功能材料
功能材料
공능재료
Journal of Functional Materials
2015年
19期
19070-19074,19079
,共6页
络合分解法%固溶体%CO2%重整甲烷%催化剂
絡閤分解法%固溶體%CO2%重整甲烷%催化劑
락합분해법%고용체%CO2%중정갑완%최화제
complex-decomposition method%solid solutions%carbon dioxide%methane reforming%catalyst
以草酸、柠檬酸、甘氨酸、聚乙烯吡咯烷酮(PVP)为络合剂,采用络合分解法制备 Ni-Ce-ZrO 2催化剂,考察了所制备 Ni-Ce-ZrO 2催化剂的 CO 2重整CH 4催化性能,并对所得催化剂进行了 XRD、BET 和H 2-TPR 表征.实验结果表明,不同络合剂对催化剂的晶型结构有很大影响,以 PVP 为络合剂更有利于形成均匀的 Ce-Zr-O 立方固溶体,且催化剂 PVP-NiCeZr具有较大的比表面积、孔容和孔径,在反应中也具有最高的 CH 4和 CO 2转化率,其初始转化率分别为83.3%和87%,合成气中 H 2/CO 接近于1.PVP-NiCeZr 表现出良好的反应稳定性,反应后100 h 其热失重率仅为1.8%,这归因于 Ce-Zr-O 立方固溶体结构更有利于活性氧的移动,增加了催化剂表面积炭与氧的接触,提高了催化剂的抗积炭性能,也有利于提高 Ni 活性组分的抗烧结团聚能力.
以草痠、檸檬痠、甘氨痠、聚乙烯吡咯烷酮(PVP)為絡閤劑,採用絡閤分解法製備 Ni-Ce-ZrO 2催化劑,攷察瞭所製備 Ni-Ce-ZrO 2催化劑的 CO 2重整CH 4催化性能,併對所得催化劑進行瞭 XRD、BET 和H 2-TPR 錶徵.實驗結果錶明,不同絡閤劑對催化劑的晶型結構有很大影響,以 PVP 為絡閤劑更有利于形成均勻的 Ce-Zr-O 立方固溶體,且催化劑 PVP-NiCeZr具有較大的比錶麵積、孔容和孔徑,在反應中也具有最高的 CH 4和 CO 2轉化率,其初始轉化率分彆為83.3%和87%,閤成氣中 H 2/CO 接近于1.PVP-NiCeZr 錶現齣良好的反應穩定性,反應後100 h 其熱失重率僅為1.8%,這歸因于 Ce-Zr-O 立方固溶體結構更有利于活性氧的移動,增加瞭催化劑錶麵積炭與氧的接觸,提高瞭催化劑的抗積炭性能,也有利于提高 Ni 活性組分的抗燒結糰聚能力.
이초산、저몽산、감안산、취을희필각완동(PVP)위락합제,채용락합분해법제비 Ni-Ce-ZrO 2최화제,고찰료소제비 Ni-Ce-ZrO 2최화제적 CO 2중정CH 4최화성능,병대소득최화제진행료 XRD、BET 화H 2-TPR 표정.실험결과표명,불동락합제대최화제적정형결구유흔대영향,이 PVP 위락합제경유리우형성균균적 Ce-Zr-O 립방고용체,차최화제 PVP-NiCeZr구유교대적비표면적、공용화공경,재반응중야구유최고적 CH 4화 CO 2전화솔,기초시전화솔분별위83.3%화87%,합성기중 H 2/CO 접근우1.PVP-NiCeZr 표현출량호적반응은정성,반응후100 h 기열실중솔부위1.8%,저귀인우 Ce-Zr-O 립방고용체결구경유리우활성양적이동,증가료최화제표면적탄여양적접촉,제고료최화제적항적탄성능,야유리우제고 Ni 활성조분적항소결단취능력.
The Ni-Ce-ZrO 2 catalyst was prepared with the complex-decomposition method using oxalic acid (OA),citric acid(CA),glycine(GA)and polyvinyl pyrrolidone(PVP)as the complexing agent.The catalytic performance of the catalysts for the CO 2 reforming of CH 4 reaction was measured.Theose catalysts were char-acterized by XRD,BET and H 2-TPR.The results showed that the complexing agent had a greater impact on the crystalline structure of catalysts.PVP was more beneficial to the formation of homogeneous cubic Ce-Zr-O solid solution.As-prepared catalyst PVP-NiCeZr had higher surface area,pore volume and pore size.The results indi-cated that catalyst prepared by PVP exhibited higher catalytic activity for CH 4 reforming with CO 2 .The original conversion rate of CH 4 and CO 2 were 83.3% and 87%;a syngas with a H 2/CO molar ratio of about 1 could be obtained on catalyst PVP-NiCeZr.The catalyst of PVP-NiCeZr exhibited good reaction stability.The four cata-lysts after reaction were characterized by TG.The weight loss rate of PVP-NiCeZr after reaction 100 h was only 1.8%.Due to the cubic Ce-Zr-O solid solution was more beneficial to the shift of active oxygen,the contact chance of carbon species on the catalysts surface and active oxygen was improved.The resistance to carbon for-mation and accumulation was greatly enhanced for the catalyst PVP-NiCeZr.The cubic Ce-Zr-O solid solution could also improve the anti-sintering and high temperature stability of the active Ni.Combined XRD,BET, TPR,TG with catalytic performance,it showed that the better activity and stability of PVP-NiCeZr was related to the homogeneous cubic Ce-Zr-O solid solution and the higher surface area.