General π‐Electron‐Assisted Strategy for Ir,Pt, Ru,Pd, Fe,Ni Single‐Atom Electrocatalysts with Bifunctional Active Sites for Highly Efficient Water Splitting |
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Authors: | Wei‐Hong Lai Li‐Fu Zhang Wei‐Bo Hua Sylvio Indris Zi‐Chao Yan Zhe Hu Binwei Zhang Yani Liu Li Wang Min Liu Rong Liu Yun‐Xiao Wang Jia‐Zhao Wang Zhenpeng Hu Hua‐Kun Liu Shu‐Lei Chou Shi‐Xue Dou |
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Abstract: | Both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) are crucial to water splitting, but require alternative active sites. Now, a general π‐electron‐assisted strategy to anchor single‐atom sites (M=Ir, Pt, Ru, Pd, Fe, Ni) on a heterogeneous support is reported. The M atoms can simultaneously anchor on two distinct domains of the hybrid support, four‐fold N/C atoms (M@NC), and centers of Co octahedra (M@Co), which are expected to serve as bifunctional electrocatalysts towards the HER and the OER. The Ir catalyst exhibits the best water‐splitting performance, showing a low applied potential of 1.603 V to achieve 10 mA cm?2 in 1.0 m KOH solution with cycling over 5 h. DFT calculations indicate that the Ir@Co (Ir) sites can accelerate the OER, while the Ir@NC3 sites are responsible for the enhanced HER, clarifying the unprecedented performance of this bifunctional catalyst towards full water splitting. |
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Keywords: | bifunctional active sites dual domains electrocatalysis single atom catalysts water splitting |
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