High-throughput Compositional Screening of PdxTi1-xHy and PdxNb1-xHy Hydrides for CO2 Reduction
© 2023 Wiley‐VCH GmbH..
Electrochemical experiments and theoretical calculations have shown that Pd-based metal hydrides can perform well for the CO2 reduction reaction (CO2RR). Our previous work on doped-PdH showed that doping Ti and Nb into PdH can improve the CO2RR activity, suggesting that the Pd alloy hydrides with better performance are likely to be found in the PdxTi1-xHy and PdxNb1-xHy phase space. However, the vast compositional and structural space with different alloy hydride compositions and surface adsorbates, makes it intractable to screen out the stable and active PdxM1-xHy catalysts using density functional theory calculations. Herein, an active learning cluster expansion (ALCE) surrogate model equipped with Monte Carlo simulated annealing (MCSA), a CO* binding energy filter and a kinetic model are used to identify promising PdxTi1-xHy and PdxNb1-xHy catalysts with high stability and superior activity. Using our approach, we identify 24 stable and active candidates of PdxTi1-xHy and 5 active candidates of PdxNb1-xHy. Among these candidates, the Pd0.23Ti0.77H, Pd0.19Ti0.81H0.94, and Pd0.17Nb0.83H0.25 are predicted to display current densities of approximately 5.1, 5.1 and 4.6 μA cm-2 at -0.5 V overpotential, respectively, which are significantly higher than that of PdH at 3.7 μA cm-2.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2024 |
|---|---|
| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:17 |
|---|---|
| Enthalten in: |
ChemSusChem - 17(2024), 6 vom: 22. März, Seite e202301277 |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Ai, Changzhi [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
Active learning |
|---|
| Anmerkungen: |
Date Revised 23.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
|---|
| doi: |
10.1002/cssc.202301277 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM364573902 |
|---|
| LEADER | 01000caa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM364573902 | ||
| 003 | DE-627 | ||
| 005 | 20240324234850.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 231226s2024 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1002/cssc.202301277 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n1344.xml |
| 035 | |a (DE-627)NLM364573902 | ||
| 035 | |a (NLM)37965780 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Ai, Changzhi |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a High-throughput Compositional Screening of PdxTi1-xHy and PdxNb1-xHy Hydrides for CO2 Reduction |
| 264 | 1 | |c 2024 | |
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a ƒaComputermedien |b c |2 rdamedia | ||
| 338 | |a ƒa Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Date Revised 23.03.2024 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a © 2023 Wiley‐VCH GmbH. | ||
| 520 | |a Electrochemical experiments and theoretical calculations have shown that Pd-based metal hydrides can perform well for the CO2 reduction reaction (CO2RR). Our previous work on doped-PdH showed that doping Ti and Nb into PdH can improve the CO2RR activity, suggesting that the Pd alloy hydrides with better performance are likely to be found in the PdxTi1-xHy and PdxNb1-xHy phase space. However, the vast compositional and structural space with different alloy hydride compositions and surface adsorbates, makes it intractable to screen out the stable and active PdxM1-xHy catalysts using density functional theory calculations. Herein, an active learning cluster expansion (ALCE) surrogate model equipped with Monte Carlo simulated annealing (MCSA), a CO* binding energy filter and a kinetic model are used to identify promising PdxTi1-xHy and PdxNb1-xHy catalysts with high stability and superior activity. Using our approach, we identify 24 stable and active candidates of PdxTi1-xHy and 5 active candidates of PdxNb1-xHy. Among these candidates, the Pd0.23Ti0.77H, Pd0.19Ti0.81H0.94, and Pd0.17Nb0.83H0.25 are predicted to display current densities of approximately 5.1, 5.1 and 4.6 μA cm-2 at -0.5 V overpotential, respectively, which are significantly higher than that of PdH at 3.7 μA cm-2 | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a CO2 reduction | |
| 650 | 4 | |a PdxM1-xHy | |
| 650 | 4 | |a active learning | |
| 650 | 4 | |a cluster expansion | |
| 650 | 4 | |a complex hydrides | |
| 650 | 4 | |a high-throughput screening | |
| 650 | 4 | |a kinetic activity | |
| 650 | 4 | |a selectivity | |
| 700 | 1 | |a Chang, Jin Hyun |e verfasserin |4 aut | |
| 700 | 1 | |a Tygesen, Alexander Sougaard |e verfasserin |4 aut | |
| 700 | 1 | |a Vegge, Tejs |e verfasserin |4 aut | |
| 700 | 1 | |a Hansen, Heine Anton |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t ChemSusChem |d 2008 |g 17(2024), 6 vom: 22. März, Seite e202301277 |w (DE-627)NLM180697102 |x 1864-564X |7 nnns |
| 773 | 1 | 8 | |g volume:17 |g year:2024 |g number:6 |g day:22 |g month:03 |g pages:e202301277 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1002/cssc.202301277 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |d 17 |j 2024 |e 6 |b 22 |c 03 |h e202301277 | ||