Enabling tandem oxidation of benzene to benzenediol over integrated neighboring V-Cu oxides in mesoporous silica

doi:10.1016/j.cjche.2022.05.029

中国化学工程学报 ›› 2023, Vol. 55 ›› Issue (3): 236-245.DOI: 10.1016/j.cjche.2022.05.029

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Enabling tandem oxidation of benzene to benzenediol over integrated neighboring V-Cu oxides in mesoporous silica

Mengting Liu¹, Xuexue Dong¹, Zengjing Guo², Aihua Yuan¹, Shuying Gao³, Fu Yang¹

1. School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China;
2. School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252000, China;
3. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China

收稿日期:2022-03-25 修回日期:2022-05-17 出版日期:2023-03-28 发布日期:2023-06-03
通讯作者: Shuying Gao,E-mail:gao415127@163.com;Fu Yang,E-mail:fuyang@just.edu.cn
基金资助:
This work was financially supported by the National Natural Science Foundation of China (21908085), Natural Science Foundation of Jiangsu Province, China (BK20190961), Postdoctoral Research Foundation of Jiangsu Province (2020Z291). The present study was also supported by the Jiangsu Provincial Key Laboratory of Environmental Science and Engineering (JSHJZDSYS-202103).

Enabling tandem oxidation of benzene to benzenediol over integrated neighboring V-Cu oxides in mesoporous silica

Mengting Liu¹, Xuexue Dong¹, Zengjing Guo², Aihua Yuan¹, Shuying Gao³, Fu Yang¹

1. School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China;
2. School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252000, China;
3. State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, China

Received:2022-03-25 Revised:2022-05-17 Online:2023-03-28 Published:2023-06-03
Contact: Shuying Gao,E-mail:gao415127@163.com;Fu Yang,E-mail:fuyang@just.edu.cn
Supported by:
This work was financially supported by the National Natural Science Foundation of China (21908085), Natural Science Foundation of Jiangsu Province, China (BK20190961), Postdoctoral Research Foundation of Jiangsu Province (2020Z291). The present study was also supported by the Jiangsu Provincial Key Laboratory of Environmental Science and Engineering (JSHJZDSYS-202103).

摘要/Abstract

摘要： The direct tandem oxidation synthesis of benzenediol from benzene could simplify or even avoid the separation and purification of reaction intermediates, which is promising but challenged because of the further required immediate consecutive activation of intermediate phenol. In this work, a synergistic benzene tandem-oxidation catalyst that V-Cu bimetallic oxides modified nanoporous silica (VCu-NS) was constructed via a facile assembly strategy which involves addictive negative anion citric acid mediating the intercalation of metal-citric acid chelate in mesopore of silica and subsequent thermal calcination inducing dual-metal active site formation. Such a tactic could make amorphous VO_x species well covered on the surface of mesopore, and ultrafine copper oxide particles surrounded and neighbored by highly dispersed VO_x with strong interplay in mesopore, which was comprehensively confirmed by various characterizations. Benefiting from the unique V-Cu neighboring effect, the desorption of formed phenol over the catalytic site might be restricted therefore easily further activated by the formed reactive oxidative species, 3VCu-NS shows synergetic tandem-oxidation catalytic activities for benzene towards benzenediol with a selectivity of 57%. The result allows optimal 3VCu-NS to be a promising catalyst for benzenediol synthesis from benzene.

关键词: Catalysis, Molecular sieve, Benzene, Synergetic effect, Tandem oxidation

Abstract: The direct tandem oxidation synthesis of benzenediol from benzene could simplify or even avoid the separation and purification of reaction intermediates, which is promising but challenged because of the further required immediate consecutive activation of intermediate phenol. In this work, a synergistic benzene tandem-oxidation catalyst that V-Cu bimetallic oxides modified nanoporous silica (VCu-NS) was constructed via a facile assembly strategy which involves addictive negative anion citric acid mediating the intercalation of metal-citric acid chelate in mesopore of silica and subsequent thermal calcination inducing dual-metal active site formation. Such a tactic could make amorphous VO_x species well covered on the surface of mesopore, and ultrafine copper oxide particles surrounded and neighbored by highly dispersed VO_x with strong interplay in mesopore, which was comprehensively confirmed by various characterizations. Benefiting from the unique V-Cu neighboring effect, the desorption of formed phenol over the catalytic site might be restricted therefore easily further activated by the formed reactive oxidative species, 3VCu-NS shows synergetic tandem-oxidation catalytic activities for benzene towards benzenediol with a selectivity of 57%. The result allows optimal 3VCu-NS to be a promising catalyst for benzenediol synthesis from benzene.

Key words: Catalysis, Molecular sieve, Benzene, Synergetic effect, Tandem oxidation

Mengting Liu, Xuexue Dong, Zengjing Guo, Aihua Yuan, Shuying Gao, Fu Yang. Enabling tandem oxidation of benzene to benzenediol over integrated neighboring V-Cu oxides in mesoporous silica[J]. 中国化学工程学报, 2023, 55(3): 236-245.

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Enabling tandem oxidation of benzene to benzenediol over integrated neighboring V-Cu oxides in mesoporous silica

Enabling tandem oxidation of benzene to benzenediol over integrated neighboring V-Cu oxides in mesoporous silica

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