P and S dual-doped graphitic porous carbon for aerobic oxidation reactions: Enhanced catalytic activity and catalytic sites

Mehulkumar A. Patel, Feixiang Luo, Keerthi Savaram, Pavel Kucheryavy, Qiaoqiao Xie, Carol Flach, Richard Mendelsohn, Eric Garfunkel, Jenny V. Lockard, Huixin He

Research output: Contribution to journalArticle

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Abstract

A highly porous graphitic carbon material, dually-doped with P and S, was studied as a metal free catalyst for aerobic oxidation reactions. Catalytic mechanism studies suggest that the active centers, originated from P-and S-doping, additively/synergistically catalyze the aerobic oxidation of benzylic alcohols but with different pathways. For the first time, catalytic centers stemming from S-doping were experimentally identified to be exocyclic S species (C-S-C, sulfur out of the carbon ring), which are different from those proposed for electrochemical oxygen reduction reactions (ORR) with a 4e pathway and oxygen evaluation reactions (OER). Notably, all the catalytic sites from both P and S doping share a similar “protruding out” pyramid structure, which is in contrast to the planar structure of the catalytic sites in N- or B-doped graphitic materials. The unique geometric structure of the catalytic sites can minimize substrate steric hindrance effects, endowing the P, S co-doped catalysts with a wide substrate scope and functional group tolerance. Furthermore, the unambiguous distinguishment of the catalytic sites from those in OER and ORR provides valuable guidance for designing and developing carbon materials with controlled active sites to satisfy different catalytic applications.

Original languageEnglish
Pages (from-to)383-392
Number of pages10
JournalCarbon
Volume114
DOIs
Publication statusPublished - Apr 1 2017

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Catalyst activity
Carbon
Oxygen
Oxidation
Doping (additives)
Catalysts
Substrates
Sulfur
Functional groups
Alcohols
Metals

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

P and S dual-doped graphitic porous carbon for aerobic oxidation reactions : Enhanced catalytic activity and catalytic sites. / Patel, Mehulkumar A.; Luo, Feixiang; Savaram, Keerthi; Kucheryavy, Pavel; Xie, Qiaoqiao; Flach, Carol; Mendelsohn, Richard; Garfunkel, Eric; Lockard, Jenny V.; He, Huixin.

In: Carbon, Vol. 114, 01.04.2017, p. 383-392.

Research output: Contribution to journalArticle

Patel, MA, Luo, F, Savaram, K, Kucheryavy, P, Xie, Q, Flach, C, Mendelsohn, R, Garfunkel, E, Lockard, JV & He, H 2017, 'P and S dual-doped graphitic porous carbon for aerobic oxidation reactions: Enhanced catalytic activity and catalytic sites', Carbon, vol. 114, pp. 383-392. https://doi.org/10.1016/j.carbon.2016.11.064
Patel, Mehulkumar A. ; Luo, Feixiang ; Savaram, Keerthi ; Kucheryavy, Pavel ; Xie, Qiaoqiao ; Flach, Carol ; Mendelsohn, Richard ; Garfunkel, Eric ; Lockard, Jenny V. ; He, Huixin. / P and S dual-doped graphitic porous carbon for aerobic oxidation reactions : Enhanced catalytic activity and catalytic sites. In: Carbon. 2017 ; Vol. 114. pp. 383-392.
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