This work is an attempt to study storing hydrogen in safe, reliable, compact, and cost-effective glass-ceramics materials for the first time. The effect of replacing K+ by Na+ or Li+ in the fluorophlogopite formula KMg(3)A1Si(3)O(10)F(2) was studied using DTA, XRD and SEM. Also the effect of the crystallized phases within glass-ceramics on the surface area and capacity of storing hydrogen under different pressures were studied. Replacement of K+ by Na+ or Li+ leads to increase the temperature of crystallization in the same order. XRD revealed crystallization of spodumene (LiAlSi2O6) and forsterite (Mg2SiO4) in GLi and Na-fluorophlogopite (NaMg(3)AISi(3)O(10)F(2)) and Na-mica (NaAl3Si3O11) in GNa while Lucite (KA(1)Si(2)O(6)) and forsterite in GK. Surface area measurements for optimum samples showed low values in the range 0.48-0.58 m(2)/g; also total pore volumes have low values 9.4 x 10(-4) -6.99 x 10(-3) cm(3)/g. The hydrogen adsorption content reached 1.25, 2.5, 1.34 sand 1.9 wt% for GLi, GNa, GK and GK samples heated for 2 h at 770,1100, 1000 and 1100 C-omicron, respectively. The results obtained that, Na-bearing samples are the proper for hydrogen storage wherein sodium mica and phlogopite with characteristic sheet structure were crystallized. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.