Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide

Abstract

Heteroatom-doped carbons have drawn increasing research interest as catalysts for various electrochemical reactions due to their unique electronic and surface structures. In particular, co-doping of carbon with boron and nitrogen has been shown to provide significant catalytic activity for oxygen reduction reaction (ORR). However, limited experimental work has been done to systematically study these materials, and much remains to be understood about the nature of the active site(s), particularly with regards to the factors underlying the activity enhancements of these boron-carbon-nitrogen (BCN) materials. Herein, we prepare several BCN materials experimentally with a facile and controlled synthesis method, and systematically study their electrochemical performance. We demonstrate the existence of h-BN domains embedded in the graphitic structures of these materials using X-ray spectroscopy. These synthesized structures yield higher activity and selectivity toward the 2e ORR to HO than structures with individual B or N doping. We further employ density functional theory calculations to understand the role of a variety of h-BN domains within the carbon lattice for the ORR and find that the interface between h-BN domains and graphene exhibits unique catalytic behavior that can preferentially drive the production of HO. To the best of our knowledge, this is the first example of h-BN domains in carbon identified as a novel system for the electrochemical production of HO.

Fluorescent Carbon‐ and Oxygen‐Doped Hexagonal Boron Nitride Powders as Printing Ink for Anticounterfeit Applications

“…The two peaks at 285.7 and 286.5 eV are due to BCN 2 and CN 3 , respectively 19a,22b. Another two components with higher binding energy at 287.8 and 288.9–289.2 eV are likely from CO and OCO bonds, respectively . In the O 1s spectrum, the most significant contribution at 532.6 eV is associated with OB bonds, along with a shoulder at 513.6 eV resulting from OC bonding .…”

Exploring Bi2Te3 Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

“…The value of N was experimentally determined to be 0.29 by using a standard ferricyanide system (Figure S7, Supporting Information). [ 35 ] Figure a shows the O 2 reduction disk currents and the simultaneously measured peroxide oxidation ring currents for the activated Bi 2 Te 3 NPs/C, the commercial Bi 2 Te 3 /C, carbon, and GC. The amount of H 2 O 2 produced was monitored at the ring electrode, where a positive current was measured once H 2 O 2 was produced at the disk.…”

Tailoring the Electrochemical Production of H2O2: Strategies for the Rational Design of High‐Performance Electrocatalysts

“…For nitrogen functionalization, the higher electronegativity of the nitrogen atom within the carbon framework breaks the integrity of the π conjugate system and induces a charge redistribution,4b changing the adsorption properties of the intermediates on the carbon materials. Furthermore, nitrogen doping is also observed to increase the overall surface area of carbon material through the formation of micro‐ and mesopores within the carbon framework, creating additional active sites …”