Chen Wei, Zhang Liang, Xu Leitao, He Yuanqing, Pang Huan, Wang Shuangyin, Zou Yuqin
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410000, P. R. China.
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225009, P. R. China.
Nat Commun. 2024 Mar 18;15(1):2420. doi: 10.1038/s41467-024-46752-4.
Preventing the deactivation of noble metal-based catalysts due to self-oxidation and poisonous adsorption is a significant challenge in organic electro-oxidation. In this study, we employ a pulsed potential electrolysis strategy for the selective electrocatalytic oxidation of glycerol to glyceric acid over a Pt-based catalyst. In situ Fourier-transform infrared spectroscopy, quasi-in situ X-ray photoelectron spectroscopy, and finite element simulations reveal that the pulsed potential could tailor the catalyst's oxidation and surface micro-environment. This prevents the overaccumulation of poisoning intermediate species and frees up active sites for the re-adsorption of OH adsorbate and glycerol. The pulsed potential electrolysis strategy results in a higher glyceric acid selectivity (81.8%) than constant-potential electrocatalysis with 0.7 V (37.8%). This work offers an efficient strategy to mitigate the deactivation of noble metal-based electrocatalysts.
防止基于贵金属的催化剂因自氧化和有毒吸附而失活是有机电氧化中的一项重大挑战。在本研究中，我们采用脉冲电位电解策略，在基于铂的催化剂上对甘油进行选择性电催化氧化生成甘油酸。原位傅里叶变换红外光谱、准原位X射线光电子能谱和有限元模拟表明，脉冲电位可以调节催化剂的氧化作用和表面微环境。这可防止中毒中间物种的过度积累，并释放活性位点以便OH吸附质和甘油重新吸附。与0.7 V恒电位电催化（37.8%）相比，脉冲电位电解策略产生了更高的甘油酸选择性（81.8%）。这项工作提供了一种减轻基于贵金属的电催化剂失活的有效策略。
