Designing cost-effective and high-performing metal catalysts is significant for many renewable energy conversion technologies. Lowering metal loading without sacrificing activity and durability is highly desired for the catalyst design, especially for those reactions where the noble metals deliver the best catalyzing performance. Single-atom catalysts (SACs) with maximal metal-atom utilization, homogeneous and tailorable active sites have emerged as promising catalyst candidates, where the local coordination structures of the metal atoms in SACs largely determine the reaction kinetics. Previous design strategies of constructing strong metal-support interactions can stabilize the individual metal atoms in SACs, but present obstacles to provide a flexible manipulation platform for elaborately tailoring the coordination structures to achieve performance optimization towards a specifically targeted reaction. Here, for the proof-of-concept study, we report a novel design of SAC with iridium (Ir) single atoms supported on conjugated polymer, in which the adsorption energies of reaction intermediates on Ir atoms and the reaction kinetics towards acidic water oxidation can be readily optimized through modulating the formed cation-π interactions that can be tailored by adjusting the molecular structures of conjugated polymers. This strategy establishes a general route to develop targeted SACs for various catalytic reactions.

设计经济高效且高性能的金属催化剂对于许多可再生能源转换技术具有重要意义。催化剂设计非常需要在不牺牲活性和耐久性的情况下降低金属负载量，特别是对于那些贵金属提供最佳催化性能的反应。具有最大金属原子利用率、均匀且可定制活性位点的单原子催化剂（SAC）已成为有前途的催化剂候选者，其中SAC中金属原子的局部配位结构在很大程度上决定了反应动力学。先前构建强金属-载体相互作用的设计策略可以稳定SAC中的单个金属原子，但在提供灵活的操纵平台来精心定制配位结构以实现特定目标反应的性能优化方面存在障碍。在这里，为了进行概念验证研究，我们报告了一种新颖的 SAC 设计，其中铱 (Ir) 单原子负载在共轭聚合物上，其中反应中间体在 Ir 原子上的吸附能和酸性水氧化的反应动力学可以通过调节形成的阳离子-π相互作用可以很容易地进行优化，而阳离子-π相互作用可以通过调整共轭聚合物的分子结构来定制。该策略建立了开发用于各种催化反应的靶向 SAC 的通用途径。