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Selective catalytic oxidation (SCO) of hydrogen sulfide (H2S) to sulfur exhibits significant advantages for H2S removal, including high efficiency, mild operating conditions and thermodynamic unlimitation for H2S removal. Recently, polymeric carbon nitride (PCN) has emerged as a candidate for H2S selective oxidation reactions, benefiting from its aromatic C-N hybridized p-conjugated system for H2S adsorption/dissociation and good sulfur tolerance. However, its performance is greatly hampered by the lack of sufficient surface active sites for O-2 adsorption and activation. Herein, we demonstrate that the incorporation of carbon atoms in PCN matrix to constructure carbon-rich carbon nitride nanosheets is a facile strategy to advance the desulfurization performance. The carbon atoms uniformly incorporated in PCN backbones can effectively extend the aromatic p-conjugated electronic system and create abundant oxygen-containing functional groups on the surface. The improved electronic configurations and surface properties are beneficial for the adsorption and activation of H2S and O-2. In addition, the nanosheet morphology favors for increasing the surface area of the material, thereby promoting the mass transfer of H2S and O-2 during the desulfurization process. The optimized carbon-rich carbon nitride nanosheets exhibit a H2S conversion of 99% and a S selectivity up to 95% for H2S selective oxidation at 200 degrees C, and the reaction is not restricted by mass transportation and heat transfer at such a high conversion rate. This synthetic strategy allows ample choice of low-cost and easy-available organic precursors for the large-scale production of the desulfurization catalysts. (C) 2022 Elsevier Inc. All rights reserved.
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JOURNAL OF CATALYSIS
ISSN: 0021-9517
Year: 2022
Volume: 413
Page: 992-1004
7 . 3
JCR@2022
6 . 5 0 0
JCR@2023
ESI Discipline: CHEMISTRY;
ESI HC Threshold:74
JCR Journal Grade:1
CAS Journal Grade:2
Cited Count:
WoS CC Cited Count: 20
SCOPUS Cited Count: 20
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 2