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Optimizing the binding of the *OOH intermediate via axially coordinated Co-N5 motif for efficient electrocatalytic H2O2 production.
- Source :
-
Applied Catalysis B: Environmental . Dec2023, Vol. 338, pN.PAG-N.PAG. 1p. - Publication Year :
- 2023
-
Abstract
- Electrochemical production of hydrogen peroxide (H 2 O 2) is a sustainable and environmentally benign process. The electrochemical oxygen reduction process (ORR) via a two electron pathway (2e- ORR) offers a practical method for on-site H 2 O 2 generation. As an earth-abundant catalyst, the cobalt-nitrogen coordinated systems integrated into the carbon matrix (Co-NC) has caused wide attention for its high activity in 2e- ORR. Even though most of the reported Co-NC catalysts have classical planar Co-N 4 coordination, axial coordination engineering has recently emerged as an effective way to control the active sites in the axial direction by using different coordination ligands. The structure-function link between the Co-N configuration of non-planar coordination and 2e- ORR activity is, however, not fully understood. An axial-N coordinated Co-N 5 motif embedded in hierarchically porous graphite-3R carbon (Co-N 5 C) was effectively synthesized using a template-sacrificing method. The Co-N 5 C has a high selectivity for 2e- ORR and a high H 2 O 2 molar production rate of up to 6.78 mol peroxide/g catalyst /h in acidic media, both of which are better than its Co-N 4 counterpart. DFT analyses demonstrate that axial-N ligands regulated the d -band center of the Co atom in the Co-N 5 C catalyst, inducing a shift in Δ G *OOH near the Sabatier volcano plot's peak (Δ G *OOH = 4.22 eV). This optimized the binding of the *OOH intermediate and then enhanced the protonation of *OOH to produce H 2 O 2 more efficiently. [Display omitted] • A Co-N 5 C catalyst containing an axial-N ligand was synthesized for the effective ORR. • Co-N 5 C, with graphite-3R phase, showed a specific BET surface area of 801.6 m2/g. • Co-N 5 C exhibited a high selectivity for 2e- ORR and H 2 O 2 molar production rate. • Co-N 5 C possessed a high active SD and high intrinsic kinetic TOF. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 09263373
- Volume :
- 338
- Database :
- Academic Search Index
- Journal :
- Applied Catalysis B: Environmental
- Publication Type :
- Academic Journal
- Accession number :
- 164962476
- Full Text :
- https://doi.org/10.1016/j.apcatb.2023.123078