The development of multi-dimensional statistical methods has been demonstrated on variable contact time (VCT) 29Si{1H} cross-polarization magic angle spinning (CP/MAS) data sets collected using Carr-Purcell-Meiboom-Gill (CPMG) type acquisition. These methods utilize the transformation of the collected 2D VCT data set into a 3D data set and use tensor-rank decomposition to extract the spectral components that vary as a function of transverse relaxation time (T2) and CP contact time. The result is a data dense spectral set that can be used to reconstruct CP/MAS spectra at any contact time with a high signal to noise ratio and with an excellent agreement to 29Si{1H} CP/MAS spectra collected using conventional acquisition. These CPMG data can be collected in a fraction of time that would be required to collect a conventional VCT data set. We demonstrate the method on samples of functionalized mesoporous silica materials and show that the method can provide valuable surface specific information about their functional chemistry.