Photoinduced loading of electron-rich Cu single atoms by moderate coordination for hydrogen evolution

Weiwei Fu, Jin Wan, Huijuan Zhang, Jian Li, Weigen Chen, Yuke Li, Zaiping Guo and Yu Wang ()
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Weiwei Fu: Chongqing University
Jin Wan: Chongqing University
Huijuan Zhang: Chongqing University
Jian Li: Chongqing University
Weigen Chen: Chongqing University
Yuke Li: Chinese University of Hong Kong
Zaiping Guo: University of Adelaide
Yu Wang: Chongqing University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Single-atom catalysts offer maximal atom utilization efficiencies and high-electronegativity heteroatoms play a crucial role in coordinating reactive single metal atoms to prevent agglomeration. However, these strong coordination bonds withdraw electron density for coordinated metal atoms and consequently affect their catalytic activity. Herein we reveal the high loading (11.3 wt%) and stabilization of moderately coordinated Cu-P3 structure on black phosphorus support by a photochemical strategy with auxiliary hydrogen. Single-atom Cu sites with an exceptional electron-rich feature show the $$\triangle {G}_{{{{{{\rm{H}}}}}}*}$$ △ G H * close to zero to favor catalysis. Neighboring Cu atoms work in synergy to lower the energy of key water adsorption and dissociation intermediates. The reported catalyst shows a low overpotential of only 41 mV at 10 mA cm−2 and Tafel slope of 53.4 mV dec−1 for the alkaline hydrogen evolution reaction, surpassing both isolated Cu single atoms and Cu nanoclusters. The promising materials design strategy sheds light on the design and fabrication of high-loading single metal atoms and the role of neighboring single atoms for enhanced reaction kinetics.

Date: 2022
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DOI: 10.1038/s41467-022-33275-z

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