促进光催化 H2O2 生成和增强环己烷选择性氧化的 Z 型 g-C3N4-Au-MoO3-x 异质结

IF 2.1 3区 化学 Q3 CHEMISTRY, INORGANIC & NUCLEAR
Xuyang Feng , Jincheng Liu , Jia Zheng , Yijun Luo , Wei Cai , Zewei Liao , Yanxiong Fang
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引用次数: 0

摘要

合理设计具有出色电荷分离能力和强大氧化还原能力的 Z-Scheme 光催化剂,用于在温和条件下光催化生成 HO 和氧化环己烷,仍然是一个重大挑战。为了应对这一挑战,我们采用超声液相法,将原位还原的 MoO-Au 复合材料和剥离的 g-CN 纳米片结合起来,开发出了 g-CN-Au-MoO 三元复合催化剂。此外,通过改变合成程序制备了 g-CNMoO、g-CN-Au 和 Au-g-CNMoO 复合材料,旨在探索它们在生产 HO 和催化环己烷氧化方面的有效性。值得注意的是,g-CN-Au-MoO 复合材料的 HO 生成光学速率高达 723.18 µmol-,与 Au-g-CNMoO 相比提高了 11.94 倍。同时,环己烷的转化率达到 11.59%,对 KA 油(环己醇和环己酮)的选择性高达 97.43%,KA 油的生成率为 1166.86 µmol-。通过分析光电化学特性和能带结构,可以确定金介质的参与对于 g-CN-Au-MoO 中的 Z 型电子转移至关重要。Z 型异质结的加入增加了光吸收,降低了电荷重组率,并大幅提高了 -O 和 -OH 自由基的水平,从而显著提高了 HO 生成和环己烷氧化的光催化效率。这项研究为现场即时产生过氧化氢、提高光催化环己烷氧化过程的氧化效率打开了大门。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Z-Scheme g-C3N4-Au-MoO3-x heterojunction for boosted photocatalytic H2O2 production and enhanced selective oxidation of cyclohexane

Z-Scheme g-C3N4-Au-MoO3-x heterojunction for boosted photocatalytic H2O2 production and enhanced selective oxidation of cyclohexane

Rational design of Z-Scheme photocatalyst with outstanding charge separation and robust redox capabilities for photocatalytic H2O2 generation and cyclohexane oxidation under mild conditions still poses a significant hurdle. In response to this challenge, ternary g-C3N4-Au-MoO3-x composite catalyst was developed though combining in-situ reduced MoO3-x-Au composite and exfoliated g-C3N4 nanosheets using an ultrasonic liquid-phase approach. In addition, variations in the synthesis procedures led to the preparation of g-C3N4MoO3-x, g-C3N4-Au, and Au-g-C3N4MoO3-x composites, aimed at exploring their effectiveness in both H2O2 production and catalyzing cyclohexane oxidation. Notably, the g-C3N4-Au-MoO3-x composite exhibited an impressive optical rate of H2O2 generation at 723.18 µmol·L−1·h−1, achieving a 11.94-fold enhancement compared to Au-g-C3N4MoO3-x. Meanwhile, the conversion rate of cyclohexane reached 11.59 %, with a high selectivity of 97.43 % towards KA oil (cyclohexanol and cyclohexanone), and a KA oil production rate of 1166.86 µmol·L−1·g−1. Through analyzing the photoelectrochemical properties and band energy structures, it has been established that the involvement of an Au mediator was essential and vital for the Z-Scheme electron transfer in g-C3N4-Au-MoO3-x. The incorporation of a Z-scheme heterojunction has resulted in increased light absorption, reduced charge recombination rates, and a substantial elevation in the levels of ·O2 and ·OH radicals, leading to a significant enhancement in photocatalytic efficiency for both H2O2 generation and cyclohexane oxidation. This study opens the door to on-site immediate production of hydrogen peroxide to boost the oxidation efficiency in the photocatalytic cyclohexane oxidation process.

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来源期刊
Journal of Organometallic Chemistry
Journal of Organometallic Chemistry 化学-无机化学与核化学
CiteScore
4.40
自引率
8.70%
发文量
221
审稿时长
36 days
期刊介绍: The Journal of Organometallic Chemistry targets original papers dealing with theoretical aspects, structural chemistry, synthesis, physical and chemical properties (including reaction mechanisms), and practical applications of organometallic compounds. Organometallic compounds are defined as compounds that contain metal - carbon bonds. The term metal includes all alkali and alkaline earth metals, all transition metals and the lanthanides and actinides in the Periodic Table. Metalloids including the elements in Group 13 and the heavier members of the Groups 14 - 16 are also included. The term chemistry includes syntheses, characterizations and reaction chemistry of all such compounds. Research reports based on use of organometallic complexes in bioorganometallic chemistry, medicine, material sciences, homogeneous catalysis and energy conversion are also welcome. The scope of the journal has been enlarged to encompass important research on organometallic complexes in bioorganometallic chemistry and material sciences, and of heavier main group elements in organometallic chemistry. The journal also publishes review articles, short communications and notes.
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