Liu, Chaofan;
Xie, Tian;
Xue, Guohao;
Xu, Xiaobo;
Guo, Hele;
Guan, Yawen;
Wang, Tianlu;
... Lai, Feili; + view all
(2025)
Polymer-Mediated Confined Assembly of High-Entropy Perovskite Hydroxide Nanocubes for Ammonia Production and Zinc–Nitrate Battery Energy Supply.
Advanced Functional Materials
, Article e25869. 10.1002/adfm.202525869.
(In press).
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Abstract
High-entropy perovskites, with their compositional diversity and structural tunability, have recently emerged as a versatile platform for electrocatalysis. Among them, high-entropy perovskite hydroxides (HEPHs) offer abundant active sites and flexible electronic structures, yet their controllable synthesis with well-defined morphology remains a major challenge. In this study, a polymer-mediated confined assembly strategy is presented that enables the controllable synthesis of nanocubic Sn(CuMgCoZnNi)(OH)6 (HEPH-2). HEPH-2, with highly accessible active sites and a large electrochemically active surface area, delivers outstanding electrocatalytic nitrate reduction to ammonia (eNRA) performance, achieving an ammonia (NH3) yield rate of 9.28 mg h−1 mg−1cat. and a high Faradaic efficiency (FE) of 90.06% in alkaline media, significantly outperforming irregular HEPH nanoparticles (HEPH-0) synthesized without polyvinylpyrrolidone. Density functional theory (DFT) calculations reveal that Sn acts as the dominant active site with the strongest NO3− adsorption, while the hydrogenation of *NO to *NOH constitutes the rate-determining step. Meanwhile, when used as the cathode material in a zinc-nitrate battery, HEPH-2 demonstrates a high NH3 yield rate (3.70 mg h−1 cm−2) and a high FE value (94.21%). This work introduces a simple yet effective strategy for engineering well-defined perovskite hydroxides, demonstrating their potential as next-generation materials for sustainable ammonia production and energy conversion.
| Type: | Article |
|---|---|
| Title: | Polymer-Mediated Confined Assembly of High-Entropy Perovskite Hydroxide Nanocubes for Ammonia Production and Zinc–Nitrate Battery Energy Supply |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/adfm.202525869 |
| Publisher version: | https://doi.org/10.1002/adfm.202525869 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. It has been made open access under the Creative Commons (CC BY) licence under the terms of the UCL Intellectual Property (IP) Policy and UCL Publications Policy. |
| Keywords: | Ammonia production; electrocatalytic nitrate reduction; high-entropy perovskite hydroxides; polymer-mediated confined assembly; zinc-nitrate battery |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10219617 |
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