Fe改性Zr基蒙脱土对新疆和丰煤热解行为的影响  

Effect of Fe modified Zr-based montmorillonites on the pyrolysis behavior of Xinjiang Hefeng coal

作　　者：张照曦 钟梅[1] 亚力昆江·吐尔逊[1] 李建[1] ZHANG Zhao-xi;ZHONG Mei;YALKUN·Tursun;LI Jian(State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources and Xinjiang Key Laboratory of Coal Clean Conversion&Chemical Engineering,School of Chemical Engineering and Technology Xinjiang University,Urumqi 830046,China)

机构地区：[1]新疆大学化工学院省部共建碳基能源资源化学与利用国家重点实验室新疆煤炭清洁转化与化工过程重点实验室,新疆乌鲁木齐830046

出　　处：《燃料化学学报》2022年第6期683-692,共10页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21766035);新疆维吾尔自治区杰出青年基金(2020Q001);国家自然科学基金与新疆维吾尔自治区政府联合基金重点项目(U1703252)资助。

摘　　要：采用机械球磨法制备不同Fe盐改性Zr基蒙脱土催化剂,通过X射线衍射仪(XRD)、物理吸附仪(BET)、化学吸附仪(NH_(3)-TPD、H2-TPR)和X射线光电子能谱仪(XPS)分析其组成和结构。结果表明,与24ZrAM相比,以FeCl_(3)·6H2O和FeCl2·4H2O为铁源时,3Cl−-24ZrAM和2Cl−-24ZrAM中生成了Fe–O–Zr结构。Fe的硫酸盐存在时,催化剂的比表面积显著减小。引入Fe后,催化剂的总酸量均降低,3Cl−-24ZrAM的酸量与强酸强度最高。H2-TPR显示,3Cl−-24ZrAM、2Cl−-24ZrAM和3NO_(3)^(-)-24ZrAM中Fe2O3还原为Fe3O4的温度均低于500℃。在固定床反应器中考察了催化剂对新疆和丰煤热解行为及含不同桥键模型化合物的断键机制的影响。与24ZrAM相比,不同Fe源改性蒙脱土均能降低焦油中沥青的质量分数,其中,3Cl−-24ZrAM的裂解活性最高,轻质焦油分率增加至63%,比24ZrAM提高了18.9%,轻油和酚油质量分数分别为24ZrAM的1.3倍和1.4倍,长链烃含量进一步降低,降幅为0.7%。引入Fe后,苄基苯基醚(BPE)、联苄和联苯的转化率分别比24ZrAM提高了5%、1.6%和43.9%。A serial of Fe modified Zr-based montmorillonites were prepared by mechanical ball milling and their characteristics were depicted by X-ray diffractometer(XRD),N2 adsorption-desorption instrument(BET),temperature-programmed desorption of ammonia(NH_(3)-TPD,H2-TPD),X-ray photoelectron spectrometer(XPS).The results show that compared with 24ZrAM,when FeCl_(3)·6H_(2)O and FeCl_(2)·4H_(2)O are used as iron sources,Fe-O-Zr structure appears on the 3Cl−-24ZrAM and 2Cl−-24ZrAM catalysts.In the presence of Fe sulfate,the specific surface area of the catalysts decreases markedly.With the introducing of Fe,the total acid content of catalysts reduces.Wherein,3Cl−-24ZrAM has the highest acid content and strongest acid strength.H_(2)-TPR shows that the temperature for Fe_(2)O_(3) reduced to Fe_(3)O_(4) in 3Cl−-24ZrAM,2Cl−-24ZrAM and3NO_(3)^(-)-24ZrAM is lower than 500℃.Then,the effect of catalysts on the pyrolysis behavior of Xinjiang Hefeng coal and the bridge bond cleavage mechanism of different model compounds were investigated in a fixed bed reactor.It is noted that compared with 24ZrAM,the fraction of coal tar pitch all declines under the action of Fe species.Among them,3Cl−-24ZrAM has the highest cracking activity with the light tar fraction of 63%,which is 18.9%higher than that of 24ZrAM.Meanwhile,the content of light oil and phenol oil are 1.3 times and 1.4 times higher than that of 24ZrAM,respectively.As for long-chain hydrocarbons,a further decline by 0.7%is observed.In addition,the conversion rates of benzyl phenyl ether(BPE),dibenzyl and biphenyl increase by 5%,1.6%and 43.9%,respectively.

关 键 词：Fe改性Zr基蒙脱土 新疆和丰煤 模型化合物 催化热解 焦油品质 

分 类 号：TQ530.2[化学工程—煤化学工程]