期刊
JOURNAL OF CATALYSIS
卷 342, 期 -, 页码 158-163出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2016.08.001
关键词
Sulfated zirconia; Enthalpy of formation; Heterogeneous catalysis; Thermodynamics; Calorimetry; Olefins conversion; Stability and activity
资金
- United States Department of Energy, Office of Basic Energy Sciences [DE-FG02-05ER15667]
- China Scholarship Council for the State Scholarship Fund [201506740047]
- Gene and Linda Voiland School of Chemical Engineering and Bioengineering at Washington State University
A series of sulfated zirconia (SZ) catalysts were synthesized by immersion of amorphous zirconium hydroxide in sulfuric acid of various concentrations (1-5 N). These samples were fully characterized by X-ray diffraction (XRD), thermogravimetric analysis and mass spectrometry (TGA-MS), and aqueous sulfuric acid immersion and high temperature oxide melt solution calorimetry. We investigated the enthalpies of the complex interactions between sulfur species and the zirconia surface (Delta H-SZ) for the sulfated zirconia precursor (SZP), ranging from - 109.46 +/- 7.33 (1 N) to -42.50 +/- 0.89 (4 N) S. Delta H-SZ appears to be a roughly exponential function of sulfuric acid concentration. On the other hand, the enthalpy of SZ formation (Delta H-f), becomes more exothermic linearly as sulfur surface coverage increases, from -147.90 +/- 4.16 (2.14 nm(-2)) to -317.03 +/- 4.20 (2.29 nm(-2)) kJ/mol S, indicating formation of energetically more stable polysulfate species. (C) 2016 Elsevier Inc. All rights reserved.
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