Transition Metal-like Carbocatalyst (NACs) for Activating Strong Bonds

Scientific Achievement

Discovery of the first metal-free carbocatalyst (nitrogen assembly carbons, NACs) capable of activating strong covalent bonds, H-H, C-O, and C-H, with high selectivity. The unique activity arises from the closely-placed graphitic N, as indicated by mechanistic and kinetic studies together with DFT calculations. NACs

Significance and Impact

The discovery of new active sites provides guidelines for rationale design of novel metal-free catalysts. NACs are broadly applicable for processing fossil and renewable feedstocks, electrocatalysis, and fuel cells.

Research Details

•Reactions: NACs catalyze hydrogenolysis of aryl ethers and dehydrogenation of ethylbenzene and tetrahydroquinoline as well as for hydrogenation of common unsaturated functionalities.

•Mechanism: The similarity and disparity of NACs from transition metals are demonstrated by H2/D2 exchange, D2/2-PrOH exchange, and selective styrene deuteration.

Luo, Z.; Nie, R.; Nguyen, V. T.; Biswas, A.; Behera, R. K.; Wu, X.; Kobayashi, T.; Sadow, A.; Wang, B.;* Huang, W.;* Qi, L.* Transition metal-like carbocatalyst. Nat. Commun. 2020, 11, 4091. DOI: 10.1038/s41467-020-17909-8.