Mechanistic Insights into the Structure-Dependent Selectivity of Catalytic Furfural Conversion on Platinum Catalysts

Cai, Qiuxia; Wang, Jianguo; Wang, Yang-Gang; Mei, Donghai

doi:10.1002/aic.14902

Title: Mechanistic Insights into the Structure-Dependent Selectivity of Catalytic Furfural Conversion on Platinum Catalysts

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Abstract

The effects of structure and size on the selectivity of catalytic furfural conversion over supported Pt catalysts in the presence of hydrogen have been studied using first principles density functional theory (DFT) calculations and microkinetic modeling. Four Pt model systems, i.e., periodic Pt(111), Pt(211) surfaces, as well as small nanoclusters (Pt13 and Pt55) are chosen to represent the terrace, step, and corner sites of Pt nanoparticles. Our DFT results show that the reaction routes for furfural hydrogenation and decarbonylation are strongly dependent on the type of reactive sites, which lead to the different selectivity. On the basis of the size-dependent site distribution rule, we correlate the site distributions as a function of the Pt particle size. Our microkinetic results indicate the critical particle size that controls the furfural selectivity is about 1.0 nm, which is in good agreement with the reported experimental value under reaction conditions. This work was supported by National Basic Research Program of China (973 Program) (2013CB733501) and the National Natural Science Foundation of China (NSFC-21306169, 21176221, 21136001, 21101137 and 91334103). This work was also partially supported by the US Department of Energy (DOE), the Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences.more »« less

Authors:: Cai, Qiuxia; Wang, Jianguo; Wang, Yang-Gang; Mei, Donghai

Publication Date:: Sun Nov 01 00:00:00 EDT 2015

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1226402

Report Number(s):: PNNL-SA-104546
Journal ID: ISSN 1547-5905; 47800; KC0302010

DOE Contract Number:: AC05-76RL01830

Resource Type:: Journal Article

Journal Name:: AIChE Journal (Online)

Additional Journal Information:: Journal Volume: 6; Journal Issue: 11; Journal ID: ISSN 1547-5905

Country of Publication:: United States

Language:: English

Subject:: catalysis; biomass conversion; size-dependent selectivity; density functional theory; microkinetic modeling; Environmental Molecular Sciences Laboratory

Citation Formats


                    Cai, Qiuxia, Wang, Jianguo, Wang, Yang-Gang, and Mei, Donghai. Mechanistic Insights into the Structure-Dependent Selectivity of Catalytic Furfural Conversion on Platinum Catalysts.  United States: N. p., 2015. 
        Web.  doi:10.1002/aic.14902.

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                    Cai, Qiuxia, Wang, Jianguo, Wang, Yang-Gang, & Mei, Donghai. Mechanistic Insights into the Structure-Dependent Selectivity of Catalytic Furfural Conversion on Platinum Catalysts.  United States.  https://doi.org/10.1002/aic.14902

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                    Cai, Qiuxia, Wang, Jianguo, Wang, Yang-Gang, and Mei, Donghai. 2015.  
        "Mechanistic Insights into the Structure-Dependent Selectivity of Catalytic Furfural Conversion on Platinum Catalysts".  United States.  https://doi.org/10.1002/aic.14902.

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@article{osti_1226402,

  title        = {Mechanistic Insights into the Structure-Dependent Selectivity of Catalytic Furfural Conversion on Platinum Catalysts},

  author       = {Cai, Qiuxia and Wang, Jianguo and Wang, Yang-Gang and Mei, Donghai},

  abstractNote = {The effects of structure and size on the selectivity of catalytic furfural conversion over supported Pt catalysts in the presence of hydrogen have been studied using first principles density functional theory (DFT) calculations and microkinetic modeling. Four Pt model systems, i.e., periodic Pt(111), Pt(211) surfaces, as well as small nanoclusters (Pt13 and Pt55) are chosen to represent the terrace, step, and corner sites of Pt nanoparticles. Our DFT results show that the reaction routes for furfural hydrogenation and decarbonylation are strongly dependent on the type of reactive sites, which lead to the different selectivity. On the basis of the size-dependent site distribution rule, we correlate the site distributions as a function of the Pt particle size. Our microkinetic results indicate the critical particle size that controls the furfural selectivity is about 1.0 nm, which is in good agreement with the reported experimental value under reaction conditions. This work was supported by National Basic Research Program of China (973 Program) (2013CB733501) and the National Natural Science Foundation of China (NSFC-21306169, 21176221, 21136001, 21101137 and 91334103). This work was also partially supported by the US Department of Energy (DOE), the Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. Computing time was granted by the grand challenge of computational catalysis of the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL). EMSL is a national scientific user facility located at Pacific Northwest National Laboratory (PNNL) and sponsored by DOE’s Office of Biological and Environmental Research.},

  doi          = {10.1002/aic.14902},

  url          = {https://www.osti.gov/biblio/1226402},
  journal      = {AIChE Journal (Online)},

  issn         = {1547-5905},

  number       = 11,

  volume       = 6,

  place        = {United States},

  year         = {Sun Nov 01 00:00:00 EDT 2015},

  month        = {Sun Nov 01 00:00:00 EDT 2015}

}

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