Yu Zhiyong, Deng Hao, Yao Qing, Zhao Liangqun, Xue Fei, He Tianou, Hu Zhiwei, Huang Wei-Hsiang, Pao Chih-Wen, Yang Li-Ming, Huang Xiaoqing
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Wuhan, 430074, China.
Nat Commun. 2024 Oct 29;15(1):9346. doi: 10.1038/s41467-024-53607-5.
Developing efficient electrocatalysts for acidic electrosynthesis of hydrogen peroxide (HO) 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 HO in acids. The Se‒Pt nanoparticles, with optimized shell thickness, exhibit over 95% selectivity for HO production, while suppressing its decomposition. In flow cell reactor, Se‒Pt nanoparticles maintain current density of 250 mA cm for 400 h, yielding a HO concentration of 113.2 g L with productivity of 4160.3 mmol g h for effective organic dye degradation. The constructed amorphous Pt-Se shell leads to desirable O 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 ORR pathway.
开发用于酸性电合成过氧化氢(HO)的高效电催化剂具有重要意义,然而大多数材料在酸性条件下的选择性和稳定性会受到影响。在此,我们证明在结晶态Pt核上构建非晶态铂 - 硒(Pt - Se)壳层可以调控氧还原反应(ORR)途径,从而在酸性条件下高效催化HO的电合成。具有优化壳层厚度的Se - Pt纳米颗粒对HO生成的选择性超过95%,同时抑制其分解。在流动池反应器中,Se - Pt纳米颗粒在400小时内保持250 mA cm的电流密度,产生113.2 g L的HO浓度,有效有机染料降解的生产率为4160.3 mmol g h。构建的非晶态Pt - Se壳层导致理想的O吸附模式以提高选择性,并诱导应变以优化OOH*结合,加速反应动力学。这种硒化方法可推广到其他贵金属以调整2e ORR途径。