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具有碳空位超薄g-C3N4纳米片可见光下产过氧化氢

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光催化产过氧化氢(H2O2)作为一种绿色可持续发展技术,相比于工业上常用的蒽醌法,具有清洁无污染、安全、低能耗及低成本等优点.石墨相氮化碳(g-C3N4)作为一种无机非金属材料,是一种很有前景的产H2O2光催化剂.然而,块体g-C3N4存在光生电子空穴复合严重以及光生电荷迁移能力弱等问题,导致其光催化产H2O2效率低.为了提高g-C3N4的光催化产H2O2活性.本文通过简单的连续两步高温煅烧制备了含有碳空位的超薄g-C3N4纳米片(CNS580),通过X射线衍射仪、扫描电子显微镜、原子力显微镜、电子顺磁共振仪、紫外可见漫反射、瞬态光电流、电化学阻抗谱测试等对光催化剂进行了一系列的结构形貌、光吸收性能以及电化学性能表征.结果表明,该光催化剂具有超薄纳米片结构,厚度约为2.15nm,可提高光生电荷的传输效率;同时引入的碳空位可捕获光生电子,这将改善其光生电子空穴的分离能力.在光催化产H2O2的实验中,CNS580光催化反应6h,其产H2O2浓度可达到0.091mmol/L,是块体g-C3N4的4.13倍.此外,讨论并提出CNS580光催化产H2O2可能的机理.
Enhanced hydrogen peroxide production performance in visible light from ultra-thin g-C3N4 nanosheets with carbon vacancies
Photocatalytic production of hydrogen peroxide(H2O2),as a green and sustainable technology,has the advantages of clean and pollution-free,safety,low energy consumption and low cost compared with the anthraquinone method commonly used in industry.Graphitic phase carbon nitride(g-C3N4),as an inorganic nonmetallic material,is a promising H2O2producing photocatalyst.However,bulk g-C3N4 suffers from severe photogenerated electrons-holes complexation and weak photogenerated charge transfer ability,resulting in its low photocatalytic H2O2 production efficiency.In order to improve the photocatalytic H2O2 production activity of g-C3N4,ultrathin g-C3N4 nanosheets containing carbon vacancies(CNS580)were prepared by simple sequential two-step high-temperature calcination in this paper,and the structure and morphology,light absorption properties and electrochemical properties of photocatalysts were characterized by XRD,SEM,AFM,ESR,UV-Vis,TPC and EIS.The results showed that the photocatalyst had an ultrathin nanosheet structure with a thickness of about 2.15nm,which could improve the transmission efficiency of photogenerated charge.Meanwhile,the introduced carbon vacancies could capture photogenerated electrons,which would improve its photogenerated electrons-holes separation ability.In the experiment of photocatalytic H2O2 production,the H2O2 production concentration by CNS580 via photocatalytic reaction for 6h could reach 0.091mmol/L,which was 4.13 times higher than that of the bulk g-C3N4.In addition,the possible mechanism of photocatalytic H2O2 production for CNS580 was discussed and proposed.

graphitic phase carbon nitrideultra-thin nanosheetscarbon vacancyvisible lighthydrogen peroxide

石家汀、王辉、蒲凯凯、赵婷、聂丽君、郑娜、高宇航、薛坤坤、石建惠

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太原理工大学环境科学与工程学院,山西太原 030024

石墨相氮化碳 超薄纳米片 碳空位 可见光 过氧化氢

国家自然科学基金

52100101

2024

化工进展
中国化工学会,化学工业出版社

化工进展

CSTPCD北大核心
影响因子:1.062
ISSN:1000-6613
年,卷(期):2024.43(7)