Li Xijuan, Li Zhiqian, Zhang Zining, Zhao Yuxiao, Fang Qi, Tang Jing, He Jianping
College of Materials Science and Technology, Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China.
Nanoscale. 2024 Sep 26;16(37):17527-17536. doi: 10.1039/d4nr02240h.
Electroreduction of carbon dioxide (CO) to multiple carbon products plays a significant role in carbon neutrality and the production of valuable chemicals. Herein, we developed a magnesium-modified copper oxide nanosheet catalyst (Mg-CuO) using a post-impregnation method. Comprehensive elemental analysis demonstrated the effective incorporation of magnesium into CuO nanosheets, resulting in a noticeable alteration of the electron density of Cu atoms. Consequently, the Mg-CuO nanosheets exhibited an increased efficiency for CO electroreduction in comparison with the unmodified CuO nanosheets. The optimized Mg-CuO catalyst exhibited faradaic efficiencies of 46.33% for ethylene production and 62.64% for C production at -1.3 V reversible hydrogen electrode (RHE). DFT proved that the introduction of Mg species could increase the charge density of Cu and decrease the adsorption energy of *CO, which promoted C-C coupling and enhanced the selectivity of C products. This study presents an effective way to adjust the electronic structure of common copper-based electrocatalysts and the corresponding interaction with *CO, resulting in an improved faradaic efficiency of C products.
将二氧化碳（CO₂）电还原为多碳产物在碳中和及有价值化学品的生产中发挥着重要作用。在此，我们采用后浸渍法制备了一种镁修饰的氧化铜纳米片催化剂（Mg-CuO）。全面的元素分析表明镁有效地掺入到CuO纳米片中，导致Cu原子的电子密度发生显著变化。因此，与未修饰的CuO纳米片相比，Mg-CuO纳米片对CO₂电还原表现出更高的效率。优化后的Mg-CuO催化剂在-1.3 V可逆氢电极（RHE）下对乙烯生成的法拉第效率为46.33%，对C₂产物生成的法拉第效率为62.64%。密度泛函理论（DFT）证明，Mg物种的引入可增加Cu的电荷密度并降低CO的吸附能，从而促进C-C偶联并提高C₂产物的选择性。本研究提出了一种有效方法来调节常见铜基电催化剂的电子结构及其与CO的相应相互作用，从而提高C₂产物的法拉第效率。
