ReactionMechanismGenerator / ReactionMechanismGenerator/RMG-database

LHM & ERM NO oxidation and the adsorption configurations of NO2* bidentate

Open
#477 2 comments 0 reactions 0 assignees View on GitHub

Nobody has claimed this yet.

Topic: Catalysis
Dominant language
Python
Stars
127
Forks
160
Avg merge
6d 2h
Merged PRs (30d)
2

Description

Inspired by this paper, NO oxidation can proceed by

  1. NO* + O* <=> NO2* Langmuir–Hinshelwood Mechanism(LHM)
  2. NOgas + O* <=> NO2* Eley–Rideal Mechanism (ERM)

This paper also proposed a more stable O,O' bidentate structure of NO2 adsorbate on the bimetallic surface that
image
We have thermo data for both structures, it can be found by searching these two adjcencyLists
image

multiplicity 2
1 O u0 p2 c0 {3,S} {5,S}
2 O u1 p2 c0 {3,S}
3 N u0 p1 c0 {1,S} {2,S} {4,S}
4 X u0 p0 c0 {3,S}
5 X u0 p0 c0 {1,S}

and

image

multiplicity 2
1 O u0 p2 c0 {3,S} {5,S}
2 O u0 p2 c0 {3,S} {4,S}
3 N u1 p1 c0 {1,S} {2,S}
4 X u0 p0 c0 {2,S}
5 X u0 p0 c0 {1,S}

Presently, we don’t have a family or library to deal with these mechanisms (both LHM and ERM). One similar template is from the Surface_Dissociation family

 *1--*2                 *1     *2                        *O--*N=O               *O     *N=O
  |            ---->    ||      |        which is         |            ---->    ||      | 
~*3~ + ~*4~~           ~*3~ + ~*4~~                     ~*3~ + ~*4~~           ~*3~ + ~*4~~

Another similar one is in the Surface_Bidentate_Dissociation family

 *1--*2              *1   +   *2                      *O--*N-O              *O   +   *N-O      
  |   |     ---->    ||       ||          and          |   |     ---->      ||       ||          
~*3~~*4~~           ~*3~~ +  ~*4~~                   ~*3~~*4~~             ~*3~~ +  ~*4~~             

while X=N-O is not a representative species in RMG and we don't have thermo data of this adsorbate
image

Maybe we can consider a template or library like this?

 *1       *2=*5          *1--*2-*5              *O       *N=*O          *O--*N-*O
 ||        |    ---->     |   |         and     ||        |    ---->     |   |
~*3~  +  ~*4~~          ~*3~~*4~~              ~*3~  +  ~*4~~          ~*3~~*4~~

One more thing to discuss is the value of sticking coefficient for reaction NO2gas + * <=> NO2* reported in table I, which is:
A= ((2.24E2 /bar)/ s)(2.483E-9 mol/cm2)sqrt(2pi46 g/mol * molar gas constant * 298 kelvin)= 1.4884E-6
Comparing the value reported in RMG is A= 0.2, which is very different.
image
I am not confident with this value and not sure if we could include this in the training reactions.

Contributor guide

No contributing guide indexed for this repository

First steps

  1. Read the whole issue, then the project's contributing guide.
  2. Comment on the issue to say you are picking it up — it saves two people doing the same work.
  3. Fork the repository and make your change on a branch.
  4. Open a pull request that references the issue number.

Research direction

Start by reviewing the Surface_Dissociation and Surface_Bidentate_Dissociation families, then inspect the two supplied adjacencyLists and their thermo data. The work is complete only when the intended LHM and ERM representations, bidentate adsorption configurations, and the proposed NO2 sticking coefficient or training-reaction treatment are explicitly decided and supported.

Written by the indexing model from the issue text.

Assessment

Domain
databases
Issue type
Feature
Difficulty
5/5
Estimated time
Over a week
Activity status
Stale
Clarity
Needs clarification
Newbie friendliness
25/100

Get new issues in your inbox

A short digest of beginner-friendly GitHub issues.