Ni/Pd co-modified graphene hydrogen storage materials were successfully prepared by a solvothermal method using NiCl2·6H2O and Pd(OAc)2 and reduced graphene oxide (rGO). By adjusting the hydrothermal temperature, Pd–Ni is successfully alloyed, and the size of the obtained nanoparticles is uniform. The electronic structure of Pd was changed by alloying, and the center of the D-band moved down, which promoted the adsorption of hydrogen. The NiPd-rGO-180 sample, in which 180 represents the solvothermal temperature in centigrade (°C), has the highest hydrogen storage capacity of 2.65 wt% at a moderate condition (RT/4MPa). The excellent hydrogen storage performance benefits from the synergistic hydrogen spillover effect of Pd–Ni bimetal. The calculated hydrogen adsorption energies of Ni2Pd2-rGO are within the ideal range (−0.20 to −0.60 eV) of hydrogen ads/desorption; however, the introduction of substrate defects and the cluster orientation alter the hydrogen adsorption energy. This work provides an effective reference for the design and optimization of carbon-based hydrogen storage materials.
