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Stabilisation of reactive intermediates in molecular sieves

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This paper presents studies on paramagnetic intermediates, free atoms and radicals produced in γ-irradiated molecular sieves and their reactions with adsorbate molecules or exchangeable cations. Four different systems have been investigated using EPR spectroscopy, Na-A/CH4, AgNa-A/CH3OH, Ag-SAPO-11/C2H4 and AgCs-rho/NH3. It was found that methyl radicals are formed in two different sites in Na-A/CH4 and in one of them they are stable at room temperature. The formation of Ag•CH2OH+ radical cation with one-electron bond between silver and carbon has been established in AgNa-A/CH3OH by EPR experiments with [13C]CH3OH and DFT calculations. In Ag-SAPO-11/C2H4 the stabilisation of biligand silver/ethylene complex, Ag0(C2H4)2 was postulated based on EPR and DFT results. Tetrameric silver clusters (Ag3+4) produced radiolytically in AgCs-rho/NH3strongly interact with two ammonia molecules as was deduced from the changes in superhyperfine structure of high-field EPR line of Ag3+4 pentet for zeolite exposed to [14N]NH3 and [15N]NH3. The presented examples clearly show that the combination of radiation methods with EPR technique is very useful to study the structure and reactivity of paramagnetic intermediates.

Affiliations: 1: Institute of Nuclear Chemistry and Technology, Dorodna 16, 03-195 Warsaw, Poland


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