Multivariate curve resolution combined with on-line infrared spectroscopy for researching the synthesis mechanism of 3,4-bis(4′-aminofurazano-3′)furoxan

Abstract

3,4-Bis(4′-aminofurazano-3′)furoxan(DATF), one of a new generation of high energy density materials, shows lots of interesting properties such as lower sensitivity, excellent thermal stability and superior detonation performance in chemistry and physics. In this paper, on-line infrared(IR) spectroscopy was used to monitor the synthesis process of DATF. The concentration profiles and IR spectra of the components were determined by analyzing the IR data via principal component analysis(PCA), evolving factor analysis(EFA) and multivariate curve resolution-alternating least squares(MCR-ALS). The geometric configurations of reactant, intermediates and product were optimized with the density functional theory(DFT) at B3LYP/6-31+G(d, p) level. Their vibrational frequencies and IR spectra were obtained on the basis of vibrational analysis. The result obtained by the chemometric resolution methods agreed well with that obtained by quantum chemical calculation method, which demonstrated the reliability of the proposed chemometric resolution methods. The unstable intermediate 3-amino-4-oxycyanofurazan(AOF) was confirmed via comparing the IR spectra resloved by chemometric resolution methods with those calculated by B3LYP/6-31+G(d,p) and analyzed by MCR-ALS. Finally, the possible synthesis mechanism of DATF was deduced by analyzing the above IR spectra.

Keywords

Evolving factor analysis(EFA) / Multivariate curve resolution-alternating least square(MCR-ALS) / On-line infrared spectrum / Quantum chemical calculation method / Synthesis mechanism

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