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通过溶剂-前驱体相互作用构建具有氮缺陷的石墨相氮化碳促进纯水中过氧化氢的生成:探索压电光催化中的复杂情况

Promoted Hydrogen Peroxide Production from Pure Water on g-CN with Nitrogen Defects Constructed through Solvent-Precursor Interactions: Exploring a Complex Story in Piezo-Photocatalysis.

作者信息

Minh Phan Pham Duc, Nguyen Duc-Viet, Nguyen Minh Chien, Anh Nguyen Hoai, Toan Huynh Phuoc, Ly Pho Phuong, Nguyen Ngoc Linh, Van Nguyen Tiep, Pham Minh-Thuan, Ung Thuy Dieu Thi, Bich Do Danh, Hue Pham Thu, Hue Nguyen Thi Ngoc, Dang Van-Han, Yu Woo Jong, Hur Seung Hyun, Nguyen Quang Hung, Tuyen Luu Anh, Vuong Hoai-Thanh

机构信息

Faculty of Chemical Engineering, Ho Chi Minh City University of Technology (HCMUT), 268 Ly Thuong Kiet, District 10, Ho Chi Minh City, 700000, Vietnam.

Vietnam National University Ho Chi Minh City (VNU-HCM), Linh Trung Ward, Thu Duc City, Ho Chi Minh City, 700000, Vietnam.

出版信息

Small Methods. 2025 Jan;9(1):e2400797. doi: 10.1002/smtd.202400797. Epub 2024 Jul 31.

DOI:10.1002/smtd.202400797
PMID:39082067
Abstract

Hydrogen peroxide (HO) production via oxygen (O) reduction reaction (ORR) in pure water (HO) through graphitic carbon nitrides (g-CN)-based piezo-photocatalysts is an exciting approach in many current studies. However, the low Lewis-acid properties of g-CN limited the catalytic performance because of the low O adsorption efficacy. To overcome this challenge, the interaction of g-CN precursors with various solvents are utilized to synthesize g-CN, possessing multiple nitrogen-vacant species via thermal shocking polymerization. These results suggest that the lack of nitrogen in g-CN and the incident introduction of oxygen-functional groups enhance the Lewis acid-base interactions and polarize the g-CN lattices, leading to the enormous enhancement. Furthermore, the catalytic mechanisms are thoroughly studied, with the formation of HO proceeding via radical and water oxidation pathways, in which the roles of light and ultrasound are carefully investigated. Thus, these findings not only reinforce the potential view of metal-free photocatalysts, accelerating the understanding of g-CN working principles to generate HO based on the oxygen reduction and water oxidation reactions, but also propose a facile one-step way for fabricating highly efficient and scalable photocatalysts to produce HO without using sacrificial agents, pushing the practical application of in situ solar HO toward real-world scenarios.

摘要

通过基于石墨相氮化碳(g-CN)的压电光催化剂在纯水(H₂O)中经由氧(O₂)还原反应(ORR)生成过氧化氢(H₂O₂)是当前许多研究中一种令人兴奋的方法。然而,g-CN的低路易斯酸性由于O₂吸附效率低而限制了催化性能。为了克服这一挑战,利用g-CN前驱体与各种溶剂的相互作用来合成g-CN,通过热冲击聚合拥有多个氮空位物种。这些结果表明,g-CN中氮的缺乏以及氧官能团的意外引入增强了路易斯酸碱相互作用并使g-CN晶格极化,从而导致巨大的增强。此外,对催化机制进行了深入研究,H₂O₂的形成通过自由基和水氧化途径进行,其中仔细研究了光和超声的作用。因此,这些发现不仅强化了无金属光催化剂的潜在观点,加速了对基于氧还原和水氧化反应生成H₂O₂的g-CN工作原理的理解,而且还提出了一种简便的一步法来制备高效且可扩展的光催化剂以在不使用牺牲剂的情况下生产H₂O₂,推动原位太阳能H₂O₂在实际场景中的实际应用。

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引用本文的文献

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Synthesis, Characterization, and Roles of Vacancy Defects in Polymer and Graphitized Carbon Nitride Photocatalysts: A Comprehensive Review.聚合物和石墨化氮化碳光催化剂中空位缺陷的合成、表征及作用:综述
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