DFT calculation of AsH3 adsorption and dissociation on Ni- and Cu-doped graphene.

This work explores the adsorption and dissociation of AsH3 on Ni- and Cu-doped graphene by density functional theory (DFT) method. The most stable configurations, adsorption energy, and dissociation pathways are calculated thoroughly. In addition, the electron density difference (EDD), charge transfer, partial density of states (PDOS), and frontier orbitals are performed to describe the adsorption and dissociation process. The first dehydrogenation step on PG-Cu is easier than on PG-Ni due to the lower energy barrier. But further dissociation is becoming difficult in both systems. The third dehydrogenation steps are the rate determining steps for the whole reactions on PG-Ni and PG-Cu, as the energy barrier is 2.01 and 1.72 eV. In conclusion, PG-Ni and PG-Cu has similar AsH3 sensitivity, but the dissociation of AsH3 on PG-Cu is easier than on PG-Ni. It indicates that PG-Cu has better catalytic activity as an AsH3 removal catalyst than PG-Ni. This work may provide useful information for further experimental studies to develop efficient and long-term AsH3 removal catalysts. Graphical abstract.