Fabricating Lattice-Confined Pt Single Atoms With High Electron-Deficient State for Alkali Hydrogen Evolution Under Industrial-Current Density.

Cao, Dong; Gao, Peng; Shen, Yuge; Qiao, Liang; Ma, Mengyao; Guo, Xiaoyan; Cheng, Daojian · Adv Mater · 2025

basic_science · Level V

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Abstract

The confining effect is essential to regulate the activity and stability of single-atom catalysts (SACs), but the universal fabrication of confined SACs is still a great challenge. Here, various lattice-confined Pt SACs supported by different carriers are constructed by a universal co-reduction approach. Notably, Pt single atoms confined in the lattice of Ni(OH)<sub>2</sub> (Pt<sub>1</sub>/Ni(OH)<sub>2</sub>) with a high electron-deficient state exhibit excellent activity for basic hydrogen evolution reaction (HER). Specifically, Pt<sub>1</sub>/Ni(OH)<sub>2</sub> just requires 15 mV to get 10 mA cm<sup>-2</sup> and the mass activity of Pt<sub>1</sub>/Ni(OH)<sub>2</sub> is 15 times of commercial Pt/C. Moreover, Pt<sub>1</sub>/Ni(OH)<sub>2</sub> assembled in an alkaline water electrolyzer shows 1030 h durability under the industrial current density of 800 mA cm<sup>-2</sup>. In situ spectroscopy techniques reveal Pt─H and "free" OH radical can be directly observed for Pt<sub>1</sub>/Ni(OH)<sub>2</sub>, confirming the lattice-confined Pt single atoms play a key role during HER. Further density functional theory uncovers the Pt 3d orbital strongly hybridizes with O 2p and Ni 3d orbitals in Ni(OH)<sub>2</sub>, which quickly optimizes the electronic state of the Pt site, thus largely reducing the energy barrier of the rate-determining step to 0.16 eV for HER. Finally, this synthesis method is extended to construct other 9 lattice-confined SACs.