Selective and durable H<sub>2</sub>O<sub>2</sub> electrosynthesis catalyst in acid by selenization induced straining and phasing.

Yu, Zhiyong; Deng, Hao; Yao, Qing; Zhao, Liangqun; Xue, Fei; He, Tianou; Hu, Zhiwei; Huang, Wei-Hsiang et al. · Nat Commun · 2024

basic_science · Level V

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Abstract

Developing efficient electrocatalysts for acidic electrosynthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) holds considerable significance, while the selectivity and stability of most materials are compromised under acidic conditions. Herein, we demonstrate that constructing amorphous platinum-selenium (Pt-Se) shells on crystalline Pt cores can manipulate the oxygen reduction reaction (ORR) pathway to efficiently catalyze the electrosynthesis of H<sub>2</sub>O<sub>2</sub> in acids. The Se<sub>2</sub>‒Pt nanoparticles, with optimized shell thickness, exhibit over 95% selectivity for H<sub>2</sub>O<sub>2</sub> production, while suppressing its decomposition. In flow cell reactor, Se<sub>2</sub>‒Pt nanoparticles maintain current density of 250 mA cm<sup>-2</sup> for 400 h, yielding a H<sub>2</sub>O<sub>2</sub> concentration of 113.2 g L<sup>-1</sup> with productivity of 4160.3 mmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup> for effective organic dye degradation. The constructed amorphous Pt-Se shell leads to desirable O<sub>2</sub> adsorption mode for increased selectivity and induces strain for optimized OOH* binding, accelerating the reaction kinetics. This selenization approach is generalizable to other noble metals for tuning 2e<sup>‒</sup> ORR pathway.