350 mV versus RHE. Additionally, the improved stability of CN-FeOx-OH suppresses migration and aggregation. The DFT calculations revealed a distinct catalytic mechanism in which the active center composed of multisites modified by hydroxyl exhibited a strong synergistic effect to modulate the adsorption behaviors of OH and O intermediates, which possessed the optimal adsorption energy for enhanced activity as compared with a single site in the CN-FeOx-OH and CN-FeOx, respectively. The adopted strategies in this paper can effectively promote the application of Fe-based catalysts in OER.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.2c01153.

    • Methods for material synthesis and characterization, XRD patterns, FT-IR spectra, Raman spectra, 1H MAS NMR spectrum, TEM images, XPS analysis, EXAFS spectra and fit results, and experimental and computational data (PDF)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 5 publications.

    1. Jing Hou, Yingying Cheng, Hui Pan, Peng Kang. Tailored Bimetallic Ni–Sn Catalyst for Electrochemical Ammonia Oxidation to Dinitrogen with High Selectivity. Inorganic Chemistry 2023, 62 (9) , 3986-3992. https://doi.org/10.1021/acs.inorgchem.2c04440
    2. Yue Zhou, Yanmin Wang, Deqiang Kong, Qianqian Zhao, Lei Zhao, Jialin Zhang, Xuemin Chen, Yanan Li, Yan Xu, Chao Meng. Revealing the Reactant Mediation Role of Low‐Valence Mo for Accelerated Urea‐Assisted Water Splitting. Advanced Functional Materials 2023, 33 (8) , 2210656. https://doi.org/10.1002/adfm.202210656
    3. Yu Zhu, Xuan Wang, Xiaoheng Zhu, Zixin Wu, Dongsheng Zhao, Fei Wang, Dongmei Sun, Yawen Tang, Hao Li, Gengtao Fu. Improving the Oxygen Evolution Activity of Layered Double‐Hydroxide via Erbium‐Induced Electronic Engineering. Small 2023, 19 (5) , 2206531. https://doi.org/10.1002/smll.202206531
    4. Jingxi Qin, Ke Tian, Taiping Qing, Siqi Zhong. Efficient Degradation of Ofloxacin with Pyridine Nitrogen Regulation Using Co/Fe Bimetal-Doped Carbon Nitride as Peroxymonosulfate Activator. SSRN Electronic Journal 2023, 626 https://doi.org/10.2139/ssrn.4349393
    5. Xiaoqing Mao, Pei Kang Shen. Interface engineering of NiMoSx heterostructure nanorods for efficient oxygen evolution reaction. Journal of Colloid and Interface Science 2022, 628 , 513-523. https://doi.org/10.1016/j.jcis.2022.07.157

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