Abstract
AbstractDeveloping metal‐free heterogeneous catalysts with high efficiency for the elimination of H2S into eco‐friendly products are very important for both fundamental catalytic science and industrial chemistry. Herein, we design a new modified carbon nitride catalyst engrafted with Br‐substituted aromatic heterocycle (CNU−Br) through a simple copolymerization and exfoliation method. CNU−Br exhibits excellent H2S conversion efficiency, high sulfur selectivity, and outstanding stability in the catalytic desulfurization reaction, which is better than most of the reported catalysts. The experiments and theoretical calculations show that the grafting of bromophenyl groups into the fundamental carbon nitride structural network leads to π‐delocalization, surface modification, as well as enhances the basicity of the structural active N sites. The regulation of the H and S affinity of CNU−Br that mediate the facile cleavage of H2S hydrogen‐sulfur bonds and the release of S atoms in thermodynamics. Furthermore, the superior surface area and mass transfer over CNU−Br accelerate the adsorption and oxidation of H2S in kinetics compared with the ordinary carbon nitride.
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