Enhancing the catalytic properties of a biochar-supported copper oxide in nitric oxide selective reduction with hydrogen

IF 16.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Ibrahim Yakub, Khairul Anwar Mohamad Said, Rubiyah Baini, Mohamed Afizal Mohamed Amin
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Abstract

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.

Abstract Image

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
在生物炭上支撑的氧化铜可能存在氮选择性低和碳燃烧的问题,尽管它在替代使用不可再生材料作为催化剂支撑以减少一氧化氮方面具有可持续发展的前景。双金属催化是提高催化性能(包括转化率和选择性)的一种手段。因此,本研究通过将铁或锰与铜共同浸渍,研究如何提高碳支撑铜氧化物在使用氢气进行一氧化氮选择性还原时的性能。双金属催化剂是通过序贯萌发湿润法制备的,即在浸渍和煅烧助催化剂之前先浸渍和煅烧氧化铜。铁与铜配对后,氮的选择性在 200 °C 时提高了 20%(几乎 100%),而在更高温度(300 °C )下,碳的燃烧率降低了 20%。这种改善被视为双金属氧化物催化剂的协同效应,是元素组成(从 60% 碳含量到 50% )、催化剂酸度(从 12 毫摩尔 NH3 脱附/克到 16 毫摩尔 NH3d/克)和氧化还原特性(从 5 毫摩尔 H2 消耗/克到 3 毫摩尔 H2/克)发生变化的结果。闪烁元素分析仪显示,这种催化剂的碳含量较低,但氧含量较高(30%,而不是 19%),这与较高的酸性位点有关,温度编程解吸分析和傅立叶变换红外光谱也证实了这一点。改变两种催化剂的比例可以发现,不同的反应机制可能是理解氮选择性增强的关键。不过,要确保该催化系统在工业中的适用性,还需要进一步的研究。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Accounts of Chemical Research
Accounts of Chemical Research 化学-化学综合
CiteScore
31.40
自引率
1.10%
发文量
312
审稿时长
2 months
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.
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