催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2012年
12期
1965-1973
,共9页
朱艺%潘浩%陈山虎%王世丹%赵明%龚茂初%陈耀强
硃藝%潘浩%陳山虎%王世丹%趙明%龔茂初%陳耀彊
주예%반호%진산호%왕세단%조명%공무초%진요강
锰氧化物%负载量%碳烟%催化燃烧%氧化铈%氧化锆%氧化镧%氧化铝
錳氧化物%負載量%碳煙%催化燃燒%氧化鈰%氧化鋯%氧化鑭%氧化鋁
맹양화물%부재량%탄연%최화연소%양화시%양화고%양화란%양화려
manganese oxide%loading amount%soot%catalytic combustion%ceria%zirconia%lanthana%alumina
采用等体积浸渍法制备了一系列不同 MnOx 含量的 MnOx/Ce0.7Zr0.2La0.1O2-Al2O3(Ce0.7Zr0.2La0.1O2/Al2O3质量比=1)催化剂,并用 X 射线衍射、低温 N2吸附-脱附、X 射线光电子能谱、O2程序升温脱附和 H2程序升温还原等手段对催化剂进行了表征,考察了催化剂催化柴油车排放碳烟颗粒物燃烧的反应性能.结果表明,催化剂表面吸附的活性氧物种和 MnOx 的低温区还原性能是决定催化剂活性的两大关键因素.当 MnOx 负载量为5%时,催化反应所需的活性氧减少,因而活性降低;但 MnOx负载量增至10%时,催化剂中 Mn 物种的可还原量提高,从而增加其活性;增至20%时, MnOx 与表面吸附氧物种的可还原量间达平衡最佳值,活性最佳,碳烟起燃温度比无催化剂时降低了179 oC;负载量达30%后,由于载体表面吸附氧物种数量的降低和还原峰温的上升使催化剂活性下降.
採用等體積浸漬法製備瞭一繫列不同 MnOx 含量的 MnOx/Ce0.7Zr0.2La0.1O2-Al2O3(Ce0.7Zr0.2La0.1O2/Al2O3質量比=1)催化劑,併用 X 射線衍射、低溫 N2吸附-脫附、X 射線光電子能譜、O2程序升溫脫附和 H2程序升溫還原等手段對催化劑進行瞭錶徵,攷察瞭催化劑催化柴油車排放碳煙顆粒物燃燒的反應性能.結果錶明,催化劑錶麵吸附的活性氧物種和 MnOx 的低溫區還原性能是決定催化劑活性的兩大關鍵因素.噹 MnOx 負載量為5%時,催化反應所需的活性氧減少,因而活性降低;但 MnOx負載量增至10%時,催化劑中 Mn 物種的可還原量提高,從而增加其活性;增至20%時, MnOx 與錶麵吸附氧物種的可還原量間達平衡最佳值,活性最佳,碳煙起燃溫度比無催化劑時降低瞭179 oC;負載量達30%後,由于載體錶麵吸附氧物種數量的降低和還原峰溫的上升使催化劑活性下降.
채용등체적침지법제비료일계렬불동 MnOx 함량적 MnOx/Ce0.7Zr0.2La0.1O2-Al2O3(Ce0.7Zr0.2La0.1O2/Al2O3질량비=1)최화제,병용 X 사선연사、저온 N2흡부-탈부、X 사선광전자능보、O2정서승온탈부화 H2정서승온환원등수단대최화제진행료표정,고찰료최화제최화시유차배방탄연과립물연소적반응성능.결과표명,최화제표면흡부적활성양물충화 MnOx 적저온구환원성능시결정최화제활성적량대관건인소.당 MnOx 부재량위5%시,최화반응소수적활성양감소,인이활성강저;단 MnOx부재량증지10%시,최화제중 Mn 물충적가환원량제고,종이증가기활성;증지20%시, MnOx 여표면흡부양물충적가환원량간체평형최가치,활성최가,탄연기연온도비무최화제시강저료179 oC;부재량체30%후,유우재체표면흡부양물충수량적강저화환원봉온적상승사최화제활성하강.
A series of MnOx/Ce0.7Zr0.2La0.1O2-Al2O3 supported catalysts with the Ce0.7Zr0.2La0.1O2:Al2O3 mass ratio of 1:1 and different MnOx loadings were prepared by the incipient wetness method. The catalysts were characterized by X-ray diffraction, low temperature N2 adsorp-tion-desorption, X-ray photoelectron spectroscopy, O2 temperature-programmed desorption, and H2 temperature-programmed reduction. The catalytic performance of these catalysts for the combustion of diesel soot was investigated. It is found that surface-adsorbed active oxygen species and low-temperature reducibility of MnOx are the determinants of catalytic activity. When the MnOx loading is 5%, the catalyst activ-ity decreases owing to the loss of active oxygen species, which are necessary for the catalytic combustion. When the MnOx loading is in-creased to 10%, the catalyst activity is dramatically increased because of the enhanced reducible manganese species. Interestingly, the opti-mal values for reducible manganese species and surface-adsorbed oxygen species can be achieved in the catalyst with 20% MnOx, and so the catalyst exhibits the best catalytic activity, giving a light-off temperature about 179 oC lower than that of the non-catalytic soot combustion. With a further addition of MnOx species up to 30%, its catalytic activity is deteriorated mainly due to the decrease in surface-trapped oxygen species and upper shift of the reduction temperature.