Surface distortion as a unifying concept and descriptor in oxygen reduction reaction electrocatalysis

Nature Materials
Raphaël ChattotFrédéric Maillard

Abstract

Tuning the surface structure at the atomic level is of primary importance to simultaneously meet the electrocatalytic performance and stability criteria required for the development of low-temperature proton-exchange membrane fuel cells (PEMFCs). However, transposing the knowledge acquired on extended, model surfaces to practical nanomaterials remains highly challenging. Here, we propose 'surface distortion' as a novel structural descriptor, which is able to reconciliate and unify seemingly opposing notions and contradictory experimental observations in regards to the electrocatalytic oxygen reduction reaction (ORR) reactivity. Beyond its unifying character, we show that surface distortion is pivotal to rationalize the electrocatalytic properties of state-of-the-art of PtNi/C nanocatalysts with distinct atomic composition, size, shape and degree of surface defectiveness under a simulated PEMFC cathode environment. Our study brings fundamental and practical insights into the role of surface defects in electrocatalysis and highlights strategies to design more durable ORR nanocatalysts.

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Citations

Feb 26, 2019·Advanced Materials·Dmitry I SharapaSilke Behrens
May 18, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Bo LinZhanhu Guo
May 16, 2019·Chemical Society Reviews·Zhonghong Xia, Shaojun Guo
Oct 20, 2018·Chemical Record : an Official Publication of the Chemical Society of Japan ... [et Al.]·Xiao ZhaoYasuhiro Iwasawa
Jun 12, 2019·Advanced Materials·Zipeng ZhaoYu Huang
Jan 11, 2020·Chemical Society Reviews·Xiao WangHongjie Zhang
Dec 5, 2019·Angewandte Chemie·Kavita KumarFrédéric Maillard
Mar 17, 2020·Advanced Materials·Wei LiShuangyin Wang
Jul 10, 2020·Chemical Communications : Chem Comm·Qiang LiJinlan Wang
Sep 29, 2020·Nanoscale·Junming ZhangShigang Sun
Nov 6, 2018·The Journal of Chemical Physics·Lei YanOsamu Sugino
Jul 21, 2020·Journal of Applied Crystallography·Cedric J GommesJakub Drnec
Apr 2, 2020·Chemical Communications : Chem Comm·Zhicheng LinZhigang Zou
Jul 6, 2020·Nature Communications·Zhanxi FanHua Zhang
Dec 12, 2018·Advanced Materials·Bin Cai, Alexander Eychmüller
Dec 21, 2019·Chemical Science·Batyr GarlyyevFederico Calle-Vallejo
Jul 22, 2020·Nature Materials·Pietro P LopesVojislav R Stamenkovic
Oct 15, 2020·ChemSusChem·Ahmed BadreldinAhmed Abdel-Wahab
Apr 2, 2021·ACS Nano·Rafael A VicentePablo S Fernández
Apr 24, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Xian-Kai WanMizuki Tada
Jun 2, 2021·Nano Letters·Yonggang FengXiaoqing Huang

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Methods Mentioned

BETA
X-ray
transmission electron microscopy
scanning

Software Mentioned

Nova
Vienna ab initio simulation package ( VASP )
pyFAI
Fullprof
JEOL

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