安徽理工大学学报（自然科学版）
安徽理工大學學報（自然科學版）
안휘리공대학학보（자연과학판）
JOURNAL OF ANHUI UNIVERSITY OF SCIENCE AND TECHNOLOGY(NATURAL SCIENCE)
2013年
2期
12-16
,共5页
Ni/CeO2(La2O3)-MgO-Al2O3催化剂%制备%CH4-重整%合成气
Ni/CeO2(La2O3)-MgO-Al2O3催化劑%製備%CH4-重整%閤成氣
Ni/CeO2(La2O3)-MgO-Al2O3최화제%제비%CH4-중정%합성기
Ni/CeO2(La2O3)-MgO-Al2O3catalyst%preparation%CH4-reforming%synthesisgas
以稀土氧化物（CeO2、La2 O3）为助剂对Ni/类水滑石催化剂进行改性，用于CH4三自热重整反应，旨在改善催化剂的活性和稳定性。以共沉淀法先制得铈（镧）掺杂的镁铝类水滑石（LDHs），焙烧后再以浸渍法负载镍活性组分得到Ni/LDHs前驱体，再焙烧得到NiO/CeO2（La2 O3）-MgO-Al2 O3催化剂。用ICP-AES进行Ni、Mg、Al元素分析，BET法测试催化剂比表面积， XRD表征催化剂物相， H2-TPR表征催化剂活性中心。考察了原料气组成为n （CH4）∶n （CO2）∶n （H2 O）∶n （O2）＝1∶0．5∶1．8∶0．1时催化剂在750℃、0．1 MPa条件下CH4三自热催化重整的稳定性及积炭性能。结果表明，制得的Ni/CeO2（La2 O3）-MgO-Al2 O3催化剂中， Ni组分以NiO形式存在于催化剂表面，能降低催化剂还原活化温度；在催化剂中掺杂CeO2（La2 O3）对其活性有一定程度的调控作用，且能够很好地改善催化剂的抗积碳性能；当Ni的质量分数为10％、Al与Mg的质量比为1．7时，催化活性较好，750℃、0．1 MPa时， CH4转化率达到92．3％， CO2转化率达到98．3％；反应100 h后， Ni/CeO2（La2 O3）-MgO-Al2 O3催化剂上的CH4转化率仍可维持在75％以上。
以稀土氧化物（CeO2、La2 O3）為助劑對Ni/類水滑石催化劑進行改性，用于CH4三自熱重整反應，旨在改善催化劑的活性和穩定性。以共沉澱法先製得鈰（鑭）摻雜的鎂鋁類水滑石（LDHs），焙燒後再以浸漬法負載鎳活性組分得到Ni/LDHs前驅體，再焙燒得到NiO/CeO2（La2 O3）-MgO-Al2 O3催化劑。用ICP-AES進行Ni、Mg、Al元素分析，BET法測試催化劑比錶麵積， XRD錶徵催化劑物相， H2-TPR錶徵催化劑活性中心。攷察瞭原料氣組成為n （CH4）∶n （CO2）∶n （H2 O）∶n （O2）＝1∶0．5∶1．8∶0．1時催化劑在750℃、0．1 MPa條件下CH4三自熱催化重整的穩定性及積炭性能。結果錶明，製得的Ni/CeO2（La2 O3）-MgO-Al2 O3催化劑中， Ni組分以NiO形式存在于催化劑錶麵，能降低催化劑還原活化溫度；在催化劑中摻雜CeO2（La2 O3）對其活性有一定程度的調控作用，且能夠很好地改善催化劑的抗積碳性能；噹Ni的質量分數為10％、Al與Mg的質量比為1．7時，催化活性較好，750℃、0．1 MPa時， CH4轉化率達到92．3％， CO2轉化率達到98．3％；反應100 h後， Ni/CeO2（La2 O3）-MgO-Al2 O3催化劑上的CH4轉化率仍可維持在75％以上。
이희토양화물（CeO2、La2 O3）위조제대Ni/류수활석최화제진행개성，용우CH4삼자열중정반응，지재개선최화제적활성화은정성。이공침정법선제득시（란）참잡적미려류수활석（LDHs），배소후재이침지법부재얼활성조분득도Ni/LDHs전구체，재배소득도NiO/CeO2（La2 O3）-MgO-Al2 O3최화제。용ICP-AES진행Ni、Mg、Al원소분석，BET법측시최화제비표면적， XRD표정최화제물상， H2-TPR표정최화제활성중심。고찰료원료기조성위n （CH4）∶n （CO2）∶n （H2 O）∶n （O2）＝1∶0．5∶1．8∶0．1시최화제재750℃、0．1 MPa조건하CH4삼자열최화중정적은정성급적탄성능。결과표명，제득적Ni/CeO2（La2 O3）-MgO-Al2 O3최화제중， Ni조분이NiO형식존재우최화제표면，능강저최화제환원활화온도；재최화제중참잡CeO2（La2 O3）대기활성유일정정도적조공작용，차능구흔호지개선최화제적항적탄성능；당Ni적질량분수위10％、Al여Mg적질량비위1．7시，최화활성교호，750℃、0．1 MPa시， CH4전화솔체도92．3％， CO2전화솔체도98．3％；반응100 h후， Ni/CeO2（La2 O3）-MgO-Al2 O3최화제상적CH4전화솔잉가유지재75％이상。
In order to improve activity and stability of catalyst being used in reaction of methane tri -reforming , Ni/LDHs was modified with rare earth (CeO2 , La2 O3 ).Ce (La)-doped Mg-Al layered double oxide support (LDO) was obtained through calcination at 500℃ from the corresponding Ce (La) -doped Mg -Al layered double hydroxides (LDHs), which was prepared by co -precipitation method.Then the active component nickel was loaded on Ce (La)-LDO by impregnation to reconstruct the Ni/LDHs precursor .After roasting, the NiO/Ce (La)-MgO-Al2 O3 catalyst was prepared from the precursor at last .The Ni, Mg, Al elements in the cata-lyst was analyzed via ICP-AES.The specific surface area of the catalyst was tested by the BET method .The phase of the catalyst was characterized by XRD .The active center of the catalyst was characterized via H 2 -TPR techniques.The catalytic performance of the catalysts for tri -reforming of CH4 -CO2 to Synthesis Gas were test-ed with the feed gas which composition was n (CH4 )∶n (CO2 )∶n (H2O )∶n (O2 ) =1∶0.5∶1.8∶0.1 under 750℃and 0.1MPa.The results show that the NiO component was distributed on the surface of NiO /Ce (La)-MgO-Al2 O3 catalyst, and the reduction temperature of NiO was decreased largely .The doping component CeO 2 (or La2 O3 ) within the catalyst could adjust catalytic activity in a certain extent , and could improve the resistance performance to coke deposit greatly .The catalytic activity is better when the mass fraction of Ni is10%, the mass ratio of Al, and Mg is 1.7.Under the condition of 750℃and 0.1MPa, the CH4 conversion rate is 92.3%, and CO2 conversion rate is 98.3%.After having reacted 100 h, the CH4 conversion rate of Ni/CeO2 (La2 O3 )-MgO-Al2 O3 catalyst still remains above 75%.
