Sn/nitrogen-doped carbon composites with enhanced CO2 electroreduction toward formate

IF 6.3 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Surfaces and Interfaces Pub Date : 2025-02-15 Epub Date: 2025-02-08 DOI:10.1016/j.surfin.2025.105990
Xiaohui Zhong , Tingting Yang , Qingqing Zhang , Jingwen Wang , Hong Deng , Yong Zhou
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Abstract

Electrochemical CO2 reduction reaction (CO2RR) using renewable energy resources is a promising method for both mitigating the atmospheric CO2 level and producing valuable chemicals. The morphology design and interface charge transfer of catalysts play a critical role in the activity and selectivity of CO2RR. Herein, Sn@nitrogen-doped carbon (Sn@NC) was successfully developed by the loading procedure, enabling the direct conversion of CO2 to C1 products with excellent electrocatalytic performances. The target electrocatalyst Sn@NC-700 exhibits a high Faradaic efficiency of up to 93.2 % for formate product, with a partial current density of 22.3 mA cm-2 at -1.03 V versus RHE. Moreover, the Sn@NC-700 electrocatalyst has remarkable stability in generating formate during CO2RR, without obvious attenuation over the reaction time of 50 h. The electrochemical data and density functional theory calculations indicate that the inherent structural features, such as superior conductivity and rapid charge transfer, promote the Sn@NC electrode to stabilize the *OCHO intermediates, thereby accelerating the production of formate. This study is beneficial for reducing carbon emissions, promoting resource recycling, and advancing a green and sustainable production of formate to serve the chemical industry.

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锡/氮掺杂碳复合材料对甲酸盐的强化CO2电还原
利用可再生能源的电化学CO2还原反应(CO2RR)是一种既能降低大气CO2浓度又能生产有价值化学品的有前途的方法。催化剂的形态设计和界面电荷转移对CO2RR的活性和选择性起着至关重要的作用。其中,通过负载过程成功开发了Sn@nitrogen-doped碳(Sn@NC),使CO2直接转化为具有优异电催化性能的C1产物成为可能。目标电催化剂Sn@NC-700对甲酸产物具有高达93.2%的法拉第效率,在-1.03 V时相对于RHE的偏电流密度为22.3 mA cm-2。此外,Sn@NC-700电催化剂在CO2RR过程中生成甲酸具有显著的稳定性,在50 h的反应时间内没有明显的衰减。电化学数据和密度泛函理论计算表明,Sn@NC电极固有的结构特征,如优越的电导率和快速的电荷转移,促进了*OCHO中间体的稳定,从而加速了甲酸的生成。本研究有利于减少碳排放,促进资源循环利用,推进甲酸酯的绿色可持续生产,为化工行业服务。
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sodium borohydride
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tin (IV) chloride pentahydrate
来源期刊
Surfaces and Interfaces
Surfaces and Interfaces Chemistry-General Chemistry
CiteScore
8.50
自引率
6.50%
发文量
753
审稿时长
35 days
期刊介绍: The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results. Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)
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