Constructing Hydrogen Migration Channel from Atomic Clusters to Single Atom for Superior Electrocatalytic Hydrogen Evolution with Ultralow Pt Loading
Abstract
Abstract Developing highly active and durable cathode catalysts using minimal use of noble metal remains a grand challenge for proton exchange membrane water electrolyzer. Herein we design a Pt‐based sub‐nanometric catalysts featuring coexisting single atoms and atomic clusters anchored on sulfur‐doped carbon. This dual‐active‐site architecture enables independent optimization of active hydrogen (H*) formation and subsequent recombination kinetics, thus breaking the limitation of Sabatier principle. Specially, by introducing a secondary transition metal such as Mn, the interfacial charge distribution and work function of Pt clusters is regulated, promoting both H* formation and migration. Meanwhile, the neighboring electron‐deficient Pt single atoms facilitate H* recombination kinetics. The catalyst with 3.6 wt% Pt loading achieves a recorded mass activity of 14.48 A mg −1 at 15 mV, exceeding commercial 40wt% Pt/C by 41‐fold. When integrated into an electrolyzer, the catalyst demonstrates exceptional activity and stability with only 10% Pt loading relative to commercial benchmark, representing a critical advancement toward practical green hydrogen production. Also, the direct evidences of H* formation, migration and recombination process are confirmed by operando experiments and theoretical calculations for the first time, which offers new concept for decoupling of HER reaction and rational design of catalysts.
Article Details
Authors (13)
Zexing He
School of Chemical Engineering and Technology Key Laboratory for Green Chemical Technology of Ministry of Education Tianjin University Tianjin China
Xiaokang Liu
State Key Laboratory of Geomicrobiology and Environmental Changes, School of Earth Sciences, China University of Geosciences
Minghui Zhang
Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering
Yajun Wang
State Key Laboratory of Coordination Chemistry, Jiangsu Key Laboratory of Advanced Organic Materials, Chemistry and Biomedicine Innovation Center, ChemBioMed Interdisciplinary Research Center, School of Chemistry
Zhen‐Feng Huang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry‐Education Platform for Energy Storage Tianjin University Tianjin 300072 China
Chengxiang Shi
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Ruijie Gao
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Lun Pan
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Chong Peng
Wanliang Mi
Xiangwen Zhang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Jinlong Gong
School of Chemical Engineering and Technology, Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University
Ji‐Jun Zou
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry‐Education Platform for Energy Storage Tianjin University Tianjin 300072 China