以氧化鈦及氧化鋯擔載鎳及鐵之載氧體製備與測試

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题名:	以氧化鈦及氧化鋯擔載鎳及鐵之載氧體製備與測試
作者:	林欣志;Hsin-Chih Lin
贡献者:	化學工程與材料工程研究所
关键词:	化學環路燃燒;載氧體;擔體;oxygen carrier;Chemical looping combustion;support
日期:	2011-07-25
上传时间:	2012-01-05 11:22:18 (UTC+8)
摘要:	本研究以氧化鈦、氧化鋯為擔體，附載鐵、鎳活性金屬作為載氧體，進行化學循環燃燒(Chemical looping combustion)之實驗。擔體及活性金屬都是以固定之pH值下中和沉澱法製備。所獲得之氫氧化鈦、氫氧化鋯、氫氧化鎳及氫氧化鐵沉澱物經凝絮沈降及離心清洗後，依照活性金屬與擔體摩爾比6:4的比例，配出單一活性金屬或雙活性金屬，及擔成分擔體與複合擔體等，共九種配方。經過乾燥及900oC煆燒得到九組載氧體樣品。所有的載氧體樣品都經過XRD鑑定結晶結構、氮氣吸附鑑定孔洞結構及比表面積，並以XPS分析金屬原子之化學狀態。這些樣品都以TGA設備在900oC下用甲烷還原空氣氧化之循環測試其性質。所有樣品在十次氧化還原循環中皆保持很好的穩定性。由還原態XRD圖譜看到，上述樣品中的活性金屬皆可在循環中達到完全還原及完全氧化。並無因燒結而降低活性的現象。其中鎳金屬無論是擔載在Ti或Zr上都有很好的反應性，而甲烷還原速率最快的樣品是氧化鋯上擔載之鎳金屬。所以可推論以氧化鋯擔載的鎳金屬是化學循環燃燒最有潛力的載氧體。 Nine combinations of active metals (Nickel and iron) and supports (TiO2 and ZrO2) were tested as the oxygen carrier for the Chemical looping combustion process. These metals and supports were all prepared by the precipitation of the corresponding hydroxide from an inorganic salt solution. The wet hydroxides were mixed in various combinations to make up a 6:4 atom ratio between the metal and the oxide support. Nine oxygen carriers were obtained from the mixed hydroxides after 900oC calcination. They were then characterized by XRD, Nitrogen adsorption and XPS before subjected to 900oC redox cycles in a TGA system, with 50 % methane/Nitrogen as the reducing gas and air as the oxidant. The oxygen weight gain and the XRD analysis indicated that the nickel and iron metals went through a complete reduction and oxidation cycle without sintering or decay in at least ten cycles. This must have resulted from the better dispersion of the active metals on the support through the mixing of the corresponding hydroxides. Among the samples tested, the nickel showed the best reactivity and thus the shortest cycle time, while ZrO2 appeared as the support of choice that promoted the Redox reaction of nickel
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