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【催化】福建物構所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:2018-10-15
【催化(hua)(hua)】福建物構(gou)所煤制乙二醇構(gou)筑高(gao)效穩定的銅硅催化(hua)(hua)劑取得新進展


【催化】福建物構所煤制乙二醇構筑高效穩定的銅硅催化劑取得新進展


為了(le)解(jie)決(jue)當前煤制(zhi)乙二醇技(ji)術中(zhong)草(cao)酸酯氫化催化劑存在的(de)鉻污染(ran)和(he)穩(wen)(wen)定(ding)性差的(de)問題,目前研(yan)(yan)發的(de)銅(tong)硅催化劑集(ji)中(zhong)于添加Pd、Pt、Ni、Au、Ag等其他金屬助劑和(he)TiO2、CNTs等載體改(gai)性。中(zhong)科院(yuan)福(fu)建物構研(yan)(yan)究所煤制(zhi)乙二醇實驗室的(de)姚元根(gen)研(yan)(yan)究員領導的(de)煤制(zhi)乙二醇攻關(guan)小(xiao)組在中(zhong)科院(yuan)戰略性先(xian)導科技(ji)專項(A類)和(he)國家留學基(ji)金委(wei)等項目的(de)資助下,基(ji)于金屬有(you)機框(kuang)架材料(MOFs)構筑了(le)一種高效穩(wen)(wen)定(ding)的(de)草(cao)酸酯氫化銅(tong)硅催化劑。

他(ta)們采用(yong)溶膠(jiao)凝膠(jiao)法在(zai)制備過程(cheng)中(zhong)引(yin)入Cu-MOF前(qian)驅(qu)(qu)體(ti)(ti)來調控最終(zhong)催(cui)化(hua)(hua)(hua)劑(ji)中(zhong)銅(tong)(tong)(tong)物(wu)種的(de)(de)(de)尺寸(cun)及(ji)分(fen)散(san)(san)度,改善(shan)一價銅(tong)(tong)(tong)和零價銅(tong)(tong)(tong)的(de)(de)(de)協同(tong)作(zuo)用(yong)提高催(cui)化(hua)(hua)(hua)劑(ji)的(de)(de)(de)催(cui)化(hua)(hua)(hua)性能,所得到的(de)(de)(de)Cu/SiO2-MOF催(cui)化(hua)(hua)(hua)劑(ji)在(zai)草酸(suan)二甲(jia)酯的(de)(de)(de)氫化(hua)(hua)(hua)反(fan)應中(zhong)可以穩(wen)定(ding)(ding)運行220 h,比100 h左右的(de)(de)(de)常規(gui)銅(tong)(tong)(tong)硅(gui)催(cui)化(hua)(hua)(hua)劑(ji)壽命長。溶膠(jiao)凝膠(jiao)法用(yong)于(yu)制備銅(tong)(tong)(tong)含量小于(yu)10%的(de)(de)(de)Cu/SiO2-CN催(cui)化(hua)(hua)(hua)劑(ji)時(shi)(硝酸(suan)銅(tong)(tong)(tong)作(zuo)為前(qian)驅(qu)(qu)體(ti)(ti)),銅(tong)(tong)(tong)物(wu)種可以較(jiao)為均勻地分(fen)散(san)(san)在(zai)硅(gui)膠(jiao)網(wang)絡(luo)中(zhong),但(dan)與此同(tong)時(shi),銅(tong)(tong)(tong)物(wu)種被(bei)硅(gui)膠(jiao)網(wang)絡(luo)包(bao)裹,不易與反(fan)應物(wu)接觸(chu)而(er)活性較(jiao)低。而(er)使(shi)(shi)用(yong)Cu-MOF前(qian)驅(qu)(qu)體(ti)(ti)的(de)(de)(de)優勢在(zai)于(yu)較(jiao)大(da)的(de)(de)(de)空間結構(gou)使(shi)(shi)其不易被(bei)載體(ti)(ti)二氧化(hua)(hua)(hua)硅(gui)網(wang)絡(luo)完全包(bao)裹,在(zai)銅(tong)(tong)(tong)氧硅(gui)界(jie)面(mian)容易暴露更(geng)多的(de)(de)(de)銅(tong)(tong)(tong)活性物(wu)種,又由于(yu)銅(tong)(tong)(tong)含量較(jiao)低也不易引(yin)起銅(tong)(tong)(tong)的(de)(de)(de)團聚,二氧化(hua)(hua)(hua)硅(gui)起到錨(mao)定(ding)(ding)銅(tong)(tong)(tong)物(wu)種的(de)(de)(de)作(zuo)用(yong),從而(er)提高催(cui)化(hua)(hua)(hua)劑(ji)的(de)(de)(de)穩(wen)定(ding)(ding)性。這(zhe)項技術(shu)解決了(le)低銅(tong)(tong)(tong)含量銅(tong)(tong)(tong)分(fen)散(san)(san)好但(dan)包(bao)裹后活性低的(de)(de)(de)難題,提高了(le)低銅(tong)(tong)(tong)含量催(cui)化(hua)(hua)(hua)劑(ji)的(de)(de)(de)活性和穩(wen)定(ding)(ding)性,拓(tuo)寬了(le)MOFs材料的(de)(de)(de)應用(yong)領(ling)域。相關成果近期發表(biao)在(zai)ACS Catalysis上。