Boron From Net Charge Acceptor to Donor and Its Effect on Hydrogen Uptake by Novel Mg-B-electrochemically Synthesized Reduced Graphene Oxide
Abstract Hydrogen uptake (H-uptake) is studied in ball milled Mg-B-electrochemically synthesized reduced graphene oxide (erGO) nanocomposites at PH2≈15 bar, ~320 ℃. B/C (weight ratio): 0, ~0.09, ~0.36, ~0.90 are synthesized maintaining erGO≈10wt %. B occupies octahedral interstices within Mg unit cell - revealed by electron density maps. Persistent charge donations from Mg and B to C appear as Mg-C (~283.2 eV), B-C (~283.3-283.9 eV) interactions in C-1s core X-ray photoelectron spectrometry (XPS) at all B/C. At B/C>0.09, charge reception by B from Mg yields Mg-B interaction (51.3 eV, Mg-2p XPS). This net charge acceptor role of B does not alter Mg unit cell size significantly. Despite charge donation to both C and B, the Mg charge is <+2, resulting in long incubation times (>5 h) at B/C>0.09. In B/C≈0.09, C-2p π→π* transition (~290 eV, C-1s XPS) is also seen. Absence of Mg-B interaction renders B a charge donor, resulting in Mg-B repulsion and Mg unit cell expansion. Mg-C peak shift to lower binding energies (C-1s XPS), decreases incubation time to 2.25 h and increases H-uptake kinetics. Various atomic interactions influence the reduction of incubation time in H-uptake and increase its kinetics in the order: (Mg→C; B→C)B/C≈0.09 > (Mg→C)B/C=0 > (ternary Mg→B→C)B/C>0.09.