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Enhancing oxygen reduction electrocatalysis by tuning interfacial hydrogen bonds
Nature Catalysis ( IF 37.8 ) Pub Date : 2021-09-06 , DOI: 10.1038/s41929-021-00668-0
Tao Wang 1, 2, 3 , Yirui Zhang 1, 4 , Botao Huang 1, 2 , Bin Cai 1, 4 , Reshma R. Rao 1, 2 , Livia Giordano 1, 4 , Yang Shao-Horn 1, 2, 4, 5 , Shi-Gang Sun 3
Affiliation  

Proton activity at the electrified interface is central to the kinetics of proton-coupled electron transfer (PCET) reactions for making chemicals and fuels. Here we employ a library of protic ionic liquids in an interfacial layer on platinum and gold to alter local proton activity, where the intrinsic oxygen-reduction reaction (ORR) activity is enhanced up to fivefold, exhibiting a volcano-shaped dependence on the pKa of the ionic liquid. The enhanced ORR activity is attributed to strengthened hydrogen bonds between ORR products and ionic liquids with comparable pKas, resulting in favourable PCET kinetics. This proposed mechanism is supported by in situ surface-enhanced Fourier-transform infrared spectroscopy and our simulation of PCET kinetics based on computed proton vibrational wavefunctions at the hydrogen-bonding interface. These findings highlight opportunities for using non-covalent interactions between hydrogen-bonded structures and solvation environments at the electrified interface to tune the kinetics of ORR and beyond.



中文翻译:

通过调整界面氢键增强氧还原电催化

带电界面处的质子活动对于制造化学品和燃料的质子耦合电子转移 (PCET) 反应的动力学至关重要。在这里,我们在铂和金的界面层中使用质子离子液体库来改变局部质子活性,其中固有的氧还原反应 (ORR) 活性提高了五倍,表现出对 p K的火山形依赖性a离子液体。增强的 ORR 活性归因于 ORR 产物和具有可比 p K a 的离子液体之间的氢键增强s,导致有利的 PCET 动力学。原位表面增强傅里叶变换红外光谱和我们基于氢键界面处计算的质子振动波函数对 PCET 动力学的模拟支持了这一提出的机制。这些发现突出了在带电界面处使用氢键结构和溶剂化环境之间的非共价相互作用来调节 ORR 及其他动力学的机会。

更新日期:2021-09-06
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