The first coordination shell is considered crucial in determining the performance of single atom catalysts (SACs), but the significance of the second coordination shell has been overlooked. In this study, we developed a post-doping strategy to realize predictable and controlled modulation on the second coordination shell. By incorporating a P atom into the second coordination shell of a porphyrin-like Pt SAC, the charge density at the Fermi level of Pt single atom increases, enhancing its intrinsic activity.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2024
Platinum (Pt) has been widely used as cathodic electrocatalysts for the hydrogen evolution reaction (HER) but unfortunately neglected as an anodic electrocatalyst for the oxygen evolution reaction (OER) due to excessively strong bonding with oxygen species in water splitting electrolyzers. Herein we report that fine control over the electronic-structure and local-coordination environment of Pt-rich PtPbCu nanowires (NWs) by doping of iridium (Ir) lowers the overpotential of the OER and simultaneously suppresses the overoxidation of Pt in IrPtPbCu NWs during water electrolysis. In light of the one-dimensional morphology featured with atomically dispersed IrO species and electronically modulated Pt-sites, the IrPtPbCu NWs exhibit an enhanced OER (175 mV at 10 mA cm) and HER (25 mV at 10 mA cm) electrocatalytic performance in acidic media and yield a high turnover frequency.
View Article and Find Full Text PDFIn line with current research goals involving water splitting for hydrogen production, this work aims to develop a noble-metal-free electrocatalyst for a superior hydrogen evolution reaction (HER). A single-step interfacial activation of TiCT MXene layers was employed by uniformly growing embedded WS two-dimensional (2D) nanopetal-like sheets through a facile solvothermal method. We exploited the interactions between WS nanopetals and TiCT nanolayers to enhance HER performance.
View Article and Find Full Text PDFAdv Sci (Weinh)
May 2024
Small Methods
September 2024
Defects in the crystal structure of nanomaterials are important for their diverse applications. As, defects in 2D framework allow surface confinement effects, efficient molecular accessibility, high surface-area to volume-ratio and lead to higher catalytic activity, but it is challenging to expose defects of specific metal on the surface of 2D alloy and find the correlation between defective structure and electrocatalytic properties with atomic precision. Herein, the work paves the way for the controlled synthesis of ultrathin porous Ir-Cu nanosheets (NSs) with selectively iridium (Ir) rich defects to boost their performance for acidic oxygen evolution reaction (OER).
View Article and Find Full Text PDFVisible light active g-CN/CeO/FeO ternary composite nanosheets were fabricated by facile co-precipitation routes. The density functional theory (DFT) computations investigated changes in geometry and electronic character of g-CN with CeO and FeO addition. Chemical and surface characterizations were explored with XRD, XPS, SEM, TEM, PL, DRS and Raman measurements.
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