A New Strategy for the Synthesis of Highly Active Catalysts Based on g-C3N4 for Photocatalytic Production of Hydrogen under Visible Light

IF 1.1 4区化学 Q4 CHEMISTRY, PHYSICAL Doklady Physical Chemistry Pub Date : 2024-02-28 DOI:10.1134/s0012501623700112

K. O. Potapenko, S. V. Cherepanova, E. A. Kozlova

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Abstract

Materials based on graphite-like carbon nitride g‑C₃N₄ were synthesized by heat treatment of a mixture of melamine and urea, and the effect of synthesis conditions on the photocatalytic activity of the samples was studied at various melamine : urea ratios. Platinum (1 wt %) was deposited on the surface of the synthesized g‑C₃N₄ samples as a cocatalyst. The produced photocatalysts were characterized by X-ray powder diffraction analysis, diffuse reflectance UV-Vis spectroscopy, and low-temperature nitrogen adsorption. Photocatalytic activity was determined in the reaction of hydrogen evolution from an aqueous solution of triethanolamine (10 vol %) upon irradiation with visible light (λ = 425 nm). Optimal conditions for the synthesis of the photocatalyst 1% Pt/g-C₃N₄ were found, which was obtained by calcination of a mixture of melamine and urea (1 : 3) and ensured an H₂ evolution rate of 5.0 mmol g^–1 h^–1 at an apparent quantum efficiency of 2.5%. The developed synthetic approach produces highly active catalysts because, during the synthesis, an intermediate supramolecular complex melamine–cyanuric acid is formed, which, upon further heating, is converted into g-C₃N₄ characterized by a high specific surface area exceeding 100 m² g^–1.

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基于 g-C3N4 的高活性催化剂的合成新策略，用于在可见光下光催化制氢

摘要通过对三聚氰胺和尿素的混合物进行热处理，合成了基于类石墨氮化碳 g-C3N4 的材料，并研究了不同三聚氰胺和尿素比例下合成条件对样品光催化活性的影响。铂（1 wt %）作为共催化剂沉积在合成的 g-C3N4 样品表面。通过 X 射线粉末衍射分析、漫反射紫外可见光谱和低温氮吸附对所制备的光催化剂进行了表征。在用可见光（λ = 425 nm）照射三乙醇胺（10 vol %）水溶液时，测定了其在氢进化反应中的光催化活性。通过煅烧三聚氰胺和尿素（1:3）的混合物，找到了合成 1%Pt/g-C3N4光催化剂的最佳条件，并确保了 5.0 mmol g-1 h-1 的氢气进化速率和 2.5% 的表观量子效率。所开发的合成方法能产生高活性催化剂，因为在合成过程中会形成三聚氰胺-氰尿酸超分子中间复合物，进一步加热后，该复合物会转化为 g-C3N4，其特点是具有超过 100 平方米 g-1 的高比表面积。

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来源期刊

Doklady Physical Chemistry 化学-物理化学

CiteScore

1.50

自引率

0.00%

发文量

审稿时长

6-12 weeks

期刊介绍： Doklady Physical Chemistry is a monthly journal containing English translations of current Russian research in physical chemistry from the Physical Chemistry sections of the Doklady Akademii Nauk (Proceedings of the Russian Academy of Sciences). The journal publishes the most significant new research in physical chemistry being done in Russia, thus ensuring its scientific priority. Doklady Physical Chemistry presents short preliminary accounts of the application of the state-of-the-art physical chemistry ideas and methods to the study of organic and inorganic compounds and macromolecules; polymeric, inorganic and composite materials as well as corresponding processes. The journal is intended for scientists in all fields of chemistry and in interdisciplinary sciences.