Rational design of cobalt and nitrogen co-doped carbon hollow frameworks for efficient photocatalytic degradation of gaseous toluene
Rational design of cobalt and nitrogen co-doped carbon hollow frameworks for efficient photocatalytic degradation of gaseous toluene
复制标题
钴氮共掺杂碳空心骨架的合理设计用于高效光催化降解气态甲苯
DOI：
10.1016/j.jcis.2018.05.067
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发表时间：
2018-10-15
影响因子：
9.9
通讯作者：
Li, Xinyong
中科院分区：
文献类型：
--
作者：
Li, Xinyue;Li, Jianan;Li, Xinyong
本工作通过多巴胺缩聚反应原位转化咪唑骨架分子筛（ZIF-67），成功构建了Co/N共掺杂的中空碳骨架（Co/N-C）。透射电子显微镜（TEM）观察表明，Co/N-C复合材料具有中空多孔结构。用X射线光电子能谱（XPS）对掺杂和Co-N-C活性位进行了验证。空心Co/N-C纳米粒子的紫外-可见漫反射光谱（UV-vis DRS）反映了在300-800 nm范围内光吸收的显著增强。Co/N-C具有中空的多孔结构、较强的光吸收和丰富的Co-N-C活性中心，以气态甲苯为模型污染物，表现出良好的光催化性能，在温和条件下（即室温下），对气态甲苯的降解率可达78.2%左右。温度= 273 K，压力= 1原子，2，λ>= 420 nm，t = 6 h）。通过原位傅里叶变换红外光谱（FTIR）进一步研究了甲苯的光催化降解过程和机理，发现甲苯的光催化消除过程包括多次羟基化反应和苯环开环反应，并且包括苯甲醛和苯甲酸的初始中间体物种首先源自由于羟基自由基的羟基化，随后进一步氧化成二氧化碳，水(C)2018爱思唯尔公司All rights reserved.
In this work, the hollow Co/N co-doped carbon frameworks (Co/N-C) were successfully constructed by in situ transformation of zeolitic imidazolate frameworks (ZIF-67) through polycondensation of dopamine. The hollow and porous structure of Co/N-C was demonstrated by transmission electron microscopy (TEM). The doping and Co-N-C active sites were verified by X-ray photoelectron spectroscopy (XPS). The UV-vis diffusion reflectance spectra (UV-vis DRS) of hollow Co/N-C nanoparticles reflected a significant enhancement of optical absorption in the range of 300-800 nm. With hollow porous structure, strong optical absorption and rich Co-N-C active sites, the Co/N-C exhibited a high photocatalytic performance by using gaseous toluene as a model pollutant, and the degradation efficiency of gaseous toluene was found to be around 78.2% under mild conditions (i.e., Temperature = 273 K, Pressure = 1 atom, 2, lambda >= 420 nm, t = 6 h). The photocatalytic degradation process and mechanism of toluene were further investigated by in situ Fourier transform infrared (FTIR) spectroscopy, which indicated that multiple hydroxylation and benzen ring opening are both involved in the catalytic elimination processes, and the initial intermediate species including benzaldehyde and benzoic acid were firstly derived from the hydroxylation due to the hydroxyl radical followed by further oxidation into carbon dioxide and water. (C) 2018 Elsevier Inc. All rights reserved.