Promoting CO2 Electroreduction Over Nano-Socketed Cu/Perovskite Heterostructures via A-Site-Valence-Controlled Oxygen Vacancies
© 2024 Wiley-VCH GmbH..
Despite the intriguing potential, nano-socketed Cu/perovskite heterostructures for CO2 electroreduction (CO2 RR) are still in their infancy and rational optimization of their CO2 RR properties is lacking. Here, an effective strategy is reported to promote CO2 -to-C2+ conversion over nano-socketed Cu/perovskite heterostructures by A-site-valence-controlled oxygen vacancies. For the proof-of-concept catalysts of Cu/La0.3-x Sr0.6+x TiO3-δ (x from 0 to 0.3), their oxygen vacancy concentrations increase controllably with the decreased A-site valences (or the increased x values). In flow cells, their activity and selectivity for C2+ present positive correlations with the oxygen vacancy concentrations. Among them, the Cu/Sr0.9 TiO3-δ with most oxygen vacancies shows the optimal activity and selectivity for C2+ . And relative to the Cu/La0.3 Sr0.6 TiO3-δ with minimum oxygen vacancies, the Cu/Sr0.9 TiO3-δ exhibits marked improvements (up to 2.4 folds) in activity and selectivity for C2+ . The experiments and theoretical calculations suggest that the optimized performance can be attributed to the merits provided by oxygen vacancies, including the accelerated charge transfer, enhanced adsorption/activation of reaction species, and reduced energy barrier for C─C coupling. Moreover, when explored in a membrane-electrode assembly electrolyzer, the Cu/Sr0.9 TiO3-δ catalyst shows excellent activity, selectivity (43.9%), and stability for C2 H4 at industrial current densities, being the most effective perovskite-based catalyst for CO2 -to-C2 H4 conversion.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2024 |
|---|---|
| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - year:2024 |
|---|---|
| Enthalten in: |
Small (Weinheim an der Bergstrasse, Germany) - (2024) vom: 13. März, Seite e2400615 |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Chen, Mingfa [VerfasserIn] |
|---|
| Links: |
|---|
| Themen: |
C2+ production |
|---|
| Anmerkungen: |
Date Revised 13.03.2024 published: Print-Electronic Citation Status Publisher |
|---|
| doi: |
10.1002/smll.202400615 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM369674146 |
|---|
| LEADER | 01000naa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM369674146 | ||
| 003 | DE-627 | ||
| 005 | 20240313235923.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 240313s2024 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1002/smll.202400615 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n1327.xml |
| 035 | |a (DE-627)NLM369674146 | ||
| 035 | |a (NLM)38477702 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Chen, Mingfa |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Promoting CO2 Electroreduction Over Nano-Socketed Cu/Perovskite Heterostructures via A-Site-Valence-Controlled Oxygen Vacancies |
| 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 13.03.2024 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status Publisher | ||
| 520 | |a © 2024 Wiley-VCH GmbH. | ||
| 520 | |a Despite the intriguing potential, nano-socketed Cu/perovskite heterostructures for CO2 electroreduction (CO2 RR) are still in their infancy and rational optimization of their CO2 RR properties is lacking. Here, an effective strategy is reported to promote CO2 -to-C2+ conversion over nano-socketed Cu/perovskite heterostructures by A-site-valence-controlled oxygen vacancies. For the proof-of-concept catalysts of Cu/La0.3-x Sr0.6+x TiO3-δ (x from 0 to 0.3), their oxygen vacancy concentrations increase controllably with the decreased A-site valences (or the increased x values). In flow cells, their activity and selectivity for C2+ present positive correlations with the oxygen vacancy concentrations. Among them, the Cu/Sr0.9 TiO3-δ with most oxygen vacancies shows the optimal activity and selectivity for C2+ . And relative to the Cu/La0.3 Sr0.6 TiO3-δ with minimum oxygen vacancies, the Cu/Sr0.9 TiO3-δ exhibits marked improvements (up to 2.4 folds) in activity and selectivity for C2+ . The experiments and theoretical calculations suggest that the optimized performance can be attributed to the merits provided by oxygen vacancies, including the accelerated charge transfer, enhanced adsorption/activation of reaction species, and reduced energy barrier for C─C coupling. Moreover, when explored in a membrane-electrode assembly electrolyzer, the Cu/Sr0.9 TiO3-δ catalyst shows excellent activity, selectivity (43.9%), and stability for C2 H4 at industrial current densities, being the most effective perovskite-based catalyst for CO2 -to-C2 H4 conversion | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a C2+ production | |
| 650 | 4 | |a CO2 electroreduction | |
| 650 | 4 | |a Cu/perovskite heterostructure | |
| 650 | 4 | |a Nano-socketed Cu | |
| 650 | 4 | |a Oxygen vacancy | |
| 700 | 1 | |a Xu, Yunze |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Yu |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Zhenbao |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Xueyan |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Qi |e verfasserin |4 aut | |
| 700 | 1 | |a Huang, Minghua |e verfasserin |4 aut | |
| 700 | 1 | |a Fang, Wei |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Yu |e verfasserin |4 aut | |
| 700 | 1 | |a Jiang, Heqing |e verfasserin |4 aut | |
| 700 | 1 | |a Zhu, Yongfa |e verfasserin |4 aut | |
| 700 | 1 | |a Zhu, Jiawei |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t Small (Weinheim an der Bergstrasse, Germany) |d 2005 |g (2024) vom: 13. März, Seite e2400615 |w (DE-627)NLM167400452 |x 1613-6829 |7 nnns |
| 773 | 1 | 8 | |g year:2024 |g day:13 |g month:03 |g pages:e2400615 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1002/smll.202400615 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |j 2024 |b 13 |c 03 |h e2400615 | ||