Chen Zhangsen, Zhang Gaixia, Du Lei, Zheng Yi, Sun Lixian, Sun Shuhui
Institut National de la Recherche Scientifique-Énergie Matériaux et Télécommunications, Varennes, Québec, J3 × 1S2, Canada.
Research Institute of Photocatalysis, State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou, 350116, P. R. China.
Small. 2020 Dec;16(52):e2004158. doi: 10.1002/smll.202004158. Epub 2020 Dec 1.
CO reduction reaction (CO RR) provides a promising strategy for sustainable carbon fixation by converting CO into value-added fuels and chemicals. In recent years, considerable efforts are focused on the development of transition-metal (TM)-based catalysts for the selectively electrochemical CO reduction reaction (ECO RR). Co-based catalysts emerge as one of the most promising electrocatalysts with high Faradaic efficiency, current density, and low overpotential, exhibiting excellent catalytic performance toward ECO RR for CO and HCOOH productions that are economically viable. The intrinsic contribution of Co and the synergistic effects in Co-hybrid catalysts play essential roles for future commercial productions by ECO RR. This review summarizes the rational design of Co-based catalysts for ECO RR, including molecular, single-metal-site, and oxide-derived catalysts, along with the nanostructure engineering techniques to highlight the distribution of the ECO RR products by Co-based catalysts. The density functional theory (DFT) simulations and advanced in situ characterizations contribute to interpreting the synergies between Co and other materials for the enhanced product selectivity and catalytic activity. Challenges and outlook concerning the catalyst design and reaction mechanism, including the upgrading of reaction systems of Co-based catalysts for ECO RR, are also discussed.
一氧化碳还原反应(CO RR)通过将CO转化为增值燃料和化学品,为可持续碳固定提供了一种有前景的策略。近年来,大量的研究致力于开发用于选择性电化学一氧化碳还原反应(ECO RR)的过渡金属(TM)基催化剂。钴基催化剂成为最有前景的电催化剂之一,具有高法拉第效率、电流密度和低过电位,对ECO RR生成CO和HCOOH表现出优异的催化性能,这些产物在经济上是可行的。钴的内在贡献以及钴基混合催化剂中的协同效应对于未来通过ECO RR进行商业生产起着至关重要的作用。本文综述了用于ECO RR的钴基催化剂的合理设计,包括分子催化剂、单金属位点催化剂和氧化物衍生催化剂,以及纳米结构工程技术,以突出钴基催化剂对ECO RR产物的分布情况。密度泛函理论(DFT)模拟和先进的原位表征有助于解释钴与其他材料之间的协同作用,以提高产物选择性和催化活性。还讨论了关于催化剂设计和反应机理的挑战与展望,包括用于ECO RR的钴基催化剂反应体系的升级。