Basic Research Needs for Catalysis Science Report of the Basic Energy Sciences Workshop on Basic Research Needs for Catalysis Science to Transform Energy Technologies May 8–10, 2017 Image courtesy of Argonne National Laboratory. DISCLAIMER This report was prepared as an account of a workshop sponsored by the U.S. Department of Energy. Neither the United States Government nor any agency thereof, nor any of their employees or officers, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of document authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. Copyrights to portions of this report (including graphics) are reserved by original copyright holders or their assignees, and are used by the Government’s license and by permission. Requests to use any images must be made to the provider identified in the image credits. This report is available in pdf format at https://science.energy.gov/bes/community-resources/reports/ REPORT OF THE BASIC RESEARCH NEEDS WORKSHOP FOR CATALYSIS SCIENCE Basic Research Needs for Catalysis Science TO TRANSFORM ENERGY TECHNOLOGIES Report from the U.S. Department of Energy, Office of Basic Energy Sciences Workshop May 8–10, 2017, in Gaithersburg, Maryland CHAIR: ASSOCIATE CHAIRS: Carl A. Koval, University of Colorado – Boulder Johannes Lercher, Pacific Northwest National Laboratory and Technical University of Munich Susannah L. Scott, University of California – Santa Barbara PANEL LEADS: Diversified Energy Feedstocks and Carriers Advanced Chemical Conversion Approaches Geoffrey W. Coates, Cornell University Maria Flytzani-Stephanopoulos, Tufts University Enrique Iglesia, University of California – Berkeley Daniel Resasco, University of Oklahoma Cathy L. Tway, Dow Chemical Company Novel Approaches to Energy Transformations R. Morris Bullock, Pacific Northwest Crosscutting Capabilities and Challenges: National Laboratory Synthesis, Theory, and Characterization Thomas F. Jaramillo, Stanford University Victor Batista, Yale University and SLAC National Accelerator Laboratory Karena W. Chapman, Argonne National Laboratory Sheng Dai, Oak Ridge National Laboratory PLENARY SPEAKERS: James Dumesic, University of Wisconsin Cynthia Friend, Harvard University Russ Hille, University of California – Riverside Kim Johnson, Shell International Exploration and Production Jens Nørskov, Stanford University and SLAC National Accelerator Laboratory Jim Rekoske, Honeywell UOP Reuben Sarkar, U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy BASIC ENERGY SCIENCES TEAM: Christopher Bradley Bruce Garrett Craig Henderson Raul Miranda Charles Peden Viviane Schwartz i REPORT OF THE BASIC RESEARCH NEEDS WORKSHOP FOR CATALYSIS SCIENCE SPECIAL ASSISTANCE: Administrative Katie Runkles, Basic Energy Sciences Web/Publication Staff Karen Fellner, Argonne National Laboratory Cynthia Jenks, Argonne National Laboratory Michele Nelson, Argonne National Laboratory Technical/Writing Aaron M. Appel, Pacific Northwest National Laboratory Simon Bare, SLAC National Accelerator Laboratory Bart M. Bartlett, University of Michigan Thomas Bligaard, SLAC National Accelerator Laboratory Bert D. Chandler, Trinity University Robert J. Davis, University of Virginia Vassiliki-Alexandra Glezakou, Pacific Northwest National Laboratory John Gregoire, California Institute of Technology Russ Hille, University of California – Riverside Adam S. Hock, Illinois Institute of Technology and Argonne National Laboratory John Kitchin, Carnegie Mellon University Harold H. Kung, Northwestern University Jens Nørskov, Stanford University and SLAC National Accelerator Laboratory Daniel Resasco, University of Oklahoma Roger Rousseau, Pacific Northwest National Laboratory Aaron D. Sadow, Iowa State University and Ames Laboratory Raymond E. Schaak, Pennsylvania State University Wendy J. Shaw, Pacific Northwest National Laboratory Dario J. Stacchiola, Brookhaven National Laboratory Factual Document Writers Max Delferro, Lead Technical Contact, Argonne National Laboratory Contributors Emilio Bunel, Argonne National Laboratory Adam Hock, Argonne National Laboratory John Holladay, Pacific Northwest National Laboratory Frances Houle, Lawrence Berkeley National Laboratory Cynthia Jenks, Argonne National Laboratory Ted Krause, Argonne National Laboratory Chris Marshall, Argonne National Laboratory Nathan Neale, National Renewable Energy Laboratory James Parks II, Pacific Northwest National Laboratory Aaron Sadow, Ames Laboratory Joshua Schaidle, National Renewable Energy