将甲烷以低能耗的方式直接转化为甲醇等高附加值的化学品一直是可持续化工产业的重要目标和重大挑战.本文制备了三维(3D)ZnO/CdS/NiFe层状双金属氢氧化物(LDH)核/壳/分层纳米线阵列(NWAs)结构材料并将其用于室温、模拟阳光照射下甲烷的...将甲烷以低能耗的方式直接转化为甲醇等高附加值的化学品一直是可持续化工产业的重要目标和重大挑战.本文制备了三维(3D)ZnO/CdS/NiFe层状双金属氢氧化物(LDH)核/壳/分层纳米线阵列(NWAs)结构材料并将其用于室温、模拟阳光照射下甲烷的光电催化氧化.结果表明3D ZnO/CdS/NiFe-LDH具有优异的光电化学性能及催化活性,甲烷气氛下的光电流密度达到了6.57 mA·cm^(−2)(0.9 V vs RHE),其催化甲烷生成甲醇及甲酸产量分别是纯ZnO的5.0和6.3倍,两种主要产物的总法拉第效率达到54.87%.CdS纳米颗粒(NPs)的沉积显著提升了复合物对可见光的吸收,促进了光生载流子的分离.而具有三维多孔结构的NiFe-LDH纳米片的引入改善了甲烷氧化表面反应动力学,起到了优异的助催化作用;并且有效抑制了O_(2)^(•-)的产生,防止O_(2)^(•-)进一步将甲醇及甲酸氧化为CO_(2),提高了甲醇及甲酸的选择性.最后,提出了三维ZnO/CdS/NiFe-LDH复合材料光电催化甲烷转化为甲醇及甲酸的机理,为甲烷低能耗转化为高价值化学品提供了新思路.展开更多
Targeting the problem of large amounts of gas emission from the goaf of the No.14201 working face in the Shaqu coal mine of Huajin Coking Coal Co. Ltd., we used a negative exponential function to describe the attenuat...Targeting the problem of large amounts of gas emission from the goaf of the No.14201 working face in the Shaqu coal mine of Huajin Coking Coal Co. Ltd., we used a negative exponential function to describe the attenuation process of gas emission in goaf (the stable source) based on the principle of field flow. Equations of two-component flow (gas and air) and seep- age-diffusion in a heterogeneous goaf flow field are solved by means of numerical simulation and fluid mechanics principles of air movement and gas distribution during gas emission from goaf. The results indicate that the air diversion volume has a negative, exponential relation with the volume of gas emitted from goaf to the working face and is clearly inversely related to gas concentra- tion. We calculated the minimum amount of air diversion and distributed air volume in the tailing roadway required for safe pro- duction.展开更多
文摘将甲烷以低能耗的方式直接转化为甲醇等高附加值的化学品一直是可持续化工产业的重要目标和重大挑战.本文制备了三维(3D)ZnO/CdS/NiFe层状双金属氢氧化物(LDH)核/壳/分层纳米线阵列(NWAs)结构材料并将其用于室温、模拟阳光照射下甲烷的光电催化氧化.结果表明3D ZnO/CdS/NiFe-LDH具有优异的光电化学性能及催化活性,甲烷气氛下的光电流密度达到了6.57 mA·cm^(−2)(0.9 V vs RHE),其催化甲烷生成甲醇及甲酸产量分别是纯ZnO的5.0和6.3倍,两种主要产物的总法拉第效率达到54.87%.CdS纳米颗粒(NPs)的沉积显著提升了复合物对可见光的吸收,促进了光生载流子的分离.而具有三维多孔结构的NiFe-LDH纳米片的引入改善了甲烷氧化表面反应动力学,起到了优异的助催化作用;并且有效抑制了O_(2)^(•-)的产生,防止O_(2)^(•-)进一步将甲醇及甲酸氧化为CO_(2),提高了甲醇及甲酸的选择性.最后,提出了三维ZnO/CdS/NiFe-LDH复合材料光电催化甲烷转化为甲醇及甲酸的机理,为甲烷低能耗转化为高价值化学品提供了新思路.
基金Project 50574038 supported by the National Natural Science Foundation of China
文摘Targeting the problem of large amounts of gas emission from the goaf of the No.14201 working face in the Shaqu coal mine of Huajin Coking Coal Co. Ltd., we used a negative exponential function to describe the attenuation process of gas emission in goaf (the stable source) based on the principle of field flow. Equations of two-component flow (gas and air) and seep- age-diffusion in a heterogeneous goaf flow field are solved by means of numerical simulation and fluid mechanics principles of air movement and gas distribution during gas emission from goaf. The results indicate that the air diversion volume has a negative, exponential relation with the volume of gas emitted from goaf to the working face and is clearly inversely related to gas concentra- tion. We calculated the minimum amount of air diversion and distributed air volume in the tailing roadway required for safe pro- duction.
