马新宾
一氧化碳气相催化合成草酸二乙酯、碳酸二甲酯、碳酸二苯酯的环境友好工艺的开发与研究
个性化签名
- 姓名:马新宾
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- 担任导师情况:
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学术头衔:
博士生导师, 教育部“新世纪优秀人才支持计划”入选者
- 职称:-
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学科领域:
化工系统工程
- 研究兴趣:一氧化碳气相催化合成草酸二乙酯、碳酸二甲酯、碳酸二苯酯的环境友好工艺的开发与研究
马新宾, 男,1968年生,教授,博士生导师,天津大学化工学院化学工艺系主任,绿色合成与转化教育部重点实验室副主任,教育部“新世纪优秀人才支持计划”人选。1990年7月在天津大学化学工程系获得化学工程专业学士学位;1993年3月在天津大学化学工程系获得有机化工专业工学硕士学位;1996年3月在天津大学化学工程系获得有机化工专业工学博士学位。选择“绿色化学工艺与一碳化工”作为自己的科研方向,在一氧化碳气相催化合成草酸二乙酯、碳酸二甲酯、碳酸二苯酯的环境友好工艺的开发与研究等领域开展科研与教学工作。先后主持了国家自然科学基金、天津市自然科学基金、天津市科技攻关培育项目、教育部博士点基金、教育部高等学校骨干教师资助基金、云南省省院省校合作项目等9项国家级、省部级项目。申请国家发明专利14项,其中已授权5项,获天津市科技进步二等奖1项;在国内外高水平刊物上发表论文50多篇,其中被SCI、EI收录论文达30多篇。曾获得2001年天津市新长征突击手、2001年天津大学十佳杰出青年,2003-2004年度天津大学青年师德标兵荣誉称号。
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马新宾, Xinbin Ma*, Zhenhua Li, Baowei Wang, and Genhui Xu
React. Kinet. Catal. Lett. Vol. 76, No.1, 179-187 (2002),-0001,():
-1年11月30日
In this paper, the effect of catalyst preparation on the activity of supported Cu catalyst for oxidative carbonylation of methanol to dimethyl carbonate was investigated. The results showed that after addING metal hydroxide, the supported Cu catalyst enhanced the conversion of methanol and the selectivity TO of DMC and the suitable mole ratio of OH/Cu is 1.0. The optimum Cu content lies in 6 10wt.% and varies with reaction temperature. The suitable calcination temperature range is 200~300℃ considering both factors of methanol conversion and DMC selectivity. The effect of particle size of the catalysts on the activity is negligible.
Cu,, carbon monoxide,, dimethyl carbonate,, carbonylation
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马新宾, Xin Bin MA*, Sheng Ping WANG, Hong Li GUO, Gen Hui XU
Chinese Chemical Letters Vol. 14, No.5, pp 461-464, 2003,-0001,():
-1年11月30日
Diphenyl oxalate was synthesized from transesterification of dimethyl oxalate with phenol over TS-1 (2.5 wt% Ti) catalyst. TS-1 catalyst, as a heterogeneous catalyst, showed excellent selectivity of diphenyl oxalate and methylphenyl oxalate compared with other homogeneous catalysts. Lewis acid sites on TS-1 catalyst were the active sites for transesterification of dimethyl oxalate with phenol. The high selectivity was closely related to the weak acid sites over TS-1.
Diphenyl oxalate,, transesterification,, dimethyl oxalate,, weak acid sites,, TS-1.,
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【期刊论文】Transesterification of dimethyl oxalate with phenol over TS-1 catalyst
马新宾, Xinbin Ma*, Hongli Guo, Shengping Wang, Yongli Sun
Fuel Processing Technology 83 (2003) 275-286,-0001,():
-1年11月30日
The transesterification of dimethyl oxalate with phenol to produce methyphenyl oxalate and diphenyl oxalate was carried out in liquid phase using a heterogeneous catalyst. The evaluation results showed that TS-1 had better activity and excellent selectivity to target products compared with many conventional ester exchange catalysts tested. Two hours as the duration of the reaction was appropriate. Under the catalytic reaction conditions, framework IR and the reaction results jointly proved that the best calcination temperature was 823 K at which the amount of acid sites measured by IR of adsorbed pyridine reached a maximum. X-ray diffraction of TS-1 did not show much variation with changing calcination temperatures from 723 to 923 K. The characterization of the catalyst, by means of IR of adsorbed pyridine and NH3-TPD indicated that the desired catalytic activity of TS-1 could be ascribed to its weak Lewis acidity. Tin modified TS-1 showed a better performance in activity and selectivity. The conversion of dimethyl oxalate was improved up to 50.3% when Sn loading was 2, while the selectivity was above 99% over all Tin modified TS-1 molecular sieves.
