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

Haifeng Qi, Ji Yang, Fei Liu, LeiLei Zhang (), Jingyi Yang, Xiaoyan Liu, Lin Li, Yang Su, Yuefeng Liu, Rui Hao, Aiqin Wang () and Tao Zhang ()
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Haifeng Qi: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Ji Yang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Fei Liu: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
LeiLei Zhang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Jingyi Yang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Xiaoyan Liu: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Lin Li: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yang Su: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yuefeng Liu: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Rui Hao: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Aiqin Wang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Tao Zhang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract 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 °C in N2 followed by treatment at 800 °C in NH3. The resultant Ru1-N3 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.

Date: 2021
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DOI: 10.1038/s41467-021-23429-w

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