投稿范围:煤化(hua)工(gong)(gong)(gong)(gong)(gong)、盐化(hua)工(gong)(gong)(gong)(gong)(gong)、生物化(hua)工(gong)(gong)(gong)(gong)(gong)、医(yi)药化(hua)工(gong)(gong)(gong)(gong)(gong)、石油(you)化(hua)工(gong)(gong)(gong)(gong)(gong)、农用化(hua)工(gong)(gong)(gong)(gong)(gong)、化(hua)工(gong)(gong)(gong)(gong)(gong)环保、工(gong)(gong)(gong)(gong)(gong)业(ye)水处理、精细化(hua)工(gong)(gong)(gong)(gong)(gong)、日用化(hua)工(gong)(gong)(gong)(gong)(gong)、燃气化(hua)工(gong)(gong)(gong)(gong)(gong)、橡胶与(yu)(yu)轮胎工(gong)(gong)(gong)(gong)(gong)业(ye)、化(hua)肥(fei)农药、有机与(yu)(yu)无(wu)机、涂料(liao)与(yu)(yu)油(you)墨、染(ran)料(liao)与(yu)(yu)颜(yan)料(liao)、助剂(ji)与(yu)(yu)添加剂(ji)、树(shu)脂与(yu)(yu)塑料(liao)、胶粘(zhan)剂(ji)、化(hua)工(gong)(gong)(gong)(gong)(gong)教育、化(hua)工(gong)(gong)(gong)(gong)(gong)设计、化(hua)工(gong)(gong)(gong)(gong)(gong)机械与(yu)(yu)装备
近日(ri),中国科(ke)(ke)学(xue)院(yuan)大(da)连化(hua)学(xue)物理研究(jiu)所(suo)催化(hua)基础国家重点实验室研究(jiu)员(yuan)傅强(qiang)与中科(ke)(ke)院(yuan)院(yuan)士(shi)包信和团(tuan)队,在(zai)金属(shu)(shu)与载(zai)体界面催化(hua)研究(jiu)方面取得(de)新进展。研究(jiu)发(fa)现过渡金属(shu)(shu)催化(hua)剂与惰性(xing)的(de)(de)六方氮化(hua)硼(peng)(h-BN)载(zai)体之(zhi)间存在(zai)经典的(de)(de)金属(shu)(shu)-载(zai)体强(qiang)相互(hu)作用(Strong Metal-Support Interaction, SMSI)。
金属(shu)-载(zai)体(ti)强相(xiang)互(hu)作用是多相(xiang)催(cui)化研(yan)究领域中的(de)(de)(de)重要概念之一。该现象是指当金属(shu)担载(zai)于活性的(de)(de)(de)可还(hai)原氧化物载(zai)体(ti)上时,在一定(ding)的(de)(de)(de)预(yu)处理或催(cui)化反应条件下,金属(shu)纳米粒(li)子被载(zai)体(ti)衍生的(de)(de)(de)材料包裹(guo)和去包裹(guo)的(de)(de)(de)过(guo)程,以及(ji)由此对(dui)催(cui)化反应性能产(chan)生的(de)(de)(de)重要影响(xiang)。
研究发现,惰性的h-BN片层负载金属Ni催化剂在甲烷二氧化碳干重整(DRM)反应中表现出优异的性能,原位表征证明反应气氛中的CO2和H2O组分可以促进Ni/h-BN界面处h-BN片层被氧化刻蚀形成纳米孔洞(nanopits)结构,同时Ni粒子表面被氧化硼(BOx)薄层包裹;包裹和去包裹过程可以通过DRM反应和H2还原进(jin)行可逆控(kong)制,呈现出经典的(de)(de)SMSI现象。这(zhei)(zhei)是首(shou)次在惰性(xing)的(de)(de)非(fei)氧化(hua)物(wu)载体担载金(jin)(jin)属(shu)催(cui)化(hua)剂中(zhong)发现这(zhei)(zhei)一现象,在h-BN担载的(de)(de)其他过(guo)渡金(jin)(jin)属(shu)催(cui)化(hua)剂如Fe、Co和(he)(he)Ru中(zhong)也普遍存(cun)在。此外,金(jin)(jin)属(shu)/h-BN体系中(zhong)发生的(de)(de)DRM反(fan)应诱导SMSI效应会增(zeng)强该催(cui)化(hua)过(guo)程,实(shi)验和(he)(he)理(li)论计算(suan)结果表(biao)(biao)明,界(jie)面处的(de)(de)载体通(tong)过(guo)刻蚀形成的(de)(de)纳米(mi)孔(kong)洞限域金(jin)(jin)属(shu)粒(li)(li)子并阻止(zhi)其团聚,同时金(jin)(jin)属(shu)粒(li)(li)子表(biao)(biao)面形成的(de)(de)无定形BOx包裹层与金(jin)(jin)属(shu)协同作用,使得Ni/h-BN催(cui)化(hua)剂同时具有抗(kang)积碳和(he)(he)抗(kang)烧结的(de)(de)性(xing)能。
相关研(yan)(yan)究(jiu)成果发表(biao)在上。研(yan)(yan)究(jiu)工作(zuo)得到国(guo)家自然(ran)科(ke)学基金科(ke)学中心、科(ke)技部重点研(yan)(yan)发计划、中科(ke)院(yuan)战略性先导科(ke)技专项(B类)及洁净能源(yuan)创(chuang)新研(yan)(yan)究(jiu)院(yuan)合作(zuo)基金等的资助。
大连化物(wu)所发(fa)现金属(shu)与惰性(xing)非氧化物(wu)载体之间的金属(shu)-载体强相互作用