Reactive adsorption of hydrogen sulfide by promoted sorbents Cu-ZnO/SiO2: active sites by experiment and simulation

被引：21
|
作者：
Dhage, Priyanka [1 ]
Samokhvalov, Alexander [1 ,3 ]
McKee, Michael L. [2 ]
Duin, Evert C. [2 ]
Tatarchuk, Bruce J. [1 ]
机构：
[1] Auburn Univ, Dept Chem Engn, Auburn, AL 36849 USA
[2] Auburn Univ, Dept Chem & Biochem, Auburn, AL 36849 USA
[3] Rutgers State Univ, Dept Chem, Camden, NJ 08102 USA
来源：
SURFACE AND INTERFACE ANALYSIS | 2013年 / 45卷 / 05期
关键词：
desulfurization; zinc oxide; density functional theory; hydrogen sulfide; sorbent; promoter; MIXED-METAL OXIDES; ZINC-OXIDE; TEMPERATURE REMOVAL; REGENERABLE SORBENTS; H2S REMOVAL; SOFT ACIDS; COPPER; ZNO; CATALYSTS; CU;
D O I：
10.1002/sia.5174
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
In the Cu-x-Zn(1-x)O/SiO2 sorbents for ultradeep adsorptive removal of H2S from gaseous fuel reformates for fuel cells at room temperature, Cu promoter sites significantly increase sulfur uptake capacity of the sorbents. We report characterization of the family of Cu-x-Zn(1-x)O/SiO2 sorbents for reactive adsorption of H2S using X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) surface area analysis, electron spin resonance (ESR), ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy (DRS) and calculations by the density functional theory (DFT). Both the supported ZnO phase and Cu promoter sites in the Cu-x-Zn(1-x)O/SiO2 sorbents are nano-dispersed, as shown by XRD. The Cu-x-Zn(1-x)O/SiO2 sorbents contain Cu promoter as the Cu2+ site of octahedral geometry, as found by the complementary ESR and UV-vis DRS. Mechanism of the promoter effect of the Cu2+ site in the Cu-x-Zn(1-x)O/SiO2 sorbents in reaction with H2S is proposed based on DFT calculations. Copyright (C) 2012 John Wiley & Sons, Ltd.
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收藏
页码：865 / 872
页数：8
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