Lawrence Livermore National Laboratory

Marcus Worsley


For energy-related processes, such as energy storage, catalysis, and desalination, mass transport is coupled with electrode processes. The need for fast mass transport is especially significant for flow batteries, since these systems use dilute solutions prone to forming concentration gradients, leading to efficiency losses. However, optimization of flow battery design is difficult since electrode pore size is critical, and control of pore morphology is poor.

In this project, we developed a capability enabling rapid design and production of engineered, high performance flow-through electrodes tailored for specific applications. We achieved this capability through innovations in electrode fabrication and design optimization. For electrode fabrication, we developed a light-based, 3D printing process to create hierarchical pore structures with arbitrary complexity and order-of-magnitude finer features. This fabrication technique enables the realization of electrodes based on our design optimization tool. Specifically, flow modeling and optimization were used to design the pore morphology of an electrode that effectively decouples the interdependence of mass transfer and reaction rate, i.e., surface area, on a global scale. This design allows mass transport and reaction rates to be independently optimized, resulting in significant gains for both the performance and efficiency of the flow battery.

Impact on Mission

Our work leveraged Lawrence Livermore National Laboratory's core capabilities in advanced materials and manufacturing as well as computational science and engineering. Our results directly support the energy and climate security mission focus area as they advance flow-through electrodes in energy storage and capacitive desalination.

Publications, Presentations, Etc.

Beck, V., et al. 2018. "Optimizing Nanomaterials-Based Electrodes for Electrochemical Energy Storage and Conversion." 4th International Seminar on AEROGELS-2018, Keynote, Hamburg, Germany, September 2018. LLNL-PRES-759265.

——— . 2018. "Optimally Engineered Flow-Through Electrodes Using Topology Optimization and Additive Manufacturing." Material Research Society, Boston, MA, November 2018. LLNL-ABS-752967.

——— . 2019. "Additively Manufactured Electrodes for Electrochemical Energy Storage and Conversion." ACS Spring Meeting 2019, Orlando, Florida, April 2019. LLNL-PRES-771464.

——— . 2019. "Optimally Engineered Flow-Through Electrodes Using Topology Optimization and Additive Manufacturing." Electrochemical Society Meeting, Dallas, TX, May 2019. LLNL-PRES-775408.

Chandrasekaran, S., et al. 2017. "Carbon Aerogel Evolution: Allotrope, Graphene-Inspired, and 3D-Printed Aerogels." Journal of Materials Research, 32 4166 (2017). LLNL-JRNL-735818.

——— . 2018. "Direct Ink Writing of Organic and Carbon Aerogels," Materials Horizons, 5 , 1166 (2018). LLNL-JRNL-751398.

Hensleigh, R., et al. 2018. "Additive Manufacturing of Hierarchical Three-dimensional Micro-architected Graphene Aerogels," Materials Horizons, 5, 1035 (2018). LLNL-JRNL-749080.

Liu, T., et al. 2016. "Ion Intercalation Induced Capacitance Improvement for Graphene-based Supercapacitor Electrodes." ChemNanoMat, doi: 10.1002/cnma.201600107R1. LLNL-JRNL-691106.

Qi, Z., et al. 2018. "3D-Printed, Superelastic Polypyrrole-Graphene Electrodes with Ultrahigh Areal Capacitance for Electrochemical Energy Storage." Advanced Materials Technologies 3(7): 1800053. doi: 10.1002/admt.201800053. LLNL-JRNL-744282.

Qian, F., et al. n.d. "Cross-Phase Separation of Nanowires and Nanoparticles." Issued U.S. Patent 9,975,178.

Song, Y., et al. 2018. "Three-Dimensional Carbon Architectures for Electrochemical Capacitors." Journal of Colloid and Interface Science, 509 529 (2018). LLNL-JRNL-732865.

Worsley, M. 2016. "Graphene and Related Layered Materials as Aerogels: Synthesis and Characterization." BMIC 2016, São Pedro, São Paulo, September 2016. LLNL-PRES-704104.

——— . 2017. "Printing and Optimization of Electrically Conductive Structures." Mini Workshop of CO2 Conversion to Fuels (TOTAL/Stanford/LLNL), Stanford, CA, September 2017. LLNL-PRES-739509.

——— . 2017. "The Evolution of Carbon Aerogels: Allotropes, Composites, and Graphene-Inspired." MRS Spring Meeting 2017, Phoenix, AAZ, April 2017. LLNL-PRES-729760.

Zhu, C., et al. 2016. "Supercapacitors Based on Three-Dimensional Hierarchical Graphene Aerogels with Periodic Macropores." Nano Letters, 16 3448 (2016). LLNL-JRNL-720298.

——— . 2017. "3D Printed Functional Nanomaterials for Electrochemical Energy Storage," Nano Today, 15 107 (2017). LLNL-JRNL-731179.

——— . 2017. "Colloidal Materials for 3D Printing." Annual Review of Chemical and Biomolecular Engineering, accepted (2019). LLNL-JRNL-763587.