CO2 Hydrogenation on Unpromoted and M-Promoted Co/TiO2 Catalysts (M = Zr, K, Cs): Effects of Crystal Phase of Supports and Metal-Support Interaction on Tuning Product Distribution
文献类型：期刊论文
| 作者 | Guo, Xinwen2; Li, Wenhui2; Zhang, Guanghui2; Jiang, Xiao3; Liu, Yi2; Zhu, Jie2; Ding, Fanshu2; Liu, Zhongmin4; Song, Chunshan1,2,5 |
| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2019-04-01 |
| 卷号 | 9期号:4页码:2739-2751 |
| 关键词 | CO2 hydrogenation cobalt catalyst crystal phase TiO2 C/H ratio |
| ISSN号 | 2155-5435 |
| DOI | 10.1021/acscatal.8b04720 |
| 通讯作者 | Guo, Xinwen(guoxw@dlut.edu.cn) ; Song, Chunshan(csong@psu.edu) |
| 英文摘要 | Cobalt catalysts supported on TiO2 with different crystal forms (anatase and rutile) differ sharply in CO2 conversion and product selectivity for CO2 hydrogenation. The Co/rutile-TiO2 catalyst selectively catalyzed CO2 hydrogenation to CH4, while CO is the main product on the Co/anatase-TiO2 catalyst. In situ DRIFT (diffuse reflectance infrared Fourier transform) results have partially revealed the reaction pathway of CO2 hydrogenation on these two catalysts. On Co/rutile-TiO2, the reaction proceeds through the key intermediate formate species, which is further converted to CH4. Differently, the reaction on Co/anatase-TiO2 undergoes CO2 -> *CO, which desorbs to form gas-phase CO instead of subsequent hydrogenation. The strongly bonded *CO is required to enhance the subsequent hydrogenation. By simply changing the calcination temperature of anatase TiO2, the product selectivity can be tuned from CO to CH4 with a significant increase in CO, conversion due to the surface phase transition of the anatase to the rutile phase. The addition of Zr, K, and Cs further improves the CO, CO2, and H-2 adsorption in both the capacity and strength over anatase- and rutile-supported catalysts. The Zr modification makes the reaction pathway over anatase-supported catalyst proceed via the intermediate formate species and enables the subsequent hydrogenation to CH4. In addition, the surface C/H ratio increases significantly in the presence of promoters (unpromoted < Zr-promoted < K-Zr-promoted similar to Cs-Zr-promoted), which leads to the highest C-2(+) selectivity of 17% with 70% CO, conversion over K-Zr-Co/anatase-TiO2 catalyst. These results reveal mechanistic insights into how the product distribution of Co/TiO2 catalysts can be manipulated through adjusting the adsorption performance and surface C/H ratio. |
| WOS关键词 | CARBON-DIOXIDE METHANATION ; METHANOL SYNTHESIS ; LOWER OLEFINS ; TIO2 PHOTOCATALYSTS ; HIGHER HYDROCARBONS ; COBALT CATALYSTS ; FE ; PERFORMANCE ; ANATASE ; RUTILE |
| 资助项目 | National Key Research and Development Program of China[2016YFB0600902-5] ; National Natural Science Foundation of China[21503029] ; Fundamental Research Funds for the Central Universities[DUT 18RC(3)057] ; Fundamental Research Funds for the Central Universities[R-500] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000464075700006 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; National Key Research and Development Program of China ; National Key Research and Development Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/165560]  |
| 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 | Guo, Xinwen; Song, Chunshan |
| 作者单位 | 1.Penn State Univ, Dept Energy & Mineral Engn, PSU DUT Joint Ctr Energy Res, Clean Fuels & Catalysis Program,EMS Energy Inst, University Pk, PA 16802 USA 2.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China 3.Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA 4.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Natl Engn Lab Methanol Olefins, Dalian 116023, Peoples R China 5.Penn State Univ, Dept Chem Engn, PSU DUT Joint Ctr Energy Res, Clean Fuels & Catalysis Program,EMS Energy Inst, University Pk, PA 16802 USA |
| 推荐引用方式 GB/T 7714 | Guo, Xinwen,Li, Wenhui,Zhang, Guanghui,et al. CO2 Hydrogenation on Unpromoted and M-Promoted Co/TiO2 Catalysts (M = Zr, K, Cs): Effects of Crystal Phase of Supports and Metal-Support Interaction on Tuning Product Distribution[J]. ACS CATALYSIS,2019,9(4):2739-2751. |
| APA | Guo, Xinwen.,Li, Wenhui.,Zhang, Guanghui.,Jiang, Xiao.,Liu, Yi.,...&Song, Chunshan.(2019).CO2 Hydrogenation on Unpromoted and M-Promoted Co/TiO2 Catalysts (M = Zr, K, Cs): Effects of Crystal Phase of Supports and Metal-Support Interaction on Tuning Product Distribution.ACS CATALYSIS,9(4),2739-2751. |
| MLA | Guo, Xinwen,et al."CO2 Hydrogenation on Unpromoted and M-Promoted Co/TiO2 Catalysts (M = Zr, K, Cs): Effects of Crystal Phase of Supports and Metal-Support Interaction on Tuning Product Distribution".ACS CATALYSIS 9.4(2019):2739-2751. |
入库方式： OAI收割
来源：大连化学物理研究所
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