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Stabilizing efficient structures of superwetting electrocatalysts for enhanced urea oxidation reactions
Chem Catalysis ( IF 11.5 ) Pub Date : 2022-10-13 , DOI: 10.1016/j.checat.2022.09.023
Jichao Zhang , Xuedan Song , Liqun Kang , Jiexin Zhu , Longxiang Liu , Qing Zhang , Dan J.L. Brett , Paul R. Shearing , Liqiang Mai , Ivan P. Parkin , Guanjie He

Layered hydroxides have shown superior catalytic activity for the electrocatalytic organic compound oxidation reaction. However, metal leaching can lead to uncontrollable structural phase transformation. Here, we report a Cr-Ni(OH)2 electrocatalyst as a model of a pre-catalyst for the identification of the structure-performance relationship. The optimized electrocatalyst delivered superb performances, i.e., a low potential of 1.38 V (versus reversible hydrogen electrode [RHE]) to reach 100 mA cm−2 and stable activity over 200 h at 10 mA cm−2. In situ analyses and theoretical calculations demonstrate that well-tuned electronic structures and the superhydrophilic-superaerophobic surface can enable rapid urea oxidation reaction (UOR) kinetics, which reduces the specific adsorption OH and significantly depresses Cr dopants leaching, and this helps to maintain high UOR performance. Furthermore, the crucial role of mass transfer improvement to alleviate the structural decay under high potentials is disclosed.



中文翻译:

稳定超润湿电催化剂的有效结构以增强尿素氧化反应

层状氢氧化物对电催化有机化合物氧化反应显示出优异的催化活性。然而,金属浸出会导致不可控的结构相变。在这里,我们报告了一种 Cr-Ni(OH) 2电催化剂作为预催化剂模型,用于确定结构-性能关系。优化后的电催化剂表现出卓越的性能,即在 1.38 V(相对于可逆氢电极 [RHE])的低电势下即可达到 100 mA cm -2并在 10 mA cm -2下稳定活性超过 200 小时。就地分析和理论计算表明,良好调整的电子结构和超亲水-超疏气表面可以实现快速尿素氧化反应 (UOR) 动力学,从而降低比吸附 OH -并显着抑制 Cr 掺杂剂的浸出,这有助于保持高 UOR 性能. 此外,还揭示了改善传质以减轻高电位下结构衰减的关键作用。

更新日期:2022-10-13
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