Improved Ammonia Synthesis and Energy Output from Zinc-Nitrate Batteries by Spin-State Regulation in Perovskite Oxides
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15640%2F25%3A73629161" target="_blank" >RIV/61989592:15640/25:73629161 - isvavai.cz</a>
Alternative codes found
RIV/61989100:27640/25:10258838
Result on the web
<a href="https://pubs.acs.org/doi/10.1021/jacs.4c12240" target="_blank" >https://pubs.acs.org/doi/10.1021/jacs.4c12240</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/jacs.4c12240" target="_blank" >10.1021/jacs.4c12240</a>
Alternative languages
Result language
angličtina
Original language name
Improved Ammonia Synthesis and Energy Output from Zinc-Nitrate Batteries by Spin-State Regulation in Perovskite Oxides
Original language description
Electrocatalytic nitrate reduction to ammonia (eNRA) is a promising route toward environmental sustainability and clean energy. However, its efficiency is often limited by the slow conversion of intermediates due to spin-forbidden processes. Here, we introduce a novel A-site high-entropy strategy to develop a new perovskite oxide (La0.2Pr0.2Nd0.2Ba0.2Sr0.2)CoO3-delta (LPNBSC) for eNRA. The LPNBSC possesses a higher concentration of high-spin (HS) cobalt-active centers, resulting from an increased concentration of [CoO5] structural motifs compared to conventional LaCoO3. Consequently, this material exhibits a significantly improved electrocatalytic performance toward ammonia (NH3) production, resulting in a 3-fold increase in yield rate (129 mu mol h-1 mgcat. -1) and a 2-fold increase in Faradaic efficiency (FE, 76%) compared to LaCoO3 at the optimal potential. Furthermore, the LPNBSC-based Zn-nitrate battery reaches a maximum FE of 82% and an NH3 yield rate of 57 mu mol h-1 cm-2. Density functional theory calculations reveal that A-site high-entropy management in perovskites facilitates nitrate activation and potentially optimizes the thermodynamic rate-determining step of the eNRA process, namely, *HNO3 + H+ + e- -> *NO2 + H2O. This work presents an efficient concept for modulating the spin state of the B-site metal in perovskites and offers valuable insights for the design of high-performance eNRA catalysts.
Czech name
—
Czech description
—
Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
—
OECD FORD branch
10405 - Electrochemistry (dry cells, batteries, fuel cells, corrosion metals, electrolysis)
Result continuities
Project
—
Continuities
I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Others
Publication year
2025
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN
0002-7863
e-ISSN
1520-5126
Volume of the periodical
147
Issue of the periodical within the volume
4
Country of publishing house
US - UNITED STATES
Number of pages
10
Pages from-to
"3119–3128"
UT code for WoS article
001399163600001
EID of the result in the Scopus database
2-s2.0-85215837719