Transition metal-like carbocatalyst

Zhicheng Luo, Renfeng Nie, Vy T. Nguyen, Abhranil Biswas, Ranjan K. Behera, Xun Wu, Takeshi Kobayashi, Aaron Sadow, Bin Wang (), Wenyu Huang () and Long Qi ()
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Zhicheng Luo: Iowa State University
Renfeng Nie: Iowa State University
Vy T. Nguyen: University of Oklahoma
Abhranil Biswas: Iowa State University
Ranjan K. Behera: Iowa State University
Xun Wu: Iowa State University
Takeshi Kobayashi: Iowa State University
Aaron Sadow: Iowa State University
Bin Wang: University of Oklahoma
Wenyu Huang: Iowa State University
Long Qi: Iowa State University

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Catalytic cleavage of strong bonds including hydrogen-hydrogen, carbon-oxygen, and carbon-hydrogen bonds is a highly desired yet challenging fundamental transformation for the production of chemicals and fuels. Transition metal-containing catalysts are employed, although accompanied with poor selectivity in hydrotreatment. Here we report metal-free nitrogen-assembly carbons (NACs) with closely-placed graphitic nitrogen as active sites, achieving dihydrogen dissociation and subsequent transformation of oxygenates. NACs exhibit high selectivity towards alkylarenes for hydrogenolysis of aryl ethers as model bio-oxygenates without over-hydrogeneration of arenes. Activities originate from cooperating graphitic nitrogen dopants induced by the diamine precursors, as demonstrated in mechanistic and computational studies. We further show that the NAC catalyst is versatile for dehydrogenation of ethylbenzene and tetrahydroquinoline as well as for hydrogenation of common unsaturated functionalities, including ketone, alkene, alkyne, and nitro groups. The discovery of nitrogen assembly as active sites can open up broad opportunities for rational design of new metal-free catalysts for challenging chemical reactions.

Date: 2020
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DOI: 10.1038/s41467-020-17909-8

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