Journal
CHEMICAL SCIENCE
Volume 12, Issue 13, Pages 4931-4939Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc05647b
Keywords
-
Categories
Ask authors/readers for more resources
By introducing a chemically consistent graph architecture and iterative cost-solving procedure, we have overcome the limitations of current reaction networks, enabling the identification of low-cost pathways in massive reaction networks. Using this approach, we constructed the first electrochemical reaction network and investigated the formation of a key component, lithium ethylene dicarbonate, revealing both previously proposed mechanisms and novel pathways with counter-intuitive reactions that have not been reported in the literature. Our framework and data-driven methodology are envisioned to facilitate efforts in controlling reactivity and engineering properties of complex chemical processes, such as the solid electrolyte interphase in lithium-ion batteries.
Modeling reactivity with chemical reaction networks could yield fundamental mechanistic understanding that would expedite the development of processes and technologies for energy storage, medicine, catalysis, and more. Thus far, reaction networks have been limited in size by chemically inconsistent graph representations of multi-reactant reactions (e.g. A + B -> C) that cannot enforce stoichiometric constraints, precluding the use of optimized shortest-path algorithms. Here, we report a chemically consistent graph architecture that overcomes these limitations using a novel multi-reactant representation and iterative cost-solving procedure. Our approach enables the identification of all low-cost pathways to desired products in massive reaction networks containing reactions of any stoichiometry, allowing for the investigation of vastly more complex systems than previously possible. Leveraging our architecture, we construct the first ever electrochemical reaction network from first-principles thermodynamic calculations to describe the formation of the Li-ion solid electrolyte interphase (SEI), which is critical for passivation of the negative electrode. Using this network comprised of nearly 6000 species and 4.5 million reactions, we interrogate the formation of a key SEI component, lithium ethylene dicarbonate. We automatically identify previously proposed mechanisms as well as multiple novel pathways containing counter-intuitive reactions that have not, to our knowledge, been reported in the literature. We envision that our framework and data-driven methodology will facilitate efforts to engineer the composition-related properties of the SEI - or of any complex chemical process - through selective control of reactivity.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available