催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2014年
8期
1347-1358
,共12页
孙敬方%张雷%葛成艳%汤常金%董林
孫敬方%張雷%葛成豔%湯常金%董林
손경방%장뢰%갈성염%탕상금%동림
一氧化碳氧化%氧化铜/二氧化铈%固相浸渍法%湿浸渍法%协同作用机制
一氧化碳氧化%氧化銅/二氧化鈰%固相浸漬法%濕浸漬法%協同作用機製
일양화탄양화%양화동/이양화시%고상침지법%습침지법%협동작용궤제
Carbon monoxide oxidation%Copper oxide Cerium oxide%Solid state impregnation%Wet impregnation%Synergistic mechanism
采用固相浸渍法和常规湿浸渍法制备了一系列CuO/CeO2催化剂,并结合X射线衍射(XRD)、氢气-程序升温还原(H2-TPR)、激光拉曼光谱(LRS)、原位漫反射红外光谱(in situ DRIFTS)、X射线光电子能谱(XPS)等手段考察了制备方法对催化剂结构性质及其在CO氧化反应中性能的影响. XPS和H2-TPR结果表明,固相浸渍法更有利于得到高分散的铜物种,并促进CuO物种的还原. LRS结果表明,相比于湿浸渍法,固相浸渍法能产生更多氧空位,而这些氧空位可以活化参与反应的O2. CO氧化活性测试结果表明,当铜负载量相同时,固相浸渍法制备的催化剂相比于湿浸渍法表现出更好的催化性能.结合多种表征结果发现,催化剂CO氧化性能与其表面氧空位和Cu+-CO浓度紧密相关,提出了CuO/CeO2催化剂在CO氧化反应中可能的协同作用机制.
採用固相浸漬法和常規濕浸漬法製備瞭一繫列CuO/CeO2催化劑,併結閤X射線衍射(XRD)、氫氣-程序升溫還原(H2-TPR)、激光拉曼光譜(LRS)、原位漫反射紅外光譜(in situ DRIFTS)、X射線光電子能譜(XPS)等手段攷察瞭製備方法對催化劑結構性質及其在CO氧化反應中性能的影響. XPS和H2-TPR結果錶明,固相浸漬法更有利于得到高分散的銅物種,併促進CuO物種的還原. LRS結果錶明,相比于濕浸漬法,固相浸漬法能產生更多氧空位,而這些氧空位可以活化參與反應的O2. CO氧化活性測試結果錶明,噹銅負載量相同時,固相浸漬法製備的催化劑相比于濕浸漬法錶現齣更好的催化性能.結閤多種錶徵結果髮現,催化劑CO氧化性能與其錶麵氧空位和Cu+-CO濃度緊密相關,提齣瞭CuO/CeO2催化劑在CO氧化反應中可能的協同作用機製.
채용고상침지법화상규습침지법제비료일계렬CuO/CeO2최화제,병결합X사선연사(XRD)、경기-정서승온환원(H2-TPR)、격광랍만광보(LRS)、원위만반사홍외광보(in situ DRIFTS)、X사선광전자능보(XPS)등수단고찰료제비방법대최화제결구성질급기재CO양화반응중성능적영향. XPS화H2-TPR결과표명,고상침지법경유리우득도고분산적동물충,병촉진CuO물충적환원. LRS결과표명,상비우습침지법,고상침지법능산생경다양공위,이저사양공위가이활화삼여반응적O2. CO양화활성측시결과표명,당동부재량상동시,고상침지법제비적최화제상비우습침지법표현출경호적최화성능.결합다충표정결과발현,최화제CO양화성능여기표면양공위화Cu+-CO농도긴밀상관,제출료CuO/CeO2최화제재CO양화반응중가능적협동작용궤제.
A series of CuO/CeO2 catalysts were prepared by solid state impregnation (SSI) and wet impregna-tion (WI) methods and characterized by X-ray diffraction, H2 temperature-programmed reduction (H2-TPR), laser Raman spectroscopy (LRS), in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), and X-ray photoelectron spectroscopy (XPS). XPS and H2-TPR results showed that SSI increased the dispersion of the copper species on the catalyst surface, which bene-fited the reduction of CuO species. LRS results indicated that a higher concentration of oxygen va-cancies was obtained by the SSI method unlike the WI method. CO oxidation results showed that at a given CuO loading, the activity of the catalysts prepared by SSI was higher than that of their coun-terparts prepared by WI. Based on the combined characterization results, it was suggested that the enhanced activity was closely related to the higher concentrations of oxygen vacancies and Cu+-CO species on the catalysts. Last, a possible synergetic mechanism was proposed for CO oxidation over the CuO/CeO2 catalysts.