利用不稳定的 S-O 官能团作为毽子废料中 N、S 掺杂碳点的氧气吸附和活性位点,高效光催化产生 H2O2

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-05-29 DOI:10.1016/j.jcat.2024.115579
Haoyuan Qin , Kaiqu Sun , Pengyu Hao , Hao Yuan , Yu Shen , Ang Bian , Yanhua Cui , Jianhua Hou , Weilong Shi , Chunsheng Li , Feng Guo
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引用次数: 0

摘要

对环保型过氧化氢(H2O2)生产的需求日益增长,这推动了对利用太阳光进行光催化合成策略的广泛研究。然而,目前的挑战在于如何在不依赖大气环境中的牺牲剂的情况下高效生产光催化剂。在本研究中,我们提出了一种利用废弃毽子废料中的二硫键合成 N、S 共掺杂碳点(N、S-CDs)的突破性方法,并展示了其在光催化产生 H2O2 方面的卓越性能(2062.4 µM g-1h-1)。N, S-CDs 中的 S-O 功能基团的意义并不仅限于结构元素,因为它不仅是氧气的关键吸附位点,还是光催化产生 H2O2 的氧气还原反应(ORR)过程中促进电子从体相转移到 N, S-CDs 表面的活性位点。此外,飞秒瞬态吸收光谱(fs-TA)表明,S-O 分子的存在能有效延长电子寿命,从而有效抑制电子孔的重组,从而大大提高载流子的利用率。这些发现为生物质碳基光催化剂的设计提供了新的思路,对工业应用太阳能合成 H2O2 具有重要意义。
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Efficient photocatalytic H2O2 production by using unstable S-O functional groups as oxygen adsorption and active sites in shuttlecock waste-derived N, S-doped carbon dots

The growing demand for environmentally friendly hydrogen peroxide (H2O2) production has fueled extensive research into synthesis strategy for photocatalysis though the use of the sunlight. However, the current challenge lies in the efficient production of photocatalysts without relying on sacrificial agents in the atmospheric environment. In this study, we propose a breakthrough approach to synthesize N, S co-doped carbon dots (N, S-CDs) by utilizing disulfide bonds in discarded shuttlecock waste and demonstrate its impressive performance (2062.4 µM g-1h−1) for photocatalytic H2O2 production. The significance of the S-O functional groups in N, S-CDs is not limited to the structural elements, since it is not only the key adsorption site for oxygen, but also active site to promote electron transfer from the bulk phase to surface of N, S-CDs during the oxygen reduction reaction (ORR) process for photocatalytic H2O2 production. Furthermore, femtosecond transient absorption spectroscopy (fs-TA) indicates that the presence of the S-O moiety is effective in prolonging the electron lifetime, which effectively inhibit the recombination of electron-holes, thus greatly improving carriers’ utilization. These findings provide new insight for the design of biomass carbon-based photocatalysts, which have important implications for the industrial application of solar energy for the synthesis of H2O2.

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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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