Enhancing oxygen reduction electrocatalysis by tuning interfacial hydrogen bonds

被引：0
作者：
Tao Wang
Yirui Zhang
Botao Huang
Bin Cai
Reshma R. Rao
Livia Giordano
Shi-Gang Sun
Yang Shao-Horn
机构：
[1] Massachusetts Institute of Technology,Electrochemical Energy Laboratory
[2] Massachusetts Institute of Technology,Research Laboratory of Electronics
[3] Xiamen University,Collaborative Innovation Center of Chemistry for Energy Materials, State Key Laboratory for Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering
[4] Massachusetts Institute of Technology,Department of Mechanical Engineering
[5] Massachusetts Institute of Technology,Department of Materials Science and Engineering
来源：
Nature Catalysis | 2021年 / 4卷
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摘要：
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.
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页码：753 / 762
页数：9
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