A chemically consistent graph architecture for massive reaction networks applied to solid-electrolyte interphase formation.
A chemically consistent graph architecture for massive reaction networks applied to solid-electrolyte interphase formation.
复制标题
用于大规模反应网络的化学一致的图形结构应用于固体溶解度相间的形成。
DOI：
10.1039/d0sc05647b
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发表时间：
2021-02-24
期刊：
影响因子：
8.4
通讯作者：
Persson KA
中科院分区：
文献类型：
--
作者：
Blau SM;Patel HD;Spotte-Smith EWC;Xie X;Dwaraknath S;Persson KA
用化学反应网络建模反应性可以产生基本的机理理解，这将加快储能、医药、催化等工艺和技术的发展。到目前为止，反应网络的大小受到多反应物反应（例如A + B → C）的化学不一致图形表示的限制，这些图形表示不能强制执行化学计量约束，从而排除了优化最短路径算法的使用。在这里，我们报告了一个化学一致的图形架构，克服了这些限制，使用一种新的多反应物表示和迭代成本求解程序。我们的方法能够识别包含任何化学计量反应的大规模反应网络中获得所需产物的所有低成本途径，从而能够研究比以前可能的更加复杂的系统。利用我们的架构，我们从第一性原理热力学计算构建了有史以来第一个电化学反应网络，以描述锂离子固体电解质中间相（SEI）的形成，这对负极的钝化至关重要。使用这个由近6000种物质和450万个反应组成的网络，我们询问了一个关键的SEI组分，乙烯二碳酸锂的形成。我们自动识别先前提出的机制，以及多个新的途径，含有反直觉的反应，没有，据我们所知，在文献中报道。我们设想，我们的框架和数据驱动的方法将有助于通过选择性控制反应性来设计SEI或任何复杂化学过程的组成相关特性。化学上一致的图形架构使得能够从大规模反应网络中自主识别新的固体电解质界面形成途径。
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. A chemically consistent graph architecture enables autonomous identification of novel solid-electrolyte interphase formation pathways from a massive reaction network.
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影响因子：
5.5
作者：
Rappoport, Dmitrij;Aspuru-Guzik, Alan
通讯作者：
Aspuru-Guzik, Alan
影响因子：
4.3
作者：
Jinich A;Flamholz A;Ren H;Kim SJ;Sanchez-Lengeling B;Cotton CAR;Noor E;Aspuru-Guzik A;Bar-Even A
通讯作者：
Bar-Even A
影响因子：
3.7
作者：
Goldsmith, C. Franklin;West, Richard H.
通讯作者：
West, Richard H.
影响因子：
16.6
作者：
Qian, Jiangfeng;Henderson, Wesley A.;Xu, Wu;Bhattacharya, Priyanka;Engelhard, Mark;Borodin, Oleg;Zhang, Ji-Guang
通讯作者：
Zhang, Ji-Guang
影响因子：
21.8
作者：
Isaacman-VanWertz G;Massoli P;O'Brien R;Lim C;Franklin JP;Moss JA;Hunter JF;Nowak JB;Canagaratna MR;Misztal PK;Arata C;Roscioli JR;Herndon ST;Onasch TB;Lambe AT;Jayne JT;Su L;Knopf DA;Goldstein AH;Worsnop DR;Kroll JH
通讯作者：
Kroll JH