Atomic‐Level Platinum Filling into Ni‐Vacancies of Dual‐Deficient NiO for Boosting Electrocatalytic Hydrogen Evolution

Abstract

Developing low‐cost and high‐efficiency catalysts for sustainable hydrogen production through electrocatalytic hydrogen evolution reaction (HER) is crucial yet remains challenging. Here, a strategy is proposed to fill Ni‐vacancy (Niv) sites of dual‐deficient NiO (D‐NiO‐Pt) deliberately created by Ar plasma with homogeneously distributed Pt atoms driven by oxygen vacancies (Ov). The incorporated Pt atoms filling the Niv reduce the formation energy to increase crystal stability, and subsequently combine with additional Ov to tune the electronic structure of the surrounding Ni sites. Thus, a more ideal hydrogen adsorption free energy (ΔGH*) closer to 0 of Ni sites and Pt sites can be achieved. As a result, the D‐NiO‐Pt electrode achieves superior mass activity of ≈1600 mA mg−1 (normalized by platinum) and nearly negligible loss of activity during long‐term operation, which is much better than as‐prepared Pt‐containing NiO catalysts without plasma treatment. A low overpotential of 20 mV is required for the D‐NiO‐Pt at 10 mA cm−2 in alkaline HER, outperforming that of the commercial Pt/C. In addition, the universal access to the other Ni‐based compounds including nickel phosphide (Ni2P), nickel sulfide (Ni0.96S), and nickel selenide (NiSe2) is also demonstrated by employing a vacancy‐driven Pt filling mechanism.

One-Step Electrochemical Synthesis of Co0.8Fe0.2Se@NiF Spheres Enclosed with Nanoparticles and Integrated Porous FeSe2@NiF as Electrode Materials for High-Performance Asymmetric Supercapacitor

“…These nanoparticles can form a more porous nanostructure and produce a sufficient active site that enhances the interfacial surface between the electrode material and the electrolyte, resulting in improvement and increased electrochemical performance. Furthermore, the porous nanoarchitecture leads to high electrochemical active surface areas (ECSAs) that may facilitate the diffusion of electrolyte ions, leading to the rapid charge transfer reaction. , This structure is appropriate for improving electrochemical properties as an electrode active material for supercapacitors. As shown in the EDX mapping (Figure E–H), the synthesized Co 0.8 Fe 0.2 Se@NiF electrode material includes cobalt (Co), iron (Fe), selenium (Se), and oxygen (O), which support the results of the XPS test.…”

“…Furthermore, the porous nanoarchitecture leads to high electrochemical active surface areas (ECSAs) that may facilitate the diffusion of electrolyte ions, leading to the rapid charge transfer reaction. 56,57 This structure is appropriate for improving electrochemical properties as an electrode active material for supercapacitors. As shown in the EDX mapping (Figure 3E− H), the synthesized Co 0.8 Fe 0.2 Se@NiF electrode material includes cobalt (Co), iron (Fe), selenium (Se), and oxygen (O), which support the results of the XPS test.…”

Alloy-Type Lithium Anode Prepared by Laser Microcladding and Dealloying for Improved Cycling/Rate Performance

“…Energy carriers such as batteries, capacitors, and hydrogen are critical for replacing fossil fuels with renewable resources and reducing environmental issues. − Nowadays, with the urgent market demand for the rechargeable batteries with high energy density, great attention has been drawn to high-capacity alloy-type materials (Si, Ge, Sn, etc.) in next-generation lithium-ion batteries (LIBs), sodium-ion batteries, and potassium-ion batteries. − However, they undergo significant volume change during ion insertion and extraction, resulting in serious degradation in capacity and cycling life, which is a major and catastrophic problem for further practical applications. − …”

Three-Dimensional Graphene-Supported CoP-RuP2 with Artificial Heterointerfaces for an Enhanced Universal-pH Hydrogen Evolution Reaction

“…Of note, the construction of heterostructures is conducive to modulate the heterointerfacial electronic redistribution, produce rich active sites, and promote electron transfer, thereby leading to the improvement of catalytic performance. − On the other hand, anchoring TMPs on conductive substrates (e.g., porous carbon, − carbon tubes, − and graphene − ) has been proposed as an effective solution, which can effectively prevent TMPs from agglomerating and elevate their catalytic properties and stability. Especially, in comparison with solid materials, a 3D porous robust carbon matrix may offer a large surface area for exposing plentiful active sites, hierarchical micro-/mesopores for shortening the ion diffusion distance, and high conductivity. − Nevertheless, how to construct highly dispersed heterostuctures of TMPs on 3D porous carbon architectures by an easily scalable method remains an enormous challenge.…”