We observed a significant reorganization in the structure during the constant temperature portion. Several S atoms began to move from the Ni3S2 section to pure Ni. These atoms were mobile on the surface of Ni but did not move back to Ni3S2 phase. In addition, some Inspection of the surface, reveals this structure to be poorly suited for alkaline HER just as the pristine Ni3S2 surface is. As in our previous publication, the formation of an unfavorable S-H bond is still required to break an O-H bond. In addition, the H adsorption energies on this amorphous Ni3S2-like phase show it to have a poor performance. Some representative hydrogen adsorption energies are listed in Table .