Exploring efficient and inexpensive oxygen evolution reaction (OER) electrocatalysts is of great importance for various electrochemical energy storage and conversion technologies. Ni-based electrocatalysts have been actively pursued because of their promising activity and earth abundance. However, the OER efficiency for most of the developed Ni-based electrocatalysts has been intrinsically limited due to their low electrical conductivity and poor active site exposure yield. Herein, we report metallic Ni3N nanosheets as an efficient OER electrocatalyst for the first time. The first-principles calculations and electrical transport property measurements unravel that the Ni3N is intrinsically metallic, and the carrier concentration can be remarkably improved with dimensional confinement. The EXAFS spectra provide solid evidence that the Ni3N nanosheets have disordered structure resultant of dimensional reduction, which then could provide more active sites for OER. Benefiting from enhanced electrical conductivity with metallic behavior and atomically disordered structure, the Ni3N nanosheets realize intrinsically improved OER activity compared with bulk Ni3N and NiO nanosheets. Our finding suggests that metallic nitride nanosheets could serve as a new group of OER electrocatalysts with excellent property.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1021/ja5119495 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
School of Chemistry and Chemical Engineering, Shandong University, 250100, Jinan, China.
Rational regulation of active hydrogen (*H) behavior is crucial for advancing electrocatalytic nitrate reduction reaction (NORR) to ammonia (NH), yet in-depth understanding of the *H generation, transfer, and utilization remains ambiguous, and explorations for *H dynamic optimization are urgently needed. Herein we engineer a NiN nanosheet array intimately decorated with Cu nanoclusters (NF/NiN-Cu) for remarkably boosted NORR. From comprehensive experimental and theoretical investigations, the NiN moieties favors water dissociation to generate *H, and then *H can rapidly transfer to the Cu via unique reverse hydrogen spillover mediating interfacial Ni-N-Cu bridge bond, thus increasing *H coverage on the Cu site for subsequent deoxygenation/hydrogenation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
School of Chemical Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu, 610065, P. R. China.
Alkaline methanol-water electrolysis system is regarded as an appealing strategy for electro-reforming methanol into formate and producing hydrogen with low energy-consumption compared with alkaline water electrolysis. However, stability and selectivity under high current densities for practical application remain challenging. Herein, a CeF@NiN nanosheets array anchored on carbon cloth (CeF@NiN/CC) was fabricated.
View Article and Find Full Text PDFSmall
December 2024
School of Materials Science and Engineering, Nankai University, Tianjin, 300350, China.
Nickel (Ni)-based materials represent a compelling avenue as platinum alternatives in the realm of alkaline hydrogen electrocatalysis. However, conventional nickel nitrides (NiN) have long been hindered by sluggish hydrogen evolution kinetics in alkaline environments, owing to inadequate adsorption strengths of both hydrogen and water molecules. Herein, a novel approach is presented involving the design of vanadium (V)-doped NiN/MoO heterogeneous nanosheets (V-NiN@MoO), engineered to achieve optimized adsorption strengths for hydrogen evolution and oxidation reactions (HER/HOR).
View Article and Find Full Text PDFChemSusChem
September 2024
State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014, Zhejiang, P.R. China.
Glycerol oxidation-assisted water electrolysis has emerged as a cost-effective way of co-producing green hydrogen and HCOOH. Still, preparing highly selective and stable nickel-based metal electrocatalysts remains a challenge. Herein, heterostructure NiN/WO nanosheet arrays of bifunctional catalysts with large specific surface areas loaded on nickel foam (denoted as NiN/WO/NF) were synthesized.
View Article and Find Full Text PDFNanoscale
February 2024
Department of Gastroenterology and Hepatology, Guangzhou First People's Hospital, School of Medicine, South China University of Technology, Guangzhou, 510180, China.
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!