Toward Practical Design of High‐Entropy Catalysts for Chlorine Evolution Reaction via Pareto‐Guided Multi‐Objective Bayesian Optimization Enabled by a Robotic AI‐Chemist

R Ruyu Yang D Donglai Zhou (State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science) Z Zijin Jia (State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China) Y Yulan Han (Department of Chemistry and Biochemistry) L Lianyou Tang (State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China) Z Zifan Jiang (State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China) X Xiaolin Tai (State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science) Y Yuhai Cai (State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China) W Wenhui Zhong (Institute of Intelligent Innovation, Henan Academy of Sciences) Y Yue Lin H Hao Wang (Division of Quantitative Sciences, Department of Oncology Johns Hopkins University School of Medicine Baltimore Maryland USA) J Jixian Xu (State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China) Y Yan Huang J Jun Jiang (State Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science) Q Qing Zhu

Abstract

ABSTRACT The electrocatalytic chlorine evolution reaction (CER) is essential to modern chlor‐alkali industry, yet conventional RuO 2 catalysts suffer from parasitic oxygen evolution. High‐entropy ruthenium oxides (Ru‐HEO) are promising alternatives, but their practical design is hindered by complex composition‐structure‐performance relationship. Herein, we construct a Pareto‐guided multi‐objective Bayesian optimization framework to enable autonomous high‐throughput exploration of quinary Ru‐HEO system. Through this trade‐off strategy, we identify compositions that efficiently balance mass activity, Cl 2 selectivity and material cost. The leading Ru‐HEO catalyst with only 8.4 at% Ru achieves a remarkable activity of 5083 A g −1 Ru at 1.50 V versus RHE and maintains excellent 100‐h stability, outperforming commercial RuO 2 and the state‐of‐the‐art catalysts reported. Integrated into a photovoltaic‐electrochemical (PV‐EC) prototype device and tested under simulated diurnal illumination, it sustains >95% selectivity, a maximum solar‐to‐chemical (STC) efficiency of 14.6% and projected Cl 2 production costs as low as $0.177 per kg. Our work establishes a closed‐loop, AI‐accelerated research paradigm that integrates multi‐objective optimization with robotic experimentation, offering a generalizable and expedited pathway toward high‐performance electrocatalysts for sustainable chemicals manufacturing.

Article Details

Volume / Issue Vol. 65, Issue 27
Published July 01, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (15)

R

Ruyu Yang

D

Donglai Zhou

State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science

Z

Zijin Jia

State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China

Y

Yulan Han

Department of Chemistry and Biochemistry

L

Lianyou Tang

State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China

Z

Zifan Jiang

State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China

X

Xiaolin Tai

State Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science

Y

Yuhai Cai

State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China

W

Wenhui Zhong

Institute of Intelligent Innovation, Henan Academy of Sciences

Y

Yue Lin

H

Hao Wang

Division of Quantitative Sciences, Department of Oncology Johns Hopkins University School of Medicine Baltimore Maryland USA

J

Jixian Xu

State Key Laboratory of Precision and Intelligent Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei China

Y

Yan Huang

J

Jun Jiang

State Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science

Q

Qing Zhu