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重庆大学 化学化工学院,重庆 401331
余结贞(1999—),硕士研究生,研究方向为催化作用,E-mail:2324322194@qq.com。
杜军(1964—),博士,教授,博士研究生导师,研究方向为催化过程与催化材料、环境催化与污染物控制,E-mail:dujune@cqu.edu.cn。
收稿:2025-05-16,
修回:2025-05-23,
网络出版:2026-01-04,
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余结贞,陶长元,杜军.MTiO3型复合催化剂催化尿素醇解制碳酸丙烯酯性能[J].低碳化学与化工,
YU Jiezhen,TAO Changyuan,DU Jun.Catalytic performances of MTiO3-type composite catalysts for urea alcoholysis to propylene carbonate[J].Low-Carbon Chemistry and Chemical Engineering,
余结贞,陶长元,杜军.MTiO3型复合催化剂催化尿素醇解制碳酸丙烯酯性能[J].低碳化学与化工, DOI:10.12434/j.issn.2097-2547.20250228.
YU Jiezhen,TAO Changyuan,DU Jun.Catalytic performances of MTiO3-type composite catalysts for urea alcoholysis to propylene carbonate[J].Low-Carbon Chemistry and Chemical Engineering, DOI:10.12434/j.issn.2097-2547.20250228.
碳酸丙烯酯(PC)在电池、化工领域应用广泛。尿素醇解法制PC具有原料廉价易得、反应条件温和等特点,具有广阔的工业应用前景。然而,常用的金属氧化物催化剂具有活性组分流失严重、重复使用性能差等问题,严重限制了尿素醇解法的工业化发展,亟需开发兼具高活性与稳定性的催化剂。采用溶胶凝胶法制备了MTiO
3
型复合催化剂,通过TGA-DSC、XRD和SEM等多种表征手段,研究了制备条件对催化剂结构和催化尿素醇解制PC性能的影响,并优化了反应条件。结果表明,经750 ℃焙烧制备的MgTiO
3
-750催化活性最佳,在反应温度170 ℃、反应时间3 h、
n
(1
2-丙二醇):
n
(尿素) = 1.5:1.0和催化剂质量分数1%条件下,PC产率达91.2%。该条件下重复使用5次MgTiO
3
-750,其PC产率可维持在80.0%~90.0%。进一步构建了复合催化剂MgTiO
3
+ ZnO,发现通过MgTiO
3
+ ZnO中的中强碱位点协同作用,在相同反应条件下PC产率提升至95.7%,重复使用多次MgTiO
3
+ ZnO,其PC产率仍超91.0%,且通过补充ZnO进行再生处理可恢复催化剂催化活性。
Propylene carbonate (PC) is widely used in battery and chemical industry. Urea alcoholysis to PC has a broad industrial application prospect with the features of cheap and easy-to-obtain raw materials
mild reaction conditions
etc. However
the commonly used metal oxide catalysts suffer from serious loss of active components and poor reproducibility
which severely limit the industrial development of urea alcoholysis method
so it is urgent to develop catalysts with both high activity and stability. MTiO
3
-type composite catalysts were prepared by sol-gel method
and the effects of preparation conditions on the structures and catalytic performances for urea alcoholysis to PC of catalysts were studied by various characterization methods
such as TGA-DSC
XRD
SEM
etc.
and the reaction conditions were optimized. The results show that MgTiO
3
-750 calcined at 750 ℃ shows the best catalytic activity. Under the conditions of reaction temperature of 170 ℃
reaction time of 3 h
n
(1
2-propanediol):
n
(urea) = 1.5:1.0 and catalyst’s mass fraction of 1%
the PC yield reaches 91.2%. The PC yield maintains from 80.0% to 90.0% catalyzed by MgTiO
3
-750 reused five times under the same conditions. The composite catalyst MgTiO
3
+ ZnO was further constructed. It is found that through the synergistic effect of medium-strong base sites in MgTiO
3
+ ZnO
the PC yield increases to 95.7% under the same reaction conditions. What’s more
the PC yield still exceeds 91.0% catalyzed by MgTiO
3
+ ZnO reused multiple times. The catalytic activity can be restored by supplementing ZnO for regeneration treatment.
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