Air-Promoted Adsorptive Desulfurization of Diesel Fuel Over Ti-Ce Mixed Metal Oxides

被引:57
作者
Xiao, Jing [1 ,2 ,3 ]
Sitamraju, Siddarth [1 ,2 ]
Chen, Yongsheng [1 ,2 ]
Watanabe, Shingo [1 ,2 ]
Fujii, Mamoru [1 ,2 ]
Janik, Michael [1 ,2 ,4 ]
Song, Chunshan [1 ,2 ,4 ]
机构
[1] Penn State Univ, EMS Energy Inst, Clean Fuels & Catalysis Program, University Pk, PA 16802 USA
[2] Penn State Univ, Dept Energy & Mineral Engn, University Pk, PA 16802 USA
[3] S China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510640, Guangdong, Peoples R China
[4] Penn State Univ, Dept Chem Engn, University Pk, PA 16802 USA
基金
中国国家自然科学基金; 美国国家科学基金会;
关键词
desulfurization; adsorption; metal oxides; diesel; HOT GAS DESULFURIZATION; ULTRA-DEEP DESULFURIZATION; TOTAL-ENERGY CALCULATIONS; SELECTIVE ADSORPTION; TRANSPORTATION FUELS; ACTIVATED CARBONS; SULFUR; ADSORBENTS; THIOPHENE; SORBENTS;
D O I
10.1002/aic.14647
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Air-promoted adsorptive desulfurization (ADS) of commercial diesel fuel over a Ti-Ce mixed oxide adsorbent in a flow system is investigated in this work. The fresh/spent adsorbents were characterized using X-ray absorption near edge structure spectroscopy. Results show that sulfoxide species are formed during air-promoted ADS over Ti0.9Ce0.1O2 adsorbent. Adsorption selectivity of various compounds in fuel follows the order of dibenzothiophene sulfone>dibenzothiophene similar or equal to benzothiophene>4-methyldibenzothiophene> 4,6-dimethyldibenzothiophene>phenanthrene>methylnaphthalene>fluorene>naphthalene. The high adsorption affinity of sulfoxide/sulfone is attributed to stronger Ti-OSR2 than Ti-SR2 interactions, resulting in significantly enhanced ADS capacity. Adsorption affinity was calculated using ab initio methods. For Ti-Ce mixed oxides, reduced surface sites lead to O-vacancy sites for O-2 activation for oxidizing thiophenic species. Low temperature is preferred for air-promoted ADS, and the Ti-Ce adsorbent can be regenerated via oxidative air treatment. This study paves a new path of designing regenerable adsorbents. (c) 2014 American Institute of Chemical Engineers AIChE J, 61: 631-639, 2015
引用
收藏
页码:631 / 639
页数:9
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