Ideal heterogeneous metal hydrogenation catalysts are featured by simultaneously high activity, selectivity, and stability. Herein, we report a general yet powerful strategy to design and fabricate dual-active-sites Co@C core-shell nanoparticle for boosting selective hydrogenation of various N-heteroarenes. It can break the limitation of scaling relation on traditional metal surfaces, and thus afford unprecedentedly high selectivity, activity, and stability. Combining kinetics analysis and DFT calculations with multiple techniques directly unveil that the critical porous carbon shell with a pore size of 0.53 nm not only allows H₂ diffusion to Co sites for activation and blocks accessibility of N-heteroarenes but also catalyzes hydrogenation of N-heteroarenes via hydrogen spillover from Co sites. In addition, the presence of surface/subsurface carbon at the Co sites shows high anti-sulfur poisoning and anti-oxidant capability. This work is valuable for guiding the design and manipulation of cost-effective and robust hydrogenation catalysts.

理想的非均相金属加氢催化剂的特点是同时具有高活性，选择性和稳定性。在这里，我们报告了一个通用而强大的策略，以设计和制造双活性位点Co @ C核壳纳米粒子，以促进各种N-杂芳烃的选择性氢化。它可以打破传统金属表面上比例关系的限制，从而提供前所未有的高选择性，活性和稳定性。将动力学分析和DFT计算与多种技术相结合，直接揭示了孔径为0.53 nm的关键多孔碳壳不仅允许H ₂扩散到Co位置进行活化，并阻止N-杂芳烃的可及性，还催化N的氢化-杂芳烃通过氢从Co站点溢出而来。另外，在Co位点处存在表面/地下碳表现出高的抗硫中毒和抗氧化能力。这项工作对于指导设计和操作具有成本效益的耐用型氢化催化剂具有重要意义。