文献类型：期刊文献

英文题名：Thermodynamic complexity of sulfated zirconia catalysts

作者：Liu, Naiwang[1,2,3];Guo, Xiaofeng[4];Navrotsky, Alexandra[2,3];Shi, Li[1];Wu, Di[5]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Univ Calif Davis, Peter A Rock Thermochem Lab, One Shields Ave, Davis, CA 95616 USA;[3]Univ Calif Davis, NEAT ORU, One Shields Ave, Davis, CA 95616 USA;[4]Los Alamos Natl Lab, Div Earth & Environm Sci, Earth Syst Observat, Los Alamos, NM 87545 USA;[5]Washington State Univ, Gene & Linda Voiland Sch Chem Engn & Bioengn, Pullman, WA 99163 USA

年份：2016

卷号：342

起止页码：158

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20163502763825);WOS:【SCI-EXPANDED(收录号:WOS:000384864600016)】；

基金：This work was supported by the United States Department of Energy, Office of Basic Energy Sciences, Grant DE-FG02-05ER15667. N.L. thanks the China Scholarship Council for the State Scholarship Fund (No. 201506740047). D.W. thanks the institutional funds from the Gene and Linda Voiland School of Chemical Engineering and Bioengineering at Washington State University.

语种：英文

外文关键词：Sulfated zirconia; Enthalpy of formation; Heterogeneous catalysis; Thermodynamics; Calorimetry; Olefins conversion; Stability and activity

摘要：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.