Investigation of kinetic mechanisms of photocatalytic hydrogen generation from formic aside using metal-ceramic composites under visible-light irradiation

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Processes of photocatalytic hydrogen generation from the formic acid water solution under vis-light irradiation with tantalum contained metal-ceramic silicon nitride-based composites were investigated depending on pH of the solution and hydrogen peroxide adding. These compounds were obtained by self-propagated high temperature (SHS) synthesis in the way of the ferrosilicoaluminum (FSA) and silicon-aluminum powders ignition in a nitrogen atmosphere with the tantalum addition. During the investigation it was found out that the reaction rate of the hydrogen production without hydrogen peroxide can be described within the Langmuir–Hinshelwood mechanism. There is the reaction mechanism changing simultaneously with a formic acid concentration increasing in the presence of H2O2. The most significant reaction rate of hydrogen production from HCOOH is observed with the Fe-contained composite synthesized from FSA in the solution system without H2O2 addition, the reaction turns of frequency (TOF) is 4.55 µmol/min.

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作者简介

L. Skvortsova

National Research Tomsk State University

编辑信件的主要联系方式.
Email: lnskvorcova@inbox.ru
俄罗斯联邦, Lenin Ave., 36, Tomsk, 634050

I. Artyukh

National Research Tomsk State University

Email: lnskvorcova@inbox.ru
俄罗斯联邦, Lenin Ave., 36, Tomsk, 634050

T. Tatarinova

National Research Tomsk State University

Email: lnskvorcova@inbox.ru
俄罗斯联邦, Lenin Ave., 36, Tomsk, 634050

K. Bolgaru

Tomsk Scientific Center, Siberian Branch, Russian Academy of Sciences

Email: lnskvorcova@inbox.ru
俄罗斯联邦, Akademichesky Ave., 10/4, Tomsk, 634055

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2. Fig. 1. Emission spectrum of the DIORA 30 LED lamp.

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3. Fig. 2. Fragments of diffraction patterns of nitrided samples of a mixture of powders (Si + Al + Ta, 10 wt.%) (Si3N4/Ta) and (FSA + Ta, 10 wt.%) (Si3N4/Ta/Fe): 1 – β-Si3N4, 2 – AlN, 3 – Si, 4 – TaN, 5 – TaON, 6 – TaO, 7 – α-Fe, 8 – FexSiy, 9 – Ta2O5.

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4. Fig. 3. SEM images of composites (a, b) synthesized from FSA and a mixture of silicon and aluminum powders with the addition of tantalum, and distribution maps (c, d) of Ta over the surface.

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5. Fig. 4. Dependence of the absorption coefficient on the photon energy for composites Si3N4/Ta/Fe (a), Si3N4/Ta (b).

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6. Fig. 5. Adsorption isotherms of HCOOH on composites.

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7. Fig. 6. Dependence of the rate of H2 evolution from HCOOH on the Si3N4/Ta/Fe composite on the pH of the solution.

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8. Fig. 7. Dependence of the rate of H2 evolution on composites on the initial concentration of HCOOH in the absence and with the addition of H2O2.

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9. Fig. 8. Approximation in coordinates of the Langmuir–Hinshelwood equation of experimental data under different experimental conditions: a – Si3N4/Ta; b – Si3N4/Ta/Fe; c – Si3N4/Ta/H2O2, d – Si3N4/Ta/Fe/H2O2 (С0 = 0.026–0.26 M); d – Si3N4/Ta/H2O2, e – Si3N4/Ta/Fe/H2O2 (С0 = 0.4–1.0 M).

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