Duong Nghia Tuan, Trébosc Julien, Lafon Olivier, Amoureux Jean-Paul
Univ. Lille, Centrale Lille, ENSCL, Univ. Artois, CNRS-8181, UCCS - Unit of Catalysis and Chemistry of Solids, F-59000 Lille, France.
Univ. Lille, Centrale Lille, ENSCL, Univ. Artois, CNRS-8181, UCCS - Unit of Catalysis and Chemistry of Solids, F-59000 Lille, France; Univ. Lille, CNRS-FR2638, Fédération Chevreul, F-59000 Lille, France.
Solid State Nucl Magn Reson. 2019 Aug;100:52-62. doi: 10.1016/j.ssnmr.2019.03.007. Epub 2019 Mar 26.
We demonstrate the possibility to use UDEFT (Uniform Driven Equilibrium Fourier Transform) technique in order to improve the sensitivity and the quantification of one-dimensional Si NMR experiments under magic-angle spinning (MAS). We derive an analytical expression of the signal-to-noise ratios of UDEFT and single-pulse (SP) experiments subsuming the contributions of transient and steady-state regimes. Using numerical spin dynamics simulations and experiments on Si-enriched amorphous silica and borosilicate glass, we show that 5929859 refocusing composite π-pulse and the adiabatic inversion using tanh/tan modulation improve the robustness of UDEFT technique to rf-inhomogeneity, offset, and chemical shift anisotropy. These pulses combined with a two-step phase cycle limit the pulse imperfections and the artifacts produced by stimulated echoes. The sensitivity of SP, UDEFT and CPMG (Carr-Purcell-Meiboom-Gill) techniques are experimentally compared on functionalized and non-functionalized mesoporous silica. Furthermore, experiments on a flame retardant material prove that UDEFT technique provides a better quantification of Si sites with higher sensitivity than SP method.
我们证明了使用均匀驱动平衡傅里叶变换(UDEFT)技术来提高魔角旋转(MAS)下一维硅核磁共振实验的灵敏度和定量分析的可能性。我们推导了UDEFT和单脉冲(SP)实验信噪比的解析表达式,其中包括瞬态和稳态的贡献。通过对富含硅的无定形二氧化硅和硼硅酸盐玻璃进行数值自旋动力学模拟和实验,我们表明5929859重聚焦复合π脉冲以及使用tanh/tan调制的绝热反转提高了UDEFT技术对射频不均匀性、偏移和化学位移各向异性的鲁棒性。这些脉冲与两步相位循环相结合,限制了脉冲缺陷和受激回波产生的伪影。在功能化和非功能化介孔二氧化硅上对SP、UDEFT和CPMG(Carr-Purcell-Meiboom-Gill)技术的灵敏度进行了实验比较。此外,对一种阻燃材料的实验证明,UDEFT技术比SP方法能以更高的灵敏度对硅位点进行更好的定量分析。