吸附型复合催化剂光催化消除煤矿瓦斯的机理

Mechanism on photocatalytic elimination of coal-mine gas over adsorption-type composite catalysts

  • 摘要: 为研究自制的氧化镓/煤基活性炭吸附型催化剂(15%Ga2O3/AC)光催化消除矿井瓦斯机理,开展了复合催化剂光助消除模拟矿井瓦斯中甲烷气体的实验。采用X-射线衍射(XRD)、高分辨透射电镜(HRTEM)、N2吸附-脱附技术对催化剂的复合效果、微观界面结构、孔体积、孔径分布和比表面进行表征,利用荧光发射谱、电子自旋共振谱(ESR)对光生电荷分离、光电子迁移和活性物种的产生进行测定;结合对甲烷降解动力学的分析可知,15%Ga2O3/AC可循环多次用于低浓度煤矿瓦斯的光助消除,煤基活性炭在增强复合催化剂对CH4分子吸附能力的同时还促进光生电荷分离以产生更多光空穴(h+)和超氧自由基(O2·-),使CH4经h+抽氢产生的·CH3进一步被O2·-氧化,提高催化剂消除瓦斯性能,为利用光氧化技术治理矿井局部瓦斯提供理论依据。

     

    Abstract: To investigate the mechanism for the photocatalytic degradation of coal-mine gas over self-made adsorption- type composite catalyst(15% Ga2 O3 / AC),the experiments of photo-assisted removing methane in simulated coal-mine gas are carried out. The compound effect,interfacial microstructure,pore volume,pore size distribution and specific surface area of composite catalysts are characterized by X-ray diffraction(XRD),high-resolution transmission electron microscopy(HRTEM) and low temperature N2 adsorption-desorption technique,respectively. The separation of photo- induced charge carriers,the transfer of photo-generated electrons and the generation of reactive species are studied by using photoluminescence spectrum(PLs) and electron spin resonance( ESR) spectra. Based on the analysis of meth- ane degradation kinetics,the effective photo-assisted degradation of low concentration coal-mine gas can be implemen- ted repeatedly,keeping almost unchanged removal efficiency. The introduction of coal-based AC can enhance the ad- sorption of methane,meanwhile improve the separation of photo-generated charge carriers,which contributes to producing more photo-hole(h+ ) and superoxide radical(O2·- ). The generated ·CH3 via CH4 hydrogen abstraction by h+ is further oxidized through the reaction with O2·- ,promoting the removal efficiency of methane. These results provide a theoretical basis for the gas control in the local region of coal mine using photo-oxidation technology.

     

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