Proton multiple-quantum (MQ) spin-counting experiment has been employed to study arrangement of hydrogen atoms in 9 angstrom/11 angstrom natural/synthetic tobermorites. Even though all tobermorite samples give similar characterless, broad static-powder H-1 NMR spectra, their MQ spin-counting spectra are markedly different; higher quanta in 11 angstrom tobermorite do not grow with the MQ excitation time, while those in 9 angstrom one do. A statistical analysis of the MQ results recently proposed [26] is applied to show that hydrogens align in 9 angstrom tobermorite one dimensionally, while in 11 angstrom tobermorite they exist as a cluster of 5-8 hydrogen atoms. (C) 2014 Elsevier Ltd. All rights reserved.