journal article·2024-08

Universal Formation of Single Atoms from Molten Salt for Facilitating Selective CO2 Reduction

Qi Hao, Cheng Zhen, Qi Tang, Jiazhi Wang, Peiyu Ma, Junxiu Wu, Tianyang Wang, Dongxue Liu, Linxuan Xie, Xiao Liu, M. Danny Gu, Michael R. Hoffmann, Gang Yu, Kai Liu, Jun Lu

Advanced Materials· Volume 36· Issue 33
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Abstract

Abstract Clarifying the formation mechanism of single‐atom sites guides the design of emerging single‐atom catalysts (SACs) and facilitates the identification of the active sites at atomic scale. Herein, a molten‐salt atomization strategy is developed for synthesizing zinc (Zn) SACs with temperature universality from 400 to 1000/1100 °C and an evolved coordination from Zn‐N2Cl2 to Zn‐N4. The electrochemical tests and in situ attenuated total reflectance‐surface‐enhanced infrared absorption spectroscopy confirm that the Zn‐N4 atomic sites are active for electrochemical carbon dioxide (CO2) conversion to carbon monoxide (CO). In a strongly acidic medium (0.2 m K2SO4, pH = 1), the Zn SAC formed at 1000 °C (Zn1NC) containing Zn‐N4 sites enables highly selective CO2 electroreduction to CO, with nearly 100% selectivity toward CO product in a wide current density range of 100–600 mA cm−2. During a 50 h continuous electrolysis at the industrial current density of 200 mA cm−2, Zn1NC achieves Faradaic efficiencies greater than 95% for CO product. The work presents a temperature‐universal formation of single‐atom sites, which provides a novel platform for unraveling the active sites in Zn SACs for CO2 electroreduction and extends the synthesis of SACs with controllable coordination sites.
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Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Catalytic Processes in Materials Science

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Materials Science & Engineering Zhejiang University Hangzhou Zhejiang 310027 China

School of Engineering Westlake University Hangzhou Zhejiang 310030 China

Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China

Eastern Institute for Advanced Study Eastern Institute of Technology Ningbo Zhejiang 315200 China

State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun Jilin 130022 China

School of Applied Chemistry and Engineering University of Science and Technology of China Hefei Anhui 230026 China

Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 China

Key Laboratory of Precision and Intelligent Chemistry National Synchrotron Radiation Laboratory iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) University of Science and Technology of China Hefei Anhui 230026 China

College of Chemical and Biological Engineering Zhejiang University Hangzhou Zhejiang 310027 China

Key Laboratory of Automobile Materials Ministry of Education and College of Materials Science and Engineering Jilin University Changchun Jilin 130022 China

Department of Environmental Science and Engineering California Institute of Technology 1200 E California Blvd Pasadena CA 91125 USA

Merging Contaminants Research Center Beijing Normal University Zhuhai Guangdong 519087 China

Funding

China Postdoctoral Science Foundation

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