Kinetic Mechanisms of the Photocatalytic Generation of Hydrogen from Formic Acid Using Metal–Ceramic Composites under Visible-Light Irradiation

IF 16.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
L. N. Skvortsova, I. A. Artyukh, T. V. Tatarinova, K. A. Bolgaru
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Abstract

The photocatalytic generation of hydrogen from aqueous solutions of formic acid under irradiation with visible light with the use of tantalum-containing metal–ceramic composites based on silicon nitride was investigated depending on the substrate concentration and the pH of suspension in the absence and with the addition of hydrogen peroxide. These compounds were obtained by self-propagating high temperature synthesis (SHS) using the combustion of ferrosilicon aluminum (FSA) and a mixture of silicon and aluminum powders with tantalum additives in an atmosphere of nitrogen. It was found that the dependence of the rate of photocatalytic hydrogen production on the concentration of formic acid without hydrogen peroxide was described by the Langmuir–Hinshelwood mechanism. In the presence of hydrogen peroxide, the rate of the photocatalytic process sharply increased with the concentration of formic acid. The highest rate of hydrogen evolution from formic acid was observed on an iron-containing composite synthesized from FSA without the addition of hydrogen peroxide, and it amounted to 4.55 µmol/min.

Abstract Image

Abstract Image

金属陶瓷复合材料在可见光照射下光催化甲酸制氢的动力学机制
摘要 研究了在没有过氧化氢和添加过氧化氢的情况下,利用基于氮化硅的含钽金属陶瓷复合材料,在可见光照射下从甲酸水溶液中光催化产生氢气的情况。这些化合物是通过在氮气环境下燃烧硅铁铝(FSA)和含有钽添加剂的硅铝混合物粉末,进行自蔓延高温合成(SHS)而获得的。研究发现,在没有过氧化氢的情况下,光催化产氢速率与甲酸浓度的关系可用 Langmuir-Hinshelwood 机制来描述。在有过氧化氢的情况下,光催化过程的速率随着甲酸浓度的增加而急剧增加。在不添加过氧化氢的情况下,由 FSA 合成的含铁复合材料从甲酸中演化出氢气的速率最高,达到 4.55 µmol/分钟。
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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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