Diphenyl carbonate, Dimethyl oxalate, Diphenyl oxalate, Methyl phenyl oxalate, Transesterification, TS-1, Green chemistry
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【期刊论文】Transesterification of dimethyl oxalate with phenol over MoO3/SiO2 catalysts
马新宾, Jinlong Gong, Xinbin Ma*, Shengping Wang, Moyi Liu, Xia Yang, Genhui Xu
Journal of Molecular Catalysis A: Chemical 207 (2004) 213-218,-0001,():
-1年11月30日
The transesterification of dimethyl oxalate (DMO) with phenol to methyl phenyl oxalate (MPO) and diphenyl oxalate (DPO) was carried out in liquid phase using a variety of solid catalysts. The evaluation results showed that MoO3/SiO2 had a better activity and excellent selectivity to target products compared with many conventional ester exchange catalysts. The effects of supports, loading amount of Mo, catalyst amount and reaction time were investigated. Under catalytic reaction conditions, the total selectivities to methyl phenyl oxalate and diphenyl oxalate were up to 98%. And 49.3% yield of methyl phenyl oxalate and 17.3% yield of diphenyl oxalate were obtained at 453K in the presence of MoO3/SiO2. A plausible mechanism for the transesterification of dimethyl oxalate with phenol to methyl phenyl oxalate over MoO3/SiO2 was proposed.
Diphenyl carbonate, Dimethyl oxalate, Diphenyl oxalate, Methyl phenyl oxalate, Transesterification, MoO3/, SiO2
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马新宾, Xinbin Ma*, , Jinlong Gong, Shengping Wang, Ning Gao, Dali Wang, Xia Yang, Fei He
Catalysis Communications 5 (2004) 101-106,-0001,():
-1年11月30日
A series of MoO3/SiO2 catalysts were prepared with Mo loadings ranging from 1 to 16 wt% and applied to the transesterification of dimethyl oxalate (DMO) with phenol. The results showed that the catalyst of MoO3/SiO2 with 1 wt% Mo content performed best, giving 54.6% conversion of DMO and 99.6% selectivity to target products, methyl phenyl oxalate (MPO) and diphenyl oxalate (DPO). The surface properties were investigated by means of X-ray diffraction (XRD), X-ray photoelectron (XPS), BET specific surface area, temperature-programmed desorption (TPD) of ammonia, and FTIR analysis of adsorbed pyridine. XPS and XRD analyses indicated that Mo(VI) species was highly dispersed at low Mo loading and MoO3 of the crystal structure appeared at higher loading. NH3-TPD characterization and FTIR analysis of adsorbed pyridine demonstrated that only Lewis weak acids were present on catalyst surface and the amount of Mo loading has little effect on the strength of the surface acid on MoO3/SiO2. The catalytic results exhibited that the synergetic effect of Mo active centers with weak Lewis acid sites catalyzed transesterification of DMO with phenol.
Diphenyl carbonate, Dimethyl oxalate, Diphenyl oxalate, Methyl phenyl oxalate, Transesterification, MoO3/, SiO2 catalysts, Acid sites
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马新宾, Jinlong Gong a, Xinbin Ma a, *, Xia Yang a, Shengping Wang a, Shoudong Wen b
Catalysis Communications 5 (2004) 179-184,-0001,():
-1年11月30日
The transesterification of dimethyl oxalate (DMO) with phenol to methyl phenyl oxalate (MPO) and diphenyl oxalate (DPO) was carried out in liquid phase under facile catalytic conditions. A series of bimetallic, MoO3-SnO2/SiO2, catalysts with various Mo and Sn content were prepared by sequential impregnation of cationic Mo species and cationic Sn complexes using impregnation method. The effects of mass ratio of Mo:Sn, amount of Sn additive, and Mo(Sn) laoding amount on activities of transesterification of dimethyl oxalate with phenol were investigated. The evaluation results showed that MoO3-SnO2/SiO2 catalyst with 14 wt% Mo(Sn) content performed best, giving 74.6% DMO conversion and 99.5% selectivity to MPO and DPO. This new heterogeneous catalyst provided not only an excellent selectivity (99% to MPO and DPO) and high yield of MPO and DPO but also a simple and practical protocol for DPC synthesis.
Diphenyl carbonate, Diphenyl oxalate, Methyl phenyl oxalate, Transesterification, Dimethyl oxalate, Bimetallic MoO3-SnO2/, SiO2 catalysts
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马新宾, Shengping Wang, Xinbin Ma*, Hongli Guo, Jinlong Gong, Xia Yang, Genhui Xu
Journal of Molecular Catalysis A: Chemical 214 (2004) 273-279,-0001,():
-1年11月30日
The transesterification of dimethyl oxalate (DMO) with phenol to produce methyl phenyl oxalate (MPO) and diphenyl oxalate (DPO) was carried out over TiO2/SiO2 catalyst. The evaluation results showed that TiO2/SiO2 had better activity and excellent selectivity to target products compared with many conventional ester exchange catalysts. The total selectivity to MPO and DPO kept about 99.0% over TiO2/SiO2 and the conversion of DMO was 66.7% at 10% Ti loading, which was the maximum at different Ti loading. The structure and the chemical state of titanium species in TiO2/SiO2 had been investigated by XRD and XPS. The surface Ti(Ⅳ) species in the form of a monolayer was dominant until 6% Ti loading, while crystalline TiO2 was detected at 8% Ti loading. IR of adsorbed pyridine and NH3-TPD characterization indicated that the desirable catalytic activity of TiO2/SiO2 could be ascribed to its weak Lewis acid. Lewis acid sites cooperated with TiO2 to catalyze the synthesis of MPO and DPO.
