Nanoporous Surface High‐Entropy Alloys as Highly Efficient Multisite Electrocatalysts for Nonacidic Hydrogen Evolution Reaction

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  • Rui‐Qi Yao
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China
  • Yi‐Tong Zhou
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China
  • Hang Shi
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China
  • Wu‐Bin Wan
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China
  • Qing‐Hua Zhang
    Beijing National Laboratory for Condensed Matter Physics The Institute of Physics Chinese Academy of Sciences Beijing 100190 China
  • Lin Gu
    Beijing National Laboratory for Condensed Matter Physics The Institute of Physics Chinese Academy of Sciences Beijing 100190 China
  • Yong‐Fu Zhu
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China
  • Zi Wen
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China
  • Xing‐You Lang
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China
  • Qing Jiang
    Key Laboratory of Automobile Materials (Jilin University) Ministry of Education and School of Materials Science and Engineering Jilin University Changchun 130022 China

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<jats:title>Abstract</jats:title><jats:p>Electrocatalytic hydrogen evolution in alkaline and neutral media offers the possibility of adopting platinum‐free electrocatalysts for large‐scale electrochemical production of pure hydrogen fuel, but most state‐of‐the‐art electrocatalytic materials based on nonprecious transition metals operate at high overpotentials. Here, a monolithic nanoporous multielemental CuAlNiMoFe electrode with electroactive high‐entropy CuNiMoFe surface is reported to hold great promise as cost‐effective electrocatalyst for hydrogen evolution reaction (HER) in alkaline and neutral media. By virtue of a surface high‐entropy alloy composed of dissimilar Cu, Ni, Mo, and Fe metals offering bifunctional electrocatalytic sites with enhanced kinetics for water dissociation and adsorption/desorption of reactive hydrogen intermediates, and hierarchical nanoporous Cu scaffold facilitating electron transfer/mass transport, the nanoporous CuAlNiMoFe electrode exhibits superior nonacidic HER electrocatalysis. It only takes overpotentials as low as ≈240 and ≈183 mV to reach current densities of ≈1840 and ≈100 mA cm<jats:sup>−2</jats:sup> in 1 <jats:sc>m </jats:sc>KOH and pH 7 buffer electrolytes, respectively; ≈46‐ and ≈14‐fold higher than those of ternary CuAlNi electrode with bimetallic Cu–Ni surface alloy. The outstanding electrocatalytic properties make nonprecious multielemental alloys attractive candidates as high‐performance nonacidic HER electrocatalytic electrodes in water electrolysis.</jats:p>

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