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

被引：0

作者：

Sheng, Beibei ^{[1
,2
]}

Cao, Dengfeng ^{[1
]}

Qi, Zhenghang ^{[1
,3
]}

Shou, Hongwei ^{[4
]}

Xia, Yujian ^{[5
]}

Su, Xiaozhi ^{[6
]}

Chen, Shuangming ^{[1
]}

Wu, Chuanqiang ^{[7
]}

Liu, Hengjie ^{[1
]}

Chimtali, Peter Joseph ^{[1
]}

Chu, Yongheng ^{[1
]}

Liu, Chongjing ^{[1
]}

Wu, Xiaojun ^{[4
]}

Song, Li ^{[1
]}

机构：

[1] Univ Sci & Technol China, CAS Ctr Excellence Nanosci, Sch Nucl Sci & Technol, Natl Synchrotron Radiat Lab,Key Lab Precis & Intel, Hefei 230029, Peoples R China

[2] SINOPEC Shanghai Res Inst Petrochem Technol Co Ltd, Shanghai 201208, Peoples R China

[3] Tarim Univ, Coll Chem & Chem Engn, Engn Lab Chem Resources Utilizat South Xinjiang Xi, Alar 843300, Peoples R China

[4] 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

[5] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA

[6] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China

[7] Anhui Univ, Inst Phys Sci & Informat Technol, Informat Mat & Intelligent Sensing Lab Anhui Prov, Hefei 230601, Peoples R China

来源：

MATERIALS TODAY | 2025年 / 83卷

基金：

中国博士后科学基金; 国家重点研发计划;

关键词：

CARBON-DIOXIDE; ELECTROLYSIS; ELECTRODES; REDUCTION; CO;

D O I：

10.1016/j.mattod.2024.12.007

中图分类号：

T [工业技术];

学科分类号：

08 ;

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.

引用

页码：54 / 63

页数：10