An efficient preparation and local coordination environment regulation of isolated single-atom sites catalysts (ISASC) for improved activity is still challenging. Herein, we develop a solid phase thermal diffusion strategy to synthesize Mn ISASC on highly uniform nitrogen-doped carbon nanotubes by employing MnO₂ nanowires@ZIF-8 core-shell structure. Under high-temperature, the Mn species break free from core-MnO₂ lattice, which will be trapped by carbon defects derived from shell-ZIF-8 carbonization, and immobilized within carbon substrate. Furthermore, the poly-dispersed Mn sites with two nitrogen-coordinated centers can be controllably renovated into four-nitrogen-coordinated Mn sites using NH₃ treatment technology. Both experimental and computational investigations indicate that the symmetric coordinated Mn sites manifest outstanding oxygen reduction activity and superior stability in alkaline and acidic solutions. This work not only provides efficient way to regulate the coordination structure of ISASC to improve catalytic performance but also paves the way to reveal its significant promise for commercial application.

孤立单原子位点催化剂（ISASC）的有效制备和局部协调环境调节以提高活性仍然具有挑战性。在此，我们开发了一种固相热扩散策略，通过采用 MnO ₂纳米线@ZIF-8 核壳结构在高度均匀的氮掺杂碳纳米管上合成 Mn ISASC 。在高温下，Mn 物质脱离核-MnO ₂晶格，被壳-ZIF-8碳化产生的碳缺陷捕获，并固定在碳基质中。此外，具有两个氮配位中心的多分散 Mn 位点可以使用 NH ₃可控地改造为四氮配位的 Mn 位点。处理技术。实验和计算研究表明，对称配位的 Mn 位点在碱性和酸性溶液中表现出出色的氧还原活性和优异的稳定性。这项工作不仅为调节 ISASC 的配位结构以提高催化性能提供了有效的方法，而且为揭示其商业应用的重要前景铺平了道路。