催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2014年
7期
1196-1205
,共10页
赵坤%何方%黄振%郑安庆%李海滨%赵增立
趙坤%何方%黃振%鄭安慶%李海濱%趙增立
조곤%하방%황진%정안경%리해빈%조증립
钙钛矿%晶格氧%热重循环%部分氧化%合成气
鈣鈦礦%晶格氧%熱重循環%部分氧化%閤成氣
개태광%정격양%열중순배%부분양화%합성기
Perovskite%Lattice oxygen%Thermogravimetric redox%Partial oxidation%Syngas
采用燃烧法制备了Sr掺杂钙钛矿型氧化物La1-xSrxFeO3(x =0,0.3,0.5,0.9)载氧体,对载氧体分别进行X射线衍射、扫描电镜和H2程序升温还原反应表征,在热重循环装置和固定床反应装置上考察甲烷与载氧体晶格氧的部分氧化反应.结果表明, La1-xSrxFeO3氧化物中的晶格氧适用于甲烷部分氧化制合成气,晶格氧的得失是一个可逆过程, Sr的掺杂提高了载氧体的供氧能力,5次循环后载氧体得失晶格氧的能力没有明显的衰减.从甲烷转化率、n(H2)/n(CO)比以及H2和CO的选择性等方面来考虑, x =0.3-0.5比较理想,甲烷转化率维持在70%左右,气体产物中n(H2)/n(CO)约为2, CH4没有发生明显的裂解.
採用燃燒法製備瞭Sr摻雜鈣鈦礦型氧化物La1-xSrxFeO3(x =0,0.3,0.5,0.9)載氧體,對載氧體分彆進行X射線衍射、掃描電鏡和H2程序升溫還原反應錶徵,在熱重循環裝置和固定床反應裝置上攷察甲烷與載氧體晶格氧的部分氧化反應.結果錶明, La1-xSrxFeO3氧化物中的晶格氧適用于甲烷部分氧化製閤成氣,晶格氧的得失是一箇可逆過程, Sr的摻雜提高瞭載氧體的供氧能力,5次循環後載氧體得失晶格氧的能力沒有明顯的衰減.從甲烷轉化率、n(H2)/n(CO)比以及H2和CO的選擇性等方麵來攷慮, x =0.3-0.5比較理想,甲烷轉化率維持在70%左右,氣體產物中n(H2)/n(CO)約為2, CH4沒有髮生明顯的裂解.
채용연소법제비료Sr참잡개태광형양화물La1-xSrxFeO3(x =0,0.3,0.5,0.9)재양체,대재양체분별진행X사선연사、소묘전경화H2정서승온환원반응표정,재열중순배장치화고정상반응장치상고찰갑완여재양체정격양적부분양화반응.결과표명, La1-xSrxFeO3양화물중적정격양괄용우갑완부분양화제합성기,정격양적득실시일개가역과정, Sr적참잡제고료재양체적공양능력,5차순배후재양체득실정격양적능력몰유명현적쇠감.종갑완전화솔、n(H2)/n(CO)비이급H2화CO적선택성등방면래고필, x =0.3-0.5비교이상,갑완전화솔유지재70%좌우,기체산물중n(H2)/n(CO)약위2, CH4몰유발생명현적렬해.
We prepared perovskite-type oxides La1-xSrxFeO3 (x = 0, 0.3, 0.5, 0.9) by a combustion method and used these as oxygen carriers for the partial oxidation of methane. X-ray diffration, scanning elec-tron microscopy and H2 temperature-programmed reduction techniques were used to characterize the samples. Their reduction and oxidation activities were investigated using a thermogravimetric analysis reactor and fixed-bed reaction equipment, respectively. The results showed that the lattice oxygen in La1-xSrxFeO3 was suitable for the partial oxidation of methane to produce syngas. Their capacity to provide oxygen was enhanced by the partial substitution of La3+ by Sr2+ and the synthe-sized materials have good regenerability. The optimal degree of Sr substitution was found to be x =0.3-0.5 for La1-xSrxFeO3 with regard to reactivity, selectivity, and oxygen-donating ability. CH4 con-version was higher than 70%, and the n(H2)/n(CO) ratio remained about 2:1 and no obvious de-composition of CH4 occurred.