{"title":"提高生物炭支撑的氧化铜在氢气选择性还原一氧化氮过程中的催化性能","authors":"Ibrahim Yakub, Khairul Anwar Mohamad Said, Rubiyah Baini, Mohamed Afizal Mohamed Amin","doi":"10.1007/s43153-024-00453-z","DOIUrl":null,"url":null,"abstract":"<p>Copper oxide supported on a biochar could suffer from a low nitrogen-selectivity and carbon combustion, despite the sustainability prospect it provides in replacing the utilization of non-renewable materials as the catalyst support to reduce nitric oxide. Bimetallic catalysis is a means to improve catalytic properties including conversion and selectivity. Therefore, this work investigates the enhancement of carbon-supported copper oxides in nitric oxide selective reduction using hydrogen by co-impregnating iron or manganese with copper. The bimetallic catalysts were prepared via sequential incipient wetness method where copper oxide was impregnated and calcined prior to the impregnation and calcination of the co-catalyst. As iron was paired with copper, the nitrogen selectivity was enhanced by 20% (almost 100% selective) at 200 °C while reducing the carbon combustion rate by 20% at a higher temperature (300 °C). This improvement was regarded as the synergistic effects obtained by the bimetallic oxide catalysts as a result of the altered elemental composition (from 60% carbon content to 50%), catalyst acidity (from 12 mmol NH<sub>3</sub> desorbed/g to 16 mmol NH<sub>3</sub>d/g) and redox properties (from 5 mmol H<sub>2</sub> consumed/g to 3 mmol H<sub>2</sub>/g). Flash elemental analyser showed that this catalyst has lower carbon content but higher oxygen amount (30% compared to 19%) which is correlated to the higher acidic sites, as confirmed via temperature-programmed desorption analysis and Fourier-Transform infra-red spectroscopy. Varying the ratio between the two catalysts revealed that different mechanisms govern the reaction that could be the key to understanding the enhancement of the nitrogen-selectivity. Nevertheless, further studies are required to ensure the applicability of this catalytic system in the industry.</p>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":null,"pages":null},"PeriodicalIF":16.4000,"publicationDate":"2024-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing the catalytic properties of a biochar-supported copper oxide in nitric oxide selective reduction with hydrogen\",\"authors\":\"Ibrahim Yakub, Khairul Anwar Mohamad Said, Rubiyah Baini, Mohamed Afizal Mohamed Amin\",\"doi\":\"10.1007/s43153-024-00453-z\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Copper oxide supported on a biochar could suffer from a low nitrogen-selectivity and carbon combustion, despite the sustainability prospect it provides in replacing the utilization of non-renewable materials as the catalyst support to reduce nitric oxide. Bimetallic catalysis is a means to improve catalytic properties including conversion and selectivity. Therefore, this work investigates the enhancement of carbon-supported copper oxides in nitric oxide selective reduction using hydrogen by co-impregnating iron or manganese with copper. The bimetallic catalysts were prepared via sequential incipient wetness method where copper oxide was impregnated and calcined prior to the impregnation and calcination of the co-catalyst. As iron was paired with copper, the nitrogen selectivity was enhanced by 20% (almost 100% selective) at 200 °C while reducing the carbon combustion rate by 20% at a higher temperature (300 °C). This improvement was regarded as the synergistic effects obtained by the bimetallic oxide catalysts as a result of the altered elemental composition (from 60% carbon content to 50%), catalyst acidity (from 12 mmol NH<sub>3</sub> desorbed/g to 16 mmol NH<sub>3</sub>d/g) and redox properties (from 5 mmol H<sub>2</sub> consumed/g to 3 mmol H<sub>2</sub>/g). Flash elemental analyser showed that this catalyst has lower carbon content but higher oxygen amount (30% compared to 19%) which is correlated to the higher acidic sites, as confirmed via temperature-programmed desorption analysis and Fourier-Transform infra-red spectroscopy. Varying the ratio between the two catalysts revealed that different mechanisms govern the reaction that could be the key to understanding the enhancement of the nitrogen-selectivity. Nevertheless, further studies are required to ensure the applicability of this catalytic system in the industry.</p>\",\"PeriodicalId\":1,\"journal\":{\"name\":\"Accounts of Chemical Research\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":16.4000,\"publicationDate\":\"2024-03-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Accounts of Chemical Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1007/s43153-024-00453-z\",\"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":"Accounts of Chemical Research","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1007/s43153-024-00453-z","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Enhancing the catalytic properties of a biochar-supported copper oxide in nitric oxide selective reduction with hydrogen
Copper oxide supported on a biochar could suffer from a low nitrogen-selectivity and carbon combustion, despite the sustainability prospect it provides in replacing the utilization of non-renewable materials as the catalyst support to reduce nitric oxide. Bimetallic catalysis is a means to improve catalytic properties including conversion and selectivity. Therefore, this work investigates the enhancement of carbon-supported copper oxides in nitric oxide selective reduction using hydrogen by co-impregnating iron or manganese with copper. The bimetallic catalysts were prepared via sequential incipient wetness method where copper oxide was impregnated and calcined prior to the impregnation and calcination of the co-catalyst. As iron was paired with copper, the nitrogen selectivity was enhanced by 20% (almost 100% selective) at 200 °C while reducing the carbon combustion rate by 20% at a higher temperature (300 °C). This improvement was regarded as the synergistic effects obtained by the bimetallic oxide catalysts as a result of the altered elemental composition (from 60% carbon content to 50%), catalyst acidity (from 12 mmol NH3 desorbed/g to 16 mmol NH3d/g) and redox properties (from 5 mmol H2 consumed/g to 3 mmol H2/g). Flash elemental analyser showed that this catalyst has lower carbon content but higher oxygen amount (30% compared to 19%) which is correlated to the higher acidic sites, as confirmed via temperature-programmed desorption analysis and Fourier-Transform infra-red spectroscopy. Varying the ratio between the two catalysts revealed that different mechanisms govern the reaction that could be the key to understanding the enhancement of the nitrogen-selectivity. Nevertheless, further studies are required to ensure the applicability of this catalytic system in the industry.
期刊介绍:
Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance.
Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.