Screening methods and related catalysts, materials, compositions, methods and systems

Patent metadata

Field	Value
Publication number	US-2020168300-A1
Application number	US-201916698909-A
Country	US
Kind code	A1
Filing date	Nov 27, 2019
Priority date	Nov 27, 2018
Publication date	May 28, 2020
Grant date	—

Abstract

Provided herein are screening methods to select catalysts having a desired set of target properties from a reference catalyst, and catalysts so obtained, as well as related catalysts material, composition, methods and systems.

First claim

1 . A computer-based method for hierarchically screening for activity for a target chemical reaction under a target condition, of a plurality of candidate catalysts having structural and/or compositional difference with respect to a reference catalyst of the target chemical reaction, the method comprises
determining rate-limiting steps of the chemical reaction under the target reaction condition, by analyzing a free-energy diagram of the reference catalyst; ranking said rate-limiting steps according to their energy barrier values in a descending order to provide ranked rate-limiting steps; defining a plurality of criteria according to the ranked rate-limiting steps to estimate a change on an energy barrier value of each rate-limiting step caused by the structural and/or stoichiometric difference of each candidate catalyst with respect to the reference catalyst; for each candidate catalyst, evaluating, on a computer, each criterion of the plurality of criteria sequentially in the descending order to provide rate-selected candidate catalysts, wherein candidate catalysts having a negative change on the energy barrier value of a rate-limiting step in a criterion are evaluated in a next criterion; constructing, on a computer, a free-energy diagram for each rate selected candidate catalyst and performing a time evolution simulation method, on a computer, for each candidate catalyst to obtain a reaction rate of each selected candidate catalyst; and further selecting the rate selected candidate catalysts having a reaction rate for the target chemical reaction higher than the reaction rate of the reference catalysts under the target reaction condition to provide a rate selected active catalyst for the chemical reaction under the target condition.

2 . The method of claim 1 , wherein determining rate-limiting steps comprises identifying a plurality of reaction steps in the free energy diagram and portioning them into the rate-limiting steps.

3 . The method of claim 1 , wherein the determining further comprises identifying a minimum-barrier path connecting a reactant and a product of the chemical reaction, sectioning the path into a sequence of resting states and transition states, and identifying a set of free energy barrier values between each couple of transition and resting states.

4 . The method of claim 1 , wherein the defining a plurality of criteria further comprises associating a reaction connecting an initial state to a final state to each energy barrier and estimating the change in the energy barrier.

5 . The method of claim 4 , wherein estimating the change in the free energy barrier comprises calculating the electronic energy difference with the vibrational contributions (phonons) between the initial state and the final state of the reaction associated to each barrier.

6 . The method of claim 1 , wherein evaluating each criterion further comprises calculating the energy barrier value of each rate-limiting step for each candidate and comparing the free energy value of the candidate catalyst to the corresponding value of the reference catalyst.

7 . The method of claim 1 , further comprising providing a free energy diagram of the reference catalyst.

8 . The method of claim 1 , further comprising providing a plurality of candidate catalysts by modifying the reference catalyst to introduce the structural difference.

9 . The method of claim 1 , wherein the time evolution simulation method is kinetic Monte Carlo method.

10 . (canceled)

11 . The method of claim 1 , wherein the structural, and/or compositional difference comprises a single or multiple substitutional or interstitial dopants.

12 . (canceled)

13 . The method of claim 1 , wherein the reference catalyst is a multicomponent multilayer catalyst.

14 . (canceled)

15 . The method of claim 13 , wherein the single or multiple interstitial and/or substitutional dopant comprise substitutional dopants selected from the group consisting of Rh, Pd, Pt, Cu, Zn, Ag, Au, Cd, Ni, Co, Cr, and Si, or any combination thereof.

16 . A computer-based method for hierarchically screening activity and stability in a target chemical reaction under a target reaction condition of a plurality of candidate catalysts having structural and/or stoichiometric difference with respect to a reference catalyst of the target chemical reaction, the method comprising:
hierarchically screening the plurality of candidate catalysts for activity for the target chemical reaction under the target condition, by performing a computer-based method according to claim 1 ,
the method further comprising
testing on a computer, stability of the candidate catalysts, to select candidate catalysts having a stable configuration before the evaluating;
testing on a computer, stability of the rate selected candidate catalysts, to select rate selected candidate catalysts having a stable configuration before the constructing and/or the selecting; and/or
testing on a computer, stability of the rate-selected active catalyst, to further select rate selected active catalyst having a stable configuration,

to provide rate-selected active catalyst stable for the chemical reaction under the target condition.

17 . The method of claim 16 , wherein the catalyst is a multicomponent multilayer catalyst having three outer layers, and wherein at least one of the
testing on a computer, stability of the candidate catalysts testing on a computer, stability of the rate selected candidate catalysts testing on a computer, stability of the rate-selected active catalyst
comprises stability testing directed to select a catalyst having one or more dopant atoms predominantly located in one or more specific layer of the three outer layers of the multicomponent multilayer catalyst.

18 . A computer-based method for hierarchically screening activity and selectivity for a target chemical reaction under a target chemical reaction condition of a plurality of active catalysts having a structural and/or compositional difference with respect to a reference catalyst of the target chemical reaction, the method comprising
providing a plurality of rate-selected active catalysts for the chemical reactions under the target condition by hierarchically screening a plurality of candidate catalysts with a computer-based method according to claim 1 , each rate-selected active catalyst having a target reaction rate; for each rate-selected active catalyst, constructing, on a computer, a free-energy diagram of a second chemical reaction different from the target chemical reaction and performing a time evolution simulation method on a computer to obtain a second reaction rate of each rate-selected active catalyst; obtaining a selectivity ratio between the target reaction rate and the second reaction rate of each rate-selected active catalyst; and selecting the rate-selected active catalyst having a selectivity ratio greater than 1 to provide a rate-selected active catalyst selective for the chemical reaction under the reaction condition.

19 - 20 . (canceled)

21 . A computer-based method for hierarchically screening activity, stability and selectivity for a target chemical reaction under a target reaction condition of a plurality of active catalysts having structural and/or compositional differences with respect to a reference catalyst of the target chemical reaction, the method comprising
providing a rate-selected active catalyst selective for the target chemical reaction under the target condition by hierarchically scree

Assignees

• California Inst Of Techn
• Board Of Regents Of The Nevada System Of Higher Education On Behalf Of The Univ Of Nevada Ren

Inventors

• Goddard Iii William A
• FORTUNELLI Alessandro
• An Qi

Classifications

• G16C20/10 Primary

  Analysis or design of chemical reactions, syntheses or processes · CPC title

• G16C20/30

  Prediction of properties of chemical compounds, compositions or mixtures · CPC title

• B01J23/745

  Iron · CPC title

• G06F30/20

  Design optimisation, verification or simulation (optimisation, verification or simulation of circuit designs G06F30/30) · CPC title

• B01J23/80

  with zinc, cadmium or mercury · CPC title