Quaternary ammonium-functionalized rosin-derived resin for the high-performance capture of caramels: Experiments and quantum chemical theory simulations.
Quaternary ammonium-functionalized rosin-derived resin for the high-performance capture of caramels: Experiments and quantum chemical theory simulations.
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DOI：
10.1016/j.jhazmat.2023.132633
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发表时间：
2023-09
影响因子：
13.6
通讯作者：
Li Jiao;Wei Wei-Wei;Chun-Yu Liao;Yan-Hong Wei;Fu-Hou Lei;Wen Li
中科院分区：
文献类型：
--
作者：
Li Jiao;Wei Wei-Wei;Chun-Yu Liao;Yan-Hong Wei;Fu-Hou Lei;Wen Li
含有着色剂的废洗涤液的排放造成的水污染仍然存在争议。在这项研究中，松香衍生的强碱性大孔阴离子吸附树脂（RSBMAR）被设计为一种先进的吸附剂，用于清除焦糖，焦糖是废洗涤液中最顽固的着色剂。毒性测试表明RSBMAR对环境友好，几乎不威胁水生生物。 RSBMAR因其丰富的目标季铵(−R4N+)和质子化叔胺(−R3NH+)基团、丰富的多孔结构、大的比表面积、优异的热稳定性和良好的球形度而表现出出色的焦糖捕获效率。 RSBMAR对焦糖的吸附量为165.86 mg/g，脱色效率达到96.75%。经过五个循环后，废RSBMAR仍保持较高的脱色率，表明具有良好的可再生性。多重表征表明，焦糖捕获很大程度上是由−R4N+/-R3NH+（RSBMAR）和−RCOO−/−RCOOH（焦糖）之间的电荷相互作用介导的，其次是氢键。量子化学理论模拟，包括静电势、局部电离能、前沿分子轨道和独立梯度模型分析，进一步在原子水平上可视化焦糖捕获机制。 Hirshfeld 表面分析表明，RSBMAR 在焦糖吸收过程中既充当氢键供体又充当受体。通过动态吸附处理真实废水，为RSBMAR的工业应用奠定了基础。
Water contamination caused by discharge of spent washes containing colorants remains controversial. In this study, rosin-derived strongly basic macroporous anion-adsorption resin (RSBMAR) was designed as an advanced adsorbent for scavenging caramel, the most recalcitrant colorant in spent washes. Toxicity tests suggest that RSBMAR is environmentally friendly and hardly threatens aquatic organisms. RSBMAR exhibits outstanding caramel capture efficiency because of its rich target quaternary ammonium (−R4N+) and protonated tertiary amine (−R3NH+) groups, abundant porous structure, large specific surface area, excellent thermal stability, and good sphericity. The caramel adsorption capacity of RSBMAR was 165.86 mg/g and the decolorization efficiency reached 96.75%. After five cycles, the spent RSBMAR maintained a high decolorization rate, indicating excellent renewability. Multiple characterizations indicated that caramel capture was largely mediated by charge interaction between −R4N+/−R3NH+(RSBMAR) and −RCOO−/−RCOOH (caramel), followed by H-bonds. Quantum chemical theory simulations, including electrostatic potential, local ionization energy, frontier molecular orbitals, and independent gradient model analyses, further visualized caramel capture mechanisms at atomic level. Hirshfeld surface analysis revealed that RSBMAR acts as both an H-bond donor and acceptor during caramel uptake. Dynamic adsorption was performed to treat real wastewater, laying the foundation for the industrial application of RSBMAR.