Conference proceeding
A large sample volume magic angle spinning nuclear magnetic resonance probe for in situ investigations with constant flow of reactants
PCCP. Physical chemistry chemical physics (Print), Vol.14(7), pp.2137-2143
2012
Handle:
https://hdl.handle.net/2376/104522
PMID: 22025270
Abstract
A large-sample-volume constant-flow magic angle sample spinning (CF-MAS) NMR probe is reported for in situ studies of the reaction dynamics, stable intermediates/transition states, and mechanisms of catalytic reactions. In our approach, the reactants are introduced into the catalyst bed using a fixed tube at one end of the MAS rotor while a second fixed tube, linked to a vacuum pump, is attached at the other end of the rotor. The pressure difference between both ends of the catalyst bed inside the sample cell space forces the reactants flowing through the catalyst bed, which improves the diffusion of the reactants and products. This design allows the use of a large sample volume for enhanced sensitivity and thus permitting in situ13C CF-MAS studies at natural abundance. As an example of application, we show that reactants, products and reaction transition states associated with the 2-butanol dehydration reaction over a mesoporous silicalite supported heteropoly acid catalyst (HPA/meso-silicalite-1) can all be detected in a single 13C CF-MAS NMR spectrum at natural abundance. Coke products can also be detected at natural 13C abundance and under the stopped flow condition. Furthermore, 1H CF-MAS NMR is used to identify the surface functional groups of HPA/meso-silicalite-1 under the condition of in situ drying. We also show that the reaction dynamics of 2-butanol dehydration using HPA/meso-silicalite-1 as a catalyst can be explored using 1H CF-MAS NMR.
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Details
- Title
- A large sample volume magic angle spinning nuclear magnetic resonance probe for in situ investigations with constant flow of reactants
- Creators
- Jian Zhi Hu - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesJesse A SEARS - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesHardeep S MEHTA - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesJoseph J FORD - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesJa HUN KWAK - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesKake ZHU - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesYong Wang - Washington State University, School of Chemical Engineering and BioengineeringJun Liu - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesDavid W HOYT - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United StatesCharles H. F PEDEN - Institute for Integrated Catalysis, and Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory Richland, Washington 99354, United States
- Publication Details
- PCCP. Physical chemistry chemical physics (Print), Vol.14(7), pp.2137-2143
- Academic Unit
- School of Chemical Engineering and Bioengineering
- Publisher
- Royal Society of Chemistry; Cambridge
- Identifiers
- 99900546885301842
- Language
- English
- Resource Type
- Conference proceeding