Department of Applied Physics, The Hong Kong Polytechnic University, Kowloon, Hong Kong, P. R. China.
Key Laboratory of Material Chemistry for Energy Conversion and Storage (Huazhong University of Science and Technology), Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
Adv Sci (Weinh). 2022 Dec;9(36):e2205299. doi: 10.1002/advs.202205299. Epub 2022 Nov 11.
Nearly theoretical 100% atomic utilization (supposing each atom could serve as independent sites to play a role in catalyz) of single-atom catalysts (SACs) makes it highly promising for various applications. However, for most SACs, single-atom sites are trapped in a solid carbon matrix, which makes the inner parts hardly available for reaction. Herein, a hollow N-doped carbon confined single-atom Rh (Rh-SACs/HNCR) is developed via a coordination-template method. Both aberration-corrected scanning transmission electron microscopy and energy dispersive X-ray spectroscopy mapping confirm the uniform distribution of Rh single atoms. Owning to the unique hollow structure and effective carbon confinement, excessive conversion from pyridinic/pyrrolic N to graphic N is hindered. As a proof of concept, Rh-SACs/HNCR exhibits superior activity, stability, selectivity, and anti-poisoning capability in formic acid oxidation reaction compared with the counterpart Rh/C, Pd/C, and Pt/C catalysts. This work provides a powerful strategy for synthesizing hollow carbon confined single-atom catalysts apply in various energy-related systems.
单原子催化剂（SACs）几乎可以实现理论上 100%的原子利用率（假设每个原子都可以作为独立的活性位在催化中发挥作用），这使其在各种应用中极具前景。然而，对于大多数 SACs 来说，单原子位点被捕获在固体碳基质中，这使得内部部分很难参与反应。在此，通过配位模板法开发了一种空心 N 掺杂碳限制的单原子 Rh（Rh-SACs/HNCR）。球差校正扫描透射电子显微镜和能量色散 X 射线能谱映射都证实了 Rh 单原子的均匀分布。由于独特的空心结构和有效的碳限制，阻碍了吡啶/吡咯 N 向石墨 N 的过度转化。作为概念验证，与 Rh/C、Pd/C 和 Pt/C 催化剂相比，Rh-SACs/HNCR 在甲酸氧化反应中表现出优异的活性、稳定性、选择性和抗中毒能力。这项工作为合成空心碳限制的单原子催化剂提供了一种强大的策略，可应用于各种与能源相关的系统。
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