Novel two-dimensional boron-centered graphdiyne analogue as multifunctional electrocatalyst for hydrogen evolution, oxygen evolution, and oxygen reduction reactions

Seeking multifunctional electrocatalysts capable of driving the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) is becoming increasingly crucial in the realm of sustainable energy development. Herein, the multifunctional electrocatalytic activities of HER, OER, and ORR in two-dimensional (2D) boron-centered graphdiyne analogue (B-GDY) are identified by first-principles computations, and its low overpotentials of HER/OER/ORR (0.02/0.55/0.52 V) are comparable to, or even surpasses, well-developed noble-metal-based catalysts. The remarkable multifunctional electrocatalytic activity of B-GDY can be attributed to the unique orbital distribution of the 2D framework as evidenced by its highest occupied molecular orbitals (HOMO), and synergistic interplay of boron-centered carbocycles and diacetylene linkages in its unique 2D framework. More importantly, the data confirm our motivation by replacing the central C in small aromatic groups with the adjacent element of B can realize/create multi-active sites in the original aromatic functional groups (the simplest boron-centered triangulene-like units). Hence, this study not only provides cost-effective alternatives to metal-based catalysts but also paves the way for designing and developing novel, multifunctional electrocatalysts.