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Tuning Catalytic Selectivity of Oxidative Catalysis through Deposition of Nonmetallic Atoms in Surface Lattice of Metal Oxide

文献类型：期刊论文

作者Liu, Juanjuan1,2,3; Zhang, Shiran2,3; Zhou, Yan4; Fung, Victor5; Nguyen, Luan2,3; Jiang, De-en5; Shen, Wenjie4; Fan, Jie1; Tao, Franklin Feng2,3
刊名ACS CATALYSIS
出版日期2016-07-01
卷号6期号:7页码:4218-4228
关键词Catalytic Selectivity Oxidative Dehydrogenation Ethane Ethylene Surface Lattice Oxygen Oxygen Vacancies Cobalt Oxide
ISSN号2155-5435
DOI10.1021/acscatal.5b02900
文献子类Article
英文摘要Catalytic selectivity for producing an ideal product is a key topic for chemical transformations through heterogeneous catalysis. Tuning catalytic selectivity by integrating the second metal to form an alloy has been well demonstrated in the literature. Here we report a method to tune catalytic selectivity in oxidative catalysis on another category of heterogeneous catalysts, transition-metal oxides. By choosing the oxidative dehydrogenation (ODH) of ethane to ethylene as a probe reaction, we demonstrated that doping nonmetallic atoms to the surface lattice of catalyst of a transition-metal oxide can enhance catalytic selectivity through suppression of complete oxidation of the reactant molecules. Catalysts of Co3O4 with doped silicon atoms (Si-x-Co3O4) maintaining the spinel structure of pure Co3O4 exhibit much higher selectivity for the production of ethylene through ODH of ethane in comparison to pure Co3O4 at 600 degrees C by 40%. The suppression of activity of surface lattice oxygen atoms was evidenced by the observation that the surface lattice oxygen atoms of Si-x-Co3O4 cannot exchange oxygen atoms with gas-phase oxygen at low temperatures while pure Co3O4 can. The difference in releasing surface lattice oxygen atoms and dissociating molecular oxygen between pure Co3O4 and Si-x-Co3O4, was supported by DFT calculations. The calculated activation barriers for dissociation of molecular O-2 and energy barriers for hopping surface oxygen vacancies of Si-x-Co3O4, are obviously higher than those of pure Co3O4, respectively. These experimental exploration and computational studies established a correlation between increase of catalytic selectivity and suppression of the activity of surface lattice oxygen atoms/oxygen vacancies. This correlation suggests an approach for increasing the catalytic selectivity of oxidative catalysis through suppressing activity of surface lattice oxygen atoms/vacancies via doping atoms of a nonmetallic element. This new approach was further confirmed by the observed higher catalytic selectivity for production of ethylene on Geol-Co3O4 in comparison to pure Co3O4.
WOS关键词O MIXED OXIDES ; THERMAL-STABILITY ; NIO CATALYSTS ; NICKEL-OXIDE ; ETHANE ODH ; DEHYDROGENATION ; PYROLYSIS ; ETHYLENE ; NANOPARTICLES ; PROPANE
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000379457300021
出版者AMER CHEMICAL SOC
源URL[http://cas-ir.dicp.ac.cn/handle/321008/170440]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Fan, Jie; Tao, Franklin Feng
作者单位1.Zhejiang Univ, Dept Chem, Hangzhou 310027, Zhejiang, Peoples R China
2.Univ Kansas, Dept Chem & Petr Engn, Lawrence, KS 66045 USA
3.Univ Kansas, Dept Chem, Lawrence, KS 66045 USA
4.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
5.Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA
推荐引用方式
GB/T 7714		 Liu, Juanjuan,Zhang, Shiran,Zhou, Yan,et al. Tuning Catalytic Selectivity of Oxidative Catalysis through Deposition of Nonmetallic Atoms in Surface Lattice of Metal Oxide[J]. ACS CATALYSIS,2016,6(7):4218-4228.
APA Liu, Juanjuan.,Zhang, Shiran.,Zhou, Yan.,Fung, Victor.,Nguyen, Luan.,...&Tao, Franklin Feng.(2016).Tuning Catalytic Selectivity of Oxidative Catalysis through Deposition of Nonmetallic Atoms in Surface Lattice of Metal Oxide.ACS CATALYSIS,6(7),4218-4228.
MLA Liu, Juanjuan,et al."Tuning Catalytic Selectivity of Oxidative Catalysis through Deposition of Nonmetallic Atoms in Surface Lattice of Metal Oxide".ACS CATALYSIS 6.7(2016):4218-4228.

入库方式： OAI收割

来源：大连化学物理研究所

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