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On the importance of the electric double layer structure in aqueous electrocatalysis SCIE SCOPUS

Title
On the importance of the electric double layer structure in aqueous electrocatalysis
Authors
Shin, Seung-JaeKim, Dong HyunBae, GeunsuRinge, StefanChoi, HansolLim, Hyung-KyuChoi, Chang HyuckKim, Hyungjun
Date Issued
2022-01
Publisher
Nature Publishing Group
Abstract
AbstractTo design electrochemical interfaces for efficient electric-chemical energy interconversion, it is critical to reveal the electric double layer (EDL) structure and relate it with electrochemical activity; nonetheless, this has been a long-standing challenge. Of particular, no molecular-level theories have fully explained the characteristic two peaks arising in the potential-dependence of the EDL capacitance, which is sensitively dependent on the EDL structure. We herein demonstrate that our first-principles-based molecular simulation reproduces the experimental capacitance peaks. The origin of two peaks emerging at anodic and cathodic potentials is unveiled to be an electrosorption of ions and a structural phase transition, respectively. We further find a cation complexation gradually modifies the EDL structure and the field strength, which linearly scales the carbon dioxide reduction activity. This study deciphers the complex structural response of the EDL and highlights its catalytic importance, which bridges the mechanistic gap between the EDL structure and electrocatalysis.
URI
https://oasis.postech.ac.kr/handle/2014.oak/109582
DOI
10.1038/s41467-021-27909-x
ISSN
2041-1723
Article Type
Article
Citation
Nature Communications, vol. 13, no. 174, 2022-01
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