摘要
针对甲醇气相氧化羰基化直接合成碳酸二甲酯(DMC)反应中催化剂活性低和稳定性差的问题,制备了一系列氧化石墨烯复合金属催化剂,并对其进行活性评价。结果表明:催化剂PdCl_2-CuCl_2-KOAc/AC@GO-HCl表现出最佳的催化活性和稳定性:DMC的空时收率(STY)为800～900 g·(L cat)^(-1)·h^(-1),且反应16 h内活性无明显下降;甲醇选择性保持在95%以上,CO选择性为35%～40%。结合XRD和XPS表征发现,活性物种Cu_2Cl(OH)_3的生成,提高了催化剂催化活性,而CuO和KCl均可导致催化剂的失活。
A series of graphene oxide composite metal catalysts were prepared and evaluated for their activity in the direct synthesis of dimethyl carbonate(DMC)by methanol vapor phase oxidative carbonylation.The results show that the catalyst PdCl2-CuCl2-KOAc/AC@GO-HCl has the best catalytic activity and stability.The space time yield(STY)of DMC was between 800-900 g·(L cat)^-1·h^-1,and the catalytic activity was stable in 16 h without significant decrease.Methanol selectivity was maintained above 95%,and CO selectivity was between 35%-40%.Combined with results of XRD and XPS analyses,it was found that the formation of the active species Cu2Cl(OH)3 improved the catalytic activity of the catalyst,while both CuO and KCl could cause the deactivation of the catalyst.
作者
宋宇淙
丁晓墅
闫亚辉
王淑芳
王延吉
SONG Yucong;DING Xiaoshu;YAN Yahui;WANG Shufang;WANG Yanji(Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficiency Energy Saving,School of Chemical Engineering and Technology,Hebei University of Technology,Tianjin 300130,China;China Shipbuilding Industry Corp.,Handan 056027,Hebei,China)
出处
《化工学报》
EI
CAS
CSCD
北大核心
2019年第4期1401-1408,共8页
CIESC Journal
基金
国家青年自然科学基金项目(21606070)
河北省青年科学基金项目(B2016202256)
国家自然科学基金重点项目(21236001)
国家自然科学基金项目(21576069)
关键词
氧化石墨烯
催化剂
固定床
多相反应
氧化羰基化
graphene oxide
catalyst
fixed-bed
multiphase reaction
oxidative carbonylation
