期刊
AICHE JOURNAL
卷 61, 期 2, 页码 631-639出版社
WILEY
DOI: 10.1002/aic.14647
关键词
desulfurization; adsorption; metal oxides; diesel
资金
- National Energy Technology Laboratory of the US Department of Energy [DE-NT0004396]
- US Office of Naval Research [N00014-06-1-0158]
- US Environmental Protection Agency-US National Science Foundation Joint TSE Program [R831471]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- U.S. DOE [DE-AC02-06CH11357]
- National Natural Science Foundation of China [21306054]
- Guangdong Natural Science Foundation [S2013040014747]
- PetroChina Innovation Foundation
- EPA [R831471, 908902] Funding Source: Federal RePORTER
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
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