TY - JOUR
T1 - A new operando surface restructuring pathway via ion-pairing of catalyst and electrolyte for water oxidation
AU - Zhuang, Linzhou
AU - Li, Zhiheng
AU - Li, Mengran
AU - Tao, Haolan
AU - Mao, Xin
AU - Lian, Cheng
AU - Ge, Lei
AU - Du, Aijun
AU - Xu, Zhi
AU - More Authors, null
PY - 2023
Y1 - 2023
N2 - The highly efficient and stable electrolysis needs the rational control of the catalytically active interface during the reactions. Here we report a new operando surface restructuring pathway activated by pairing catalyst and electrolyte ions. Using SrCoO3-δ-based perovskites as model catalysts, we unveil the critical role of matching the catalyst properties with the electrolyte conditions in modulating catalyst ion leaching and steering surface restructuring processes toward efficient oxygen evolution reaction catalysis in both pH-neutral and alkaline electrolytes. Our results regarding multiple perovskites show that the catalyst ion leaching is controlled by catalyst ion solubility and anions of the electrolyte. Only when the electrolyte cations are smaller than catalyst's leaching cations, the formation of an outer amorphous shell can be triggered via backfilling electrolyte cations into the cationic vacancy at the catalyst surface under electrochemical polarization. Consequently, the current density of reconstructed SrCoO3-δ is increased by 21 folds compared to the pristine SrCoO3-δ at 1.75 V vs reversible hydrogen electrode and outperforms the benchmark IrO2 by 2.1 folds and most state-of-the-art electrocatalysts in the pH-neutral electrolyte. Our work could be a starting point to rationally control the electrocatalyst surface restructuring via matching the compositional chemistry of the catalyst with the electrolyte properties.
AB - The highly efficient and stable electrolysis needs the rational control of the catalytically active interface during the reactions. Here we report a new operando surface restructuring pathway activated by pairing catalyst and electrolyte ions. Using SrCoO3-δ-based perovskites as model catalysts, we unveil the critical role of matching the catalyst properties with the electrolyte conditions in modulating catalyst ion leaching and steering surface restructuring processes toward efficient oxygen evolution reaction catalysis in both pH-neutral and alkaline electrolytes. Our results regarding multiple perovskites show that the catalyst ion leaching is controlled by catalyst ion solubility and anions of the electrolyte. Only when the electrolyte cations are smaller than catalyst's leaching cations, the formation of an outer amorphous shell can be triggered via backfilling electrolyte cations into the cationic vacancy at the catalyst surface under electrochemical polarization. Consequently, the current density of reconstructed SrCoO3-δ is increased by 21 folds compared to the pristine SrCoO3-δ at 1.75 V vs reversible hydrogen electrode and outperforms the benchmark IrO2 by 2.1 folds and most state-of-the-art electrocatalysts in the pH-neutral electrolyte. Our work could be a starting point to rationally control the electrocatalyst surface restructuring via matching the compositional chemistry of the catalyst with the electrolyte properties.
KW - Cation size-matching
KW - Non-acidic medium
KW - Operando surface restructuring
KW - Oxygen evolution
KW - Strontium ion leaching
UR - http://www.scopus.com/inward/record.url?scp=85140952212&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2022.140071
DO - 10.1016/j.cej.2022.140071
M3 - Article
AN - SCOPUS:85140952212
SN - 1385-8947
VL - 454
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 140071
ER -