Catalytic adsorptive desulfurization of mercaptan, sulfide and disulfide using bifunctional Ti-based adsorbent for ultra-clean oil

doi:10.1016/j.cjche.2021.08.031

中国化学工程学报 ›› 2022, Vol. 42 ›› Issue (2): 25-34.DOI: 10.1016/j.cjche.2021.08.031

• Recent Advances in Adsorptive Separation Materials and Technologies • 上一篇下一篇

Catalytic adsorptive desulfurization of mercaptan, sulfide and disulfide using bifunctional Ti-based adsorbent for ultra-clean oil

Cuiting Yang¹, Bowen Wu¹, Zewei Liu¹, Guang Miao¹, Qibin Xia¹, Zhong Li¹, Michael J. Janik², Guoqing Li¹, Jing Xiao¹

1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China;
2. Department of Chemical Engineering, Pennsylvania State University, PA 16802, USA

收稿日期:2021-06-25 修回日期:2021-08-12 出版日期:2022-02-28 发布日期:2022-03-30
通讯作者: Jing Xiao,E-mail:cejingxiao@scut.edu.cn
基金资助:
The authors gratefully acknowledge the research grants provided by the National Natural Science Foundation of China (22022806, 21776097), and Natural Science Foundation of Guangdong Province (2017A030312005).

Catalytic adsorptive desulfurization of mercaptan, sulfide and disulfide using bifunctional Ti-based adsorbent for ultra-clean oil

Cuiting Yang¹, Bowen Wu¹, Zewei Liu¹, Guang Miao¹, Qibin Xia¹, Zhong Li¹, Michael J. Janik², Guoqing Li¹, Jing Xiao¹

1. School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China;
2. Department of Chemical Engineering, Pennsylvania State University, PA 16802, USA

Received:2021-06-25 Revised:2021-08-12 Online:2022-02-28 Published:2022-03-30
Contact: Jing Xiao,E-mail:cejingxiao@scut.edu.cn
Supported by:
The authors gratefully acknowledge the research grants provided by the National Natural Science Foundation of China (22022806, 21776097), and Natural Science Foundation of Guangdong Province (2017A030312005).

摘要/Abstract

摘要： Ultra-deep desulfurization of transformer oil is of great demand among power industry. In this work, the effective and deep removal of various types of organosulfurs, including mercaptan, sulfide and disulfide via catalytic adsorptive desulfurization (CADS) using bifunctional Ti-based adsorbent is reported. Compared to adsorptive desulfurization (ADS), dramatically improvement of the organosulfur uptakes were achieved under CADS process. The equilibrium adsorption capacity at 5 μg·g^-1 S reached up to 15.7, 33.4, 11.6 and 11.9 mg·g^-1 for propyl mercaptan(n-PM), dimethyl sulfide(DMS), di-t-butyl disulfide (DTBDS) and dibenzyl disulfide (DBDS), which was 262, 477, 97 and 128 times to that of ADS process, respectively, and was the highest among the reported desulfurization adsorbents. Moreover, it achieved superior breakthrough capacity of 2050, 530 and 210 ml F·(g A)^-1 at the breakthrough S concentration of 1 μg·g^-1 of the commercial transformer oil S containing 10, 50 and 150 μg·g^-1, respectively. The effectiveness of CADS is associated to the transformation of sulfur species to higher polar sulfonic species with the assistance of mild oxidant, which can be readily captured by silanol groups on SiO₂ through H-bonding interaction. The excellent recyclability of the adsorbent can be realized through solvent washing or oxidative air treatment. This work provides an effective and economic approach for the elimination of trace amount of mercaptan, sulfide and disulfide from transformer oil.

关键词: Adsorption, Catalysis, Selectivity, Ultra-deep desulfurization, Transformer oil

Abstract: Ultra-deep desulfurization of transformer oil is of great demand among power industry. In this work, the effective and deep removal of various types of organosulfurs, including mercaptan, sulfide and disulfide via catalytic adsorptive desulfurization (CADS) using bifunctional Ti-based adsorbent is reported. Compared to adsorptive desulfurization (ADS), dramatically improvement of the organosulfur uptakes were achieved under CADS process. The equilibrium adsorption capacity at 5 μg·g^-1 S reached up to 15.7, 33.4, 11.6 and 11.9 mg·g^-1 for propyl mercaptan(n-PM), dimethyl sulfide(DMS), di-t-butyl disulfide (DTBDS) and dibenzyl disulfide (DBDS), which was 262, 477, 97 and 128 times to that of ADS process, respectively, and was the highest among the reported desulfurization adsorbents. Moreover, it achieved superior breakthrough capacity of 2050, 530 and 210 ml F·(g A)^-1 at the breakthrough S concentration of 1 μg·g^-1 of the commercial transformer oil S containing 10, 50 and 150 μg·g^-1, respectively. The effectiveness of CADS is associated to the transformation of sulfur species to higher polar sulfonic species with the assistance of mild oxidant, which can be readily captured by silanol groups on SiO₂ through H-bonding interaction. The excellent recyclability of the adsorbent can be realized through solvent washing or oxidative air treatment. This work provides an effective and economic approach for the elimination of trace amount of mercaptan, sulfide and disulfide from transformer oil.

Key words: Adsorption, Catalysis, Selectivity, Ultra-deep desulfurization, Transformer oil

Cuiting Yang, Bowen Wu, Zewei Liu, Guang Miao, Qibin Xia, Zhong Li, Michael J. Janik, Guoqing Li, Jing Xiao. Catalytic adsorptive desulfurization of mercaptan, sulfide and disulfide using bifunctional Ti-based adsorbent for ultra-clean oil[J]. 中国化学工程学报, 2022, 42(2): 25-34.

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Catalytic adsorptive desulfurization of mercaptan, sulfide and disulfide using bifunctional Ti-based adsorbent for ultra-clean oil

Catalytic adsorptive desulfurization of mercaptan, sulfide and disulfide using bifunctional Ti-based adsorbent for ultra-clean oil

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