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

IF 1.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Kinetics and Catalysis Pub Date : 2024-05-09 DOI:10.1134/S0023158423601195
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.

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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
Kinetics and Catalysis
Kinetics and Catalysis 化学-物理化学
CiteScore
2.10
自引率
27.30%
发文量
64
审稿时长
6-12 weeks
期刊介绍: Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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