首页> 中文期刊>功能材料 >络合法制备 Ce-Zr-O固溶体作为 CO2重整 CH4催化剂载体的研究∗

络合法制备 Ce-Zr-O固溶体作为 CO2重整 CH4催化剂载体的研究∗

     

摘要

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.%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.

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