TY - JOUR
T1 - Mesoporous-molecular-sieve-supported nickel sorbents for adsorptive desulfurization of commercial ultra-low-sulfur diesel fuel
AU - Sentorun-Shalaby, Cigdem
AU - Saha, Shyamal Kumar
AU - Ma, Xiaoliang
AU - Song, Chunshan
N1 - Funding Information:
The authors are pleased to acknowledge the support of this work in part by the U.S. Department of Energy, National Energy Technology Laboratory under Contract No. DE-FC26-08NT0004396 . The authors are grateful to Dr. Xiaoxing Wang for his help in preparation of SBA-15 and Chao Xie for his help in H 2 chemisorption analysis.
PY - 2011/1/14
Y1 - 2011/1/14
N2 - A high-performance nickel-based sorbent was developed by loading nickel on a mesoporous molecular sieve, MCM-48, for adsorptive desulfurization (ADS) of commercial ultra low sulfur diesel (ULSD) for fuel cell applications. The prepared sorbents were characterized by the N2 adsorption-desorption, X-ray diffraction (XRD), H2 chemisorption, and transmission electron microscope (TEM), and the ADS performance was evaluated in a fixed-bed flow sorption system at 220°C using a commercial ULSD with a sulfur content of 14.5ppmw. Effects of the ultrasonic aid in incipient wetness impregnation (IWI), nickel loading amount and support materials on the sorbent performance were examined. It was found that the incipient wetness impregnation with the ultrasonic aid improved significantly the ADS performance of the sorbent by increasing the dispersion of nickel on the surface. Using MCM-48 as a support with 20wt% nickel loading (Ni20/MCM-48) can lead to an excellent nickel-based sorbent with a breakthrough capacity of 2.1mg-S/g-sorb for ADS of the ULSD at a breakthrough sulfur level of 1ppmw. The alkyl dibenzothiophenes are likely adsorbed on the sorbent surface directly through an interaction between the sulfur atom and the exposed nickel atoms, and a part (∼6%) of the adsorbed alkyl dibenzothiophenes react further with the surface nickel to release the corresponding hydrocarbons. The desulfurization reactivity of the alkyl dibenzothiophenes is dependent on not only the number, but also the size of the alkyl substituents at the 4- and 6-positions of alkyl dibenzothiophenes.
AB - A high-performance nickel-based sorbent was developed by loading nickel on a mesoporous molecular sieve, MCM-48, for adsorptive desulfurization (ADS) of commercial ultra low sulfur diesel (ULSD) for fuel cell applications. The prepared sorbents were characterized by the N2 adsorption-desorption, X-ray diffraction (XRD), H2 chemisorption, and transmission electron microscope (TEM), and the ADS performance was evaluated in a fixed-bed flow sorption system at 220°C using a commercial ULSD with a sulfur content of 14.5ppmw. Effects of the ultrasonic aid in incipient wetness impregnation (IWI), nickel loading amount and support materials on the sorbent performance were examined. It was found that the incipient wetness impregnation with the ultrasonic aid improved significantly the ADS performance of the sorbent by increasing the dispersion of nickel on the surface. Using MCM-48 as a support with 20wt% nickel loading (Ni20/MCM-48) can lead to an excellent nickel-based sorbent with a breakthrough capacity of 2.1mg-S/g-sorb for ADS of the ULSD at a breakthrough sulfur level of 1ppmw. The alkyl dibenzothiophenes are likely adsorbed on the sorbent surface directly through an interaction between the sulfur atom and the exposed nickel atoms, and a part (∼6%) of the adsorbed alkyl dibenzothiophenes react further with the surface nickel to release the corresponding hydrocarbons. The desulfurization reactivity of the alkyl dibenzothiophenes is dependent on not only the number, but also the size of the alkyl substituents at the 4- and 6-positions of alkyl dibenzothiophenes.
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U2 - 10.1016/j.apcatb.2010.11.014
DO - 10.1016/j.apcatb.2010.11.014
M3 - Article
AN - SCOPUS:78650309746
SN - 0926-3373
VL - 101
SP - 718
EP - 726
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
IS - 3-4
ER -