微纤复合硫氮共掺杂碳纳米管的制备及吸附性能研究

Fabrication and adsorption performance of microfiber-reinforced S,N-co-doped carbon nanotubes

  • 摘要: 随着工业化进程加速,挥发性有机化合物(VOCs)污染对生态环境构成严重威胁。对二甲苯(PX)作为典型持久性有毒污染物,其高效治理技术开发迫在眉睫。本研究聚焦碳纳米管(CNTs)吸附技术瓶颈——团聚效应及稳定性不足,采用纸状烧结不锈钢纤维载体(PSSF)为基底,通过化学气相沉积法分别以升华硫、硫脲为前驱体,制备硫掺杂(SCNT/PSSF)和硫氮共掺杂碳纳米管复合材料(SNCNT/PSSF)。表征分析表明:氮掺杂显著提升材料石墨化程度(SNCNT/PSSF的ID/IG=0.92,sp2-C占比67.78%),促进碳管有序生长,其残炭率(42.71%)较SCNT/PSSF(20.86%)提升104.7%。结构化固定床吸附实验显示:SNCNT/PSSF床层利用效率达51.37%,显著高于SCNT/PSSF(33.63%),证实氮掺杂增强吸附性能。对比不同床层的装填比例研究结果显示:提高SNCNT/PSSF床层占比可提升传质效率(无效床层厚度减小,利用率增大);低入口流速(≤100 mL/min)与低PX浓度(≤2.17 mg/L)更利于吸附过程。此外,结构化固定床的吸附过程可以被Yoon-Nelson模型良好拟合。本研究为开发高稳定性、可工程化的VOCs吸附材料提供了新策略。

     

    Abstract: The increasing industrial emissions of volatile organic compounds (VOCs) pose severe threats to ecological systems. Efficient abatement of P-Xylene (PX), a representative persistent toxic pollutant, is urgently required. To address the agglomeration instability of carbon nanotubes (CNTs) in adsorption processes, this study innovatively engineered paper-like sintered stainless steel fibers (PSSF) as substrates. Using chemical vapor deposition with sublimed sulfur and thiourea as precursors, sulfur-doped (SCNT/PSSF) and sulfur-nitrogen co-doped CNT composites (SNCNT/PSSF) were synthesized.Multimodal characterization demonstrated that nitrogen doping significantly enhanced graphitization (ID/IG = 0.92, sp2-C content: 67.78%) and promoted ordered CNT growth, yielding a 104.7% increase in char yield (42.71% vs. 20.86% for SCNT/PSSF). Structured fixed-bed adsorption experiments revealed 51.37% bed utilization efficiency for SNCNT/PSSF, surpassing SCNT/PSSF (33.63%) by 53%, confirming the adsorption enhancement via N-doping.A comparative study of packing ratios across different bed configurations demonstrates: Increasing SNCNT/PSSF bed proportion improved mass transfer efficiency, reducing the length of unused bed (LUB) and raising utilization to 59.32%; Optimal operation required low inlet flow rates (≤100 mL/min) and PX concentrations (≤2.17 mg/L).Furthermore, the adsorption process in structured packed-bed systems is accurately described by the Yoon-Nelson model. This work presents a novel development strategy for fabricating high-stability, engineerable VOCs adsorption materials.

     

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