Direct oxidation of H2 to H2O2 and decomposition of H2O2 over oxidized and reduced Pd-containing zeolite catalysts in acidic medium

被引:68
作者
Choudhary, VR [1 ]
Sansare, SD [1 ]
Gaikwad, AG [1 ]
机构
[1] Natl Chem Lab, Div Chem Engn, Pune 411008, Maharashtra, India
关键词
oxidation of H-2 to H2O2; decomposition of H2O2; zeolite supported Pd catalysts; Pd/H-ZSM-5; Pd/H-GaAlMFI; Pd/H-beta;
D O I
10.1023/A:1021032819400
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Both the conversion and H2O2 selectivity (or yield) in direct oxidation of H-2-to-H2O2 (using 1.7 mol% H-2 in O-2 as a feed) and also the H2O2 decomposition over zeolite (viz. H-ZSM-5, H-GaAlMFI and H-beta) supported palladium catalysts (at 22 degreesC and atmospheric pressure) are strongly influenced by the zeolite support and its fluorination, the reaction medium (viz. pure water, 0.016 M or 1.0 M NaCl solution or 0.016 M H2SO4, HCl, HNO3, H3PO4 and HClO4), and also by the form of palladium (Pd-0 or PdO). The oxidized (PdO-containing) catalysts are active for the H-2-to-H2O2 conversion and show very poor activity for the H2O2 decomposition. However, the reduced (Pd-0-containing) catalysts show higher H-2 conversion activity but with no selectivity for H2O2, and also show much higher H2O2 decomposition activity. No direct correlation is observed between the H-2-to-H2O2 conversion activity (or H2O2 selectivity) and the Pd dispersion or surface acidity of the catalysts. Higher H2O2 yield and lower H2O2 decomposition activity are, however, obtained when the non-acidic reaction medium (water with or without NaCl) is replaced by the acidic one.
引用
收藏
页码:81 / 87
页数:7
相关论文
共 20 条
[1]  
Choudhary V.R., 1971, IND ENG CHEM PROD RE, V10, P218, DOI [10.1021/i360039a002, DOI 10.1021/I360039A002]
[2]  
Choudhary VR, 2001, ANGEW CHEM INT EDIT, V40, P1776, DOI 10.1002/1521-3773(20010504)40:9<1776::AID-ANIE17760>3.3.CO
[3]  
2-3
[4]   COMPARISON BETWEEN CATALYTICALLY IMPORTANT ZEOLITES FOR THEIR CATALYTIC PROPERTIES AND DEACTIVATION [J].
CHOUDHARY, VR ;
AKOLEKAR, DB .
JOURNAL OF CATALYSIS, 1990, 125 (01) :143-156
[5]   Aromatization of dilute ethylene over Ga-modified ZSM-5 type zeolite catalysts [J].
Choudhary, VR ;
Devadas, P ;
Banerjee, S ;
Kinage, AK .
MICROPOROUS AND MESOPOROUS MATERIALS, 2001, 47 (2-3) :253-267
[6]   SIMPLE APPARATUS FOR MEASURING SOLUBILITY OF GASES AT HIGH-PRESSURES [J].
CHOUDHARY, VR ;
PARANDE, MG ;
BRAHME, PH .
INDUSTRIAL & ENGINEERING CHEMISTRY FUNDAMENTALS, 1982, 21 (04) :472-474
[7]   STEP-WISE THERMAL-DESORPTION OF AMMONIA FROM X,Y AND ZSM-5 TYPE ZEOLITES [J].
CHOUDHARY, VR ;
PATASKAR, SG .
ZEOLITES, 1986, 6 (04) :307-311
[8]  
Chuang K.T., 1994, US Patent, Patent No. [5,338,531, 5338531]
[9]  
FU F, 1992, STUD SURF SCI CATAL, V72, P33, DOI DOI 10.1016/S0167-2991(08)61656-0
[10]   Direct oxidation of hydrogen to hydrogen peroxide over Pd-containing fluorinated or sulfated Al2O3, ZrO2, CeO2, ThO2, Y2O3 and Ga2O3 catalysts in stirred slurry reactor at ambient conditions [J].
Gaikwad, AG ;
Sansare, SD ;
Choudhary, VR .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2002, 181 (1-2) :143-149