The Exploration of Chemical Reaction Networks.

@article{Unsleber2020TheEO,
  title={The Exploration of Chemical Reaction Networks.},
  author={Jan P. Unsleber and M. Reiher},
  journal={Annual review of physical chemistry},
  year={2020}
}
  • Jan P. Unsleber, M. Reiher
  • Published 2020
  • Chemistry, Computer Science, Medicine, Physics
  • Annual review of physical chemistry
Modern computational chemistry has reached a stage at which massive exploration into chemical reaction space with unprecedented resolution with respect to the number of potentially relevant molecular structures has become possible. Various algorithmic advances have shown that such structural screenings must and can be automated and routinely carried out. This will replace the standard approach of manually studying a selected and restricted number of molecular structures for a chemical mechanism… Expand
View on PubMed
arxiv.org
15 Citations

15 Citations

Citation Type

Citation Type

Perspective on computational reaction prediction using machine learning methods in heterogeneous catalysis.
  • Jiayan Xu, Xiao-Ming Cao, P. Hu
  • Medicine
  • Physical chemistry chemical physics : PCCP
  • 2021
TLDR
The conventional workflow of reaction prediction, including reaction network generation, ab initio thermodynamics and microkinetic modelling, and an overview of the frequently used regression models in machine learning are summarized. Expand
Organic reactivity from mechanism to machine learning
As more data are introduced in the building of models of chemical reactivity, the mechanistic component can be reduced until ‘big data’ applications are reached. These methods no longer depend on… Expand
A chemically consistent graph architecture for massive reaction networks applied to solid-electrolyte interphase formation†
TLDR
This work constructs 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. Expand
Reactants, products, and transition states of elementary chemical reactions based on quantum chemistry
TLDR
This work used automated potential energy surface exploration to generate 12,000 organic reactions involving H, C, N, and O atoms calculated at the ω B97X-D3/def2-TZVP quantum chemistry level, and extracted atom-mapped reaction SMILES, activation energies, and enthalpies of reaction. Expand
Autonomous discovery in the chemical sciences part I: Progress
TLDR
This two-part review examines how automation has contributed to different aspects of discovery in the chemical sciences and describes many case studies of discoveries accelerated by or resulting from computer assistance and automation from the domains of synthetic chemistry, drug discovery, inorganic chemistry, and materials science. Expand
Artificial Intelligence for Computer-Aided Synthesis In Flow: Analysis and Selection of Reaction Components
Computer-aided synthesis has received much attention in recent years. It is a challenging topic in itself, due to the high dimensionality of chemical and reaction space. It becomes even more… Expand
Automation of Active Space Selection for Multireference Methods via Machine Learning on Chemical Bond Dissociation.
TLDR
An automated machine learning protocol that performs an automated selection of active spaces for chemical bond dissociation calculations of main group diatomic molecules shows that a "black-box" mode is possible for facilitating and accelerating the large-scale calculations on multireference systems where single-reference methods such as KS-DFT cannot be applied. Expand
Discovering chemical reaction pathways using accelerated molecular dynamics simulations and network analysis tools – Application to oxidation induced decomposition of ethylene carbonate
Abstract We present an automated method to clarify reaction pathways for complex reactive systems. The method uses accelerated molecular dynamics to find rare events and network graph analysis tools… Expand
Self-Parametrizing System-Focused Atomistic Models.
TLDR
This work develops and combines an automatically parametrizable quantum chemically derived molecular mechanics model with machine-learned corrections under autonomous uncertainty quantification and refinement to generate an accurate, physically motivated model from a minimum energy structure and its corresponding Hessian matrix. Expand
An automated computational approach to kinetic model discrimination and parameter estimation†
  • Connor J Taylor, H. Seki, +5 authors R. Bourne
  • Medicine
  • Reaction chemistry & engineering
  • 2021
TLDR
This report shows the first chemical applications of an autonomous tool to identify the kinetic model and parameters of a process, when considering both catalytic species and various integer and non-integer orders in the model's rate laws. Expand
...
1
2
...

References

SHOWING 1-10 OF 125 REFERENCES
Parallel optimization of synthetic pathways within the network of organic chemistry.
TLDR
This communication is the first instance in which synthetic optimizations are based on the entire body of synthetic knowledge as stored in the NOC and combined with economical descriptors, and can reduce the cost of an existing synthetic company by almost 50%. Expand
Automatic Proposal of Multistep Reaction Mechanisms using a Graph-Driven Search.
TLDR
A simple random-walk algorithm that searches for the set of elementary chemical reactions that transform defined reactant structures into target products, and illustrates how atomic coordinates for each elementary reaction can be generated under the action of a graph-restraining potential, prior to further analysis by quantum chemical calculations. Expand
Heuristics-Guided Exploration of Reaction Mechanisms.
TLDR
A computational protocol is presented that constructs chemical reaction networks in a parallelized and automated manner and applies it to the Schrock dinitrogen-fixation catalyst to study alternative pathways of catalytic ammonia production. Expand
Context-Driven Exploration of Complex Chemical Reaction Networks.
  • G. Simm, M. Reiher
  • Chemistry, Medicine
  • Journal of chemical theory and computation
  • 2017
TLDR
A computational protocol is presented that constructs reaction networks in a fully automated fashion steered in an intuitive, graph-based fashion through a single graphical user interface to study different pathways of sugar formation and to rationalize its autocatalytic nature. Expand
Rewiring chemistry: algorithmic discovery and experimental validation of one-pot reactions in the network of organic chemistry.
TLDR
The extension of chemicalnetwork concepts into methods directly relevant to experimental chemistry: 1) discovery of one-pot reactions; 2) optimization of multiple reaction pathways, and 3) the detection and blocking of synthetic pathways leading to dangerous chemicals. Expand
Exploration of Reaction Pathways and Chemical Transformation Networks.
TLDR
The different algorithmic approaches for the investigation of chemical reaction networks differ in their application range, the level of completeness of the exploration, and the amount of heuristics and human intervention required. Expand
Molecular Propensity as a Driver for Explorative Reactivity Studies
TLDR
Within the real-time quantum chemistry framework, an algorithm is developed that automatically detects and flags the predisposition of a molecular system to react across different electronic states in certain nuclear configurations or with other reactants present in the reaction liquor. Expand
Sampling reactive pathways with random walks in chemical space: Applications to molecular dissociation and catalysis.
  • S. Habershon
  • Chemistry, Medicine
  • The Journal of chemical physics
  • 2015
TLDR
This work outlines a computational approach to allow automated sampling of chemical reaction pathways, including sampling of different chemical species at the reaction end-points, and provides a route to automated generation of a "roadmap" describing chemical reactivity. Expand
Methods for exploring reaction space in molecular systems
The area of reaction mechanism discovery simulation has taken considerable strides in recent years. Novel methods that make hypotheses for elementary steps and complementary means for reaction path… Expand
Studying chemical reactivity in a virtual environment.
TLDR
An analysis of modern semi-empirical methods which already today are candidates for the interactive study of chemical reactivity and implications of manual structure manipulations for their physical meaning and chemical relevance are carefully analysed in order to provide sound theoretical foundations for the interpretation of the interactive reactivity exploration. Expand
...
1
2
3
4
5
...