Coupling Value-Added Methanol Oxidation with CO 2 Electrolysis by Low-Coordinated Atomic Ni Sites

作者：Kang Lian, Sanshuang Gao, Wenxian Liu, Qian Liu, Yanhong Feng, Jun Luo, Guangzhi Hu, Ke Chu, Dingsheng Wang, Xijun Liu · 发表于：ACS Nano · 年份：2025 · DOI：10.1021/acsnano.5c03677 · 被引用次数：53 · 研究领域：CO2 Reduction Techniques and Catalysts、Electrocatalysts for Energy Conversion、Catalytic Processes in Materials Science

The combination of CO 2 fixation and small organic molecule oxidation offers a promising solution to increasing severe environmental issues and energy crises. Here, low-coordinated NiN 3 sites were anchored onto nitrogen-doped ordered mesoporous carbon (Ni-SAs/NOMC), which is capable of efficiently catalyzing the coupled methanol oxidation reaction and CO 2 reduction reaction (MOR||CO 2 RR), thereby reducing the energy required for CO 2 conversion and enhancing the economic value of the CO 2 electrolytic system. In the membrane electrode assembly electrolyzer-based MOR||CO 2 RR, Ni-SAs/NOMC achieved Faradaic efficiencies (FEs) of 95.4% for formate at the anode and 96.3% for CO at the cathode. Moreover, at a current density of 0.8 A cm –2, Ni-SAs/NOMC demonstrated stable electrolysis for up to 100 h, with FEs at both the anode and cathode remaining stable at approximately 90%. In situ spectroscopy analyses and theoretical calculations identified the formation of critical intermediate species and the origin of activity improvement, guiding the development of efficient electrosynthesis of valuable chemicals.