Trace Chlorine‐Induced Lattice Oxygen Activation for Enhanced High‐Temperature CO <sub>2</sub> Electrolysis
Abstract
Abstract Tuning lattice oxygen activity in perovskite oxides (ABO 3 ) offers a promising approach to overcome the intrinsic trade‐off between catalytic activity and stability in redox reactions. However, precise modulation and mechanistic understanding of lattice oxygen activation remain elusive under high‐temperature CO 2 electrolysis conditions. Herein, a novel anion activation strategy is proposed by incorporating trace chloride ions (Cl − ) into the O‐sites of Sr 2 Fe 1.5 Mo 0.5 O 6−δ perovskite forming an oxychloride cathode. This Cl − substitution activates lattice oxygen reactivity by weakening Mo−O/Fe−O covalency, thereby facilitating the formation and redistribution of oxygen vacancies, accelerating bulk oxygen ion transport, enhancing CO 2 adsorption and carbonate intermediate formation, and ultimately promoting CO 2 reduction kinetics. As a result, the oxychloride cathode achieves a 60.2–80.8% enhancement in CO 2 ‐to‐CO electrolysis, reaching 2.02 A cm −2 at 800 °C and 1.5 V with ≈100% Faradaic efficiency, while maintaining exceptional stability of 500 h. This work establishes a new paradigm of O‐site anion engineering to unlock lattice oxygen activity for electrocatalytic reactions.
Article Details
Authors (14)
Shaowei Zhang
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics
Xueyu Hu
School of Materials Science and Engineering
Tianfu Liu
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics
Hewei Liu
College of Light Industry and Chemical Engineering
Yige Guo
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics
Geng Zou
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials)
Wenwen Zhang
Xiaomin Zhang
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials)
Peng Zhang
Runsheng Yu
Yuefeng Song
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics
Changrong Xia
CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China No. 96 Jinzhai Road Hefei 230026 P. R. China
Guoxiong Wang
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics
Xinhe Bao
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics