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Breakthrough Characteristics of Reformate Desulfurization Using

ZnO Sorbents for Logistic Fuel Cell Power Systems

Hongyun Yang†, Ryan Sothen, Donald R. Cahela and Bruce J. Tatarchuk*

Center for Microfibrous Materials Manufacturing, Department of Chemical Engineering, Auburn University,
Auburn, Alabama 36849
Ind. Eng. Chem. Res., 2008, 47 (24), pp 10064–10070
DOI: 10.1021/ie8008617
Publication Date (Web): November 21, 2008
Copyright © 2008 American Chemical Society

* To whom correspondence should be addressed. Tel.: (334) 844-2023 FREE. Fax: (334) 844-2065. E-, †
Current address: IntraMicron Inc., 368 Industry Drive, Auburn, AL 36832.

Sulfur breakthrough behaviors during reformate desulfurization were investigated using a novel ZnO-
based sorbent with minimized mass transfer resistance. The presence of CO, CO2, or water affected
the breakthrough characteristics of H2S and carbonyl sulfide (COS). CO and CO2did not significantly
affect the reaction between H2S and ZnO, but they reacted with H2S to form COS, which cannot be
efficiently removed by ZnO. The mechanisms of COS formation via two different pathways were also
investigated. CO reacted with H2S to form COS homogeneously; CO2 reacted with H2S
heterogeneously on the sulfide surface. COS formation by CO and CO2was suppressed by H2 and
water. Water also severely hindered the reaction between ZnO and H2S and significantly decreased
H2S breakthrough time. At low water concentrations, sulfur breakthrough was determined by the
homogeneous COS formation; at high water concentrations, it was controlled by H2S breakthrough.
Capacity loss due to COS formation and adsorption of water was also observed. Novel sorbent and
process designs are required to improve the desulfurization performance.