T v argeted-tuning competitive acidic CO2RR ia metalloid antagonism sites

作     者：Sheng, Beibei Cao, Dengfeng Qi, Zhenghang Shou, Hongwei Xia, Yujian Su, Xiaozhi Chen, Shuangming Wu, Chuanqiang Liu, Hengjie Chimtali, Peter Joseph Chu, Yongheng Liu, Chongjing Wu, Xiaojun Song, Li 

作者机构：Univ Sci & Technol China CAS Ctr Excellence Nanosci Sch Nucl Sci & Technol Natl Synchrotron Radiat LabKey Lab Precis & Intel Hefei 230029 Peoples R China SINOPEC Shanghai Res Inst Petrochem Technol Co Ltd Shanghai 201208 Peoples R China Tarim Univ Coll Chem & Chem Engn Engn Lab Chem Resources Utilizat South Xinjiang Xi Alar 843300 Peoples R China Univ Sci & Technol China CAS Ctr Excellence Nanosci & Synerget Innovat Quan Sch Chem & Mat Sci Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China Lawrence Berkeley Natl Lab Adv Light Source Berkeley CA 94720 USA Chinese Acad Sci Shanghai Inst Appl Phys Shanghai Synchrotron Radiat Facil Shanghai 201204 Peoples R China Anhui Univ Inst Phys Sci & Informat Technol Informat Mat & Intelligent Sensing Lab Anhui Prov Hefei 230601 Peoples R China 

出 版 物：《MATERIALS TODAY》 (Mater. Today)

年 卷 期：2025年第83卷

页      面：54-63页

核心收录：

学科分类：08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 

基　　金：National Key R&D Program of China [2022YFA1605400] NSFC [12225508, 12322515, U23A20121, 22075264, 12305370] CAS Youth Innovation Promotion Association Key Program of Research and Development of Hefei Science Cen-ter [2022HSC-KPRD003] China Postdoctoral Science Foundation [BX20220282, 2022M720136] Anhui Provincial Natural Science Foundation [2308085QA16] 

主　　题：Synchrotron radiation 

摘      要：To mitigate the high separation costs associated with conventional neutral/alkaline electrocatalysis for CO2 reduction reactions (CO2RR), acidic CO2RR offers economic advantages and improved efficiency in CO2 utilization. However, it typically involves the cleavage of M H bonds at a relatively negative potential, leading to the predominant formation of H2 and poor HCOOH selectivity. Herein, we develop a facile solid-phase thermal diffusion approach to controllably synthesize a novel metalloid- metal single atom alloys (m-SAAs) electrocatalyst Te1Bi with unique metalloid antagonistic sites, thus enabling high-efficient acidic CO2-to-HCOOH conversion. Electrochemical test and operando synchrotron radiation multi-techniques (SRMS) characterization reveal that metalloid Te sites bring steric hindrance effect and blocks *H coupling. Furthermore, it actively adsorbs OH species as a proton source, allowing for effective separation of protons and electrons in space. Thus, leading to enhanced hydrogenation in acidic CO2RR to produce HCOOH. The flow cell test results demonstrate that the carefully designed Te1Bi catalyst exhibits a milder reaction potential, along with higher HCOOH Faraday efficiency (similar to 94.5 %) and single-pass carbon efficiency (SPCE, similar to 40 %) in acidic media. This work significantly expands the family of SAAs and offers a novel perspective to analyze the regulation of competitive reactions through site-specific modifications for industrial acidic CO2RR.