How Does Structural Disorder Impact Heterogeneous Catalysts? The Case of Ammonia Decomposition on Non-Stoichiometric Lithium Imide
Among the many catalysts suggested for ammonia decomposition, Li2NH has been shown to be quite promising. In the recent past, we have performed extensive \textit{ab-initio}-quality simulations to explain the workings of this unusual catalyst. In the complex scenario that has emerged, surface dynamics and structural disorder enhanced by the interaction with the reacting ammonia molecules played a crucial role. Non-stoichiometric lithium imide Li(2-x)(NH2)x(NH)(1-x) has been reported to have better catalytic performances than pure lithium imide. Stimulated by these findings, we follow up our first study simulating the ammonia decomposition on such non-stoichiometric compound. We attribute the enhanced reactivity to the fact that the compositional disorder further enhances the fluctuations in the topmost layers of the catalyst, strengthening our dynamical picture of this catalytic process..
| Medienart: |
|
|---|
Preprint| Erscheinungsjahr: |
2024 |
|---|---|
| Erschienen: |
2024 |
| Enthalten in: |
chemRxiv.org - (2024) vom: 11. Jan. Zur Gesamtaufnahme - year:2024 |
|---|
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Mambretti, Francesco [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
|---|
| doi: |
10.26434/chemrxiv-2023-79p32 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
XCH041493036 |
|---|
| LEADER | 01000caa a22002652 4500 | ||
|---|---|---|---|
| 001 | XCH041493036 | ||
| 003 | DE-627 | ||
| 005 | 20240112103107.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 231110s2024 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.26434/chemrxiv-2023-79p32 |2 doi | |
| 035 | |a (DE-627)XCH041493036 | ||
| 035 | |a (chemrXiv)10.26434/chemrxiv-2023-79p32 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Mambretti, Francesco |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a How Does Structural Disorder Impact Heterogeneous Catalysts? The Case of Ammonia Decomposition on Non-Stoichiometric Lithium Imide |
| 264 | 1 | |c 2024 | |
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a Computermedien |b c |2 rdamedia | ||
| 338 | |a Online-Ressource |b cr |2 rdacarrier | ||
| 520 | |a Among the many catalysts suggested for ammonia decomposition, Li2NH has been shown to be quite promising. In the recent past, we have performed extensive \textit{ab-initio}-quality simulations to explain the workings of this unusual catalyst. In the complex scenario that has emerged, surface dynamics and structural disorder enhanced by the interaction with the reacting ammonia molecules played a crucial role. Non-stoichiometric lithium imide Li(2-x)(NH2)x(NH)(1-x) has been reported to have better catalytic performances than pure lithium imide. Stimulated by these findings, we follow up our first study simulating the ammonia decomposition on such non-stoichiometric compound. We attribute the enhanced reactivity to the fact that the compositional disorder further enhances the fluctuations in the topmost layers of the catalyst, strengthening our dynamical picture of this catalytic process. | ||
| 650 | 4 | |a Chemistry |7 (dpeaa)DE-84 | |
| 650 | 4 | |a 540 |7 (dpeaa)DE-84 | |
| 700 | 1 | |a Raucci, Umberto |0 (orcid)0000-0002-8219-224X |4 aut | |
| 700 | 1 | |a Yang, Manyi |4 aut | |
| 700 | 1 | |a Parrinello, Michele |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t chemRxiv.org |g (2024) vom: 11. Jan. |
| 773 | 1 | 8 | |g year:2024 |g day:11 |g month:01 |
| 856 | 4 | 0 | |u https://doi.org/10.1021/acscatal.3c05376 |z lizenzpflichtig |3 Volltext |
| 856 | 4 | 0 | |u http://dx.doi.org/10.26434/chemrxiv-2023-79p32 |z kostenfrei |3 Volltext |
| 912 | |a GBV_XCH | ||
| 951 | |a AR | ||
| 952 | |j 2024 |b 11 |c 01 | ||