A CoOxHy/β-NiOOH electrocatalyst for robust ammonia oxidation to nitrite and nitrate†

IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Green Chemistry Pub Date : 2023-09-18 DOI:10.1039/d3gc01835k
Sam Cohen , Sam Johnston , Cuong K. Nguyen , Tam D. Nguyen , Dijon A. Hoogeveen , Daniel Van Zeil , Sarbjit Giddey , Alexandr N. Simonov , Douglas R. MacFarlane
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Abstract

As the global demand for fertilisers and other nitrogenous products increases, so does the demand for robust, cost-effective and sustainable alternatives to the Ostwald process for the oxidation of ammonia to NOx compounds. Attention has turned to the electrochemical ammonia oxidation to nitrite and nitrate ([NO2/3]) – a process that could enable distributed production of these important commodity chemicals. Studies of the ammonia oxidation reaction (AOR) for the synthesis of [NO2/3] are now trending towards more selective and cheaper catalytic materials, rather than the optimisation of Pt and other known noble metal-based catalysts that are subject to poisoning and/or corrosion. Towards this goal, we describe a composite of CoOxHy and β-NiOOH on a Ni foam substrate as an electrocatalyst for the AOR that enables generation of [NO2/3] under alkaline conditions over extended periods of operation. Specifically, the average [NO2/3] yield rate of 1.5 ± 0.5 nmol s−1 cm−2 with a faradaic efficiency of 79% ± 10% is demonstrated over 4 days of continuous operation. These results represent a step forward in the development of more robust, corrosion-resistant, and industrially practical materials for the sustainable production of nitrates and nitrites.

Abstract Image

用于将氨氧化成亚硝酸盐和硝酸盐的 CoOxHy/β-NiOOH 电催化剂†
随着全球对化肥和其他含氮产品需求的增加,人们也越来越需要稳健、具有成本效益和可持续的氨氧化成氮氧化物的奥斯特瓦尔德工艺替代品。人们开始关注氨氧化成亚硝酸盐和硝酸盐([NO2/3]-)的电化学过程--该过程可实现这些重要商品化学品的分布式生产。目前,对合成 [NO2/3]- 的氨氧化反应 (AOR) 的研究趋向于选择性更强、成本更低的催化材料,而不是优化铂和其他已知的贵金属基催化剂,因为它们容易中毒和/或腐蚀。为了实现这一目标,我们在镍泡沫基底上描述了一种 CoOxHy 和 β-NiOOH 的复合材料,作为 AOR 的电催化剂,它能在碱性条件下生成 [NO2/3]-,并能长时间运行。具体来说,在连续运行 4 天后,平均[NO2/3]-产率为 1.5 ± 0.5 nmol s-1 cm-2,远红外效率为 79% ± 10%。这些结果表明,在开发更坚固耐用、耐腐蚀和工业实用的材料用于硝酸盐和亚硝酸盐的可持续生产方面,我们又向前迈进了一步。
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来源期刊
Green Chemistry
Green Chemistry 化学-化学综合
CiteScore
16.10
自引率
7.10%
发文量
677
审稿时长
1.4 months
期刊介绍: Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.
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