Laboratory Jao VandeLagemaat, National Renewable Energy Laboratory Yong Wang, Pacific Northwest National Laboratory Robert Weber, Pacific Northwest National Laboratory ii REPORT OF THE BASIC RESEARCH NEEDS WORKSHOP FOR CATALYSIS SCIENCE Table of Contents Abbreviations, Acronyms, and Initialisms .............................................................................................................................v Executive Summary ...................................................................................................................................................................1 Introduction ............................................................................................................................................................................... 3 PRD 1 Design Catalysts Beyond the Binding Site .......................................................................................................... 7 PRD 2 Understand and Control the Dynamic Evolution of Catalysts ........................................................................19 PRD 3 Manipulate Reaction Networks in Complex Environments to Steer Catalytic Transformations Selectively ..................................................................................................................................31 PRD 4 Design Catalysts for Efficient Electron-driven Chemical Transformations ..................................................43 PRD 5 Drive New Catalyst Discoveries by Coupling Data Science, Theory, and Experiment .............................53 Workshop Panel Reports .......................................................................................................................................................65 Panel 1 Diversified Energy Feedstocks and Carriers ................................................................................................67 Panel 2 Novel Approaches to Energy Transformations ............................................................................................ 81 Panel 3 Advanced Chemical Conversion Approaches ............................................................................................ 95 Panel 4 Crosscutting Capabilities and Challenges: Synthesis, Theory and Characterization ....................109 Appendices .............................................................................................................................................................................137 Appendix A: Figure Sources ............................................................................................................................................... 137 Appendix B: Workshop Agenda ........................................................................................................................................143 Appendix C: Abstracts for Plenary Talks ......................................................................................................................... 147 Appendix D: Workshop Participants .................................................................................................................................149 iii REPORT OF THE BASIC RESEARCH NEEDS WORKSHOP FOR CATALYSIS SCIENCE This page intentionally left blank. iv REPORT OF THE BASIC RESEARCH NEEDS WORKSHOP FOR CATALYSIS SCIENCE Abbreviations, Acronyms, and Initialisms AFM atomic force microscopy AIMD ab initio molecular dynamics ALD atomic layer deposition ANN artificial neural networks APO apoenzyme APT atom probe tomography AP-XPS ambient pressure X-ray photoelectron spectroscopy ATP adenosine triphosphate BAS Brønsted acid site BEEF Bayesian error estimation functional BEP Brønsted-Evans-Polanyi BES Basic Energy Sciences BN boron nitride BODIPY boron-dipyrromethene BRN Basic Research Needs CAACs cyclic (alkyl)(amino)carbenes CCSD couple cluster single double CD circular dichroism CFD computational fluid dynamics CMD concerted metalation-deprotonation COF covalent organic framework CP2K density functional based massively parallel and/or linear scaling codes CPMD density functional based massively parallel and/or linear scaling codes CVD chemical vapor deposition DFT density functional theory DFT-QM/MM density functional theory quantum mechanics/molecular mechanics DME dimethyl ether DNN deep neural network DNP NMR dynamic nuclear polarization nuclear magnetic resonance DRIFTS diffuse reflectance infrared fourier transform spectroscopy ED electroless deposition EDS