Citation: Xue Dong, Xiaofu Sun, Shuaiqiang Jia, Shitao Han, Dawei Zhou, Ting Yao, Min Wang, Minghui Fang, Haihong Wu, Buxing Han. 碳修饰的铜催化剂实现安培级电流电化学还原CO₂制C₂₊产物[J]. Acta Physico-Chimica Sinica, ;2025, 41(3): 240401. doi: 10.3866/PKU.WHXB202404012 shu

碳修饰的铜催化剂实现安培级电流电化学还原CO₂制C₂₊产物

Xue Dong ¹ ,
Xiaofu Sun ² ,
Shuaiqiang Jia ¹ ,
Shitao Han ¹ ,
Dawei Zhou ¹ ,
Ting Yao ¹ ,
Min Wang ¹ ,
Minghui Fang ¹ ,
Haihong Wu ¹ ,
Buxing Han ^1,2

1.
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China;
2.
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China

Received Date: 8 April 2024
Revised Date: 7 May 2024
Accepted Date: 7 May 2024

Fund Project: The work was supported by the National Key Research and Development Program of China (2023YFA1507901, 2020YFA0710201) and National Natural Science Foundation of China (22293015, 22121002).

铜基电催化剂在CO₂还原反应(CO₂RR)中产高附加值产物的潜力巨大，是实现碳负排放的一种很有前景的途径。同时，安培级电流是实现多碳(C₂₊)产业化的关键。然而，由于复杂的电子传递过程和不可避免的副反应，工业电流密度下的C₂₊选择性仍然不令人满意。在此，我们开发了一种碳修饰策略来优化局部环境并调节中间产物在Cu活性位点的吸附。结果表明，Cu-C_x催化剂(x为催化剂中C的原子百分数)能有效催化CO₂RR生成C₂₊产物。特别是在流动池中，Cu-C_6%在-0.72 V vs. RHE(相对可逆氢电极)条件下，电流密度可达1.25 A∙cm^-2, C₂H₄和C₂₊产物的法拉第效率(FE)分别可达54.4%和80.2%。原位光谱分析和密度泛函理论(DFT)计算表明，C的存在调节了^*CO在Cu表面的吸附，降低了C―C耦合的能垒，从而促进了C₂₊产物的生成。
- CO₂ reduction,
- Electrocatalysis,
- Multi-carbon products,
- Green chemistry,
- Ampere-level current
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碳修饰的铜催化剂实现安培级电流电化学还原CO₂制C₂₊产物