模型炭催化加氢气化反应特性研究  

The behavior of the different catalysts for model carbon hydrogasification

作　　者：曲旋[1] 王沁汾 严帅 冯俊 张建树 张荣[1] 毕继诚[1] QU Xuan;WANG Qin-fen;YAN Shuai;FENG Jun;ZHANG Jian-shu;ZHANG Rong;BI Ji-cheng(State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;School of Chemistry and Chemical Engineering/Key Laboratory for Green Process of Chemical Engineering of Xinjiang Bingtuan-Provincial Ministry of Education to Build a National Key Laboratory Breeding Base,Shihezi University,Shihezi 832003,China;Department of Energy and Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001 [2]石河子大学化学化工学院新疆兵团化工绿色过程重点实验室-省部共建国家重点实验室培育基地,新疆石河子832003 [3]华东理工大学资源与环境工程学院,上海200237 [4]中国科学院大学,北京100049

出　　处：《燃料化学学报》2022年第1期1-10,共10页Journal of Fuel Chemistry and Technology

基　　金：NSFC-新疆联合基金(U1703253);煤转化国家重点实验室青年人才基金(2021BWZ001);山西省自然科学基金(201801D121287)资助。

摘　　要：在加压热天平中研究了活性炭/烟煤半焦/无烟煤半焦等模型炭催化加氢气化(CHG)的特性,并结合GC、BET等表征对炭的物理结构和化学反应过程的分析,初步获悉了Co对炭-氢反应的催化作用过程。结果表明,炭CHG过程中过渡金属(Fe、Co、Ni)的催化活性明显高于碱金属和碱土金属(K、CaO、MgO),过渡金属催化过程存在低温(600−750℃)和高温(>800℃)两个特征催化区域,低温催化区域的出现主要归因于过渡金属催化剂氧化物与炭发生相互作用,部分炭结构得到活化的同时过渡金属嵌入到炭层结构中更为有效的发挥供氢和断键作用。Co催化剂在850℃和1 MPa氢压以上的条件下,催化剂的供氢作用可达到饱和,炭的催化加氢气化过程主要为温度促使的催化断键反应。具有高比表面积和低致密程度炭结构的模型炭在较低的催化剂负载量下即可具有高的CHG活性。The catalytic hydrogasification of activated carbon/bituminous char/anthracite char with the different catalysts were performed in a pressurized thermogravimetry analysis(PTGA).The GC,BET were used to characterize the physical structure and chemical reaction process of carbon.The function principle of Co to the carbon-hydrogen reaction was preliminarily obtained.The results showed that the catalytic activity of transition metals(Fe,Co,Ni)was significantly better than that of alkali metals and alkaline earth metals during the process of activated carbon hydrogasification.There were two catalytic zones of low temperature(600−750℃)and high temperature(>800℃)in the catalytic process.The emergence of the low temperature catalytic zone could be attributed to the interaction between the transition metal oxides and carbon.The transition metal was embedded in carbon layer structure during the activated carbon hydrogasification,then parts of carbon structure was activated,resulting in the cleavage of carbon-carbon bonds.The adequate active hydrogen could be supplied by Co at 850℃when the pressure was beyond 1 MPa.Briefly,the reaction temperature was the crucial factor for the cleavage of carbon-carbon bonds.The model carbon with higher specific surface area and weaker carbon structure could be converted efficiently even with lower loading amount of catalyst.

关 键 词：模型炭 催化加氢气化 加压热天平 

分 类 号：TQ53[化学工程—煤化学工程]