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Title: Synergistic effect of dual Brønsted acidic deep eutectic solvents for oxidative desulfurization of diesel fuel

Abstract

Deep eutectic solvents (DESs) are generally used as attractive solvents or extractants rather than catalysts in the field of synthesis and separation. Herein, dual Brønsted acidic DESs were prepared by mixing sulfonated quaternary ammonium and oxalic acid as extractants and catalysts for deep oxidative desulfurization. Compared to the DESs with single acidic group, the dual acidic DESs exhibited much higher catalytic activity likely due to the synergistic effect. The 1H NMR study indicated that the weak interaction between DES and sulfur compounds led to a low extraction capacity. However, the sulfur removal could reach 97.7% under optimized reaction conditions. Density functional theory (DFT) calculations demonstrated that sulfonic group and carboxylic group are of equal importance to desulfurization performance. Further, the desulfurization efficiency was also strongly affected by the viscosity of DESs. Here, we put forward a new strategy that the reaction time could be sharply shortened to 40 min and 100 min by adding low viscous acetonitrile and polyethylene glycol into DES to form mixing reaction system, respectively.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [2];  [3];  [2];  [2];  [2]; ORCiD logo [4];  [3]; ORCiD logo [2];  [2]; ORCiD logo [4]
  1. Jiangsu Univ., Zhenjiang (China). Inst. for Energy Research; Univ. of Tennessee, Knoxville, TN (United States)
  2. Jiangsu Univ., Zhenjiang (China). Inst. for Energy Research
  3. Hainan Normal Univ., Haikou (China)
  4. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (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:
1809999
Grant/Contract Number:  
AC05-00OR22725; 21978119; 21809092; 21766007
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Engineering Journal
Additional Journal Information:
Journal Volume: 394; Journal ID: ISSN 1385-8947
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; oxidative desulfurization; deep eutectic solvents; dual Brønsted acidity; low viscosity

Citation Formats

Jiang, Wei, Zhu, Kun, Li, Hongping, Zhu, Linhua, Hua, Mingqing, Xiao, Jin, Wang, Chao, Yang, Zhenzhen, Chen, Guangying, Zhu, Wenshuai, Li, Huaming, and Dai, Sheng. Synergistic effect of dual Brønsted acidic deep eutectic solvents for oxidative desulfurization of diesel fuel. United States: N. p., 2020. Web. doi:10.1016/j.cej.2020.124831.
Jiang, Wei, Zhu, Kun, Li, Hongping, Zhu, Linhua, Hua, Mingqing, Xiao, Jin, Wang, Chao, Yang, Zhenzhen, Chen, Guangying, Zhu, Wenshuai, Li, Huaming, & Dai, Sheng. Synergistic effect of dual Brønsted acidic deep eutectic solvents for oxidative desulfurization of diesel fuel. United States. https://doi.org/10.1016/j.cej.2020.124831
Jiang, Wei, Zhu, Kun, Li, Hongping, Zhu, Linhua, Hua, Mingqing, Xiao, Jin, Wang, Chao, Yang, Zhenzhen, Chen, Guangying, Zhu, Wenshuai, Li, Huaming, and Dai, Sheng. Sat . "Synergistic effect of dual Brønsted acidic deep eutectic solvents for oxidative desulfurization of diesel fuel". United States. https://doi.org/10.1016/j.cej.2020.124831. https://www.osti.gov/servlets/purl/1809999.
@article{osti_1809999,
title = {Synergistic effect of dual Brønsted acidic deep eutectic solvents for oxidative desulfurization of diesel fuel},
author = {Jiang, Wei and Zhu, Kun and Li, Hongping and Zhu, Linhua and Hua, Mingqing and Xiao, Jin and Wang, Chao and Yang, Zhenzhen and Chen, Guangying and Zhu, Wenshuai and Li, Huaming and Dai, Sheng},
abstractNote = {Deep eutectic solvents (DESs) are generally used as attractive solvents or extractants rather than catalysts in the field of synthesis and separation. Herein, dual Brønsted acidic DESs were prepared by mixing sulfonated quaternary ammonium and oxalic acid as extractants and catalysts for deep oxidative desulfurization. Compared to the DESs with single acidic group, the dual acidic DESs exhibited much higher catalytic activity likely due to the synergistic effect. The 1H NMR study indicated that the weak interaction between DES and sulfur compounds led to a low extraction capacity. However, the sulfur removal could reach 97.7% under optimized reaction conditions. Density functional theory (DFT) calculations demonstrated that sulfonic group and carboxylic group are of equal importance to desulfurization performance. Further, the desulfurization efficiency was also strongly affected by the viscosity of DESs. Here, we put forward a new strategy that the reaction time could be sharply shortened to 40 min and 100 min by adding low viscous acetonitrile and polyethylene glycol into DES to form mixing reaction system, respectively.},
doi = {10.1016/j.cej.2020.124831},
journal = {Chemical Engineering Journal},
number = ,
volume = 394,
place = {United States},
year = {Sat Mar 21 00:00:00 EDT 2020},
month = {Sat Mar 21 00:00:00 EDT 2020}
}

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