煤焦-Ni复合物催化甲烷干重整及其反应后形成碳材料的电化学性能研究  

Study on dry reforming of methane catalyzed by coal char-Ni composite and electrochemical performance of formed carbon materials after reaction

作　　者：周娅兰 王建友 杨文成 张磊 张建波 马晓迅[1] ZHOU Yalan;WANG Jianyou;YANG Wencheng;ZHANG Lei;ZHANG Jianbo;MA Xiaoxun(School of Chemical Engineering,Northwest University,Xi’an 710127,Shaanxi,China;Yulin Yushen Industrial Park Energy Technology Development Co.,Ltd.,Yulin 719302,Shaanxi,China;Shaanxi Coal Chemical Industry Technology Research Institute Co.,Ltd.,Xi’an 710100,Shaanxi,China)

机构地区：[1]西北大学化工学院,陕西西安710127 [2]榆林市榆神工业区能源科技发展有限公司,陕西榆林719302 [3]陕西煤业化工技术研究院有限责任公司,陕西西安710100

出　　处：《低碳化学与化工》2024年第6期54-62,共9页Low-Carbon Chemistry and Chemical Engineering

基　　金：国家自然科学基金(21878248);陕西省自然科学基础研究计划-陕煤联合基金(2021JLM-22);榆林市科技计划(CXY-2022-163)。

摘　　要：甲烷干重整(DRM)反应能够将CH_(4)和CO_(2)两种温室气体转化为合成气,具有突出的环境和经济效益。但DRM反应过程的高温条件和产出的积炭易造成Ni等金属催化剂的失活,限制了其在工业上的应用。中低温煤热解半焦(简称“煤焦”)具有作为高效Ni基催化剂载体的良好潜力。为了提升DRM反应性能并促进煤焦利用,设计并制备了一种煤焦-Ni复合物,以K_(2)CO_(3)为助剂,考察了DRM反应性能、煤焦-Ni复合物在反应后形成碳材料的表面结构特征及其用作超级电容器电极材料的性能。研究发现,当m(煤焦):m(K_(2)CO_(3)):m(Ni)=1.00:1.00:0.05、DRM反应温度为850℃时,CH_(4)和CO_(2)初始转化率分别达71%和72%。优化反应条件(催化剂的Ni负载量、反应温度和反应时间)后,以煤焦-Ni复合物在反应后形成的碳材料为超级电容器电极材料可表现出优良的电化学性能,其中,CC-2在扫描速率为5 mV/s时,比电容为136 F/g;在电流密度为1 A/g时,比电容为143 F/g。本研究为DRM和煤焦的协同转化利用、反应后碳材料(反应中作为催化剂或催化剂载体)的回收利用提供了潜在路径。Dry reforming of methane(DRM)can convert two greenhouse gases CH_(4) and CO_(2) into syngas,which has significantly environmental and economic benefits.However,the high reaction temperature and carbon deposition during the DRM process can easily cause the deactivation of metal catalysts such as Ni,limiting its application in industry.At present,coal pyrolysis char(referred to as“coal char”)has good potential as supports of high effective Ni-based catalysts.In order to improve performance of DRM reaction and promote the utilization of coal char,a coal char-Ni complex was designed and prepared with K_(2)CO_(3) as an additive.The DRM reaction performance,surface and structural properties of the formed carbon materials from the coal char-Ni complex after the reaction and its performance as supercapacitor electrode materials were investigated.The results demonstrate that the initial CH4 and CO_(2) conversion rates reach 71% and 72%,respectively when m(coal char):m(K_(2)CO_(3)):m(Ni)=1.00:1.00:0.05 and the temperature is 850℃.After optimizing the reaction conditions(including Ni loading amounts,the temperature and reaction time of DRM reaction),the formed carbon materials from the spent char-Ni complex,serving as supercapacitor electrodes,can show good electrochemical properties.CC-2 has specific capacitances of 136 F/g at a scanning rate of 5 mV/s and 143 F/g at a current density of 1 A/g.This study provides a potential path for the synergistic conversion of DRM and coal char and recycling of the spent carbon materials(catalysts or supports of catalysts in the reaction).

关 键 词：甲烷干重整 煤焦 NI 电极材料 比电容 

分 类 号：TQ519[化学工程]