*In Journal of molecular modeling *

_{12}and χ

_{3}) by density functional theory (DFT) calculations. The results show that the early- and VIII-TM anchored β

_{12}and χ

_{3}borophenes are structurally and thermodynamically stable. The overpotentials of OER (η

^{OER}) over the Ni supported on β

_{12}and χ

_{3}borophene SACs, designated as β

_{12}-Ni and χ

_{3}-Ni, are 0.38 and 0.35 V, respectively. The η

^{ORR}of β

_{12}-Ni and χ

_{3}-Ni are estimated to be as low as 0.34 and 0.39 V, respectively. The OER/ORR activity of the SACs can be well correlated with their electronic structures. The high η

^{OER}values of early TM supported on borophene SACs correspond to high d-band center of TM. Both β

_{12}-Ni and χ

_{3}-Ni have a moderate d-band center. Since the overpotentials for OER and ORR on β

_{12}-Ni and χ

_{3}-Ni are comparable to those of Pt group metals and their oxides, β

_{12}-Ni and χ

_{3}-Ni can be considered as the promising bifunctional catalysts for OER and ORR.

*Xu Xuewen, Si Ruihao, Dong Yao, Li Lanlan, Zhang Minghui, Wu Xiaoyi, Zhang Jun, Fu Kun, Guo Yue, He Yanyan*

*2021-Feb-03*

**Borophene, Density functional theory (DFT), Oxygen evolution reaction (OER), Oxygen reduction reaction (ORR), Single-atom catalysts (SACs)**