化工学报
化工學報
화공학보
JOURNAL OF CHEMICAL INDUSY AND ENGINEERING (CHINA)
2015年
2期
88-96
,共9页
张光洁%耿艳楼%安华良%赵新强%王延吉
張光潔%耿豔樓%安華良%趙新彊%王延吉
장광길%경염루%안화량%조신강%왕연길
1,2-丙二醇%二氧化碳%碳酸丙烯酯%固定床%催化剂%反应机理
1,2-丙二醇%二氧化碳%碳痠丙烯酯%固定床%催化劑%反應機理
1,2-병이순%이양화탄%탄산병희지%고정상%최화제%반응궤리
1,2-propylene glycol%carbon dioxide%propylene carbonate%fixed-bed%catalyst%reaction mechanism
以负载型乙酸锌为催化剂,在固定床上实现了CO2和1,2-丙二醇(PG)合成碳酸丙烯酯(PC)反应。考察了不同载体和负载量对负载型乙酸锌催化性能的影响以及反应条件对 PC 合成反应的影响。结果表明:负载量为40%(质量分数)的Zn(OAc)2/AC催化性能最好。CO2与PG合成PC适宜的反应条件为:PG、乙腈和CO2的摩尔比为1:1.8:11,CO2压力4.0 MPa,反应温度160℃和液空速0.9 h?1。在此条件下,PC收率和选择性分别为6.3%和49.0%。采用原位红外结合设计实验研究了无水乙酸锌分别与CO2和PG之间的相互作用,发现CO2与乙酸锌之间的化学吸附比较弱,而PG与乙酸锌之间的化学吸附较强,能够活化PG。据此推测了乙酸锌催化CO2与PG合成PC的反应机理。
以負載型乙痠鋅為催化劑,在固定床上實現瞭CO2和1,2-丙二醇(PG)閤成碳痠丙烯酯(PC)反應。攷察瞭不同載體和負載量對負載型乙痠鋅催化性能的影響以及反應條件對 PC 閤成反應的影響。結果錶明:負載量為40%(質量分數)的Zn(OAc)2/AC催化性能最好。CO2與PG閤成PC適宜的反應條件為:PG、乙腈和CO2的摩爾比為1:1.8:11,CO2壓力4.0 MPa,反應溫度160℃和液空速0.9 h?1。在此條件下,PC收率和選擇性分彆為6.3%和49.0%。採用原位紅外結閤設計實驗研究瞭無水乙痠鋅分彆與CO2和PG之間的相互作用,髮現CO2與乙痠鋅之間的化學吸附比較弱,而PG與乙痠鋅之間的化學吸附較彊,能夠活化PG。據此推測瞭乙痠鋅催化CO2與PG閤成PC的反應機理。
이부재형을산자위최화제,재고정상상실현료CO2화1,2-병이순(PG)합성탄산병희지(PC)반응。고찰료불동재체화부재량대부재형을산자최화성능적영향이급반응조건대 PC 합성반응적영향。결과표명:부재량위40%(질량분수)적Zn(OAc)2/AC최화성능최호。CO2여PG합성PC괄의적반응조건위:PG、을정화CO2적마이비위1:1.8:11,CO2압력4.0 MPa,반응온도160℃화액공속0.9 h?1。재차조건하,PC수솔화선택성분별위6.3%화49.0%。채용원위홍외결합설계실험연구료무수을산자분별여CO2화PG지간적상호작용,발현CO2여을산자지간적화학흡부비교약,이PG여을산자지간적화학흡부교강,능구활화PG。거차추측료을산자최화CO2여PG합성PC적반응궤리。
Propylene carbonate (PC) was synthesized on a fixed-bed reactor from CO2 and propylene glycol (PG) catalyzed by supported Zn(OAc)2 catalyst. Then the effect of the kind of carrier and its loading on the catalytic performance and the influence of reaction conditions on PC synthesis reaction were investigated. The results indicates that Zn(OAc)2/AC with loading of 40%(mass) shows better catalytic performance. The suitable reaction conditions are obtained as follows: molar ratio of PG to acetonitrile(solvent) to CO2 is 1:1.8:11, reaction temperature 160℃, CO2 pressure 4.0 MPa and LHSV 0.9 h?1. Under the above conditions, the yield and selectivity of PC were 6.3% and 49.0%, respectively. The interaction between Zn(OAc)2 and CO2 or PG was investigated by in-situ IR technique combined with some designed experiments. It was found that the chemical adsorption of CO2 on Zn(OAc)2 is weaker while it is much stronger between PG and Zn(OAc)2. Chemical bond between PG and Zn(OAc)2 is found, indicating that Zn(OAc)2 can activate PG in this reaction. Accordingly, the role of Zn(OAc)2 in the catalytic reaction of CO2 and PG to PC is elucidated.