Xu Airong, Liu Tong, Liu Dong, Li Wenzhi, Huang Hui, Wang Sicong, Xu Li, Liu Xiaokang, Jiang Shuaiwei, Chen Yudan, Sun Mei, Luo Qiquan, Ding Tao, Yao Tao
School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
Institutes of Physical Science and Information Technology, Anhui University, Hefei, 230601, P.R. China.
Angew Chem Int Ed Engl. 2024 Oct 1;63(40):e202410545. doi: 10.1002/anie.202410545. Epub 2024 Aug 13.
Rational design of efficient methanol oxidation reaction (MOR) catalyst that undergo non-CO pathway is essential to resolve the long-standing poisoning issue. However, it remains a huge challenge due to the rather difficulty in maximizing the non-CO pathway by the selective coupling between the key *CHO and *OH intermediates. Here, we report a high-performance electrocatalyst of patchy atomic-layer Pt epitaxial growth on CeO nanocube (Pt ALs/CeO) with maximum electronic metal-support interaction for enhancing the coupling selectively. The small-size monolayer material achieves an optimal geometrical distance between edge Pt-O-Ce sites and *OH absorbed on CeO, which well restrains the dehydrogenation of *CHO, resulting in the non-CO pathway. Meanwhile, the *CHO/*CO intermediate generated at inner Pt-O-Ce sites can migrate to edge, inducing the subsequent coupling reaction, thus avoiding poisoning while promoting reaction efficiency. Consequently, Pt ALs/CeO exhibits exceptionally catalytic stability with negligible degradation even under 1000 s pure CO poisoning operation and high mass activity (14.87 A/mg), enabling it one of the best-performing alkali-stable MOR catalysts.
设计高效的、遵循非CO路径的甲醇氧化反应（MOR）催化剂对于解决长期存在的中毒问题至关重要。然而，由于通过关键的CHO和OH中间体之间的选择性偶联来最大化非CO路径相当困难，这仍然是一个巨大的挑战。在此，我们报道了一种高性能的电催化剂，即斑片状原子层Pt在CeO纳米立方体上外延生长（Pt ALs/CeO），其具有最大的电子金属-载体相互作用以选择性地增强偶联。这种小尺寸的单层材料在边缘的Pt-O-Ce位点和吸附在CeO上的OH之间实现了最佳的几何距离，很好地抑制了CHO的脱氢反应，从而产生了非CO路径。同时，在内侧Pt-O-Ce位点生成的*CHO/*CO中间体可以迁移到边缘，引发随后的偶联反应，从而在促进反应效率的同时避免中毒。因此，Pt ALs/CeO表现出异常的催化稳定性，即使在1000 s纯CO中毒操作下也几乎没有降解，并且具有高质量活性（14.87 A/mg），使其成为性能最佳的碱稳定MOR催化剂之一。
