非均相羰基氧化一步合成碳酸二苯酯的研究(Ⅴ)筛选催化剂及优化合成条件

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非均相羰基氧化一步合成碳酸二苯酯的研究(Ⅴ)筛选催化剂及优化合成条件

张光旭^a,b; 吴元欣^b; 马沛生^a; 田崎峰^b; 吴广文^b; 李定或^b; 王存文^b

^a State Key Laboratory of C1 Chemistry and Technology, Tianjin University, Tianjin,300072,
China
^b Department of Chemical Engineering, Wuhan Institute of Chemical Technology, Wuhan,430074,
China

收稿日期:1900-01-01 修回日期:1900-01-01 出版日期:2003-10-28 发布日期:2003-10-28
通讯作者: 张光旭

Study on Direct Synthesis of Diphenyl Carbonate with Heterogeneous Catalytic Reaction (Ⅴ)
Screening Catalysts and Optimizing Synthesis Conditions

ZHANG Guangxu^a,b; WU Yuanxin^b; MA Peisheng^a; TIAN Qifeng^b; WU Guangwen^b; Li Dinghuo^b; WANG Cunwen^b

^a State Key Laboratory of C1 Chemistry and Technology, Tianjin University, Tianjin,300072,
China
^b Department of Chemical Engineering, Wuhan Institute of Chemical Technology, Wuhan,430074,
China

Received:1900-01-01 Revised:1900-01-01 Online:2003-10-28 Published:2003-10-28
Contact: ZHANG Guangxu

摘要/Abstract

摘要： Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct
synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and
the results of DPC synthesis indicated that the catalyst Pd/LaxPbyMnOz had higher activity.
The Pd/LaxPbyMnOz catalyst and the support was characterized by XRD, SEM and TEM, the main
phase was La0.62Pb0.38MnO3 and the average diameter could be about 25.4nm. The optimum
conditions for synthesis of DPC with Pd/LaxPbyMnOz were determined by orthogonal
experiments and the experimental results showed that reaction temperature was the first
factor of effect on the selectivity and yield of DPC, and the concentration of O2 in gas
phase also had significant effect on selectivity of DPC. The optimum reaction conditions
were catalyst/phenol mass ratio 1 to 50, pressure 4.5 MPa,volume concentration of O2 25%,
reaction temperature 60℃ and reaction time 4 h. The maximum yield and average selectivity
could reach 13% and 97% respectively in the batch operation.

关键词: diphenyl carbonate;supported catalyst;heterogeneous catalytic reaction;optimum conditions

Abstract: Pd/LaxPbyMnOz, Pd/C, Pd/molecular sieve and Pd-heteropoly acid catalysts for direct
synthesis of diphenyl carbonate (DPC) by heterogeneous catalytic reaction were compared and
the results of DPC synthesis indicated that the catalyst Pd/LaxPbyMnOz had higher activity.
The Pd/LaxPbyMnOz catalyst and the support was characterized by XRD, SEM and TEM, the main
phase was La0.62Pb0.38MnO3 and the average diameter could be about 25.4nm. The optimum
conditions for synthesis of DPC with Pd/LaxPbyMnOz were determined by orthogonal
experiments and the experimental results showed that reaction temperature was the first
factor of effect on the selectivity and yield of DPC, and the concentration of O2 in gas
phase also had significant effect on selectivity of DPC. The optimum reaction conditions
were catalyst/phenol mass ratio 1 to 50, pressure 4.5 MPa,volume concentration of O2 25%,
reaction temperature 60℃ and reaction time 4 h. The maximum yield and average selectivity
could reach 13% and 97% respectively in the batch operation.

Key words: diphenyl carbonate, supported catalyst, heterogeneous catalytic reaction, optimum conditions

张光旭, 吴元欣, 马沛生, 田崎峰, 吴广文, 李定或, 王存文. 非均相羰基氧化一步合成碳酸二苯酯的研究(Ⅴ)筛选催化剂及优化合成条件[J]. CIESC Journal.

ZHANG Guangxu, WU Yuanxin, MA Peisheng, TIAN Qifeng, WU Guangwen, Li Dinghuo, WANG Cunwen. Study on Direct Synthesis of Diphenyl Carbonate with Heterogeneous Catalytic Reaction (Ⅴ)
Screening Catalysts and Optimizing Synthesis Conditions[J]. .

