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Reduced graphene oxide: a metal-free catalyst for aerobic oxidative desulfurization
Gu, Qingqing; Wen, Guodong; Ding, Yuxiao; Wu, Kuang-Hsu; Chen, Chengmeng; Su, Dangsheng; Su, DS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China.
2017-02-21
发表期刊ROYAL SOC CHEMISTRY
ISSN1463-9262
卷号19期号:4页码:1175-1181
摘要Nanocarbons have been extensively used as metal-free alternatives to metal catalysts in many oxidative processes owing to their functional groups or defects, which have the activation ability toward oxygen molecules. Herein, reduced graphene oxide (rGO) could be used as catalysts in oxidative desulfurization reactions for the first time to remove sulfur-containing compounds from fuels. Superior catalytic activity and stability are obtained in the aerobic oxidative desulfurization process catalyzed by rGO. A broad range of sulfur-containing aromatic substrates could be removed effectively in this catalytic system. Carbonyl groups have proved to play crucial roles during the oxidation process based on an XPS analysis, a chemical titration method and a series of comparative experiments. The chemically active defects are also beneficial to the catalytic performance because carbonyl groups could be generated in situ on these defects under the reaction conditions. Based on the EPR results, a radical pathway is proposed. Oxygen molecules could interact with the carbon atoms adjacent to carbonyl groups to form adsorbed super oxygen anion radicals (rGO-OO), which then attack the adjacent sulfur-centered cation radicals and generate the final product sulfone.; Nanocarbons have been extensively used as metal-free alternatives to metal catalysts in many oxidative processes owing to their functional groups or defects, which have the activation ability toward oxygen molecules. Herein, reduced graphene oxide (rGO) could be used as catalysts in oxidative desulfurization reactions for the first time to remove sulfur-containing compounds from fuels. Superior catalytic activity and stability are obtained in the aerobic oxidative desulfurization process catalyzed by rGO. A broad range of sulfur-containing aromatic substrates could be removed effectively in this catalytic system. Carbonyl groups have proved to play crucial roles during the oxidation process based on an XPS analysis, a chemical titration method and a series of comparative experiments. The chemically active defects are also beneficial to the catalytic performance because carbonyl groups could be generated in situ on these defects under the reaction conditions. Based on the EPR results, a radical pathway is proposed. Oxygen molecules could interact with the carbon atoms adjacent to carbonyl groups to form adsorbed super oxygen anion radicals (rGO-OO), which then attack the adjacent sulfur-centered cation radicals and generate the final product sulfone.
部门归属[gu, qingqing ; wen, guodong ; wu, kuang-hsu ; su, dangsheng] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, liaoning, peoples r china ; [ding, yuxiao] max planck inst chem energy convers, stiftstr 34-36, d-45470 mulheim, germany ; [chen, chengmeng] chinese acad sci, inst coal chem, taiyuan 030001, shanxi, peoples r china
学科领域Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology
资助者Ministry of Science and Technology of China [2011CBA00504]; National Science Foundation of China [21133010, 51221264, 91545119, 91545110, 21261160487, 21411130120, 21473223, 21503241]; "Strategic Priority Research Program" of the Chinese Academy of Sciences [XDA09030103]; CAS/SAFEA International Partnership Program for Creative Research Teams; Doctoral Starting up Foundation of Liaoning Province, China [20121068]
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/79187
专题中国科学院金属研究所
通讯作者Su, DS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China.
推荐引用方式
GB/T 7714
Gu, Qingqing,Wen, Guodong,Ding, Yuxiao,et al. Reduced graphene oxide: a metal-free catalyst for aerobic oxidative desulfurization[J]. ROYAL SOC CHEMISTRY,2017,19(4):1175-1181.
APA Gu, Qingqing.,Wen, Guodong.,Ding, Yuxiao.,Wu, Kuang-Hsu.,Chen, Chengmeng.,...&Su, DS .(2017).Reduced graphene oxide: a metal-free catalyst for aerobic oxidative desulfurization.ROYAL SOC CHEMISTRY,19(4),1175-1181.
MLA Gu, Qingqing,et al."Reduced graphene oxide: a metal-free catalyst for aerobic oxidative desulfurization".ROYAL SOC CHEMISTRY 19.4(2017):1175-1181.
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