Assembling graphene quantum dots on aminophenol-formaldehyde resin towards efficient artificial photocatalytic hydrogen peroxide synthesis†

IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Journal of Materials Chemistry A Pub Date : 2025-01-31 DOI:10.1039/D4TA08165J
Yuanjie Peng, Jiahong Lin, Jiewei Xiao, Xincheng Xie, Wenjie Yu, Hao Yan and Dongting Yue
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Abstract

Artificial photocatalytic hydrogen peroxide (H2O2) production via metal-free catalysts has attracted increasing attention as an alternative strategy to inorganic photocatalysts because of their affordability, high stabilities, and safety. The relatively low photocatalytic efficiency of these catalysts limits their practical application. In this work, graphene quantum dots (GQDs) were successfully loaded on aminophenol-formaldehyde polymer (APF-GQDs) through a straightforward modification method, and can catalyze the water oxidation reaction and oxygen reduction reaction for H2O2 generation. With the help of GQDs, APF-GQDs show a stronger light absorption capacity, narrower bandgap for exciton dissociation, and higher separation and transfer efficiency of photogenerated electrons than that of the pristine APF, which contributes to an excellent H2O2 synthesis (apparent quantum efficiency, 12.9% at 420 nm and solar-to-chemical conversion efficiency, 1.14%). Our photocatalytic system retains high activity (2361.8–2826.0 μmol g−1) for solar-driven H2O2 synthesis under both pure O2 and air conditions even in harsh water environments (tap water, lake water, and seawater). Thus our study offers a new pathway for designing innovative catalysts for green chemical synthesis and environmental remediation.

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在氨基酚甲醛树脂上组装石墨烯量子点用于高效的人工光催化过氧化氢合成
利用无金属催化剂制备人工光催化过氧化氢(H2O2)作为无机光催化剂的替代方案,因其经济、高稳定性和安全性而受到越来越多的关注。但这些催化剂的光催化效率相对较低,限制了它们的实际应用。本研究通过直接修饰的方法将石墨烯量子点(GQDs)负载在氨基酚-甲醛聚合物(APF-GQDs)上,可以催化水氧化反应和氧还原反应生成H2O2。在GQDs的帮助下,APF-GQDs表现出比原始APF更强的光吸收能力,激子解离带隙更窄,光电子的分离和转移效率更高,这有助于出色的H2O2合成(420 nm的表观量子效率为12.9%,太阳-化学转换效率为1.14%)。我们的光催化系统在纯O2和空气条件下,即使在恶劣的水环境(自来水、湖水和海水)下,对太阳能驱动的H2O2仍保持较高的活性(2361.8~2826.0 μmol·g-1)。因此,本研究为设计创新的绿色化学合成催化剂和环境修复提供了一条新的途径。
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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