Zhou Dawei, Chen Chunjun, Zhang Yichi, Wang Min, Han Shitao, Dong Xue, Yao Ting, Jia Shuaiqiang, He Mingyuan, Wu Haihong, Han Buxing
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China.
State Key Laboratory of Petroleum Molecular and Process engineering, SKLPMPE, Sinopec research institute of petroleum processing Co., LTD., Beijing, 100083, China.
Angew Chem Int Ed Engl. 2024 Apr 8;63(15):e202400439. doi: 10.1002/anie.202400439. Epub 2024 Feb 29.
Electroreduction of CO to C products provides a promising strategy for reaching the goal of carbon neutrality. However, achieving high selectivity of C products at high current density remains a challenge. In this work, we designed and prepared a multi-sites catalyst, in which Pd was atomically dispersed in Cu (Pd-Cu). It was found that the Pd-Cu catalyst had excellent performance for producing C products from CO electroreduction. The Faradaic efficiency (FE) of C products could be maintained at approximately 80.8 %, even at a high current density of 0.8 A cm for at least 20 hours. In addition, the FE of C products was above 70 % at 1.4 A cm. Experiments and density functional theory (DFT) calculations revealed that the catalyst had three distinct catalytic sites. These three active sites allowed for efficient conversion of CO, water dissociation, and CO conversion, ultimately leading to high yields of C products.
将CO电还原为含碳产物为实现碳中和目标提供了一种很有前景的策略。然而，在高电流密度下实现含碳产物的高选择性仍然是一个挑战。在这项工作中，我们设计并制备了一种多位点催化剂，其中Pd原子分散在Cu中（Pd-Cu）。研究发现，Pd-Cu催化剂在CO电还原制备含碳产物方面具有优异的性能。即使在0.8 A cm的高电流密度下至少20小时，含碳产物的法拉第效率（FE）仍可维持在约80.8%。此外，在1.4 A cm时，含碳产物的FE高于70%。实验和密度泛函理论（DFT）计算表明，该催化剂有三个不同的催化位点。这三个活性位点实现了CO的高效转化、水的解离和CO的转化，最终实现了含碳产物的高产率。
