基于钴离子交换分子筛为模板的三维有序微孔炭低温合成及其宏量制备  

Large-scale synthesis of 3D ordered microporous carbon at low temperature using cobalt ions exchanged zeolite Y as a template

作　　者：赵宏伟[1] 李莉香[1,2] 左怀洋 曲迪 张涵 陶林 孙呈郭 巨东英 安百钢[1,2] ZHAO Hong-wei;LI Li-xiang;ZUO Huai-yang;QU Di;ZHANG Han;TAO Lin;SUN Cheng-guo;JU Dong-ying;AN Bai-gang(Key Laboratory of Energy Materials and Electrochemistry Research Liaoning Province,School of Chemical Engineering,University of Science and Technology Liaoning,Anshan 114051,China;Hainan Provincial Key Lab of Fine Chemistry,School of Chemical Engineering and Technology,Hainan University,Haikou 570228,China.;School of Chemical Engineering,Nanjing University of Science and Technology,Nanjing 210094,China)

机构地区：[1]辽宁科技大学化学工程学院,辽宁省能源材料与电化学重点实验室,辽宁鞍山114051 [2]海南大学化学工程与技术学院,海南省精细化学重点实验室,海南海口570228 [3]南京理工大学化学与化工学院,江苏南京210094

出　　处：《新型炭材料（中英文）》2023年第5期861-874,共14页New Carbon Materials

基　　金：国家自然科学基金(51872131,51972156,51672117,51672118);辽宁省特聘教授项目;辽宁省博士科研启动基金(2023-BS-184);辽宁科技大学人才项目(6003000315).

摘　　要：沸石模板炭(ZTCs)由于具有独特的三维有序微孔结构和高比表面积,在吸附和能量存储等方面表现出诸多优异的性能。然而,ZTCs有效合成方法的缺乏和大规模合成的困难严重限制其发展。本文通过使用钴离子交换的Y型沸石分子筛作为模板,采用直接乙炔化学气相沉积(CVD)的方法,开发出一种低温CVD合成及宏量制备ZTCs的简单工艺路线。沸石中的钴离子作为Lewis酸位点,通过d-π配位效应催化乙炔在400℃低温热解,使碳沉积选择性地发生在沸石内部。通过对CVD温度和时间的优化,ZTC_((Co))-400-8h具有优异的三维有序微孔结构、高比表面积(3000 m^(2) g^(-1))、大的孔体积(1.33 cm^(3) g^(-1)),CO_(2)吸附容量和选择性分别为2.78 mmol g^(-1)(25℃,100 kPa)和98。本工作中,利用简单的合成方法实现了高质量ZTCs的宏量制备,使用10.0 g/批次沸石模板制备的ZTC_((Co))-400-8h(L)的比表面和孔体积可达到2700 m^(2) g^(-1)和1.27 cm^(3) g^(-1)。Zeolite-templated carbons(ZTCs)have a unique three-dimensional(3D)ordered microporous structure and an extralarge surface area,and have excellent properties in adsorption and energy storage.Unfortunately,the lack of efficient synthesis strategies and the difficulty of doing this on a large-scale have seriously limited their development.We have developed a large-scale simple production route using a relatively low synthesis temperature and direct acetylene chemical vapor deposition(CVD)using Co ion-exchanged zeolite Y(CoY)as the template.The Co^(2+)confined in the zeolite acts as Lewis acid sites to catalyze the pyrolysis of acetylene through the d-πcoordination effect,making carbon deposition occur selectively inside the zeolite at 400℃ rather than on the external surface.By systematically investigating the CVD temperature and time,the optimum conditions of 8 h deposition at 400℃ produces an excellent 3D ordered-microporous structure and outstanding structure parameters(3000 m^(2) g^(-1),1.33 cm^(3) g^(-1)).Its CO_(2) adsorption capacity and selectivity are 2.78 mmol g^(-1)(25℃,100 kPa)and 98,respectively.This simple CVD process allows the synthesis of high-quality ZTCs on a large scale at a low cost.

关 键 词：沸石模板炭 钴离子交换 低温化学气相沉积 有序微孔 二氧化碳吸附剂 

分 类 号：TB33[一般工业技术—材料科学与工程]