TY - JOUR
T1 - Synthesis of propylene carbonate from carbon dioxide and propylene oxide using Zn-Mg-Al composite oxide as high-efficiency catalyst
AU - Dai, Wei Li
AU - Yin, Shuang Feng
AU - Guo, Rui
AU - Luo, Sheng Lian
AU - Du, Xin
AU - Au, Chak Tong
N1 - Funding Information:
Acknowledgments This work was financially supported by the National Natural Science Foundation of China (Grant Nos 20873038 and 20507005), Outstanding Young Research Award of National Natural Science Foundation of China (Grant No E50725825), and National 863 Program of China (2009AA05Z319). CTA thanks the Hunan University for an adjunct professorship and the Hong Kong Baptist University for financial support (FRG/08-09/II-09).
PY - 2010/5
Y1 - 2010/5
N2 - A series of Zn-Al composite oxides that were modified with alkaline earth metals, Zn-M-Al-O (M = Mg, Ca, Sr, and Ba) were fabricated via calcination of the corresponding hydrotalcite precursors, and evaluated as catalysts for the synthesis of propylene carbonate (PC) from CO2 and propylene oxide. Among the Zn-M-Al-O catalysts, Zn-Mg-Al-O (Zn/Mg = 4.0, pH = 10, without hydrothermal treatment) is the best in performance, showing PC selectivity of 99.2% and yield of 88.8% (140 °C, 12 h). Furthermore, the Zn-Mg-Al-O catalyst can be readily reused and recycled without any loss of activity in a test of five cycles. Through detailed studies of the basic nature of the Zn-M-Al-O catalysts, it was found that a moderate basicity (6.1 ≤ H 0 < 8.9) is beneficial to the cycloaddition reaction. The NH 3- and CO2-TPD results also indicate that the Zn-Mg-Al-O catalyst has acid-base bifunctional properties, and a reaction mechanism is proposed. Graphic Abstract: Zn-Mg-Al composite oxides were prepared via calcination of the corresponding hydrotalcite precursors, and used as catalysts for the synthesis of propylene carbonate from CO2 and propylene oxide. We achieved high catalytic efficiency under mild conditions, easy separation of catalyst from the product, and good recyclability of the catalyst. A plausible reaction mechanism has been proposed for the catalytic action.
AB - A series of Zn-Al composite oxides that were modified with alkaline earth metals, Zn-M-Al-O (M = Mg, Ca, Sr, and Ba) were fabricated via calcination of the corresponding hydrotalcite precursors, and evaluated as catalysts for the synthesis of propylene carbonate (PC) from CO2 and propylene oxide. Among the Zn-M-Al-O catalysts, Zn-Mg-Al-O (Zn/Mg = 4.0, pH = 10, without hydrothermal treatment) is the best in performance, showing PC selectivity of 99.2% and yield of 88.8% (140 °C, 12 h). Furthermore, the Zn-Mg-Al-O catalyst can be readily reused and recycled without any loss of activity in a test of five cycles. Through detailed studies of the basic nature of the Zn-M-Al-O catalysts, it was found that a moderate basicity (6.1 ≤ H 0 < 8.9) is beneficial to the cycloaddition reaction. The NH 3- and CO2-TPD results also indicate that the Zn-Mg-Al-O catalyst has acid-base bifunctional properties, and a reaction mechanism is proposed. Graphic Abstract: Zn-Mg-Al composite oxides were prepared via calcination of the corresponding hydrotalcite precursors, and used as catalysts for the synthesis of propylene carbonate from CO2 and propylene oxide. We achieved high catalytic efficiency under mild conditions, easy separation of catalyst from the product, and good recyclability of the catalyst. A plausible reaction mechanism has been proposed for the catalytic action.
KW - Carbon dioxide
KW - Heterogeneous catalysis
KW - Propylene carbonate
KW - Propylene oxide
KW - Zn-Mg-Al-O composite oxide
UR - http://www.scopus.com/inward/record.url?scp=77951620508&partnerID=8YFLogxK
U2 - 10.1007/s10562-009-0198-2
DO - 10.1007/s10562-009-0198-2
M3 - Journal article
AN - SCOPUS:77951620508
SN - 1011-372X
VL - 136
SP - 35
EP - 44
JO - Catalysis Letters
JF - Catalysis Letters
IS - 1-2
ER -