期刊
ACS CATALYSIS
卷 12, 期 14, 页码 8623-8631出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01329
关键词
single-atom catalyst; aerobic oxidation; deep desulfurization; carbon nanotube; chromium
资金
- National Natural Science Foundation of China [21978119, 22078135, 22178154]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program
By using single-atom chromium catalysts on multiwalled carbon nanotubes, efficient oxidative desulfurization reactions have been achieved, with promising catalytic performance and cycling stability, providing a potential catalyst for sulfur removal in practical fuels.
Oxidative desulfurization (ODS) plays critical roles in the production of high-quality sulfur impurity-free fuels, especially procedures using molecular oxygen as the sole oxidant. However, the state-of-the-art systems still rely on noble metal nanocatalysts, with deactivation issues caused by coking and sintering still present. Herein, leveraging the merits of single-atom catalysts (SACs) with earth-abundant metal cores and robust nanoporous supports, a series of catalysts composed of homogeneously distributed single chromium atoms anchored on multiwalled carbon nanotubes were fabricated and deployed to catalyze the aerobic ODS transformation. Adopting aromatic sulfur compound (ASC)-containing alkanes as a model system with molecular oxygen as the oxidant, efficient oxygen-to-active O-2(center dot-) transformation and subsequent ASCs-to-sulfone conversion have been achieved, with the former benefiting from the chromium-active sites and the latter arising from the robust, nanoporous, and pi-conjugated architecture of the supports. The attractive catalytic performance and cycling stability of the chromium-based SACs make them promising candidates in practical sulfur species removal from liquid fuels, supplying an alternative guidance on the catalyst design toward cost-effective and energy-efficient ODS procedures.
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