Cross Cutting Computation: panel members

1. Cross Cutting Computation: panel members Brian Anderson Paulette Clancy* Michael Deem Laura Gagliardi Maciej Haranczyk Rajamani Krishna Berend Smit* * Panel co-lead 1

2. Cross Cutting Computation:technology challenges Conceiving a material that can be synthesized from CO2 at such a low energy cost and such a high stability that it can be disposed and/or capture CO2. Establishing theoretical limits for proposed capture materials The lack of experimental data is a bottleneck for the design of capture processes There is a need for capture processes that can be tailor-made to the availability of “low grade” energy sources 2

3. Cross Cutting Computation:current status From a scientific point of view CO2 has not been seen as an interesting molecule. Consequently there is a lack of basic computational knowledge on CO2-material interactions Computational methods for amorphous materials lag behind those of crystalline materials, since the detailed molecular structures are unknown No reliable means to go from electrons to processes (simulations across length and time scales) 3

4. Cross Cutting Computation:basic-science challenges, opportunities, and needs Use two to three slides to summarize the basic-science challenges, opportunities, and research needs associated with the focus of your panel. 4

5. Cross-Cutting Computation:PRD 1: Fundamental gas–material interactions Scientific challenges Summary of research direction • Develop classical potentials to enable the scale-up of molecular simulations informed by quantum calculations and experiment • Quantitative predictions of dispersive interactions and charge distributions in capture materials • Use appropriate quantum calculations in situations where this level of theory is essential, including situations involving reactive interactions • The availability of accurate force fields is key to the success of molecular simulations to predict the thermodynamic and transport properties of materials. Accurate potentials are not always readily available for materials of interest and mixtures, even for relatively simple gases. • This requires a better understanding of the interactions gas, e.g. CO2, CH4, N2, O2, H2O, etc. with complex materials, e.g. ionic liquids, polymers, MOFs, etc. Potential scientific impact Potential impact on Carbon Capture • Intermolecular interactions are the fundamental building blocks of molecular simulation. Their availability would be an enormous asset to the scientific community in general. • The availability of thermodynamic and transport properties could be of immediate benefit to process designers • For known capture materials these interactions could be available in 5-10 years

6. Cross-Cutting Computation:PRD 2: Building molecular models of materials with complex molecular structures Scientific challenges Summary of research direction • Integrated experimental/computational methods to build models of non-crystalline materials • Enable the prediction of structural property changes, including instances where prompted by the presence of CO2 • The inclusion of processing conditions and their effects on material structure and properties • Provide links to multiscale models • Rational approach to materials selection • A better understanding of polymer membranes is needed at the molecular level. Differences in process conditions may contribute to macromolecular structure differences and inhomogeneities • Developing a rational approach for selecting composites or mixed-matrix materials and optimization of the performance Potential scientific impact Potential impact on Carbon Capture • Applications of complex molecular structure models will go well beyond the carbon capture community – e.g. polymers and semiconductors, including solar applications • Better materials would lead to improved permeability/permeance and selectivity for membrane separations • Models of composite materials such as nanotube composites • Models could be available in 5-10 years, but widespread industrial deployment would be 20+ years 6

7. Cross-Cutting Computation:PRD 3: Multiscale modeling techniques Scientific challenges Summary of research direction • Connecting atomistic and continuum scales • Mixed gas adsorption and diffusion predictions • Mesoscale modeling of defects • Coarse-graining complex topologies • All-atom and coarse grained models for systems with complex geometries • Grain boundaries, crystallites, and defects affect the transport properties • Equilibrium and non-equilibrium states of materials • Guest-induced structural transformations • Bridging phenomena at hierarchy of scales Potential scientific impact Potential impact on Carbon Capture • Results will have impact on the way we model diffusion and adsorption in diverse areas in the chemical industries • Optimization of process • Reduction of the time scale for process development and commercialization 7

