Isolated Au Atom Anchored on Porous Boron Nitride as a Promising Electrocatalyst for Oxygen Reduction Reaction (ORR): A DFT Study

Abstract

The development of efficient, stable, and low-cost catalytic material for the oxygen reduction reaction (ORR) is currently highly desirable but challenging. In this work, based on first-principles calculation, the stabilities, catalytic activities and catalytic mechanisms of isolated Au atom supported on defective porous BN (p-BN) have been studied in detail. The results reveal that the defective p-BN anchor Au atom strongly to ensure the stability of Au/p-BN. Based on frontier molecular orbital and charge-density analysis, isolated Au atom supported on porous BN with VN defect (Au/p-BN-VN) is an effective ORR catalyst. Especially, the low barriers of the formation (0.38 eV) and dissociation (0.31 eV) of *OOH and the instability of H2O2 on Au/p-BN-VN catalyst suggest that ORR proceeds via 4-electron pathway. Along the favorable pathway, the reduction of O2 to *OOH is the rate-limiting step with the largest activation barrier of 0.38 eV and the maximum free energy change is 1.88 eV. Our results provide a useful guidance for the design and fabrication of new Au-base catalyst with high-efficiency and are beneficial for the developing of novel isolated metal atom catalysts for ORR.

Single transition metal atom centered clusters activating semiconductor surface lattice atoms for efficient solar fuel production

“…These obvious changes in the pDOS curves evidence the strong interactions between the Ni(O 1.5 H) 6 clusters and the CZS host, implying the excellent stability of the joining structure. 60,61 Moreover, the formation of defect states across the Fermi level will probably improve the electronic conductivity and electron transport, 62–64 thereby promoting the separation of charge carriers, which is in line with the findings in photoluminescence analysis. However, for the shallow acceptor level above the Fermi level, it should be responsible for the enhanced light absorption at wavelengths ranging from 500 to 700 nm in Fig.…”

Bimetallic AuPd Nanoparticles Loaded on Amine-Functionalized Porous Boron Nitride Nanofibers for Catalytic Dehydrogenation of Formic Acid

“…The strong interactions indicate that h-BN can favorably support metal atoms in thermodynamics. 48 It is also noteworthy that as compared with Figure 7d,e, Figure 7f shows several new peaks around the Fermi energy level in both Pd PDOS and TDOS after the formation of the AuPd alloy. The increased density of states near the Fermi energy level facilitates the electron transfer at the carrier metal interface, which is generally regarded as a sign of the high catalytic activity.…”

“…The obvious resonance between the d orbitals of metal atoms and the partial 2p orbitals of B/N atoms (especially N atoms) can be observed, revealing the strong interactions between metal atoms and h-BN. The strong interactions indicate that h-BN can favorably support metal atoms in thermodynamics . It is also noteworthy that as compared with Figure d,e, Figure f shows several new peaks around the Fermi energy level in both Pd PDOS and TDOS after the formation of the AuPd alloy.…”

Advances in platinum-based and platinum-free oxygen reduction reaction catalysts for cathodes in direct methanol fuel cells

“…The parasitic reactions on the cathode caused by the sluggish ORR kinetics and methanol crossing should be minimized to further develop advanced cathodic catalysts for DMFCs. Catalysts such as Ag (Park et al, 2016), Au (Li et al, 2019b), Pt (Zhu et al, 2021), Pd (Ejaz and Jeon, 2018), and nitrogendoped carbon nanotubes (NCNTs) (Ejaz and Jeon, 2018), have all shown enhanced ORR activities. Based on current progress in this field, it is necessary to explore platinum-free cathodic catalysts with high performance and methanol resistance.…”