Diphenyl carbonate, Dimethyl oxalate, Diphenyl oxalate, Methyl phenyl oxalate, Transesterification, TiO2/, SiO2, Weak Lewis acid sites
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马新宾, Jinlong Gong a, Xinbin Ma a*, Shengping Wang a, Xia Yang a, Gang Wang a, and Shoudong Wen b
React. Kinet. Catal. Lett. Vol. 83, No.1, 113-120 (2004),-0001,():
-1年11月30日
The influence of molybdenum content on the catalytic performance in the transesterification of dimethyl oxalate (DMO) with phenol to methyl phenyl oxalate (MPO) and diphenyl oxalate (DPO) was investigated. The results indicated that the MoO3/Al2O3 catalyst with 14wt% Mo content gave maximal DPO yield with 6.1% and 75.1% DMO conversion. The component, structure and phase of MoO3/Al2O3 catalysts were characterized by means of X-ray diffraction (XRD), BET specific surface area, temperature-programmed desorption of ammonia (NH3-TPD), and FTIR analysis of adsorbed pyridine.
Diphenyl carbonate,, diphenyl oxalate,, methyl phenyl oxalate,, MoO3/, γ-Al2O3,, Lewis acid
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【期刊论文】Transesterification of Dimethyl Oxalate with Phenol under SnO2/SiO2 Catalysts
马新宾, Shengping Wang, Xinbin Ma, *, Jinlong Gong, Xia Yang, Hongli Guo, and Genhui Xu
Ind. Eng. Chem. Res. 2004, 43, 4027-4030,-0001,():
-1年11月30日
The transesterification of dimethyl oxalate (DMO) with phenol to produce methyl phenyl oxalate (MPO) and diphenyl oxalate (DPO) was carried out over a SnO2/SiO2 catalyst. The evaluation results showed that SnO2/SiO2 had better activity and total selectivity to MPO and DPO than many conventional ester exchange catalysts. Especially, SnO2/SiO2 was in favor of the disproportionation of MPO into DPO compared with TS-1, MoO3/SiO2, and MoO3-SnO2/SiO2 catalysts. The conversion of DMO was 46.7% and the selectivity to DPO was 22.5% at 8% Sn loadings, which was the maximum at different Sn loadings. IR of adsorbed pyridine and NH3-TPD characterization indicated that the desirable catalytic activity of SnO2/SiO2 could be ascribed to its weak Lewis acidity. The structure and chemical state of tin species in SnO2/SiO2 had been investigated by X-ray diffraction. SnO2 active centers dispersed on a SiO2 carrier with a high specific surface area were of benefit to the transesterification.
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马新宾, Shengping Wang, Xinbin Ma*, Jinlong Gong, Ning Gao, Hongli Guo, Xia Yang, Genhui Xu
Catalysis Today 93-95 (2004) 377-381,-0001,():
-1年11月30日
The transesterification of dimethyl oxalate (DMO) with phenol over stannum modifiedH was conducted to prepare diphenyl oxalate (DPO) used to produce diphenyl carbonate (DPC). The component, structure and phase of Hβ catalysts with various Sn loadings were investigated. The relationship between the catalytic properties and the amount of Sn loadings was discussed. The catalyst of H with 2wt.% Sn loading based on metal performed best, giving 75.3% conversion of DMO and 24.0% selectivity to DPO. At Sn loadings below 2wt.%, Sn was highly dispersed as monolayer, but at higher loadings it was crystallized into bulk tin dioxide, and the catalytic activity decreased. The curve of XPS peak intensity ratio of Sn 3d/Si 2p versus Sn loadings estimated the dispersed capacity of Sn on Hβ to be 2.1% Sn loading, which was in good agreement with the value obtained from XRD analysis. NH3-TPD results showed that the amount of Sn loading had effect only on the strength of the weak surface acid sites on Hβ. And the decrease of selectivity to anisole was not due to the change of the weak acid sites. Maybe, SnO2 accelerated to the formation of MPO and DPO. FTIR analysis of adsorbed pyridine showed that many Lewis acid sites and few Brönsted acid sites were present on Hβ catalysts with or without Sn modified. The acid sites together with SnO2 active centers catalyzed the transesterification of DMO with phenol. Especially, SnO2 active centers were in favor of the disproportionation of MPO into DPO.
Diphenyl carbonate, Diphenyl oxalate, Methyl phenyl oxalate, Dimethyl oxalate, Transesterification, Stannum modified Hβ
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