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Title
Mechanism on photocatalytic elimination of coal-mine gas over adsorption-type composite catalysts
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作者
杨娟郝静怡魏建平王云刚戴俊
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Author
YANG Juan1,2,3 ,HAO Jingyi1,2 ,WEI Jianping1,2,3 ,WANG Yungang1,2,3 ,DAI Jun1,2
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单位
河南省瓦斯地质与瓦斯治理重点实验室—省部共建国家重点实验室培育基地河南理工大学安全科学与工程学院煤炭安全生产河南省协同创新中心
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Organization
1. State Key Laboratory Cultivation Base for Gas Geology and Gas Control,Henan Polytechnic University,Jiaozuo 454000,China; 2. School of Safety Science and Engineering,Henan Polytechnic University,Jiaozuo 454000,China; 3. The Collaborative Innovation Center of Coal Safety Production of Henan,Jiaozuo 454000,China
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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。
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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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关键词
瓦斯机理研究光催化煤基活性炭复合催化剂
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KeyWords
coal-mine gas;mechanism study;photo-catalysis;coal-based activated carbon;composite catalyst
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基金项目(Foundation)
国家自然科学基金资助项目(U1704129);中国博士后科学基金资助项目(2017M622344);教育部创新团队发展支持计划资助项目(IRT_16R22);
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DOI
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Citation
YANG Juan,HAO Jingyi,WEI Jianping,et al. Mechanism on photocatalytic elimination of coal-mine gas over adsorption-type composite catalysts[J]. Journal of China Coal Society,2018,43(8):2250-2255.
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