挥发性组分对煤结构变形及煤吸附甲烷的影响（英文）

研究了煤中的挥发性物质对煤结构变形的作用,考察了此类结构变形对煤吸附甲烷的影响.实验过程采用溶剂抽提方式逐步移除了煤的挥发性物质.使用热重分析、X射线衍射及N2吸附/脱附等技术方法,考察了抽提前后样品的晶体结构、织构结构以及样品对甲烷吸附能力的差异.结果表明,移除挥发性物质导致煤结构变形,并导致煤吸附甲烷量的改变.微观结构表征证明,挥发性物质以两种形态存在于煤结构中:即其镶嵌在孔道中,或者以交联的方式附着在煤大分子网络中.其中,镶嵌在孔道中的挥发性物质是构筑煤孔道结构重要组成部分,因此影响气体在孔中的储存量;交联在煤大分子网络中的挥发性物质,影响煤与煤之间的分子相互作用,是煤晶体结构的重要参数,其可影响煤的孔结构变形程度.     

CH4, CO2和H2O在非金属原子修饰石墨烯表面的吸附

煤层气(矿井瓦斯)是一种有望替代传统化石燃料,如煤、石油和天然气的非常规气体. 作为可得的清洁能源,它的利用被认为是节能和经济的选择. 在本工作中,非金属原子X(X=H,O,N,S,P,Si,F,Cl)修饰的石墨烯(Gr)被用来代表具有结构异性的煤表面模型. 通过密度泛函理论系统地研究了煤层气组分Y(Y=CH₄,CO₂,H₂O)在非金属原子修饰石墨烯上的吸附作用. 结果表明Y在非金属原子修饰石墨烯上的吸附均为物理吸附. 态密度和差分电荷密度共同表明了这种弱的相互作用.其中,H和Cl对CH₄的作用较大; N、O、F、Cl对CO₂的作用较强; N,Cl对H₂O的影响不容忽视. 总的来说,吸附能大小依次为：H₂O>CO₂>CH₄. 因此,在CH₄富集的煤层里注入H₂O或CO₂可以与CH₄形成竞争吸附,进而提高煤层气采收率. 本工作提供了在分子水平下煤层气与非金属原子修饰石墨烯之间的相互作用的详情,并为煤层瓦斯的开采与分离提供了有用的信息.     

Ni/Al2O3催化剂上甲烷部分氧化制合成气反应积炭的研究

合成气制备;Ni/Al2O3催化剂上甲烷部分氧化制合成气反应积炭的研究     

热液法合成四苯基卟啉

以苯甲醛和吡咯为原料,采用热液法合成了四苯基卟啉,其结构经UV, 1H NMR和IR表征.较适宜的反应条件为:苯甲醛25 mmol, n(苯甲醛) : n(吡咯) : n(水杨酸)=1 : 1 : 1,在二甲苯(80 mL)中于140 ℃反应5 h,收率15.38%.     

贵金属助剂对费-托合成用钴基催化剂的促进作用

贵金属助剂促进的费-托合成用钴基催化剂具有高活性和长链烃(C₅⁺)选择性优越等特点,被广泛应用于由合成气制清洁燃料的合成反应中。 本文重点讨论了贵金属助剂对活性钴物种的结构（还原度、分散度、双金属颗粒或合金的构成）, 钴基催化剂稳定性以及其对费-托合成的反应速率和产物选择性的影响规律。     

介孔二氧化硅负载磷钨杂多酸催化合成聚四氢呋喃

采用浸渍法制备了介孔二氧化硅(SiO2)负载的磷钨杂多酸(PW12)催化剂(PW12/SiO2),其物化性质和表面酸强度经BET,IR,TG-DTG和Hammett指示剂法表征.以PW12/SiO2催化四氢呋喃开环聚合合成聚四氢呋喃(PTHF),考察了PW12的负载量[w(PW12)]和焙烧温度对催化剂活性的影响.实验结果表明,在w(PW12)为35.0%,于230 ℃焙烧活化3 h的条件下制备的催化剂(35Cat)活性最高.以35Cat为催化剂,用量占反应物总质量的15.0%时,PTHF收率达60.2%.     

