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加氫催化劑,羰化合成催化劑,煤制乙二醇催化劑

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煤制乙二醇構筑高效穩定的銅硅催化劑取得新進展

瀏覽次數: 日期:2018-09-19
為了(le)解決當(dang)前煤(mei)(mei)制乙二醇(chun)技(ji)術中(zhong)草酸(suan)酯氫化催化劑存在(zai)的鉻(ge)污染和穩定性(xing)差的問題,目前研發的銅硅催化劑集(ji)中(zhong)于(yu)添(tian)加Pd、Pt、Ni、Au、Ag等(deng)其他(ta)金屬(shu)(shu)助劑和TiO2、CNTs等(deng)載體改(gai)性(xing)。中(zhong)科院福建物構研究所煤(mei)(mei)制乙二醇(chun)實(shi)驗(yan)室的姚元根研究員(yuan)領導(dao)的煤(mei)(mei)制乙二醇(chun)攻關小組在(zai)中(zhong)科院戰略性(xing)先導(dao)科技(ji)專項(xiang)(A類)和國家留學基金委等(deng)項(xiang)目的資助下,基于(yu)金屬(shu)(shu)有機框架材料(MOFs)構筑了(le)一種(zhong)高效穩定的草酸(suan)酯氫化銅硅催化劑。


煤制乙二醇催化劑


他們(men)采用溶膠(jiao)(jiao)(jiao)凝(ning)膠(jiao)(jiao)(jiao)法(fa)(fa)在(zai)制備過(guo)程中(zhong)引(yin)入(ru)Cu-MOF前驅體(ti)來調控最終催化(hua)劑(ji)(ji)中(zhong)銅(tong)(tong)(tong)(tong)物種(zhong)的(de)(de)(de)尺寸(cun)及分(fen)散度,改善一(yi)價銅(tong)(tong)(tong)(tong)和零價銅(tong)(tong)(tong)(tong)的(de)(de)(de)協同(tong)作(zuo)用提高(gao)催化(hua)劑(ji)(ji)的(de)(de)(de)催化(hua)性(xing)(xing)(xing)能,所得到(dao)的(de)(de)(de)Cu/SiO2-MOF催化(hua)劑(ji)(ji)在(zai)草酸二甲酯的(de)(de)(de)氫化(hua)反應(ying)中(zhong)可以穩(wen)定(ding)運行220 h,比100 h左右的(de)(de)(de)常(chang)規銅(tong)(tong)(tong)(tong)硅(gui)催化(hua)劑(ji)(ji)壽(shou)命長。溶膠(jiao)(jiao)(jiao)凝(ning)膠(jiao)(jiao)(jiao)法(fa)(fa)用于制備銅(tong)(tong)(tong)(tong)含量(liang)小于10%的(de)(de)(de)Cu/SiO2-CN催化(hua)劑(ji)(ji)時(shi)(shi)(硝酸銅(tong)(tong)(tong)(tong)作(zuo)為前驅體(ti)),銅(tong)(tong)(tong)(tong)物種(zhong)可以較為均勻地分(fen)散在(zai)硅(gui)膠(jiao)(jiao)(jiao)網(wang)絡(luo)中(zhong),但與此同(tong)時(shi)(shi),銅(tong)(tong)(tong)(tong)物種(zhong)被(bei)硅(gui)膠(jiao)(jiao)(jiao)網(wang)絡(luo)包裹(guo)(guo),不(bu)易(yi)與反應(ying)物接觸而活性(xing)(xing)(xing)較低(di)。而使用Cu-MOF前驅體(ti)的(de)(de)(de)優(you)勢在(zai)于較大的(de)(de)(de)空間(jian)結構使其不(bu)易(yi)被(bei)載(zai)體(ti)二氧(yang)化(hua)硅(gui)網(wang)絡(luo)完全(quan)包裹(guo)(guo),在(zai)銅(tong)(tong)(tong)(tong)氧(yang)硅(gui)界面容(rong)易(yi)暴露(lu)更多的(de)(de)(de)銅(tong)(tong)(tong)(tong)活性(xing)(xing)(xing)物種(zhong),又由于銅(tong)(tong)(tong)(tong)含量(liang)較低(di)也不(bu)易(yi)引(yin)起(qi)銅(tong)(tong)(tong)(tong)的(de)(de)(de)團聚(ju),二氧(yang)化(hua)硅(gui)起(qi)到(dao)錨(mao)定(ding)銅(tong)(tong)(tong)(tong)物種(zhong)的(de)(de)(de)作(zuo)用,從而提高(gao)催化(hua)劑(ji)(ji)的(de)(de)(de)穩(wen)定(ding)性(xing)(xing)(xing)。這項技術解決(jue)了(le)低(di)銅(tong)(tong)(tong)(tong)含量(liang)銅(tong)(tong)(tong)(tong)分(fen)散好但包裹(guo)(guo)后(hou)活性(xing)(xing)(xing)低(di)的(de)(de)(de)難題,提高(gao)了(le)低(di)銅(tong)(tong)(tong)(tong)含量(liang)催化(hua)劑(ji)(ji)的(de)(de)(de)活性(xing)(xing)(xing)和穩(wen)定(ding)性(xing)(xing)(xing),拓寬了(le)MOFs材料的(de)(de)(de)應(ying)用領域。相關成果(guo)近期發表在(zai)ACS Catalysis上。