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富铟液态金属电极上的硝酸盐到氨的转化

Nitrate-to-Ammonia Conversion at an InSn-Enriched Liquid-Metal Electrode.

作者信息

Crawford Jessica, Yin Hanqing, Du Aijun, O'Mullane Anthony P

机构信息

School of Chemistry and Physics, Queensland University of Technology (QUT), Brisbane, QLD 4001, Australia.

Centre for Materials Science, Queensland University of Technology (QUT), Brisbane, QLD 4001, Australia.

出版信息

Angew Chem Int Ed Engl. 2022 Jun 7;61(23):e202201604. doi: 10.1002/anie.202201604. Epub 2022 Apr 5.

DOI:10.1002/anie.202201604
PMID:35322508
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9324788/
Abstract

The renewable energy driven electrochemical conversion of nitrates to ammonia is emerging as a viable route for the creation of this hydrogen carrier. However, the creation of highly efficient electrocatalysts that show prolonged stability is an ongoing challenge. Here we show that room temperature liquid metal Galinstan can be used as an efficient and stable electrocatalyst for nitrate conversion to ammonia achieving rates of up to 2335 μg h  cm with a Faradaic efficiency of 100 %. Density functional theory (DFT) calculations and experimental observation indicated the activity is due to InSn alloy enrichment within the liquid metal that occurs during the electrocatalytic reaction. This high selectivity for NH is also due to additional suppression of the competing hydrogen evolution reaction at the identified In Sn active site. This work adds to the increasing applicability of liquid metals based on Ga for clean energy technologies.

摘要

可再生能源驱动的硝酸盐电化学转化为氨正成为一种可行的途径来制造这种氢载体。然而,开发出具有长期稳定性的高效电催化剂仍是一个持续存在的挑战。在此,我们表明室温液态金属镓铟锡合金可作为一种高效且稳定的电催化剂用于将硝酸盐转化为氨,实现了高达2335 μg h⁻¹ cm⁻² 的速率,法拉第效率达100%。密度泛函理论(DFT)计算和实验观察表明,活性源于电催化反应过程中液态金属内部铟锡合金的富集。对NH₃ 的这种高选择性还归因于在确定的铟锡活性位点上对竞争性析氢反应的额外抑制。这项工作增加了基于镓的液态金属在清洁能源技术中的应用范围。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/fa9318dc3f95/ANIE-61-0-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/1e54db1222f0/ANIE-61-0-g005.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/5a7aadcd3f5b/ANIE-61-0-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/fa9318dc3f95/ANIE-61-0-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/1e54db1222f0/ANIE-61-0-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/e4082f332046/ANIE-61-0-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/89347c4c0461/ANIE-61-0-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/5a7aadcd3f5b/ANIE-61-0-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dbdd/9324788/fa9318dc3f95/ANIE-61-0-g001.jpg

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