Hydrogen energy is critical for achieving carbon neutrality. Heterostructured materials with single metal-atom dispersion are desirable for hydrogen production. However, it remains a great challenge to achieve large-scale fabrication of single atom-anchored heterostructured catalysts with high stability, low cost, and convenience. Here, we report single iron (Fe) atom-dispersed heterostructured Mo-based nanosheets developed from a mineral hydrogel. These rationally designed nanosheets exhibit excellent hydrogen evolution reaction (HER) activity and reliability in alkaline condition, manifesting an overpotential of 38.5 mV at 10 mA cm, and superior stability without performance deterioration over 600 h at current density up to 200 mA cm, superior to most previously reported non-noble-metal electrocatalysts. The experimental and density functional theory results reveal that the O-coordinated single Fe atom-dispersed heterostructures greatly facilitated HO adsorption and enabled effective adsorbed hydrogen (H*) adsorption/desorption. The green, scalable production of single-atom-dispersed heterostructured HER electrocatalysts reported here is of great significance in promoting their large-scale implementation.
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http://dx.doi.org/10.1038/s41467-022-33725-8 | DOI Listing |
Inorg Chem
January 2025
School of Materials Science and Chemical Engineering, Ningbo University, Ningbo, Zhejiang 315211, P. R. China.
It is especially essential to develop high-performance and low-cost nonprecious metal catalysts for large-scale hydrogen production. A large number of electrochemical catalysts composited by transition metal centers has been reported; however, it is still a great challenge to design and manipulate target electrocatalysts to realize high overall water-splitting activity at the atomic level. Herein, we develop totally new P-(Fe,V)-codoped metastable-phase β-NiMoO.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Nanjing University, College of Engineering and Applied Sciences, No. 163 Xianlin Avenue, Qixia District, Nanjing, Nanjing, CHINA.
Electrolyte engineering has emerged as an effective strategy for stabilizing Zn-metal anodes. However, a single solute or solvent additive is far from sufficient to meet the requirements for electrolyte cycling stability. Here, we report a new-type high-entropy electrolyte composed of equal molar amounts of Zn(OTf)2 and LiOTf, along with equal volumes of H2O, triethyl phosphate, and dimethyl sulfoxide, which enhances electrolyte stability by increasing solvation entropy.
View Article and Find Full Text PDFSmall
January 2025
College of Ecology and Environment, Co-Innovation Center for the Sustainable Forestry in Southern China, Nanjing Forestry University, Nanjing, 210037, P. R. China.
Constructing heterojunctions between phase interfaces represents a crucial strategy for achieving excellent photocatalytic performance, but the absence of sufficient interface driving force and limited charge transfer pathway leads to unsatisfactory charge separation processes. Herein, a doping-engineering strategy is introduced to construct a In─N bond-bridged InS nanocluster modified S doped carbon nitride (CN) nanosheets Z-Scheme van der Waals (VDW) heterojunctions (InS/CNS) photocatalyst, and the preparation process just by one-step pyrolysis using the pre-coordination confinement method. Specifically, S atoms doping enhances the bond strength of In─N and forms high-quality interfacial In─N linkage which serves as the atomic-level interfacial "highway" for improving the interfacial electrons migration, decreasing the charge recombination probability.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Shanghai Jiaotong University, 800 Dongchuan Road, Minhang District, Shanghai, CHINA.
Diabetes significantly increases the risk of serious health issues, including prolonged skin inflammation and delayed wound healing, owing to inferior glucose control and suppression of the immune system. Although traditional hydrogen (H2) therapy is slightly effective, its ability to tailor the release of H2 on the skin is limited. Accordingly, this study proposed a novel strategy for electrocatalytic H2 release under neutral conditions to promote wound healing in diabetic mice and rabbit.
View Article and Find Full Text PDFChemistry
January 2025
Southeast University, School of Chemistry and Chemical Engineering, Dongnan Daxue Road 2, 211189, Nanjing, CHINA.
The design of well-engineered bifunctional electrocatalysts is crucial for achieving durable and efficient performance in overall water splitting. In this study, Ru-doped FeMn-MOF-74 itself has Ru sites and generates FeMnOOH under catalytic conditions, forming dual active sites for overall water splitting. Density functional theory (DFT) calculations demonstrate that the Ru dopants exhibit optimized binding strength for H* and enhanced hydrogen evolution reaction (HER) performance.
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