Unconventional grain fragmentation creates high-density boundaries for efficient CO2-to-C2+ electro-conversion at ampere-level current density
2024; Elsevier BV; Volume: 128; Linguagem: Inglês
10.1016/j.nanoen.2024.109945
ISSN2211-3282
AutoresJunjie Ding, Qianling Song, Lu Xia, Lujie Ruan, Min Zhang, Chaogang Ban, Jiazhi Meng, Jiangping Ma, Yajie Feng, Yang Wang, Xiaoping Tao, Danmei Yu, Jiyan Dai, Li‐Yong Gan, Xiaoyuan Zhou,
Tópico(s)Electrocatalysts for Energy Conversion
ResumoElectrocatalytic CO2 reduction reaction (CO2RR) to produce multi-carbon products (C2+) is one of the most sustainable manners to achieve net-zero carbon emissions. Among many approaches, enriching grain boundaries (GBs) in copper (Cu) catalysts has been demonstrated to enable enhancement for C2+ production. However, it still lacks effective strategies to controllably synthesize abundant GBs, rendering efficient C2+ production a persistent challenge, especially at ampere-level current density. Herein, we propose a novel strategy, which can achieve unconventional grain fragmentation during thermal annealing and thus create controllable GB densities. The catalyst with the utmost GB density exhibits a peak C2+ faradaic efficiency (FE) of ca. 70.0% in an H-type cell and 68.2% in a flow cell; even more impressively, it delivers an ultra-high C2+ current density of 0.768 A cm-2, outperforming most recently reported results. A combination of in situ spectroscopies and theoretical calculations reveal that the enrichment of GBs yields more active sites for a higher ⁎CO coverage, leading to promotion of the ⁎CO-⁎CO coupling process and ultimately high C2+ production performance.
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