Tunable Ag-Ox coordination for industrial-level carbon-negative CO2 electrolysis

作者：Hao Chen, Qi Huang, Kang Yang, Sheng Chen, Hao Feng, Jia Chen, Qiang Li, Zhao Chuan, Jingjing Duan · 发表于：Nano Energy · 年份：2024 · DOI：10.1016/j.nanoen.2024.110265 · 被引用次数：8 · 研究领域：CO2 Reduction Techniques and Catalysts、Carbon dioxide utilization in catalysis、Ammonia Synthesis and Nitrogen Reduction

The electrochemical CO 2 reduction (eCO 2 RR) is promising for eliminating CO 2 , generate valuable chemicals and utilize spare electricity. However, its industrialization is greatly hindered by low CO 2 single-pass conversion efficiency (SPCE) in alkaline/neutral electrolytes, and poor compatibility between the electrolysis and intermittent energy system. Herein, a carbon-negative acidic eCO 2 RR system is developed using acidic-tolerant Ag based metal-organic frameworks (Ag-MOFs), achieving a high Faradaic efficiency of CO above 97 % in a broad working window of 10–400 mA cm −2 for unsaturated Ag-O2 clusters, and a high CO 2 SPCE of 46.3 % even under industrial-level 400 mA cm −2 . Being connected to solar cells, the acidic eCO 2 RR system displays a remarkable solar-to-chemical efficiency of 19.74 %, offering great potential for industrial eCO 2 RR directly driven by renewable energy . Specifically, the CO/HCOOH selectivity could be manipulated by adjusting the coordination number of Ag atoms in Ag-MOFs, and thus a Pourbaix-diagram is proposed to explain the tunable selectivity theoretically.