Trace Chlorine-Induced Lattice Oxygen Activation for Enhanced High-Temperature CO_2 Electrolysis

Shaowei Zhang ¹Xueyu Hu ²Tianfu Liu ¹Hewei Liu ¹Yige Guo ³Geng Zou ³Wenwen Zhang ¹Xiaomin Zhang ¹Peng Zhang ⁴Runsheng Yu ⁴Yuefeng Song ¹Changrong Xia ⁵Guoxiong Wang ⁶Xinhe Bao⁶

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作者信息

1. 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 Chinese Academy of Sciences Dalian 116023,China
2. School of Materials Science and Engineering Georgia Institute of Technology Atlanta,GA 30332-0245,USA
3. 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 Chinese Academy of Sciences Dalian 116023,China||College of Energy University of Chinese Academy of Sciences Beijing 100049,China
4. Multi-disciplinary Research Division Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049,China
5. 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||Energy Materials Center Anhui Estone Materials Technology Co.Ltd 2-A-1,No.106,Chuangxin Avenue,Hefei 230088,P.R.China
6. 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 Chinese Academy of Sciences Dalian 116023,China||Advanced Institute for Future Energy Shanghai Key Laboratory of Electrochemical and Thermochemical Conversion for Resources Recycling State Key Laboratory of Porous Materials for Separation and Conversion iChEM (Collaborative Innovation Center of Chemistry for Energy Materi
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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 ℃ 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.

Key words

chloride substitution/CO_2 electrolysis/lattice oxygen activation/perovskite/oxychloride/solid oxide electrolysis cells

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出版年

2026

Advanced Materials

ISSN：0935-9648

参考文献量53

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