物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2015年
5期
948-954
,共7页
张晓晴%徐艳%杨春辉%张燕平%印永祥%尚书勇
張曉晴%徐豔%楊春輝%張燕平%印永祥%尚書勇
장효청%서염%양춘휘%장연평%인영상%상서용
甲烷二氧化碳重整%水滑石%镍基催化剂%催化活性%稳定性%抗积碳性
甲烷二氧化碳重整%水滑石%鎳基催化劑%催化活性%穩定性%抗積碳性
갑완이양화탄중정%수활석%얼기최화제%최화활성%은정성%항적탄성
Dry reforming of methane%Layered double hydroxide%Ni-based catalyst%Catalytic activity%Stability%Coke resistance
通过原位共沉淀的方法在γ-Al2O3表面上合成了Ni-Mg-Al-LDHs (水滑石),合成的Ni-Mg-Al-LDHs/γ-Al2O3作为催化前驱体经过不同的热处理还原方式得到催化剂Cat-1、Cat-2和Cat-3.用X射线衍射(XRD)、透射电镜(TEM)、N2吸附-脱附测试(BET)以及热重-差热分析(TG-DTA)对催化剂的形貌结构和抗积碳能力进行了表征测试;通过甲烷二氧化碳重整反应体系对催化剂的反应活性和稳定性进行了评价.结果表明催化剂前驱体的预处理方式对催化剂的反应性能具有较大的影响. Ni-Mg-Al-LDHs/γ-Al2O3直接经过H2/Ar常压高频冷等离子体炬的分解还原所获得的催化剂Cat-3表现出了最佳的催化活性和稳定性. TEM表征表明催化活性组分在Cat-3上的分散性更好,颗粒粒径更小. BET结果证明Cat-3具备较大的比表面积(195.8 m2?g-1). Ni-Mg-Al水滑石的结构赋予了催化剂活性组分在载体γ-Al2O3上均匀的分散性,同时常压高频冷等离体炬对催化剂的表面结构以及活性组分的还原具有进一步的优化作用,两者的协同作用使Ni-Mg-Al-LDHs/γ-Al2O3在甲烷二氧化碳反应体系中具备优良的催化活性和抗积碳性能.
通過原位共沉澱的方法在γ-Al2O3錶麵上閤成瞭Ni-Mg-Al-LDHs (水滑石),閤成的Ni-Mg-Al-LDHs/γ-Al2O3作為催化前驅體經過不同的熱處理還原方式得到催化劑Cat-1、Cat-2和Cat-3.用X射線衍射(XRD)、透射電鏡(TEM)、N2吸附-脫附測試(BET)以及熱重-差熱分析(TG-DTA)對催化劑的形貌結構和抗積碳能力進行瞭錶徵測試;通過甲烷二氧化碳重整反應體繫對催化劑的反應活性和穩定性進行瞭評價.結果錶明催化劑前驅體的預處理方式對催化劑的反應性能具有較大的影響. Ni-Mg-Al-LDHs/γ-Al2O3直接經過H2/Ar常壓高頻冷等離子體炬的分解還原所穫得的催化劑Cat-3錶現齣瞭最佳的催化活性和穩定性. TEM錶徵錶明催化活性組分在Cat-3上的分散性更好,顆粒粒徑更小. BET結果證明Cat-3具備較大的比錶麵積(195.8 m2?g-1). Ni-Mg-Al水滑石的結構賦予瞭催化劑活性組分在載體γ-Al2O3上均勻的分散性,同時常壓高頻冷等離體炬對催化劑的錶麵結構以及活性組分的還原具有進一步的優化作用,兩者的協同作用使Ni-Mg-Al-LDHs/γ-Al2O3在甲烷二氧化碳反應體繫中具備優良的催化活性和抗積碳性能.
통과원위공침정적방법재γ-Al2O3표면상합성료Ni-Mg-Al-LDHs (수활석),합성적Ni-Mg-Al-LDHs/γ-Al2O3작위최화전구체경과불동적열처리환원방식득도최화제Cat-1、Cat-2화Cat-3.용X사선연사(XRD)、투사전경(TEM)、N2흡부-탈부측시(BET)이급열중-차열분석(TG-DTA)대최화제적형모결구화항적탄능력진행료표정측시;통과갑완이양화탄중정반응체계대최화제적반응활성화은정성진행료평개.결과표명최화제전구체적예처리방식대최화제적반응성능구유교대적영향. Ni-Mg-Al-LDHs/γ-Al2O3직접경과H2/Ar상압고빈랭등리자체거적분해환원소획득적최화제Cat-3표현출료최가적최화활성화은정성. TEM표정표명최화활성조분재Cat-3상적분산성경호,과립립경경소. BET결과증명Cat-3구비교대적비표면적(195.8 m2?g-1). Ni-Mg-Al수활석적결구부여료최화제활성조분재재체γ-Al2O3상균균적분산성,동시상압고빈랭등리체거대최화제적표면결구이급활성조분적환원구유진일보적우화작용,량자적협동작용사Ni-Mg-Al-LDHs/γ-Al2O3재갑완이양화탄반응체계중구비우량적최화활성화항적탄성능.
A series of novel catalysts derived from Ni-Mg-Al-LDHs (LDHs:layered double hydroxides) were synthesized in-situ onγ-Al2O3 and evaluated in CO2 reforming of CH4 (dry reforming of methane, DRM) reaction system. The catalytic precursors were decomposed and reduced by calcination and an atmospheric plasma technique, respectively. Activity and stability tests showed that the catalytic properties were greatly affected by the pretreatment method. The best catalytic performance was obtained with the catalyst that was directly reduced and decomposed using an atmospheric H2/Ar plasma jet. Compared with the pure LDH precursor, Ni-Mg-Al-LDHs/γ-Al2O3 had much greater mechanical strength, because of theγ-Al2O3 support. This feature extends the long lifetime of catalyst at high temperatures. X-ray diffraction (XRD), transmission electron microscopy (TEM), N2-adsorption-desorption, and thermogravimetry-differential thermal analysis (TG-DTA) results showed that the excel ent catalytic performance was based on the smal particle size and uniform dispersion of active Ni crystals, as wel as the high mechanical strength and large specific surface area of the catalyst.