Nature Communications ( IF 14.7 ) Pub Date : 2024-03-18 , DOI: 10.1038/s41467-024-46752-4 Wei Chen 1, 2 , Liang Zhang 1, 3 , Leitao Xu 1 , Yuanqing He 1, 2 , Huan Pang 2 , Shuangyin Wang 1 , Yuqin Zou 1
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 VRHE (37.8%). This work offers an efficient strategy to mitigate the deactivation of noble metal-based electrocatalysts.
中文翻译:
脉冲电位介导的甘油电催化氧化成甘油酸的选择性
防止贵金属催化剂因自氧化和有毒吸附而失活是有机电氧化中的一个重大挑战。在这项研究中,我们采用脉冲电位电解策略,在铂基催化剂上将甘油选择性电催化氧化为甘油酸。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和表面微环境。这可以防止中毒中间物质的过度积累,并释放活性位点以重新吸附 OH 吸附物和甘油。脉冲电位电解策略比 0.7 V RHE的恒电位电催化 (37.8%) 具有更高的甘油酸选择性 (81.8%)。这项工作提供了一种有效的策略来减轻贵金属基电催化剂的失活。