CO_2重整CH_4纳米ZrO_2负载Ni催化剂的研究(Ⅰ)——与常规载体上Ni催化剂的比较  

CO_2 Reforming of CH 4 over Ni Supported on Nano-ZrO_2(Ⅰ) Comparison with Conventional Oxide Supported Nickel

作　　者：魏俊梅[1] 徐柏庆[1] 李晋鲁[1] 程振兴[1] 王亚权[1] 朱起明[1] 

机构地区：[1]清华大学化学系一碳化学与化工国家重点实验室,北京100084

出　　处：《高等学校化学学报》2002年第1期92-97,共6页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金 (批准号 :2 0 0 730 2 3);清华大学重点基础研究基金 (批准号 :JC19990 5 1)资助

摘　　要：在 Ni负载量相近 (约 5 % )时 ,比较了由超临界干燥得到的纳米 Zr O2 -AS为载体制备的 Ni/Zr O2 -AS与几种常规载体 (γ-Al2 O3,Ti O2 ,Si O2 和 Zr O2 -CP)负载的 Ni催化剂对 CO2 重整 CH4制合成气反应的催化性能 .研究结果表明 ,γ-Al2 O3,Ti O2 ,Si O2 和 Zr O2 -CP负载 Ni催化剂表现出明显的失活过程 ,而 Ni/Zr O2 -AS催化剂在反应 2 0 0 h后活性未下降 .“纯 Zr O2 -AS”载体本身不仅能催化生成合成气的反应 ,而且活性稳定 .TPO测定结果表明 ,负载在这种活性 Zr O2 -AS载体上的The catalytic activity and stability of Ni supported on γ Al 2O 3, TiO 2, SiO 2, conventional ZrO 2 CP, and nano ZrO 2 AS(15-20 nm) were comparatively studied for CO 2 reforming of CH 4 to synthesis gas. The Ni loading in these catalysts was limited to 5%(mass fraction) of the supports, and the reaction was performed in a fixed bed flow microreactor at 1 030 K with GHSV=2.4×10 4 mL/(h·g cat). The initial CH 4 conversions of the catalysts are in the order of Ni/ γ Al 2O 3>Ni/TiO 2>Ni/ZrO 2 CP> Ni/ZrO 2 AS > Ni/SiO 2 . Ni catalysts supported on γ Al 2O 3, TiO 2, ZrO 2 CP and SiO 2 deactivated rapidly in less than 50 h TOS, but Ni/ZrO 2 AS catalyst showed no deactivation for longer than 200 h. The pure ZrO 2 AS also showed a catalytic activity for the reaction and no loss of the activity was observed during 50 h on stream at 1 073 K. TPO measurements demonstrated that carbon deposition on the Ni/ZrO 2 AS catalyst was much less and was eliminated at lower temperature than those over the other catalysts. Explanation for the excellent stability of Ni/ZrO 2 AS catalyst was given based on the present data. It is suggested that Ni/ZrO 2 AS can be better expressed as a nano composite of the Ni and ZrO 2 AS, and high percentage of the metal support perimeter in the composite seems crucial for the long stability of the catalyst.

关 键 词：二氧化碳 甲烷 合成气 镍催化剂 纳米ZRO2 载体效应 抗积炭能力 二氧化锆 负载型催化剂 催化活性 

分 类 号：TE665.3[石油与天然气工程—油气加工工程] O643.361[理学—物理化学]