Tuning the reactivity of carbon surfaces with oxygen-containing functional groups

Jiahua Zhou, Piaoping Yang, Pavel A. Kots, Maximilian Cohen, Ying Chen, Caitlin M. Quinn, Matheus Dorneles Mello, J. Anibal Boscoboinik, Wendy J. Shaw, Stavros Caratzoulas, Weiqing Zheng () and Dionisios G. Vlachos ()
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Jiahua Zhou: University of Delaware
Piaoping Yang: University of Delaware
Pavel A. Kots: University of Delaware
Maximilian Cohen: University of Delaware
Ying Chen: Pacific Northwest National Laboratory
Caitlin M. Quinn: University of Delaware
Matheus Dorneles Mello: University of Delaware
J. Anibal Boscoboinik: University of Delaware
Wendy J. Shaw: Pacific Northwest National Laboratory
Stavros Caratzoulas: University of Delaware
Weiqing Zheng: University of Delaware
Dionisios G. Vlachos: University of Delaware

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Oxygen-containing carbons are promising supports and metal-free catalysts for many reactions. However, distinguishing the role of various oxygen functional groups and quantifying and tuning each functionality is still difficult. Here we investigate the role of Brønsted acidic oxygen-containing functional groups by synthesizing a diverse library of materials. By combining acid-catalyzed elimination probe chemistry, comprehensive surface characterizations, 15N isotopically labeled acetonitrile adsorption coupled with magic-angle spinning nuclear magnetic resonance, machine learning, and density-functional theory calculations, we demonstrate that phenolic is the main acid site in gas-phase chemistries and unexpectedly carboxylic groups are much less acidic than phenolic groups in the graphitized mesoporous carbon due to electron density delocalization induced by the aromatic rings of graphitic carbon. The methodology can identify acidic sites in oxygenated carbon materials in solid acid catalyst-driven chemistry.

Date: 2023
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DOI: 10.1038/s41467-023-37962-3

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