Microstructure and its influence on CH4 adsorption behavior of deep coal

In this paper we investigate the influence of microstructure on the CH4 adsorption behavior of deep coal. The coal microstructure is characterized by N2 adsorption at 77 K, scanning electron microscopy （SEM）, Raman spectroscopy, and Fourier transform infrared spectroscopy （FT-IR）. The CH4 adsorptions are measured at 298 K at pressures up to 5.0 MPa by the the volumetric method and fitted by the Langmuir model. The results show that the Langmuir model fits well with the experimental data, and there is a positive correlation with surface area, pore volume, ID/IG, and CH4 adsorption capacity. The burial depth also affects the methane adsorption capacity of the samples.     

K_2S-activated carbons developed from coal and their methane adsorption behaviors

The main purpose of this work is to prepare various activated carbons by K2S activation of coal with size fractions of 60-80 meshes, and investigate the microporosity development and corresponding methane storage capacities. Raw coal is mixed with K2S powder, and then heated at 750 ℃-900 ℃ for 30 min-150 min in N2 atmosphere to produce the adsorbents. The texture and surface morphology are characterized by a N2 adsorption/desorption isotherm at 77 K and scanning electron microscopy （SEM）. The chemical properties of carbons are confirmed by ultimate analysis. The crystal structure and degree of graphitization are tested by X-ray diffraction and Raman spectra. The relationship between sulfur content and the specific surface area of the adsorbents is also determined. K2S activation is helps to bring about better development of pore texture. These adsorbents are microporous materials with textural parameters increasing in a range of specific surface area 72.27 m2/g-657.7 m2/g and micropore volume 0.035 cm3/g-0.334 cm3/g. The ability of activated carbons to adsorb methane is measured at 298 K and at pressures up to 5.0 MPa by a volumetric method. The Langmuir model fits the experimental data well. It is concluded that the high specific surface area and micropore volume of activated carbons do determine methane adsorption capacity. The adsorbents obtained at 800 ℃ for 90 min with K2S/raw coal mass ratios of 1.0 and 1.2 show the highest methane adsorption capacities amounting to 106.98 mg/g and 106.17 mg/g, respectively.     

Synthesis of multi-walled carbon nanotubes using CoMnMgO catalysts through catalytic chemical vapor deposition

The Co Mg O and Co Mn Mg O catalysts are prepared by a co-precipitation method and used as the catalysts for the synthesis of carbon nanotubes（CNTs） through the catalytic chemical vapor deposition（CCVD）. The effects of Mn addition on the carbon yield and structure are investigated. The catalysts are characterized by temperature programmed reduction（TPR） and X-ray diffraction（XRD） techniques, and the synthesized carbon materials are characterized by transmission electron microscopy（TEM） and thermo gravimetric analysis（TG）. TEM measurement indicates that the catalyst Co Mg O enclosed completely in the produced graphite layer results in the deactivation of the catalyst. TG results suggest that the Co Mn Mg O catalyst has a higher selectivity for CNTs than Co Mg O. Meanwhile, different diameters of CNTs are synthesized by Co Mn Mg O catalysts with various amounts of Co content, and the results show that the addition of Mn avoids forming the enclosed catalyst, prevents the formation of amorphous carbon, subsequently promotes the growth of CNTs, and the catalyst with decreased Co content is favorable for the synthesis of CNTs with a narrow diameter distribution.The Co Mn Mg O catalyst with 40% Co content has superior catalytic activity for the growth of carbon nanotubes.     

甲烷与含氮有机杂环化合物吸附作用的DFT研究

根据煤中氮的存在形式,提炼出11种具有不同杂化方式及含氮量的有机环状化合物.应用密度泛函理论(DFT)模拟方法对甲烷在这11种含氮化合物上的吸附模型进行结构优化,并结合吸附能、电荷分布及静电势能面的分析,从微观角度考察了甲烷与这些化合物之间的相互作用.计算结果表明:甲烷与含氮化合物的相互作用能在3.81-6.82kJ·mol-1范围内,且通过氢键和静电力相互作用;当化合物中氮的杂化方式为sp2时,其与甲烷的作用能大于sp3杂化方式的;当化合物中的氮含量增加时,可以提供更多的甲烷吸附位点.