煤基富氮层级多孔碳制备及其催化脱硫性能  

Preparation of hierarchical nitrogen-rich porous carbon from coal tar for catalytic desulfurization

作　　者：孙明慧 陈静圆 肖南 陈奥博[2] 王旭珍 邱介山 SUN Minghui;CHEN Jingyuan;XIAO Nan;CHEN Aobo;WANG Xuzhen;QIU Jieshan(State Key Laboratory of Fine Chemical Engineering,Dalian 116024,Liaoning,China;School of Chemical Engineering&Liaoning Key Laboratory for Energy Materials and Chemical Engineering,Dalian University of Technology,Dalian 116024,Liaoning,China;School of Chemical Engineering,Beijing University of Chemical Technology,Beijing 100029,China)

机构地区：[1]精细化工国家重点实验室,辽宁大连116024 [2]大连理工大学化工学院,辽宁省功能材料化工重点实验室,辽宁大连116024 [3]北京化工大学化学工程学院,北京100029

出　　处：《化工学报》2020年第2期660-668,共9页CIESC Journal

基　　金：国家自然科学基金项目(U1610105)

摘　　要：以煤加工副产物煤焦油中蒽油馏分为碳源、多巴胺为氮源,基于纳米碳酸钙球模板在碳化过程中发生的诱导自活化作用,一步共碳化制得氮掺杂多孔碳(NPCs)材料。通过元素分析、低温氮气吸附-脱附测试、扫描及透射电镜表征,结果表明,NPCs材料的氮元素掺杂量高,且具有发达的微孔-介孔梯级孔道结构。结合室温下催化硫化氢选择性氧化为单质硫的反应性能评价,发现改变模板剂用量、碳/氮源投料比和碳化温度,可调控NPCs材料的氮掺杂量(质量分数6.4%~21.3%)、比表面积、孔道结构发达程度及相应的定向转化硫容,最佳工艺条件下合成样品的饱和硫容高达5.8 g H2S/(g催化剂)。Nitrogen-doped porous carbon(NPCs)were prepared by one-step co-carbonization used the anthracene oil fraction form coal taras the carbon source and dopamine as the nitrogen source,based on the induced selfactivation of the nano-calcium carbonate template in the carbonization process.The results from element analyses,cryogenic nitrogen adsorption-desorption test,scanning and transmission electron microscopy characterization show that NPCs have a high level of doping nitrogen and the developed micro-mesoporous hierarchical structure.Combined with the evaluation for catalytic oxidation of hydrogen sulfide to elemental sulfur at room temperature,it is found that the doped-nitrogen amount(6.4%-21.3%,mass fraction),the specific surface area,the channel texture and the corresponding desulfurization performance of NPCs can be controlled by changing the dosage of template agent,the feeding ratio of carbon/nitrogen source and the carbonization temperature.And the saturated sulfur capacity of NPCs can be up to 5.8 g H2S/(g cat.)when synthesized under the optimal process conditions.

关 键 词：碳材料 煤焦油 氮掺杂 纳米结构 催化 氧化脱硫 

分 类 号：TQ127.1[化学工程—无机化工]