Wang Huilin, Bootharaju Megalamane S, Kim Jeong Hyun, Wang Ying, Wang Ke, Zhao Meng, Zhang Rui, Xu Jing, Hyeon Taeghwan, Wang Xiao, Song Shuyan, Zhang Hongjie
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China.
J Am Chem Soc. 2023 Feb 1;145(4):2264-2270. doi: 10.1021/jacs.2c10435. Epub 2023 Jan 23.
The limitations of conventional strategies in finely controlling the composition and structure demand new promotional effects for upgrading the reverse water-gas shift (RWGS) catalysts for enhanced fuel production. We report the design and synthesis of a hetero-dual-site catalyst for boosting RWGS performance by controllably loading Fe atoms at the neighboring Pt atom on the surface of commercial CeO. The Fe-Pt/CeO exhibits a remarkably high catalytic performance (TOF: 43,519 h) for CO to CO conversion with ∼100% CO selectivity at a relatively low temperature of 350 °C. Furthermore, the catalyst retains over 80% activity after 200 h of continuous operation. The experimental and computational investigations reveal a "two-way synergistic effect", where Fe atoms can not only serve as promotors to alter the charge density of Pt atoms but also be activated by the excess active hydrogen species generated by Pt atoms, enhancing catalytic activity and stability.
传统策略在精确控制组成和结构方面的局限性要求有新的促进作用，以升级逆水煤气变换（RWGS）催化剂，从而提高燃料产量。我们报告了一种异质双位点催化剂的设计与合成，通过在商用CeO表面的相邻Pt原子上可控地负载Fe原子来提高RWGS性能。Fe-Pt/CeO在350℃的相对低温下，对CO转化为CO表现出极高的催化性能（TOF：43,519 h），CO选择性约为100%。此外，该催化剂在连续运行200小时后仍保留超过80%的活性。实验和计算研究揭示了一种“双向协同效应”，其中Fe原子不仅可以作为促进剂改变Pt原子的电荷密度，还可以被Pt原子产生的过量活性氢物种激活，从而提高催化活性和稳定性。
