State Key Laboratory of Heavy Oil Processing, School of Materials Science and Engineering, China University of Petroleum, Qingdao, 266580, PR China.
School of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao, 266042, PR China.
Nat Commun. 2023 Jun 24;14(1):3767. doi: 10.1038/s41467-023-39475-5.
Designing Pt-based electrocatalysts with high catalytic activity and CO tolerance is challenging but extremely desirable for alkaline hydrogen oxidation reaction. Herein we report the design of a series of single-atom lanthanide (La, Ce, Pr, Nd, and Lu)-embedded ultrasmall Pt nanoclusters for efficient alkaline hydrogen electro-oxidation catalysis based on vapor filling and spatially confined reduction/growth of metal species. Mechanism studies reveal that oxophilic single-atom lanthanide species in Pt nanoclusters can serve as the Lewis acid site for selective OH adsorption and regulate the binding strength of intermediates on Pt sites, which promotes the kinetics of hydrogen oxidation and CO oxidation by accelerating the combination of OH and *H/*CO in kinetics and thermodynamics, endowing the electrocatalyst with up to 14.3-times higher mass activity than commercial Pt/C and enhanced CO tolerance. This work may shed light on the design of metal nanocluster-based electrocatalysts for energy conversion.
设计具有高催化活性和 CO 耐受性的基于 Pt 的电催化剂对于碱性氢氧化反应来说极具挑战性，但又非常理想。在此，我们报告了一系列单原子镧（La、Ce、Pr、Nd 和 Lu）嵌入的超小 Pt 纳米团簇的设计，该设计基于蒸气填充和金属物种的空间受限还原/生长，用于高效碱性氢电氧化催化。机理研究表明，Pt 纳米团簇中亲氧的单原子镧物种可用作 Lewis 酸位，用于选择性 OH 吸附，并调节 Pt 位上中间体的结合强度，这通过在动力学和热力学上加速 OH 和 *H/*CO 的结合，促进了氢氧化和 CO 氧化的动力学，使电催化剂的质量活性比商业 Pt/C 提高了 14.3 倍，并增强了 CO 耐受性。这项工作可能为基于金属纳米团簇的电催化剂的能量转换设计提供启示。
