Reaction monitoring of hydrogen peroxide decomposition by NMR relaxometry

被引:18
作者
Buljubasich, L. [2 ]
Bluemich, B. [2 ]
Stapf, S. [1 ]
机构
[1] Tech Univ Ilmenau, Dept Tech Phys 2, D-98684 Ilmenau, Germany
[2] Rhein Westfal TH Aachen, Inst Tech Chem & Macromol Chem ITMC, D-52074 Aachen, Germany
关键词
Catalysis; Diffusion; Porous media; Reaction engineering; NUCLEAR-MAGNETIC-RESONANCE; SPIN-ECHO NMR; CHEMICAL-EXCHANGE; SPECTROSCOPY; RELAXATION; GRADIENT; RATES; WATER;
D O I
10.1016/j.ces.2009.10.009
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
In this contribution we suggest the feasibility to use the NMR transverse relaxation rate, R-2, as an indicator of reaction evolution during the heterogeneous catalytic hydrogen peroxide decomposition: 2H(2)O(2)(liquid)-> 2H(2)O+O-2(gas). The influence of two-site intermediate chemical exchange between protons in water and hydrogen peroxide on the relaxation rate and its concentration dependence in bulk samples is pointed out. It is demonstrated that for the system under investigation-being representative for a heterogeneously catalyzed reaction-the sample peculiarities, such as shape, metal content, internal magnetic field gradients and susceptibility effects, are minor compared to the dominating contrast produced by chemical exchange, thus rendering R2 a suitable parameter to follow the decomposition in real-time. Transverse relaxation rates as a function of reaction time are measured and discussed that were obtained during the decomposition of aqueous hydrogen peroxide solutions in the presence of a commercial Al2O3 porous particle, impregnated with Cu as catalytically active sites. (C) 2009 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1394 / 1399
页数:6
相关论文
共 25 条
[1]   ANALYSIS OF CAR-PURCELL SPIN-ECHO NMR EXPERIMENTS ON MULTIPLE-SPIN SYSTEMS .2. EFFECT OF CHEMICAL EXCHANGE [J].
ALLERHAN.A ;
THIELE, E .
JOURNAL OF CHEMICAL PHYSICS, 1966, 45 (03) :902-&
[2]   SPIN-ECHO NMR STUDIES OF CHEMICAL EXCHANGE .1. SOME GENERAL ASPECTS [J].
ALLERHAND, A ;
GUTOWSKY, HS .
JOURNAL OF CHEMICAL PHYSICS, 1964, 41 (07) :2115-&
[3]   SPIN-ECHO STUDIES OF CHEMICAL EXCHANGE .2. CLOSED FORMULAS FOR 2 SITES [J].
ALLERHAN.A ;
GUTOWSKY, HS .
JOURNAL OF CHEMICAL PHYSICS, 1965, 42 (05) :1587-&
[4]   KINETICS OF HYDROGEN EXCHANGE BETWEEN HYDROGEN PEROXIDE AND WATER STUDIED BY PROTON MAGNETIC RESONANCE [J].
ANBAR, M ;
LOEWENSTEIN, A ;
MEIBOOM, S .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1958, 80 (11) :2630-2634
[5]   Chaos in catalyst pores -: Can we use it for process development? [J].
Bluemich, Bernhard ;
Datsevich, Leonid B. ;
Jess, Andreas ;
Oehmichen, Thomas ;
Ren, Xiaohong ;
Stapf, Siegfried .
CHEMICAL ENGINEERING JOURNAL, 2007, 134 (1-3) :35-44
[6]  
Callaghan PT, 1999, CONCEPT MAGNETIC RES, V11, P181, DOI 10.1002/(SICI)1099-0534(1999)11:4<181::AID-CMR1>3.0.CO
[7]  
2-T
[8]   Treatment of high strength hexamine-containing wastewater by Electro-Fenton method [J].
Chou, SS ;
Huang, YH ;
Lee, SN ;
Huang, GH ;
Huang, CP .
WATER RESEARCH, 1999, 33 (03) :751-759
[9]  
*EUR SPAC AG, 2006, P 3 INT C GREEN PROP
[10]  
HUCKABA CE, 1948, J AM CHEM SOC, V70, P1604