Enhanced Oxygen Activation Achieved by Robust Single Chromium Atom-Derived Catalysts in Aerobic Oxidative Desulfurization
Abstract
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. In this work, 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 O2•– 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 π-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.
- Authors:
-
[1];
[2];
[1];
[3];
[1];
[1];
[4]
- Jiangsu Univ., Zhenjiang (China)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Hunan Univ., Changsha (China)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1883764
- Grant/Contract Number:
- AC05-00OR22725; 21978119; 22078135; 22178154
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 14; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; single-atom catalyst; aerobic oxidation; deep desulfurization; carbon nanotube; chromium
Citation Formats
Jiang, Wei, An, Xin, Xiao, Jin, Yang, Zhenzhen, Liu, Jixing, Chen, Hao, Li, Hongping, Zhu, Wenshuai, Li, Huaming, and Dai, Sheng. Enhanced Oxygen Activation Achieved by Robust Single Chromium Atom-Derived Catalysts in Aerobic Oxidative Desulfurization. United States: N. p., 2022.
Web. doi:10.1021/acscatal.2c01329.
Jiang, Wei, An, Xin, Xiao, Jin, Yang, Zhenzhen, Liu, Jixing, Chen, Hao, Li, Hongping, Zhu, Wenshuai, Li, Huaming, & Dai, Sheng. Enhanced Oxygen Activation Achieved by Robust Single Chromium Atom-Derived Catalysts in Aerobic Oxidative Desulfurization. United States. https://doi.org/10.1021/acscatal.2c01329
Jiang, Wei, An, Xin, Xiao, Jin, Yang, Zhenzhen, Liu, Jixing, Chen, Hao, Li, Hongping, Zhu, Wenshuai, Li, Huaming, and Dai, Sheng. Tue .
"Enhanced Oxygen Activation Achieved by Robust Single Chromium Atom-Derived Catalysts in Aerobic Oxidative Desulfurization". United States. https://doi.org/10.1021/acscatal.2c01329. https://www.osti.gov/servlets/purl/1883764.
@article{osti_1883764,
title = {Enhanced Oxygen Activation Achieved by Robust Single Chromium Atom-Derived Catalysts in Aerobic Oxidative Desulfurization},
author = {Jiang, Wei and An, Xin and Xiao, Jin and Yang, Zhenzhen and Liu, Jixing and Chen, Hao and Li, Hongping and Zhu, Wenshuai and Li, Huaming and Dai, Sheng},
abstractNote = {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. In this work, 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 O2•– 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 π-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.},
doi = {10.1021/acscatal.2c01329},
journal = {ACS Catalysis},
number = 14,
volume = 12,
place = {United States},
year = {Tue Jul 05 00:00:00 EDT 2022},
month = {Tue Jul 05 00:00:00 EDT 2022}
}
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