Sam Cohen , Sam Johnston , Cuong K. Nguyen , Tam D. Nguyen , Dijon A. Hoogeveen , Daniel Van Zeil , Sarbjit Giddey , Alexandr N. Simonov , Douglas R. MacFarlane
{"title":"用于将氨氧化成亚硝酸盐和硝酸盐的 CoOxHy/β-NiOOH 电催化剂†","authors":"Sam Cohen , Sam Johnston , Cuong K. Nguyen , Tam D. Nguyen , Dijon A. Hoogeveen , Daniel Van Zeil , Sarbjit Giddey , Alexandr N. Simonov , Douglas R. MacFarlane","doi":"10.1039/d3gc01835k","DOIUrl":null,"url":null,"abstract":"<div><p>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 NO<sub>x</sub> compounds. Attention has turned to the electrochemical ammonia oxidation to nitrite and nitrate ([NO<sub>2/3</sub>]<sup>−</sup>) – a process that could enable distributed production of these important commodity chemicals. Studies of the ammonia oxidation reaction (AOR) for the synthesis of [NO<sub>2/3</sub>]<sup>−</sup> 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 CoO<sub>x</sub>H<sub>y</sub> and β-NiOOH on a Ni foam substrate as an electrocatalyst for the AOR that enables generation of [NO<sub>2/3</sub>]<sup>−</sup> under alkaline conditions over extended periods of operation. Specifically, the average [NO<sub>2/3</sub>]<sup>−</sup> yield rate of 1.5 ± 0.5 nmol s<sup>−1</sup> cm<sup>−2</sup> 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.</p></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"25 18","pages":"Pages 7157-7165"},"PeriodicalIF":9.3000,"publicationDate":"2023-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A CoOxHy/β-NiOOH electrocatalyst for robust ammonia oxidation to nitrite and nitrate†\",\"authors\":\"Sam Cohen , Sam Johnston , Cuong K. Nguyen , Tam D. Nguyen , Dijon A. Hoogeveen , Daniel Van Zeil , Sarbjit Giddey , Alexandr N. Simonov , Douglas R. MacFarlane\",\"doi\":\"10.1039/d3gc01835k\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>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 NO<sub>x</sub> compounds. Attention has turned to the electrochemical ammonia oxidation to nitrite and nitrate ([NO<sub>2/3</sub>]<sup>−</sup>) – a process that could enable distributed production of these important commodity chemicals. Studies of the ammonia oxidation reaction (AOR) for the synthesis of [NO<sub>2/3</sub>]<sup>−</sup> 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 CoO<sub>x</sub>H<sub>y</sub> and β-NiOOH on a Ni foam substrate as an electrocatalyst for the AOR that enables generation of [NO<sub>2/3</sub>]<sup>−</sup> under alkaline conditions over extended periods of operation. Specifically, the average [NO<sub>2/3</sub>]<sup>−</sup> yield rate of 1.5 ± 0.5 nmol s<sup>−1</sup> cm<sup>−2</sup> 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.</p></div>\",\"PeriodicalId\":78,\"journal\":{\"name\":\"Green Chemistry\",\"volume\":\"25 18\",\"pages\":\"Pages 7157-7165\"},\"PeriodicalIF\":9.3000,\"publicationDate\":\"2023-09-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/org/science/article/pii/S1463926223009482\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S1463926223009482","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
A CoOxHy/β-NiOOH electrocatalyst for robust ammonia oxidation to nitrite and nitrate†
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.
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.