Effect of Metal Site Mobility of Single-Atom Catalyst on Photocatalytic Water Oxidation

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер 16(9), С. 2166 - 2174

Опубликована: Фев. 20, 2025

Understanding the impact of catalytic site diffusion on photocatalytic performance is crucial to rational design water oxidation photocatalysts. In this study, we combined ab initio nonadiabatic molecular dynamics (NAMD) with density functional theory (DFT) calculations investigate single-atom transition metals (Ni, Pd) loaded HfS2 and their effects oxidation. Transition state indicated that barriers (0.58 eV) enable possibility between most stable HS metastable HHf for Pd/1T-HfS2. Moreover, electronic structure simulations reveal distinct properties Pd/1T-HfS2:Pd adsorption at generate a deep defect (∼0.5 eV above valence band maximum (VBM)), while introduces shallow near VBM (∼0.2 VBM). Compared pristine 1T-HfS2 (6.2 ns), electron-hole recombination time extends 7 ns Pd(HS)/1T-HfS2 but decreases 1.7 Pd(HHf)/1T-HfS2, driven by position Pd-induced states. Thermodynamically, Pd(HHf)/1T-HfS2 show pronounced difference, approximately 0.08 V in limiting potential. Generally, study enhances understanding dynamic catalysts.

Язык: Английский

Copolymerization of Poly (Triazine Imide) Single Crystal Nanoplates with Enhanced Charge Transfer for Efficient Photocatalytic Overall Water Splitting

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Дек. 23, 2024

Abstract Solar‐driven photocatalytic overall water splitting represents a sustainable strategy to produce green hydrogen using metal‐free polymeric carbon nitride. However, conventional thermal polymerization with single precursor for the synthesis of poly (triazine imide) faces challenges such as slow deamination rates and mass transfer, resulting in formation undesired structural defects, which usually serve charge recombination sites decrease performance. Herein, highly crystalline by copolymerization binary precursors melamine cyanuric acid presence molten salts is reported. The results reveal that easily generate melam (intermediates nitride) subsequently facilitate polycondensation process. Solid characterizations revealed nanoplates extended π‐conjugation degrees reduced intensity defects would be obtained, largely promotes separation migration photogenerated carriers, inhibits undesirable at defect sites. Accordingly, after situ photo‐deposition CoO x Pt/Cr 2 O 3 H evolution co‐catalysts, respectively, optimized achieve an excellent solar‐to‐hydrogen conversion 0.30% under simulated sunlight irradiation.

Язык: Английский

Solid salt induced and activated semi-coke decorated carbon nitride with enhanced photocatalytic H2 production

International Journal of Hydrogen Energy, Год журнала: 2025, Номер 114, С. 368 - 377

Опубликована: Март 1, 2025

Язык: Английский