以1,5-二氨基四唑-1 H、氟偕二硝基乙醇为原料,在常温下通过曼尼希反应一步合成了N-(氟偕二硝基乙基)-1,5-二氨基四唑-1 H.采用X-射线单晶衍射分析表征了其单晶结构,表明其属于斜方晶系,空间群Pca21,173 K下的晶体密度为1.77 g·cm-3;采用Hirshfeld表面对晶体中各种作用进行了分析,晶体内占主导地位的分子间相互作用及其分布为(R为比例缩写):RO···H/H···O=27.0%,R N···H/H···N=21.5%,RF···O/O···F/F···H/H···F/N···F/F···N=15.9%,主要为氢键及卤键作用;采用热重及差示扫描量热分析(TG-DSC)研究了其热稳定性,5℃·min-1升温速率下,只有一个尖锐的分解峰温177.32℃,质量损失为92.53%,化合物分解较完全;用Kissinger法与Ozawa法分别计算了其活化能EK=213.228 kJ·mol-1,EO=209.984 kJ·mol-1.采用场发射-扫描电镜(FE-SEM)观察了产物的微观形貌,其具有类似空间网状的多孔结构.
A mini coke oven has been used to study the shrinkage crack character in the process of semi-coke formation. The results show that the section of coke cake has been clearly layered, from the inner to outward, divided into loose honeycomb semi-coke layer, small honeycomb semi-coke layer, compact semi-coke layer, cracks layer. The colour of loose honeycomb semi-coke layer and small honeycomb semi-coke layer is dark black, and its porosity about 44.8%. The colour of the compact semi-coke layer is bright black, and its porosity about 34.0%. The colour of cracks layer is silver gray, and its porosity about 46.0%. The pyrolytic plastic layer area of static and dynamics state difference, the static state pyrolytic plastic layer area is an obturation flat elliptic area, wrapped in the middle of semi-coke; the dynamic state pyrolytic plastic layer area is a placket oblate gasbag, wrapped by semi-coke from the outside. The shrinkage rate of semi-coke increases with temperature increase, the relationship between shrinkage and temperature can be described as Y=-7x10(-5) + 0.14X-56.26 (600 degrees C-850 degrees C). The thickness of semi-coke decreases, with increasing temperature, crack increases and clump decreases. Add proper humidity to coal, the crack of semi-coke decreases and the clump increases.
利用固定床反应装置研究了催化剂Co/活性炭(AC)中引入助剂Mg O对甲烷二氧化碳重整制合成气催化剂性能的影响,并通过XRD、SEM和BET技术对催化剂进行了表征。结果表明,添加适量的助剂Mg O一方面与活性物质发生协同作用,提高催化剂的比表面积;另一方面可以调节催化剂的酸碱性,提高催化剂对CO2的吸附活化,从而促进甲烷的裂解脱氢。400℃焙烧条件下制备的催化剂Co-Mg O/AC表现出最佳的催化活性和稳定性,在900℃下连续运行1 200 min,甲烷和二氧化碳转化率分别维持在96.7%和97.0%左右。
In this paper, Datong coal-based activated carbon was selected as the main research object, and the research of the effects of the activated carbon modified by different concentrations of oxidant solution in dry methane reforming reaction were carried out, using potassium permanganate as an oxidant. The results show that methane and carbon dioxide conversion reached the maximum over 0.06 mol/L KMnO4 solution modified activated carbon. Compared with origin activated carbon, the largest degree of enhancement of CO2 conversion is at 750 degrees C. While the largest degree of enhancement of CH4 conversion is at 800 degrees C. At the same time, the yield of the CO increased over modified activated carbon. The modified activated carbon catalyst has the advantages of being high in catalyst activity, good in anti-carbon performance and stability. However, it was found that there is also water generation in reforming and the yield of hydrogen decrease.
The objective of this paper is to develop, test and characterize the efficient catalyst for carbon dioxide reforming of methane. AC supported Co-Zr bimetallic catalysts for CO2 reforming of methane were prepared by impregnation method. The influence of impregnation method, impregnation amount, calcination temperature and calcination time on activity and stability of the bimetallic catalyst was studied. The reforming reactions were conducted at 650-950 degrees C and atmospheric pressure using CO2/CH4 with a feed ratio of 1/1. The catalytic performance was assessed through CH4 and CO2 conversions, synthesis gas selectivity (H-2/CO) and long-term stability. The optimum loading of Co-Zr bimetallic catalysts exhibited superior catalytic performance and presented better coke suppression. TG-DSC, XRD, SEM-EDX, H-2-TPR, XPS, BET were utilized for surface analysis of these formulations. Structural characterization and reaction results suggest that catalyst has a larger surface area, smaller metal particles and better metal dispersion and therefore gives rise to better catalytic performance. The enhanced stability is due to a strong metal metal and metal-support interaction in the catalyst. The synergistic effect between Co and Zr facilitated to migrate and form Co-Zr clusters on the AC surface, improved the Co dispersion and surface area. This may be the origin of the activity enhancement in dry reforming. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
An orthogonal experiment design was adopted for synthesis and optimization of ZrO2-Based catalyst for coke oven gas CO shift. The influence of the operating parameters on catalytic properties was investigated, with a composition being similar to typical industrial heterogeneous catalysts for WGS process. The experimental CO conversion data was analyzed by marginal and variance analysis. The optimal operating parameters for ZrO2-Al2O3 based catalyst were suggested by CO conversion.