DICP OpenIR
Exceptional stability and chemical mechanism over spinel ZnCr2O4 catalyst for HCl oxidation to Cl-2
Tian, Xin1; Guo, Chenxi3; Zhong, Hong1; Zhou, Yonghua1; Xiao, Jianping2,3
Corresponding AuthorZhou, Yonghua(zhouyonghua@csu.edu.cn) ; Xiao, Jianping(xiao@dicp.ac.cn)
KeywordChlorine recycling HCl catalytic oxidation Spinel Zinc chromate Cobalt chromate
Source PublicationMOLECULAR CATALYSIS
2019-06-01
ISSN2468-8231
DOI10.1016/j.mcat.2019.03.025
Volume470Pages:82-88
Funding ProjectNational Natural Science Foundation of China[21676303] ; National Natural Science Foundation of China[21802124] ; Hunan Provincial Science and Technology Plan Project, China[2016TP1007] ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordOXIDES ; CEO2 ; TRANSITION ; METHANE ; COPPER
AbstractDeacon process, one-step catalytic oxidation of HCl to Cl-2, is the most effective way to realize the recycling utilization of chlorine element in industry since 1868. However, the stability of non-noble metal catalysts, e.g. Cr-based catalysts, is problematic to be commercialized due to the Cr loss in reaction atmosphere. Herein, we reported a spinel ZnCr2O4 catalyst exhibiting a high activity as well as an unprecedented long-term stability, with a sustainable HCl conversion rate (chi(Hcl)) of (similar to)78% and the space time yield (STY) of 2.25 g(cl2) g(cat)(-1) h(-1) even after 300 h run at 390 degrees C and feed O-2/HCl (1:1). In addition, we conceived the control experiments and density functional theory (DFT) calculations to deeply understand the chemical mechanisms over spinel CoCr2O4 and ZnCr2O4. The XPS, O-2-TPD and H-2-TPR characterizations suggested the different surface redox behaviors of both catalysts. DFT calculations indicated that a defect surface of ZnCr2O4 was more active in HCl catalyzed oxidation and HCl preferred to be absorbed on the Zn top site and Cl* coupling to Cl-2 was the Delta G-determining step, which led to the excellent stability of ZnCr2O4 by efficiently avoiding the Cr loss. On the contrary, the higher reaction energy of HCl adsorption on the Co-Cr bridge sites of CoCr2O4 caused the decreasing of activity and stability. Consequently, the different stability performance over CoCr2O4 and ZnCr2O4 was well correlated with the two distinct chemical mechanisms and therefore an outstanding agreement was obtained from the theoretical calculations and experimental behaviors.
Language英语
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Hunan Provincial Science and Technology Plan Project, China ; Hunan Provincial Science and Technology Plan Project, China ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University ; Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University
WOS IDWOS:000469906600010
PublisherELSEVIER SCIENCE BV
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/172076
Collection中国科学院大连化学物理研究所
Corresponding AuthorZhou, Yonghua; Xiao, Jianping
Affiliation1.Cent S Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Efficient & Clean Utilizat Man, Changsha 410083, Hunan, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
3.Westlake Univ, Sch Sci, Inst Nat Sci, Westlake Inst Adv Study, Hangzhou 310024, Zhejiang, Peoples R China
Recommended Citation
GB/T 7714
Tian, Xin,Guo, Chenxi,Zhong, Hong,et al. Exceptional stability and chemical mechanism over spinel ZnCr2O4 catalyst for HCl oxidation to Cl-2[J]. MOLECULAR CATALYSIS,2019,470:82-88.
APA Tian, Xin,Guo, Chenxi,Zhong, Hong,Zhou, Yonghua,&Xiao, Jianping.(2019).Exceptional stability and chemical mechanism over spinel ZnCr2O4 catalyst for HCl oxidation to Cl-2.MOLECULAR CATALYSIS,470,82-88.
MLA Tian, Xin,et al."Exceptional stability and chemical mechanism over spinel ZnCr2O4 catalyst for HCl oxidation to Cl-2".MOLECULAR CATALYSIS 470(2019):82-88.
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