Li Minhan, Wang Haifeng, Luo Wei, Sherrell Peter C, Chen Jun, Yang Jianping
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, International Joint Laboratory for Advanced Fiber and Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, P. R. China.
Department of Chemical Engineering, The University of Melbourne, Parkville, VIC, 3010, Australia.
Adv Mater. 2020 Aug;32(34):e2001848. doi: 10.1002/adma.202001848. Epub 2020 Jul 9.
The electrochemical CO reduction reaction (CO RR) is of great importance to tackle the rising CO concentration in the atmosphere. The CO RR can be driven by renewable energy sources, producing precious chemicals and fuels, with the implementation of this process largely relying on the development of low-cost and efficient electrocatalysts. Recently, a range of heterogeneous and potentially low-cost single-atom catalysts (SACs) containing non-precious metals coordinated to earth-abundant elements have emerged as promising candidates for the CO RR. Unfortunately, the real catalytically active centers and the key factors that govern the catalytic performance of these SACs remain ambiguous. Here, this ambiguity is addressed by developing a fundamental understanding of the CO RR-to-CO process on SACs, as CO accounts for the major product from CO RR on SACs. The reaction mechanism, the rate-determining steps, and the key factors that control the activity and selectivity are analyzed from both experimental and theoretical studies. Then, the synthesis, characterization, and the CO RR performance of SACs are discussed. Finally, the challenges and future pathways are highlighted in the hope of guiding the design of the SACs to promote and understand the CO RR on SACs.
电化学CO还原反应（CO RR）对于应对大气中不断上升的CO浓度至关重要。CO RR可以由可再生能源驱动，生产珍贵的化学品和燃料，该过程的实施很大程度上依赖于低成本且高效的电催化剂的开发。最近，一系列含有与储量丰富的元素配位的非贵金属的多相且潜在低成本的单原子催化剂（SAC）已成为CO RR的有前途的候选者。不幸的是，这些SAC的真正催化活性中心以及决定其催化性能的关键因素仍然不明确。在此，通过对SAC上CO RR生成CO的过程形成基本认识来解决这一模糊性问题，因为CO是SAC上CO RR的主要产物。从实验和理论研究两方面分析了反应机理、速率决定步骤以及控制活性和选择性的关键因素。然后，讨论了SAC的合成、表征及CO RR性能。最后，强调了挑战和未来的方向，希望能指导SAC的设计，以促进并理解SAC上的CO RR。
