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Improved Ammonia Synthesis and Energy Output from Zinc-Nitrate Batteries by Spin-State Regulation in Perovskite Oxides

Guo, Hele et al. · Zenodo (CERN)
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Skip to main Communities My dashboard Log in Sign up Published April 20, 2026 | Version v1 Publication Open Improved Ammonia Synthesis and Energy Output from Zinc-Nitrate Batteries by Spin-State Regulation in Perovskite Oxides Authors/Creators Guo, Hele Zhou, Yazhou Chu, Kaibin Cao, Xueying Qin, Jingjing Zhang, Nan Roeffaers, Maarten B. J. Zboril, Radek Hofkens, Johan Muellen, Klaus et al. Show all 12 authors Authors/Creators 12 / 12 Guo, Hele Zhou, Yazhou Chu, Kaibin Cao, Xueying Qin, Jingjing Zhang, Nan Roeffaers, Maarten B. J. Zboril, Radek Hofkens, Johan Muellen, Klaus Lai, Feili Liu, Tianxi Close 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‑δ (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 μmol 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 μmol 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. Files improved-ammonia-synthesis-and-energy-output-from-zinc-nitrate-batteries-by-spin-state-regulation-in-perovskite-oxides.pdf Files (9.7 MB) Name Size Download all improved-ammonia-synthesis-and-energy-output-from-zinc-nitrate-batteries-by-spin-state-regulation-in-perovskite-oxides.pdf md5:f54a3758d67fbd2f78f0aa0757024920 9.7 MB Preview Download Additional details Dates Accepted 2025-01-16 28 Views 23 Downloads Show more details All versions This version Views Total views 28 28 Downloads Total downloads 23 23 Data volume Total data volume 262.3 MB 262.3 MB More info on how stats are collected.... Versions External resources Indexed in OpenAIRE Communities Details DOI DOI Badge DOI 10.5281/zenodo.19662550 Markdown [![DOI](https://zenodo.org/badge/DOI/10.5281/zenodo.19662550.svg)](https://doi.org/10.5281/zenodo.19662550) reStructuredText .. image:: https://zenodo.org/badge/DOI/10.5281/zenodo.19662550.svg :target: https://doi.org/10.5281/zenodo.19662550 HTML <a href="https://doi.org/10.5281/zenodo.19662550"><img src="https://zenodo.org/badge/DOI/10.5281/zenodo.19662550.svg" alt="DOI"></a> Image URL https://zenodo.org/badge/DOI/10.5281/zenodo.19662550.svg Target URL https://doi.org/10.5281/zenodo.19662550 Resource type Publication Publisher Zenodo Rights License Creative Commons Attribution 4.0 International The Creative Commons Attribution license allows re-distribution and re-use of a licensed work on the condition that the creator is appropriately credited. Read more Citation Export Technical metadata Created April 20, 2026 Modified April 20, 2026 Jump up About About Policies Infrastructure Principles Projects Roadmap Contact Blog Blog Support Help FAQ Developers REST API OAI-PMH Contribute GitHub Donate Funded by Powered by CERN Data Centre & InvenioRDM Status Privacy policy Cookie policy Terms of Use This site uses cookies. Find out more on how we use cookies Accept all cookies Accept only essential cookies

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