Ni/煤基活性炭催化剂制备及Ni负载量对准东煤直接液化的影响  

Preparation of Ni/coal-based activated carbon catalyst and effect of Ni loading on direct liquefaction of Zhundong coal

作　　者：吴志磊 刘景梅[1,3] 周晓东 陈鲁豪 刘浪[1,3] 艾沙·努拉洪 马凤云[1,2] WU Zhilei;LIU Jingmei;ZHOU Xiaodong;CHEN Luhao;LIU Lang;Aisha·Nulahong;MA Fengyun(State Key Laboratory of Chemistry and Utilization of Carbon-based Energy Resources Jointly Constructed by Xinjiang University and Ministry,Xinjiang University,830046 Urumqi,China;Xinjiang Key Laboratory of Coal Clean Conversion and Chemical Engineering Process,School of Chemical Engineering and Technology,Xinjiang University,830046 Urumqi,China;College of Chemistry,Xinjiang University,830046 Urumqi,China)

机构地区：[1]新疆大学省部共建碳基能源资源化学与利用国家重点实验室,乌鲁木齐830046 [2]新疆煤炭清洁转化与化工过程重点实验室,新疆大学化工学院,乌鲁木齐830046 [3]新疆大学化学学院,乌鲁木齐830046

出　　处：《煤炭转化》2023年第2期64-75,共12页Coal Conversion

基　　金：新疆维吾尔自治区重大科技专项(2021A01002-1).

摘　　要：催化剂是降低煤直接液化苛刻反应条件、提高液化油产率的重要因素。以新疆俄霍布拉克煤田次烟煤为碳源,以Ni(NO_(3))_(2)水溶液为镍源,采用一步原位负载煅烧还原法,制备了Ni负载量分别为7%,8%,15%和22%(质量分数)的Ni/煤基活性炭(Ni/coal-based activated carbon,Ni/CAC)催化剂。以新疆准东西沟煤田褐煤为煤样,通过液化实验,考察了Ni负载量对Ni/CAC的形貌和结构特征、液化效果及液化油组成的影响。结果表明:Ni以单质负载于CAC孔壁,随着其负载量的增加,晶粒尺寸迅速增加,晶粒比表面积和分散度以及催化剂的比表面积和孔体积均减小。准东西沟褐煤液化实验表明,随着Ni负载量的增加,转化率和油产率均呈开口向下抛物线变化,在8%的Ni负载量时,均达到最大值,分别为89.50%和75.69%;总氢耗为3.51 g(H_(2))/100 g(煤),其中,气相氢耗为2.00 g(H_(2))/100 g(煤),占总氢耗的57%。液化油的GC-MS分析表明,不同Ni负载量的四种试样的液化油中,烷烃含量均最高,约占40%;含氧化合物含量为20%~30%,以酚类为主;芳烃含量也为20%~30%,以单环芳烃和双环芳烃为主;含N,S等化合物含量为8%~11%。随着Ni负载量的增加,烷烃含量增加幅度较大,含氧化合物含量减少,芳烃等其他化合物含量变化不大。Catalyst is an important factor to reduce the restrictions of severe reaction conditions and improve the yield of oil during the process of direct coal liquefaction.Using subbituminous coal(obtained from Ehubulake coal field in Xinjiang,China)as carbon source and Ni(NO_(3))_(2) aqueous solution as nickel source,Ni/coal-based activated carbon(Ni/CAC)with Ni loading amounts of 7%,8%,15%and 22%was prepared by one-step in situ calcination and reduction method.Taking lignite from Zhunxigou Coalfield in Xinjiang as coal samples,the effects of Ni loading on the morphology and structural characteristics,liquefaction performance and oil composition of Ni/CAC were investigated.The results show that Ni is elementally loaded on the wall of CAC hole.With the increasing of Ni loadings,the grain size of Ni increases rapidly,while the specific surface area and dispersion of the grains,as well as the specific surface area and pore volume of the catalyst decrease.The results of autoclave experiments show that with the increase of Ni loading,the conversion rate of coal and the oil yield present a variation trend of opening downward parabolic curve.When the Ni loading is 8%,the conversion rate and oil yield reaches maximum value of 89.50%and 75.69%,respectively,and the total hydrogen consumption is 3.51 g(H_(2))/100 g(coal)(the gas phase hydrogen consumption is 2.00 g(H_(2))/100 g(coal),accounting for 57%of the total hydrogen consumption).The GC-MS analysis of oil shows that the content of alkanes is the highest,accounting for about 40%.The content of oxygenated compounds is 20%-30%,mainly phenols.The content of aromatics is also 20%-30%,mainly monocyclic and bicyclic.The content of compounds containing N and S is 8%-11%.With the increase of Ni loading,the content of alkanes increases greatly,the content of oxygenates decreases,and the content of aromatics and other compounds does not change significantly.

关 键 词：低阶煤 催化液化 Ni/煤基活性炭 Ni负载量 液化油组成 

分 类 号：TQ529.1[化学工程—煤化学工程]