Engineering carbon semi-tubes supported platinum catalyst for efficient oxygen reduction electrocatalysis

Manipulation of Electronic States of Pt Sites via d-Band Center Tuning for Enhanced Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cells

“…As neotype ORR electrocatalysts, atomically dispersed Pt–nitrogen–carbon (Pt–N–C) sites have been demonstrated to have unique physicochemical properties contributing to various electrochemical reactions in energy storage and conversion due to their maximum atom utilization efficiency, capability of remarkably reducing Pt usage, and excellent electrocatalytic activity. − However, the degradation of the catalytic performance of these reported Pt–N–C under long-term operation is still behind satisfactory for ORR. As an effective and reasonable strategy, the combination of metal nanoparticles and single atoms can adjust the electronic orbital of metal-N active sites, help O 2 activation on metal-N active sites through shifting the location of the d-band center of Pt, and lead to optimized adsorption binding energies between Pt and reaction oxygen-related intermediates during the ORR process. − Currently, covalent organic frameworks (COFs) are one type of burgeoning crystalline porous polymers with framework designability and precise structural tenability, which provides a unique advantage in the fabrication of materials derived from the distinct electronic configurations of in situ formed exotic metal species coordinated to N atoms. − In addition, from the perspective of functional materials, COF-derived N–C materials with a uniform M–N center and a nanosized porous channel in the carbon substrate are highly appealing in the field of heterogeneous catalysis. − With this knowledge, a question arises: whether it is conceivable to modulate the Pt site electronic environment through altering the d-band centers with Pt particles and an atomically dispersed state in the COF-derived porous nanocarbon matrix. − Moreover, it is of great theoretical and practical importance to research the corresponding reaction mechanism of the ORR process on this issue and apply it practically in PEMFCs.…”

Simple and Efficient Method for Screening Electrocatalyst Supports at the Single Nanoparticle Level

“…Among them, heteroatom-doped carbon supports have been attracting significant attention due to their superior electrochemical stability, lightweight, and low cost. , The incorporation of heteroatoms (nitrogen, sulfur, boron, or others) can induce the electron redistribution and increase the defective structure of the catalysts, thereby altering their intrinsic activity . For instance, the intrinsic ORR activity of a Pt-based catalyst is significantly improved by doping nitrogen onto the carbon substrate . In recent years, considerable efforts for screening of catalyst supports, either theoretical or experimental methods, are thriving for developing high-performance electrocatalysts; but these methods demand exhaustive experiments and characterization, resulting in long-term cycles and high cost in research. − Additionally, the electrocatalytic performance is based on the average contribution of a large number of nanoparticles (NPs) on a large electrode surface, resulting in obscuring the structure–activity relationship.…”

“…15 For instance, the intrinsic ORR activity of a Pt-based catalyst is significantly improved by doping nitrogen onto the carbon substrate. 16 In recent years, considerable efforts for screening of catalyst supports, either theoretical or experimental methods, are thriving for developing high-performance electrocatalysts; but these methods demand exhaustive experiments and character-ization, resulting in long-term cycles and high cost in research. 17−21 Additionally, the electrocatalytic performance is based on the average contribution of a large number of nanoparticles (NPs) on a large electrode surface, resulting in obscuring the structure−activity relationship.…”