催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2012年
2期
281-289
,共9页
庞潇健%陈亚中%代瑞旗%崔鹏
龐瀟健%陳亞中%代瑞旂%崔鵬
방소건%진아중%대서기%최붕
钴%氧化铈%氧化钙掺杂%柠檬酸络合%乙醇水蒸气重整%中温
鈷%氧化鈰%氧化鈣摻雜%檸檬痠絡閤%乙醇水蒸氣重整%中溫
고%양화시%양화개참잡%저몽산락합%을순수증기중정%중온
cobalt%ceria%calcium doping%citric acid complexing%ethanol steam reforming%intermediate temperature
采用柠檬酸络合法制备了Co/CeO2及其钙掺杂系列催化剂,并对催化剂进行了低温N2物理吸附、X射线衍射、H2程序升温还原、傅里叶变换红外光谱、高分辨透射电镜表征以及乙醇水蒸气重整催化性能测试.结果表明,所制Co/CeO2催化剂具有良好的乙醇水蒸气重整催化性能,500℃时乙醇能全部转化为C1,氢气产率高达85%以上.Ca掺杂减小了载体CeO2纳米颗粒尺寸,但对还原后Co0尺寸的影响较小.当Ca掺杂量大于5.0%时,催化剂氧化还原性能和乙醇水蒸气重整催化性能下降.较高的还原温度有利于体相Ce4+还原为Ce3+,并且提高了催化活性,认为金属-氧化物边界的增加提高了催化活性.初步稳定性考察结果表明,5%钙掺杂后的催化剂具有更好的抗积炭性能.
採用檸檬痠絡閤法製備瞭Co/CeO2及其鈣摻雜繫列催化劑,併對催化劑進行瞭低溫N2物理吸附、X射線衍射、H2程序升溫還原、傅裏葉變換紅外光譜、高分辨透射電鏡錶徵以及乙醇水蒸氣重整催化性能測試.結果錶明,所製Co/CeO2催化劑具有良好的乙醇水蒸氣重整催化性能,500℃時乙醇能全部轉化為C1,氫氣產率高達85%以上.Ca摻雜減小瞭載體CeO2納米顆粒呎吋,但對還原後Co0呎吋的影響較小.噹Ca摻雜量大于5.0%時,催化劑氧化還原性能和乙醇水蒸氣重整催化性能下降.較高的還原溫度有利于體相Ce4+還原為Ce3+,併且提高瞭催化活性,認為金屬-氧化物邊界的增加提高瞭催化活性.初步穩定性攷察結果錶明,5%鈣摻雜後的催化劑具有更好的抗積炭性能.
채용저몽산락합법제비료Co/CeO2급기개참잡계렬최화제,병대최화제진행료저온N2물리흡부、X사선연사、H2정서승온환원、부리협변환홍외광보、고분변투사전경표정이급을순수증기중정최화성능측시.결과표명,소제Co/CeO2최화제구유량호적을순수증기중정최화성능,500℃시을순능전부전화위C1,경기산솔고체85%이상.Ca참잡감소료재체CeO2납미과립척촌,단대환원후Co0척촌적영향교소.당Ca참잡량대우5.0%시,최화제양화환원성능화을순수증기중정최화성능하강.교고적환원온도유리우체상Ce4+환원위Ce3+,병차제고료최화활성,인위금속-양화물변계적증가제고료최화활성.초보은정성고찰결과표명,5%개참잡후적최화제구유경호적항적탄성능.
Co/CeO2 catalysts with and without calcium doping were prepared by the citric acid complexing method,and characterized by N2 adsorption,X-ray diffraction,temperature-programmed reduction,Fourier transform infrared spectroscopy,and high resolution transmission electron microscope.Their catalytic performance measurement for ethanol steam reforming (ESR) at 400-650 ℃ and atmospheric pressure with a steam-to-carbon ratio of 3.0 and gas hourly space velocity of 50000 ml/(g·h) was measured.The citric acid complexing method enhanced metal-support interaction.The Co/CeO2 catalysts gave almost 100% ethanol conversion and good hydrogen yield at 500 ℃.Calcium doping in the catalyst reduced the particle size of CeO2,but had little effect on the metallic cobalt size after reduction.Calcium doping higher than 5% deteriorated the redox properties and ESR catalytic performance,which was attributed to the fouling of CeO2 by CaO.Catalysts activated at 650 ℃ showed a better performance,which was due to a higher reduction degree of ceria and increase of the metal-oxide interface.Stability investigation of the catalysts suggested that 5% calcium doping enhanced carbon deposition resistance.