Highly selective and robust single-atom catalyst Ru1/NC for reductive amination of aldehydes/ketones

Single-atom catalysts (SACs) have emerged as a frontier in heterogeneous catalysis due to the well-defined active site structure and the maximized metal atom utilization. Nevertheless, the robustness of SACs remains a critical concern for practical applications. Herein, we report a highly active, selective and robust Ru SAC which was synthesized by pyrolysis of ruthenium acetylacetonate and N/C precursors at 900 degrees C in N-2 followed by treatment at 800 degrees C in NH3. The resultant Ru-1-N-3 structure exhibits moderate capability for hydrogen activation even in excess NH3, which enables the effective modulation between transimination and hydrogenation activity in the reductive amination of aldehydes/ketones towards primary amines. As a consequence, it shows superior amine productivity, unrivalled resistance against CO and sulfur, and unexpectedly high stability under harsh hydrotreating conditions compared to most SACs and nanocatalysts. This SAC strategy will open an avenue towards the rational design of highly selective and robust catalysts for other demanding transformations. Single-atom catalyst (SAC) has emerged as a frontier in heterogeneous catalysis yet its robustness remains a critical concern. Here, a highly active, selective and robust Ru-1-N-3 SAC is explored for a challenging reaction, reductive amination of aldehydes/ketones for synthesis of primary amines.

Automated summary

Single-atom catalyst (SAC) has emerged as a frontier in heterogeneous catalysis, yet its robustness remains a critical concern. Here, a highly active, selective, and robust Ru-1-N-3 SAC is explored for a challenging reaction, reductive amination of aldehydes/ketones for synthesis of primary amines.