Functional Group-Dependent Proton Conductivity of Phosphoric Acid-Doped Ion-Pair Coordinated Polymer Electrolytes : A Molecular Dynamics Study
Toward deployment of high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) in our daily lives, multiple research efforts have been dedicated to develop high-performance phosphate-doped polymer electrolytes. Recently, ion-pair coordinated polymers have garnered attention for their high stability and proton conductivity. However, a comprehensive understanding of how proton transport properties are modified by the functional groups present in these polymers is still lacking. In this study, we employ molecular dynamics (MD) simulations to investigate the impact of different functional group types and conversion ratios on conductivity. We find that Grotthuss-type hopping transport predominantly governs the overall conductivity, surpassing vehicular transport by factors of 100-1000. As conductivity scales with proton concentration, we observe that less-bulky functional groups offer advantages by minimizing the volume expansion associated with increased conversion ratios. Additionally, we show that a strong ion-pair interaction between the cationic functional group and the phosphate anion disrupts the suitable intermolecular orientations required for efficient proton hopping between phosphate and phosphoric acid molecules, thereby diminishing the proton conductivity. Our study underscores the importance of optimizing the strength of ion-pair interactions to balance stability and proton conductivity, thus paving the way for the development of ion-pair coordinated polymer electrolytes with improved performance.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2023 |
|---|---|
| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:127 |
|---|---|
| Enthalten in: |
The journal of physical chemistry. B - 127(2023), 41 vom: 19. Okt., Seite 8993-8999 |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Lee, Hyeonju [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
|---|
| Anmerkungen: |
Date Revised 20.10.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
|---|
| doi: |
10.1021/acs.jpcb.3c05690 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM362869073 |
|---|
| LEADER | 01000naa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM362869073 | ||
| 003 | DE-627 | ||
| 005 | 20231226092136.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 231226s2023 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1021/acs.jpcb.3c05690 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n1209.xml |
| 035 | |a (DE-627)NLM362869073 | ||
| 035 | |a (NLM)37793186 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Lee, Hyeonju |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Functional Group-Dependent Proton Conductivity of Phosphoric Acid-Doped Ion-Pair Coordinated Polymer Electrolytes |b A Molecular Dynamics Study |
| 264 | 1 | |c 2023 | |
| 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 20.10.2023 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Toward deployment of high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) in our daily lives, multiple research efforts have been dedicated to develop high-performance phosphate-doped polymer electrolytes. Recently, ion-pair coordinated polymers have garnered attention for their high stability and proton conductivity. However, a comprehensive understanding of how proton transport properties are modified by the functional groups present in these polymers is still lacking. In this study, we employ molecular dynamics (MD) simulations to investigate the impact of different functional group types and conversion ratios on conductivity. We find that Grotthuss-type hopping transport predominantly governs the overall conductivity, surpassing vehicular transport by factors of 100-1000. As conductivity scales with proton concentration, we observe that less-bulky functional groups offer advantages by minimizing the volume expansion associated with increased conversion ratios. Additionally, we show that a strong ion-pair interaction between the cationic functional group and the phosphate anion disrupts the suitable intermolecular orientations required for efficient proton hopping between phosphate and phosphoric acid molecules, thereby diminishing the proton conductivity. Our study underscores the importance of optimizing the strength of ion-pair interactions to balance stability and proton conductivity, thus paving the way for the development of ion-pair coordinated polymer electrolytes with improved performance | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Goddard, William A |c 3rd |e verfasserin |4 aut | |
| 700 | 1 | |a Cha, JinHyeok |e verfasserin |4 aut | |
| 700 | 1 | |a Choi, Won Jae |e verfasserin |4 aut | |
| 700 | 1 | |a Noh, Seung Hyo |e verfasserin |4 aut | |
| 700 | 1 | |a Shin, Hyeyoung |e verfasserin |4 aut | |
| 700 | 1 | |a Kim, Hyungjun |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t The journal of physical chemistry. B |d 1997 |g 127(2023), 41 vom: 19. Okt., Seite 8993-8999 |w (DE-627)NLM114379831 |x 1520-5207 |7 nnns |
| 773 | 1 | 8 | |g volume:127 |g year:2023 |g number:41 |g day:19 |g month:10 |g pages:8993-8999 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1021/acs.jpcb.3c05690 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |d 127 |j 2023 |e 41 |b 19 |c 10 |h 8993-8999 | ||