Corpus ID: 237494605

Autonomous Reaction Network Exploration in Homogeneous and Heterogeneous Catalysis

  title={Autonomous Reaction Network Exploration in Homogeneous and Heterogeneous Catalysis},
  author={Miguel Steiner and Markus Reiher},
Autonomous computations that rely on automated reaction network elucidation algorithms may pave the way to make computational catalysis on a par with experimental research in the field. Several advantages of this approach are key to catalysis: (i) automation allows one to consider orders of magnitude more structures than what would be accessible by manual inspection, eventually with full resolution of structural varieties and conformations as well as with respect to the type and number of… Expand


Heuristics-Guided Exploration of Reaction Mechanisms.
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
Automatic Proposal of Multistep Reaction Mechanisms using a Graph-Driven Search.
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
Mechanism Deduction from Noisy Chemical Reaction Networks.
KiNetX, a fully automated meta-algorithm for the kinetic analysis of complex chemical reaction networks derived from semiaccurate but efficient electronic structure calculations, is introduced and AutoNetGen, a semirandomly generates chemistry-mimicking reaction networks by encoding chemical logic into their underlying graph structure is developed. Expand
Automated Generation and Analysis of the Complex Catalytic Reaction Network of Ethanol Synthesis from Syngas on Rh(111)
Reactions on the surface of catalysts are rather complex, and many possible reaction pathways and intermediates are involved. We here propose a method that is able to automatically generate aExpand
Context-Driven Exploration of Complex Chemical Reaction Networks.
  • G. Simm, M. Reiher
  • Chemistry, Medicine
  • Journal of chemical theory and computation
  • 2017
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
Automated Prediction of Catalytic Mechanism and Rate Law Using Graph-Based Reaction Path Sampling.
  • S. Habershon
  • Computer Science, Medicine
  • Journal of chemical theory and computation
  • 2016
This work confirms that the automated simulation strategy enables direct analysis of catalytic mechanisms from first principles, and finds that the reaction mechanism which emerges from these simulations is exactly that originally proposed by Heck and Breslow. Expand
Kinetic modelling of heterogeneous catalytic systems.
  • M. Stamatakis
  • Physics, Medicine
  • Journal of physics. Condensed matter : an Institute of Physics journal
  • 2015
The theory behind KMC simulation is summarized, the latest KMC computational implementations in the field are presented, and present the present challenges and future directions and opportunities in computational catalysis are discussed. Expand
Concepts, models, and methods in computational heterogeneous catalysis illustrated through CO2 conversion
This review critically describes the advances in computational heterogeneous catalysis from different viewpoints and reviews the techniques used to explore the potential energy landscape and how the information obtained can be used to bridge the gap between atomistic insight and macroscale experimental observations. Expand
Dimensionality reduction of complex reaction networks in heterogeneous catalysis: From linear‐scaling relationships to statistical learning techniques
The mechanistic analysis in heterogeneous catalysis is based on listing all elementary steps and evaluating explicitly their energies. To this end, computational models based on Density FunctionalExpand
Simultaneously improving reaction coverage and computational cost in automated reaction prediction tasks
It is shown that cost can be reduced and reaction coverage can be increased simultaneously by relatively straightforward modifications of the reaction enumeration, geometry initialization and transition state convergence algorithms that are common to many prediction methodologies. Expand