Partially Pyrolyzed Binary Metal–Organic Framework Nanosheets for Efficient Electrochemical Hydrogen Peroxide Synthesis

Abstract

Herein, we developed a partially controlled pyrolysis strategy to create evenly distributed NiO nanoparticles within NiFe‐MOF nanosheets (MOF NSs) for electrochemical synthesis of H2O2 by a two‐electron oxygen reduction reaction (ORR). The elemental Ni can be partially transformed to NiO and uniformly distributed on the surface of the MOF NSs, which is crucial for the formation of the particular structure. The optimized MOF NSs‐300 exhibits the highest activity for ORR with near‐zero overpotential and excellent H2O2 selectivity (ca. 99 %) in 0.1 m KOH solution. A high‐yield H2O2 production rate of 6.5 mol gcat−1 h−1 has also been achieved by MOF NSs‐300 in 0.1 m KOH and at 0.6 V (vs. RHE). In contrast to completely pyrolyzed products, the enhanced catalytic activities of partially pyrolyzed MOF NSs‐300 originates mainly from the retained MOF structure and the newly generated NiO nanoparticles, forming the coordinatively unsaturated Ni atoms and tuning the performance towards electrochemical H2O2 synthesis.

An Efficient Interfacial Synthesis of Two‐Dimensional Metal–Organic Framework Nanosheets for Electrochemical Hydrogen Peroxide Production

“…[1] Apart from extensively investigated 2D materials such as g-C 3 N 4 , layered double hydroxides (LDH), transition-metal dichalcogenides (TMDs), and hexagonal boron nitride (h-BN), [2][3][4][5] the 2D metal-organic frameworks (MOFs) comprised of metal centers and organic linkers have aroused emerging interests in materials and catalysis. [6][7][8][9][10][11][12][13] Because of their extraordinarily high surface areas, tunable pore size and regulable internal surface, MOFs have been widely applied in many fields, such as electrocatalysis. [14][15][16][17] To date, the most reported method for synthesizing 2D MOF NSs was ultrasonication and solvo-thermal method.…”

Honeycomb Carbon Nanofibers: A Superhydrophilic O2‐Entrapping Electrocatalyst Enables Ultrahigh Mass Activity for the Two‐Electron Oxygen Reduction Reaction

“…The under‐developed direct H 2 O 2 synthesis from an H 2 –O 2 mixture is also potentially explosive [5] . Electrochemical two‐electron (2 e − ) oxygen reduction is regarded as an attractive alternative for on‐site direct H 2 O 2 production from O 2 and water at ambient conditions, and the devices can be powered by sustainable renewable electricity sources; however, it is challenged by strong competition from the four‐electron (4 e − ) oxygen reduction [6–9] . As such, it is in great need to design and develop efficient oxygen reduction reaction (ORR) electrocatalysts for selective production of H 2 O 2 via a 2 e − pathway.…”

An Efficient Interfacial Synthesis of Two‐Dimensional Metal–Organic Framework Nanosheets for Electrochemical Hydrogen Peroxide Production

“…Since the discovery of graphene in 2004, two‐dimensional (2D) materials have been attracted huge research attentions due to their unique physical, optical and electrical properties so as to many highly promising applications [1] . Apart from extensively investigated 2D materials such as g‐C 3 N 4 , layered double hydroxides (LDH), transition‐metal dichalcogenides (TMDs), and hexagonal boron nitride (h‐BN), [2–5] the 2D metal–organic frameworks (MOFs) comprised of metal centers and organic linkers have aroused emerging interests in materials and catalysis [6–13] . Because of their extraordinarily high surface areas, tunable pore size and regulable internal surface, MOFs have been widely applied in many fields, such as electrocatalysis [14–17] .…”