摘要
采用熔融法以铁、钼、铜和钨硝酸盐为原料,制备出一系列的Fe_(x)M_(y)(M=Mo、Cu、W)双金属催化剂。首先考察了一系列的Fe_(15)M_(1)(M=Mo、Cu、W)双金属催化剂的甲烷催化裂解(CDM)活性,Fe_(15)Mo_(1)的催化活性远高于Fe_(15)Cu_(1)和Fe_(15)W_(1)。通过比表面积测试(BET)、X射线衍射(XRD)、H_(2)程序升温还原(H_(2)-TPR)和拉曼光谱(Raman)等分析方法对Fe_(15)M_(1)的物理特性、结构组成、还原特性和副产物碳纳米材料(CNMs)的石墨化度等进行表征。进一步考察了金属Mo的掺杂量和焙烧温度对Fe_(x)Mo_(y)双金属催化剂的甲烷转化率和碳产率的影响。Fe_(1)Mo_(1)表现出优异的催化性能,其碳产率(6gC/gcat)高于纯Fe的碳产率(4.35gC/gcat)。XRD和X射线光电子能谱(XPS)分析表明,Fe_(1)Mo_(1)双金属形成Fe_(2)(MoO4)_(3)相,提高了其催化活性和稳定性;透射电镜(TEM)结果表明,Fe_(1)Mo_(1)催化剂CDM反应后的CNMs为竹节状的碳纳米管。
A series of FexMy(M=Mo,Cu,W)bimetallic catalysts were prepared by the fusion method using iron,molybdenum,copper and tungsten nitrate as raw materials.Fe_(15)M1(M=Mo,Cu,W)bimetallic catalysts were synthesized to investigate their catalytic decomposition of methane(CDM)activity.Results indicated that the catalytic activity of Fe_(15)Mo_(1) was much higher than that of Fe_(15)Cu_(1) and Fe_(15)W1.The physical characteristics,structural composition,reduction characteristics and the graphitization of byproduct carbon nano materials(CNMs)were characterized by means of specific surface area(BET),X‐ray powder diffraction(XRD),H_(2) temperature programmed reduction(H2-TPR)and Raman spectra,respectively.Then,the effects of Mo doping and calcination temperature on the methane conversion and carbon yield over the FexMoy catalysts for CDM were further investigated.It was found that,the Fe1Mo1 catalyst had the best catalytic activity and stability,and its carbon yield(6gC/gcat)was higher than that of pure Fe(4.35gC/gcat).XRD and X-ray photoelectron spectroscopy(XPS)results showed that Fe_(2)(MoO_(4))_(3) phase was formed in Fe1Mo1,which increased the catalytic activity and stability.Transmission electron microscope(TEM)results indicated that the deposited CNMs over the spent Fe1Mo1 catalyst were bamboolike carbon nano tubes.
作者
钱敬侠
陈天文
刘大斌
周吕
QIAN Jingxia;CHEN Tianwen;LIU Dabin;ZHOU Lyu(School of Chemistry and Chemical Engineering,Nanjing University of Science and Technology,Nanjing 210094,Jiangsu,China)
出处
《化工进展》
EI
CAS
CSCD
北大核心
2021年第11期6102-6112,共11页
Chemical Industry and Engineering Progress
基金
南京理工大学自主科研项目(AE89891,AE89991)
中央高校基本科研业务费专项项目(30920010006,30918012202)。
关键词
甲烷
裂解
催化剂
制氢
碳纳米材料
methane
decomposition
catalyst
hydrogen production
carbon nano materials
