Pb促进的Pd/γ-Al2O3催化剂上H2O2氧化甘油反应

doi:10.1016/S1872-2067(16)62531-7

催化学报 ›› 2016, Vol. 37 ›› Issue (11): 1982-1990.DOI: 10.1016/S1872-2067(16)62531-7

Pb促进的Pd/γ-Al₂O₃催化剂上H₂O₂氧化甘油反应

María L. Faroppa^a, Juan J. Musci^a, María E. Chiosso^a.b, Claudia G. Caggiano^a, Hernán P. Bideberripe^b,c, José L. García Fierro^d, Guillermo J. Siri^b,c, Mónica L. Casella^a,b

a 布宜诺斯艾利斯西北国立大学, CIBA(CIT UNNOBA, CONICET), 布宜诺斯艾利斯, 阿根廷;
b 拉普拉塔国立大学科学学院, CINDECA(CCT La Plata-CONICET, UNLP), 1900 拉普拉, 阿根廷;
c 拉普拉塔国立大学工程学院PIDCAT, 1900拉普拉, 阿根廷;
d 西班牙国家研究委员会(CSIC)催化与石油化学研究所, E-28049 马德里, 西班牙

收稿日期:2016-06-01 修回日期:2016-08-20 出版日期:2016-11-25 发布日期:2016-11-25
通讯作者: Mónica L. Casella,Tel:+542214210711; E-mail:casella@quimica.unlp.edu.ar

Oxidation of glycerol with H₂O₂ on Pb-promoted Pd/γ-Al₂O₃ catalysts

María L. Faroppa^a, Juan J. Musci^a, María E. Chiosso^a.b, Claudia G. Caggiano^a, Hernán P. Bideberripe^b,c, José L. García Fierro^d, Guillermo J. Siri^b,c, Mónica L. Casella^a,b

a CIBA (CIT UNNOBA, CONICET), Universidad Nacional del Noroeste de la Provincia de Buenos Aires, Newbery 261 (6000) Junín, Provincia de Buenos Aires, Argentina;
b CINDECA (CCT La Plata-CONICET, UNLP), Universidad Nacional de La Plata, Facultad de Ciencias Exactas, 47 N·257, 1900 La Plata, Argentina;
c PIDCAT Facultad de Ingeniería, Universidad Nacional de La Plata, 1 y 47, 1900 La Plata, Argentina;
d Instituto de Catálisis y Petroleoquímica, CSIC, Canto Blanco, E-28049 Madrid, España

Received:2016-06-01 Revised:2016-08-20 Online:2016-11-25 Published:2016-11-25
Contact: Mónica L. Casella,Tel:+542214210711; E-mail:casella@quimica.unlp.edu.ar
Supported by:
This work was supported by CONICET (PIP 0276), UNLP (Projects X 700), UNNOBA (SIB 2924/14), and Ministry of Education and Sports (Call "Jorge Sábato" Project 44-144-415), Argentina.

摘要/Abstract

摘要：

制备了Pd含量为1 wt%、不同Pb/Pd摩尔比的γ-Al₂O₃负载Pd-Pb双金属催化剂，并用于常压、45℃和pH=11条件下H₂O₂氧化甘油反应中.催化剂的形貌和分散度采用扫描电镜-X射线电子散射谱和透射电镜进行了表征；双金属催化剂中合金相用X射线光电子能谱进行了验证.单金属Pd催化剂上反应结束后甘油转化率为19%，但随着Pb的加入甘油转化率增大到约100%.所制四个不同Pb/Pd原子比的双金属催化剂PdPb0.25，PdPb0.50，PdPb1.00和PdPb1.60均可氧化甘油至二羟基丙酮（DIHA），反应结束后DIHA选择性分别可达59%，58%，34%和25%.

关键词: 钯, 双金属钯-铅催化剂, 过氧化氢, 甘油氧化, 甘油酸, 羟基乙酸

Abstract:

A series of bimetallic Pd-Pb catalysts with a constant Pd content of 1 wt% and Pb/Pd atomic ratio from 0 to 1.6 supported on γ-Al₂O₃ were prepared and used for glycerol oxidation with H₂O₂ as the oxidizing agent at atmospheric pressure, 45℃ and pH=11. The morphology and dispersion of the catalysts were characterized by scanning electron microscopy-energy dispersive X-ray spectrosco-py (SEM-EDX) and transmission electron microscopy (TEM). The presence of an alloy phase in the bimetallic catalyst was detected by X-ray photoelectron spectroscopy (XPS). Glycerol conversion obtained with the monometallic Pd catalyst was 19%, which was increased to 100% with the addi-tion of Pb. The four bimetallic PdPb catalysts were able to oxidize glycerol to dihydroxyacetone (DIHA) and the selectivity to DIHA reached 59%, 58%, 34% and 25% for PdPb0.25, PdPb0.50, PdPb1.00 and PdPb1.60 catalysts, respectively.

Key words: Palladium, Bimetallic palladium-lead catalyst, Hydrogen peroxide, Glycerol oxidation, Glyceric acid, Glycolic acid

María L. Faroppa, Juan J. Musci, María E. Chiosso, Claudia G. Caggiano, Hernán P. Bideberripe, José L. García Fierro, Guillermo J. Siri, Mónica L. Casella. Pb促进的Pd/γ-Al₂O₃催化剂上H₂O₂氧化甘油反应[J]. 催化学报, 2016, 37(11): 1982-1990.

María L. Faroppa, Juan J. Musci, María E. Chiosso, Claudia G. Caggiano, Hernán P. Bideberripe, José L. García Fierro, Guillermo J. Siri, Mónica L. Casella. Oxidation of glycerol with H₂O₂ on Pb-promoted Pd/γ-Al₂O₃ catalysts[J]. Chinese Journal of Catalysis, 2016, 37(11): 1982-1990.

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Pb促进的Pd/γ-Al₂O₃催化剂上H₂O₂氧化甘油反应

Oxidation of glycerol with H₂O₂ on Pb-promoted Pd/γ-Al₂O₃ catalysts

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