Enhanced Catalyst Durability for Bio-Based Adipic Acid Production by Atomic Layer Deposition

Amy E. Settle, Nicholas S. Cleveland, Carrie A. Farberow, Davis R. Conklin, Xiangchen Huo, Arrelaine A. Dameron, Ryon W. Tracy, Reuben Sarkar, Elizabeth J. Kautz, Arun Devaraj, Karthikeyan K. Ramasamy, Mike J. Watson, Allyson M. York, Ryan M. Richards, Kinga A. Unocic, Gregg T. Beckham, Michael B. Griffin, Katherine E. Hurst, Eric C.D. Tan, Steven T. ChristensenDerek R. Vardon

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

Abstract

Atomic layer deposition (ALD) improves the durability of metal catalysts using nanoscale metal oxide coatings. However, targeted coating strategies and economic models are lacking for process-specific deactivation challenges that account for implications at scale. Herein, we apply Al2O3 ALD to Pd/TiO2 to increase durability during hydrogenation of muconic acid, a bio-based platform chemical, to adipic acid. Initial coating development and characterization are performed on the milligram scale using stop-flow ALD. Subsequently, ALD coating scale is increased by 3 orders of magnitude using fluidized bed ALD. Activity, leaching resistance, and thermal stability are evaluated at each synthesis scale. ALD-coated catalysts retain up to 2-fold greater muconic acid hydrogenation activity and undergo significantly less physical restructuring than uncoated Pd/TiO2 after high-temperature treatments, while reducing Pd leaching by over 4-fold. Techno-economic analysis for an adipic acid biorefinery supports increased ALD material costs through catalyst lifetime extension, underscoring the potential viability of this technology. Emerging biomass conversion processes often require challenging reaction environments that shorten catalyst lifetimes through premature deactivation. Sufficient catalyst lifetimes are critical for advancing biomass conversion toward industrial scale. Here, we demonstrate that thin metal oxide coatings by atomic layer deposition (ALD) improve catalyst leaching stability in acidic media and enhance thermal stability of both the active metal sites and support. Techno-economic analysis highlights the potential of Al2O3 ALD coatings to reduce bio-based chemical production costs at the 70 kiloton per year scale through increased catalyst lifetimes and sufficient retained activity. The potential for economical ALD coatings for catalyst durability has implications beyond biomass conversion, including other renewable energy and chemical processes facing catalyst stability challenges. Biomass conversion processes often require challenging reaction environments that shorten catalyst lifetimes through deactivation. This work demonstrates that atomic layer deposition (ALD) coatings improve catalyst metal leaching stability, as well as metal and support thermal stability, for bio-based adipic acid production. Techno-economic analysis highlights the potential to reduce adipic acid production costs through increased catalyst lifetimes and retained activity. The potential for economical ALD coatings has catalyst implications beyond biomass conversion, including renewable energy and chemical processes facing stability challenges.

Original languageEnglish
Pages (from-to)2219-2240
Number of pages22
JournalJoule
Volume3
Issue number9
DOIs
StatePublished - Sep 18 2019

Funding

This work was authored in part by the Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under contract no. DE-AC36-08GO28308. Funding was provided in part by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office. This work was partially performed in collaboration with the Chemical Catalysis for Bioenergy Consortium (ChemCatBio), a member of the Energy Materials Network, and was supported by the DOE Bioenergy Technologies Office under contract no. DE-AC05-00OR22725 with Oak Ridge National Laboratory and contract no. DE-AC36-08-GO28308 with NREL. Partial support for D.R.V. M.B.G. K.E.H. and S.T.C. was provided by the Laboratory Directed Research and Development Program at NREL. APT sample preparation and analysis was conducted using facilities at the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory. We thank George Burton for help with STEM imaging at Colorado School of Mines, Nick Grundl and Mary Biddy from NREL for the Aspen and Excel modeling used for this study, and Davinia Salvachúa from NREL for the biological production of the muconic acid. In addition, we would like to thank M.J.W. from Johnson Matthey for his advising on ALD catalyst development and process integration for commercial applications. Lastly, D.R.V. and G.T.B. thank the Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, award number DE-SC0000997, for their partial support. A.E.S. N.S.C. C.A.F. D.R.C. R.W.T. X.H. A.M.Y. E.J.K. A.D. K.A.U. M.B.G. K.E.H. E.C.D.T. and S.T.C. performed research and analyzed data; A.A.D. K.K.R. R.M.R. G.T.B. M.J.W. and D.R.V. provided supervision; A.E.S. and D.R.V. wrote the paper with input from all authors. A.E.S. M.B.G. K.E.H. S.T.C. and D.R.V. are inventors on patent applications submitted by the Alliance for Sustainable Energy on the use of ALD coatings to improve catalyst leaching stability (WO 2018/094145 A1, US 2017/62157, filed November 17, 2017) and thermal stability (U.S. provisional patent application No. 62/720,444, filed August 21, 2018). R.W.T. R.S. and A.A.D. are employees and shareholders of Forge Nano Inc. an ALD-enabled materials manufacturing company that provided samples prepared by fluidized bed ALD. M.J.W. is an employee of Johnson Matthey. This work was authored in part by the Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under contract no. DE-AC36-08GO28308 . Funding was provided in part by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office . This work was partially performed in collaboration with the Chemical Catalysis for Bioenergy Consortium (ChemCatBio), a member of the Energy Materials Network, and was supported by the DOE Bioenergy Technologies Office under contract no. DE-AC05-00OR22725 with Oak Ridge National Laboratory and contract no. DE-AC36-08-GO28308 with NREL . Partial support for D.R.V., M.B.G., K.E.H., and S.T.C. was provided by the Laboratory Directed Research and Development Program at NREL. APT sample preparation and analysis was conducted using facilities at the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory. We thank George Burton for help with STEM imaging at Colorado School of Mines, Nick Grundl and Mary Biddy from NREL for the Aspen and Excel modeling used for this study, and Davinia Salvachúa from NREL for the biological production of the muconic acid. In addition, we would like to thank M.J.W. from Johnson Matthey for his advising on ALD catalyst development and process integration for commercial applications. Lastly, D.R.V. and G.T.B. thank the Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, award number DE-SC0000997 , for their partial support.

Keywords

  • biochemicals
  • catalyst deactivation
  • catalyst leaching
  • catalyst lifetime
  • muconic acid
  • structure-stability relationship
  • thermal stability

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