Carbon Dioxide Conversion to Valuable Chemical Products over Composite Catalytic Systems

Dagle, Robert A.; Hu, Jianli; Jones, Susanne B.; Wilcox, Wayne A.; Frye, John G.; White, J. F.; Jiang, Juyuan; Wang, Yong

doi:10.1016/S2095-4956(13)60047-9

Title: Carbon Dioxide Conversion to Valuable Chemical Products over Composite Catalytic Systems

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Abstract

Presented is an experimental study on catalytic conversion of carbon dioxide into methanol, ethanol and acetic acid. Catalysts having different catalytic functions were synthesized and combined in different ways to enhance selectivity to desired products. The combined catalyst system possessed the following functions: methanol synthesis, Fischer-Tropsch synthesis, water-gas-shift and hydrogenation. Results showed that the methods of integrating these catalytic functions played important role in achieving desired product selectivity. It was speculated that if methanol synthesis sites were located adjacent to the C-C chain growth sites, the formation rate of C2 oxygenates would be enhanced. The advantage of using high temperature methanol catalyst PdZnAl in the combined catalyst system was demonstrated. In the presence of PdZnAl catalyst, the combined catalyst system was stable at temperature of 380oC. It was observed that, at high temperature, kinetics favored oxygenate formation. Results implied that the process can be intensified by operating at high temperature using Pd-based methanol synthesis catalyst. Steam reforming of the byproduct organics was demonstrated as a means to provide supplemental hydrogen. Preliminary process design, simulation, and economic analysis of the proposed CO2 conversion process were carried out. Economic analysis indicates how ethanol production cost was affected by the price of CO2more » and hydrogen.« less

Authors:: Dagle, Robert A.; Hu, Jianli; Jones, Susanne B.; Wilcox, Wayne A.; Frye, John G.; White, J. F.; Jiang, Juyuan; Wang, Yong

Publication Date:: Wed May 01 00:00:00 EDT 2013

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1089610

Report Number(s):: PNNL-SA-92509
AA7020000

DOE Contract Number:: AC05-76RL01830

Resource Type:: Journal Article

Journal Name:: Journal of Energy Chemistry, 22(3):368-374

Additional Journal Information:: Journal Name: Journal of Energy Chemistry, 22(3):368-374

Country of Publication:: United States

Language:: English

Citation Formats


                    Dagle, Robert A., Hu, Jianli, Jones, Susanne B., Wilcox, Wayne A., Frye, John G., White, J. F., Jiang, Juyuan, and Wang, Yong. Carbon Dioxide Conversion to Valuable Chemical Products over Composite Catalytic Systems.  United States: N. p., 2013. 
        Web.  doi:10.1016/S2095-4956(13)60047-9.

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                    Dagle, Robert A., Hu, Jianli, Jones, Susanne B., Wilcox, Wayne A., Frye, John G., White, J. F., Jiang, Juyuan, & Wang, Yong. Carbon Dioxide Conversion to Valuable Chemical Products over Composite Catalytic Systems.  United States.  https://doi.org/10.1016/S2095-4956(13)60047-9

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                    Dagle, Robert A., Hu, Jianli, Jones, Susanne B., Wilcox, Wayne A., Frye, John G., White, J. F., Jiang, Juyuan, and Wang, Yong. 2013.  
        "Carbon Dioxide Conversion to Valuable Chemical Products over Composite Catalytic Systems".  United States.  https://doi.org/10.1016/S2095-4956(13)60047-9.

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@article{osti_1089610,

  title        = {Carbon Dioxide Conversion to Valuable Chemical Products over Composite Catalytic Systems},

  author       = {Dagle, Robert A. and Hu, Jianli and Jones, Susanne B. and Wilcox, Wayne A. and Frye, John G. and White, J. F. and Jiang, Juyuan and Wang, Yong},

  abstractNote = {Presented is an experimental study on catalytic conversion of carbon dioxide into methanol, ethanol and acetic acid. Catalysts having different catalytic functions were synthesized and combined in different ways to enhance selectivity to desired products. The combined catalyst system possessed the following functions: methanol synthesis, Fischer-Tropsch synthesis, water-gas-shift and hydrogenation. Results showed that the methods of integrating these catalytic functions played important role in achieving desired product selectivity. It was speculated that if methanol synthesis sites were located adjacent to the C-C chain growth sites, the formation rate of C2 oxygenates would be enhanced. The advantage of using high temperature methanol catalyst PdZnAl in the combined catalyst system was demonstrated. In the presence of PdZnAl catalyst, the combined catalyst system was stable at temperature of 380oC. It was observed that, at high temperature, kinetics favored oxygenate formation. Results implied that the process can be intensified by operating at high temperature using Pd-based methanol synthesis catalyst. Steam reforming of the byproduct organics was demonstrated as a means to provide supplemental hydrogen. Preliminary process design, simulation, and economic analysis of the proposed CO2 conversion process were carried out. Economic analysis indicates how ethanol production cost was affected by the price of CO2 and hydrogen.},

  doi          = {10.1016/S2095-4956(13)60047-9},

  url          = {https://www.osti.gov/biblio/1089610},
  journal      = {Journal of Energy Chemistry, 22(3):368-374},
number       = ,

  volume       = ,

  place        = {United States},

  year         = {Wed May 01 00:00:00 EDT 2013},

  month        = {Wed May 01 00:00:00 EDT 2013}

}

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