参考文献

[1] Takagi, M., Miyagi, H., Yoneyama, T., Ohgomori, Y.,"Palladium-lead catalyzed oxidative
of phenol" , J. Mol.Cat. A: Chem., 129, L1-L3 (1998).
[2] Meenakshi, G., Ritsuko, N., Sugiyama, J.I., Michihiko, A.,Mitsuru, U., "Direct
synthesis of diphenyl carbonate by oxidative carbonylation of phenol using Pd-Cu based
redox catalyst", J. Mol. Cat. A: Chem., 137, 147-154 (1999).
[3] Meenakshi, G., Ritsuko, N., Sugiyama, J.I., Michihiko, A.,Mitsuru, U., "Effect of
inorganic redox cocatalyst on Pdcatalyzed for direct synthesis of diphenyl carbonate",
Cat.Lett., 54, 29-31 (1998).
[4] Hirotoshi, I., Mistsuru, U., Kazuhiko, T., Michihiko, A.,"Oxidative carbonylation of
phenol carbonate catalyzed by Pd-Sn complexes with redox catalyst", J. Mol. Cat. A:Chem.,
138, 311-313 (1999).
[5] Hirotoshi, I., Mistsuru, U., Kazuhiko, T., Michihiko, A.,"Oxidative carbonylation of
phenol carbonate catalyzed by Pd-Sn heterotrinuclear complexes along with Mn redox catalyst
without any addition of ammonium halide", J. Mol.Cat. A: Chem., 144, 369-372 (1999).
[6] Buysch, H.J., Hess, C., Jentsch, J.D., Rechner, J.,Zirngiebl, E., "Supported platinum-
group metal for preparatiion of diaryl carbonates", EP736325 (1996).
[7] Buysch, H.J., Jentsch, J.D., Rechner, J., Zirngiebl, E.,"Supported platinum catalysts
and process for preparation of diary carbonates" , EP736324 (1996).
[8] Hesse, C., Nothesis, U., R. echner. J., "Supported platinumgroup metal for producing
diaryl carbonates form carbon monoxide", WO9908786 (1999).
[9] Takagi, W., "Preparation of aromatic carbonates as materials for polycarbonates",
JP09278716 (1997).
[10] Song, H.Y., Park, E.D., Lee, J.S., "Oxidative carbonylation of phenol to diphenyl
carbonate over supported palladium catalysts", J. Mol. Cat. A: Chem., 154, 243-250 (2000).
[11] Zhang, G.X. , Wu, Y.X. , Ma, P.S., Wu, G.W., Li,D. H., "Study on direct synthesis of
diphenyl carbonate with heterogeneous catalyzing reaction I Effect of method of preparing
Pd catalyst carriers on catalyst activity", Chin.J. Catal., 23 (2), 130-132 (2002). (in
Chinese)
[12] Zhang, G.X., Ma, P.S., Wu, Y.X., Wu, G.W., Li, D.H.,"Study on direct synthesis of
diphenyl carbonate with heterogeneous catalyzing reaction Ⅱ Effect of calcination
temperature on catalytic activity of catalyst", Chin. J. Fuel Chem. Tech., 30 (4), 362-367
(2002). (in Chinese)
[13] Zhang, G.X., Wu, Y.X., Ma, P.S., Wu, G.W., Li, D.H.,"Study on direct synthesis of
diphenyl carbonate with heterogeneous catalyzing reaction Ⅲ Effect of Lanthanumcontent on
catalytic activity of catalyst", Chin. J. Mol.Catal., 16 (4), 292-297 (2002) . (in Chinese)
[14] Zhang, G.X., Ma, P.S., Wu, Y.X., Wu, G.W, Li, D.H.,"Study on direct synthesis of
diphenyl carbonate with heterogeneous catalyzing reaction IV Effect of active components
and the supporting methods on catalytic activity of catalyst", Chin. J. Catal., 23 (5),
410-416 (2002). (in Chinese)

非均相羰基氧化一步合成碳酸二苯酯的研究(Ⅴ)筛选催化剂及优化合成条件

Study on Direct Synthesis of Diphenyl Carbonate with Heterogeneous Catalytic Reaction (Ⅴ)
Screening Catalysts and Optimizing Synthesis Conditions

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非均相羰基氧化一步合成碳酸二苯酯的研究(Ⅴ)筛选催化剂及优化合成条件

Study on Direct Synthesis of Diphenyl Carbonate with Heterogeneous Catalytic Reaction (Ⅴ) Screening Catalysts and Optimizing Synthesis Conditions

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Study on Direct Synthesis of Diphenyl Carbonate with Heterogeneous Catalytic Reaction (Ⅴ)
Screening Catalysts and Optimizing Synthesis Conditions