Interfacial Electron Distribution of Co Nanoparticles Supported on N‐Doped Mesoporous Hollow Carbon Spheres Endows Highly Efficient ORR, OER, and HER

Abstract

The tailoring of the charge transfer between support material and transition metal active phase is an effective strategy for fine tuning the electronic structure of the catalyst active site, and hence improving the activity and stability of the reaction. This works presents that Co nanoparticles supported on N‐doped mesoporous hollow carbon nanospheres (Co/NMHCS) decouple the effect of electronic structure on catalytic performance. The detailed experimental and theoretical results reveal the charge distribution at the Co/NMHCS interface due to N‐doped MHCS. With tuning the electron redistribution, the interface between Co nanoparticles and NMHCS as the active site shows the strong capability to adsorb and reduce the OOH* and proton, thus leading to the optimal ORR, OER, and HER activity in Co/NMHCS. Furthermore, Co/NMHCS‐based Zn–air battery exhibits high power density of 185 mW cm−2, and high gravimetric energy density of 753 mAh gZn−1. Density functional theory (DFT) reveals the electrons accumulate directly on the NMHCS support, which originates from an interplay between Co nanoparticles and the NMHCS support. This work provides constructive guidance for precisely regulating the interface electronic structures to achieve excellent electrocatalytic performance.

Constructing Chainmail-Structured CoP/C Nanospheres as Highly Active Anodic Electrocatalysts for Oxygen Evolution Reaction

“…Furthermore, the formation of the interface between NMHCS and Co can promote the absorption of OOH*, thus resulting in the optimal performance of the oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and hydrogen evolution reaction (HER). 31 However, how to stably synthesize the transitionmetal−supported @ hollow nanocarbon sphere catalyst with excellent activity is still a difficult problem. Herein, we successfully synthesized well-defined and structurally stable hollow nanocarbon spheres (named the Cnanosphere).…”

“…Besides, the special NMHCS structure could provide abundant active sites, promoting the kinetics of the catalytic processes. Furthermore, the formation of the interface between NMHCS and Co can promote the absorption of OOH*, thus resulting in the optimal performance of the oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and hydrogen evolution reaction (HER) . However, how to stably synthesize the transition-metal–supported @ hollow nanocarbon sphere catalyst with excellent activity is still a difficult problem.…”

Innovative Catalyst Design of Sea-Urchin-like NiCoP Nanoneedle Arrays Supported on N-Doped Carbon Nanospheres for Enhanced HER Performance

“…11,12 Recognizing these limitations, there is a growing interest in three-dimensional (3D) nanocatalysts due to their substantial specific surface area, enhanced site exposure for high activity, and improved mass transfer rates. 13,14 For example, Wei et al synthesized a graphene aerogel catalyst incorporating NiCoP nanoparticles (NiCoP-NPs@GA) that exhibited a slight collapse after 1000 CV cycles. 15 Hence, it is necessary to develop a 3D transition metal phosphide catalyst for electrocatalytic water splitting with high activity and excellent stability.…”

“…Despite the advantages of TMP, these electrocatalysts usually suffer from sluggish electron transport, slow electrolyte diffusion, and delayed bubble evolution. Even worse, they are prone to aggregation or structural collapse, resulting in poor long-term catalytic process stability of the catalysts. , Recognizing these limitations, there is a growing interest in three-dimensional (3D) nanocatalysts due to their substantial specific surface area, enhanced site exposure for high activity, and improved mass transfer rates. , For example, Wei et al synthesized a graphene aerogel catalyst incorporating NiCoP nanoparticles (NiCoP-NPs@GA) that exhibited a slight collapse after 1000 CV cycles . Hence, it is necessary to develop a 3D transition metal phosphide catalyst for electrocatalytic water splitting with high activity and excellent stability.…”

Structural design of FeCo alloy implanted into N,S co-doped carbon nanotubes via self-catalyzed growth for advanced liquid and flexible all-state-state Zn–air battery

“…Experimental and theoretical results revealed that N-doped MHCS resulted in charge distribution at the Co/NMHCS interface, showing a strong ability to adsorb and reduce OOH* and protons. 23 In addition to the introduction of nitrogen alone, co-doping N and S with different atomic radii and electronegativities can largely change the electron distribution of adjacent carbon atoms, resulting in high ORR activity. 24,25 Yan et al demonstrated that the synergistic interaction of N and S in the carbon skeleton can produce more defects and the p-N/S adsorption potential with oxygen is greatly reduced, promoting the ORR process.…”