Mild Acidolysis-Assisted Hydrothermal Carbonization of Lignin for Simultaneous Preparation of Green and Blue Fluorescent Carbon Quantum Dots,ACS Sustainable Chemistry & Engineering

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Mild Acidolysis-Assisted Hydrothermal Carbonization of Lignin for Simultaneous Preparation of Green and Blue Fluorescent Carbon Quantum Dots
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2022-07-20 , DOI: 10.1021/acssuschemeng.2c02223
Lingli Zhu ₁ , Dekui Shen ₁ , Qian Liu ₁ , Kai Hong Luo ₂ , Chong Li ₃

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Biomass waste is a renewable, cost-effective, and eco-friendly feedstock for carbon quantum dot (CQD) preparation, but its high-efficiency utilization is still a challenge. Here, we report a mild acidolysis-assisted hydrothermal strategy toward the simultaneous preparation of green and blue fluorescent CQDs from lignin. The synthesis pathway includes first the acidolysis of lignin and then hydrothermal carbonization of its supernatant and solid residue, separately. The fluorescence mechanism of the two CQDs is elucidated through the investigation of their structure, chemical composition, and optical properties combined with quantum chemistry calculations. Their formation mechanism is also explored; nuclear magnetic resonance (NMR) data demonstrate that green CQDs are derived from the side-chain scission of lignin by the bottom-up method, while blue CQDs inherit the aromatic bulk of lignin via the top-down method. The optimal yield of two CQDs can be achieved as 30.6% for green CQDs and 15.2% for blue CQDs by adjusting the acidolysis temperatures from 30 to 110 °C. This comprehensive strategy promotes the high-efficiency conversion of biomass into CQDs and provides a theoretical basis for exploring the fluorescence mechanism and formation mechanism of CQDs.

中文翻译：

木质素轻度酸解辅助水热碳化同时制备绿色和蓝色荧光碳量子点

生物质废弃物是制备碳量子点 (CQD) 的可再生、经济、环保的原料，但其高效利用仍是一个挑战。在这里，我们报告了一种温和的酸解辅助水热策略，用于从木质素同时制备绿色和蓝色荧光 CQD。合成途径包括首先酸解木质素，然后分别对其上清液和固体残渣进行水热碳化。通过研究它们的结构、化学成分和光学性质，结合量子化学计算，阐明了这两种 CQD 的荧光机制。还探讨了它们的形成机制；核磁共振 (NMR) 数据表明，绿色 CQD 是通过自下而上的方法从木质素的侧链断裂衍生而来的，而蓝色 CQD 通过自上而下的方法继承了木质素的大部分芳香族成分。通过将酸解温度从 30 调整到 110°C，两种 CQD 的最佳产率可以达到绿色 CQD 的 30.6% 和蓝色 CQD 的 15.2%。这一综合策略促进了生物质向CQDs的高效转化，为探索CQDs的荧光机制和形成机制提供了理论依据。

更新日期：2022-07-20

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