Direct production of hydrogen peroxide with palladium supported on phosphate viologen phosphonate catalysts

被引:102
作者
Krishnan, VV [1 ]
Dokoutchaev, AG [1 ]
Thompson, ME [1 ]
机构
[1] Univ So Calif, Dept Chem, Los Angeles, CA 90089 USA
关键词
hydrogen peroxide; direct production; heterogeneous catalyst; hydrothermal incorporation; viologen; palladium; kinetic study;
D O I
10.1006/jcat.2000.3036
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
The optimization of porous hafnium phosphate viologen phosphonate (HfPOPV(X)) catalyst, [(HfF)(2)(PO4)(P3PCH2CH2-4,4'-bipyridinium-CH2CH2PO3)]F . 2H(2)O with Pd-metal nanoaggregates, has been attempted. In addition to the development of a novel technique for making this catalyst by hydrothermal incorporation, an extensive optimization of the process conditions to make hydrogen peroxide from H-2 and O-2 has been carried out. The optimal reaction medium for this process was methanol in conjunction with sulfuric acid. Under atmospheric conditions, over 3.5 M H2O2 has been produced in 50 h. A technique has also been developed to measure the water formed from the undesirable H2O2 reduction step that occurs in series-parallel. to the desired H2O2 production step. The selectivity toward the production of H2O2 in the case of the hydrothermally incorporated catalysts is over 70% under atmospheric conditions. The maximum rate of production of H2O2, achieved in anhydrous methanol-H2SO4 media and hydrothermally incorporated Pd-HfPOPV(X) is about 4.1 mmol/(g min). However, the rate measured here is probably that of external mass transfer (at the liquid-gas interface) because the resistance due to it is the rate-determining step. (C) 2000 Academic Press.
引用
收藏
页码:366 / 374
页数:9
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