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通过CO₂脉冲电还原在气流细胞中的Cu纳米晶体的选择性控制

Hyo Sang Jeon¹, Janis Timoshenko¹, Clara Rettenmaier¹

¹Department of Interface Science, Fritz-Haber Institute of the Max-Planck Society, 14195 Berlin, Germany.

Journal of the American Chemical Society

|May 6, 2021

概括

使用铜催化剂的二氧化碳 (CO2RR) 脉冲电降低提高了对C2产品或甲的选择性. 这种调整是通过控制氧化和还原电位脉冲来操纵催化剂结构和局部pH值来实现的.

科学领域:

电化学
催化剂
材料科学

背景情况:

在二氧化碳电还原 (CO2RR) 中调节产品的选择性对于可持续的化学生产至关重要.
铜 (Cu) 催化剂对CO2RR具有前景,但通常具有有限的选择性.
脉冲电解提供了控制反应途径和提高催化剂性能的潜在策略.

研究的目的:

研究脉冲电还原条件对铜催化剂对CO2RR的选择性的影响.
在工业相关的电流密度下比较脉冲电解与静电条件.
阐明导致产品选择性增强的潜在机制.

主要方法:

在电静电和脉冲电解条件下使用气体供应流量电池进行二氧化碳电解.
采用不同氧化电位的脉冲电解 (0.61.5V_RHE),然后进行减电脉冲 (-0.7V_RHE).
使用XAS,SERS和SEM/TEM进行了催化剂结构和表面化学的特征.

主要成果:

在E_an=0. 9V_RHE的脉冲电解中,与静电条件相比,提高了10%的C2产品选择性 (FE_C2=43. 6%) (FE_C2=40. 9%).
在E_an=1.2 V_RHE的脉冲电解中,甲选择性显著增加 (FE_CH4=48.3%),而非静电对照 (FE_CH4=0.1%).
催化剂的结构修改 (缺陷接口,粒度边界) 和局部pH变化被确定为影响选择性的关键因素.

结论:

脉冲二氧化碳减排是一种有效的策略来调整产品的分销和提高选择性.
在脉冲条件下,形态重建和局部pH调节是控制催化剂性能的关键机制.
这种方法为实现更高效和选择性的二氧化碳电化学转化提供了途径.

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