Synthesis of Propylene Carbonate from Carbon Dioxide and Propylene Oxide Using Zn-Mg-Al Composite Oxide as High-efficiency Catalyst
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. Am...
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| Published in | Catalysis letters Vol. 136; no. 1-2; pp. 35 - 44 |
|---|---|
| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Boston
Boston : Springer US
01.05.2010
Springer US Springer Springer Nature B.V |
| Subjects | |
| Online Access | Get full text |
| ISSN | 1011-372X 1572-879X |
| DOI | 10.1007/s10562-009-0198-2 |
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| Abstract | 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 NH₃- 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. [graphic removed] |
|---|---|
| AbstractList | 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 CO
2
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 CO
2
-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 CO
2
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. 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 ≤ H0 < 8.9) is beneficial to the cycloaddition reaction. The NH3- 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 AbstractZn-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. 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 CO(2) 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 † < 8.9) is beneficial to the cycloaddition reaction. The NH(3)- and CO(2)-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 CO(2) 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. [graphic removed] 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 C[O.sub.2] 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.sub.0] < 8.9) is beneficial to the cycloaddition reaction. The N[H.sub.3]- and C[O.sub.2]-TPD results also indicate that the Zn-Mg-Al-O catalyst has acid-base bifunctional properties, and a reaction mechanism is proposed. Keywords Zn-Mg-Al-O composite oxide * Propylene carbonate * Propylene oxide * Carbon dioxide * Heterogeneous catalysis 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 NH₃- 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. [graphic removed] 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 C[O.sub.2] 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.sub.0] < 8.9) is beneficial to the cycloaddition reaction. The N[H.sub.3]- and C[O.sub.2]-TPD results also indicate that the Zn-Mg-Al-O catalyst has acid-base bifunctional properties, and a reaction mechanism is proposed. |
| Audience | Academic |
| Author | Au, Chak-Tong Luo, Sheng-Lian Yin, Shuang-Feng Du, Xin Dai, Wei-Li Guo, Rui |
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| Keywords | Propylene oxide Heterogeneous catalysis Zn Al-O composite oxide Propylene carbonate Carbon dioxide Oxides Selectivity Alkaline earth metal Precursor Base Composite material Ammonia Hydrotalcite Propene Synthesis Hydrothermal treatment Zn-Mg-Al-O composite oxide Acids Efficiency Oxirane(methyl) Reaction mechanism pH Alkalinity Carbonates Catalyst |
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| Snippet | 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... 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... |
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| SubjectTerms | Alkaline earth metals Aluminum Ammonia Barium Basicity Calcium Carbon dioxide Carbonates Catalysis Catalysts Chemical industry Chemical synthesis Chemistry Chemistry and Materials Science Cycloaddition Exact sciences and technology General and physical chemistry Heterogeneous catalysis Hydrothermal treatment Industrial Chemistry/Chemical Engineering Magnesium Organometallic Chemistry Physical Chemistry Precursors Propylene Propylene oxide Reaction mechanisms Recyclability Roasting Selectivity Strontium Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Zinc Zinc compounds |
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| Title | Synthesis of Propylene Carbonate from Carbon Dioxide and Propylene Oxide Using Zn-Mg-Al Composite Oxide as High-efficiency Catalyst |
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