8. Cross-Cutting Computation:PRD 4: Understanding and predicting diffusion Scientific challenges Summary of research direction • Reconciling large discrepancies between different types of experiments by development of theories • Improved molecular insights into mechanisms for facilitated transport • Modeling of transport of molecules across interfaces, and within bulk • Rigorous analysis of diffusion in crystalline materials and ionic liquids • Description of surface resistances • Predictive models for facilitated transport Potential scientific impact Potential impact on Carbon Capture • Dissemination of results will spur advances in related areas of catalysis and separations • Enabling novel process discovery with revolutionary new tools for process design and simulation 8

9. Cross Cutting Computation:PRD 5: Development of material screening methods Scientific challenges Summary of research direction •Describe the space of all possible materials in a principled way E.g. What are all the possible metal organic frameworks with a certain chemical composition •Can we define the Hamiltonian that allows us to search the space of materials that fit this chemical constraint •Screen these materials for determining the best for a given applications based on the properties desired based on your design constraints E.g. Screening for O2 or CO2 separation •What are the limits to achievable property ranges? •Database of potential materials •Develop methods to screen the database • Data mining to find additional information or correlations in data • Develop methods to help guide the synthesis of these materials, e.g. structure directing agents, nucleation, self-assembly Potential scientific impact Potential impact on Carbon Capture • The zero cost capture toolkit • Can we engineer a material that will provide additional, more near the optimal, options for heat integration in the power plant? Can we tailor make materials that use these sources of energies as switching mode at exactly the desired conditions • Theory of unconventional switching • Traditional separations involve pressure or temperature swing operations. Interesting new options include alternative switching mechanisms that need to be included in the various description of the models. This includes the molecular and the system thermodynamic level. • Establish the theoretical limits for materials • A theory of chemical composition space • A theory of composition/function relationship • Theories are more general than O2 and CO2 applications 9

10. Cross Cutting Computation:PRD 6: Inverse design to predict novel materials Scientific challenges Summary of research direction • • Using desired properties to design materials in silico • Can we conceive a novel form of (CO)x (e.g. graphite oxide) which for a modest energy penalty converts CO2 in a disposable material that does not need paradisium • Can we bottle (ad/absorb or contain) CO2 using a small fraction of the fuel source or CO2 itself • Inverse design: An alternative to database first and screen second paradigm • QM methods for searching space of potential structures, with constraint on desired thermodynamics • Quantify energetic costs for creation of structure • Quantification of possibility for a polymeric CO to encapsulate CO2 (timescale of encapsulation) • Quantify energy costs Potential scientific impact Potential impact on Carbon Capture • Novel materials for CO2 separation • Novel solid state material for encapsulation of CO2 – alternative to classical CO2 capture • Critical mass of people on application • New materials for CO2 separation • New forms of polymeric CO2 • New encapsulation strategies (e.g. honeycomb CO2) • Inverse design as a viable paradigm 10

11. Grand Challenges Discovery and Use-Inspired Basic Research How nature worksMaterials properties and functionalities by design Applied Research Technology Maturation & Deployment How Nature Works … to … Materials and Processes by Design to … Technologies for the 21st Century • Controlling materials processes at the level of quantum behavior of electrons • Atom- and energy-efficient syntheses of new forms of matter with tailored properties • Emergent properties from complex correlations of atomic and electronic constituents • Man-made nanoscale objects with capabilities rivaling those of living things • Controlling matter very far away from equilibrium • Inverse Design • Basic research for fundamental new understanding on materials or systems that may revolutionize or transform today’s energy technologies • Development of new tools, techniques, and facilities, including those for the scattering sciences and for advanced modeling and computation • Basic research, often with the goal of addressing showstoppers on real-world applications in the energy technologies • Research with the goal of meeting technical milestones, with emphasis on the development, performance, cost reduction, and durability of materials and components or on efficient processes • Proof of technology concepts • Scale-up research • At-scale demonstration • Cost reduction • Prototyping • Manufacturing R&D • Deployment support Bridging atomistic models to processes BESAC & BES Basic Research Needs Workshops DOE Technology Office/Industry Roadmaps BESAC Grand Challenges Report Basic Energy Sciences Goal: new knowledge / understanding Mandate: open-ended Focus: phenomena Metric: knowledge generation DOE Technology Offices: EERE, NE, FE, EM, RW… Goal: practical targets Mandate: restricted to target Focus: performance Metric: milestone achievement