物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2014年
11期
2127-2133
,共7页
韩涛%黄伟%王晓东%唐钰%刘双强%游向轩
韓濤%黃偉%王曉東%唐鈺%劉雙彊%遊嚮軒
한도%황위%왕효동%당옥%류쌍강%유향헌
Ce%CuCo/CNTs催化剂%合成气%低碳醇%乙醇
Ce%CuCo/CNTs催化劑%閤成氣%低碳醇%乙醇
Ce%CuCo/CNTs최화제%합성기%저탄순%을순
Ce%CuCo/CNTs catalyst%Syngas%Higher alcohol%Ethanol
采用共浸渍法制备了不同Ce含量的Ce-Cu-Co/CNTs催化剂,考察了其在合成气制低碳醇反应中的催化性能,借助X射线衍射(XRD)、程序升温还原(H2-TPR)、N2吸脱附实验(BET)、透射电镜(TEM)和CO程序升温脱附(CO-TPD)对这些催化剂进行了表征.结果表明,当Ce的质量分数为3%时,低碳醇的时空收率和选择性达到最高,分别为696.4 mg?g-1?h-1和59.7%,其中乙醇占总醇的46.8%,适量Ce的添加能提高Cu物种在催化剂上的分散度和催化剂的还原性能,能显著地增加催化剂吸附CO的能力,促进合成醇活性位的形成,进而明显提高催化剂的活性和总醇的选择性.研究表明,将具有高活性和高碳链增长能力的CuCo基催化剂与碳纳米管的限域效应结合,可实现缩窄产物分布、大幅度提高乙醇选择性的目的.
採用共浸漬法製備瞭不同Ce含量的Ce-Cu-Co/CNTs催化劑,攷察瞭其在閤成氣製低碳醇反應中的催化性能,藉助X射線衍射(XRD)、程序升溫還原(H2-TPR)、N2吸脫附實驗(BET)、透射電鏡(TEM)和CO程序升溫脫附(CO-TPD)對這些催化劑進行瞭錶徵.結果錶明,噹Ce的質量分數為3%時,低碳醇的時空收率和選擇性達到最高,分彆為696.4 mg?g-1?h-1和59.7%,其中乙醇佔總醇的46.8%,適量Ce的添加能提高Cu物種在催化劑上的分散度和催化劑的還原性能,能顯著地增加催化劑吸附CO的能力,促進閤成醇活性位的形成,進而明顯提高催化劑的活性和總醇的選擇性.研究錶明,將具有高活性和高碳鏈增長能力的CuCo基催化劑與碳納米管的限域效應結閤,可實現縮窄產物分佈、大幅度提高乙醇選擇性的目的.
채용공침지법제비료불동Ce함량적Ce-Cu-Co/CNTs최화제,고찰료기재합성기제저탄순반응중적최화성능,차조X사선연사(XRD)、정서승온환원(H2-TPR)、N2흡탈부실험(BET)、투사전경(TEM)화CO정서승온탈부(CO-TPD)대저사최화제진행료표정.결과표명,당Ce적질량분수위3%시,저탄순적시공수솔화선택성체도최고,분별위696.4 mg?g-1?h-1화59.7%,기중을순점총순적46.8%,괄량Ce적첨가능제고Cu물충재최화제상적분산도화최화제적환원성능,능현저지증가최화제흡부CO적능력,촉진합성순활성위적형성,진이명현제고최화제적활성화총순적선택성.연구표명,장구유고활성화고탄련증장능력적CuCo기최화제여탄납미관적한역효응결합,가실현축착산물분포、대폭도제고을순선택성적목적.
A series of Ce-Cu-Co/carbon nanotubes (CNTs) catalysts with different Ce contents were prepared by co-impregnation, and the catalytic performance was investigated for the synthesis of higher alcohols from syngas. The catalysts were characterized by X-ray diffraction (XRD), temperature-programmed reduction of H2 (H2-TPR), N2 adsorption-desorption isotherms (BET), transmission electron microscopy (TEM), and temperature-programmed desorption of CO (CO-TPD). The results showed that at a Ce content of 3%the catalyst had the highest catalytic activity. The formation rate and selectivity of alcohol reached 696.4 mg?g-1?h-1 and 59.7%, where the mass fraction of ethanol was 46.8%of the total amount of alcohols. The addition of an appropriate amount of Ce facilitated the dispersion of Cu and promoted reduction of the catalysts. It also markedly increased the adsorption capacity for CO, and significantly improved the formation of active sites for alcohols, which is favorable for the catalytic activity and to improve the selectivity of alcohols. Research showed that combining the CuCo-based catalyst, which has high activity and a high ability of carbon chain growth, with the confinement effect of CNTs can result in a narrow distribution of alcohols and significantly improve the selectivity of ethanol.