Anchoring Pd Single Atoms on N-Doped MOF-Derived TiO2 for Photocatalytic Hydrogen Evolution With an Ultra-High Rate up to 185.8 mmol g-1 h-1.

Abstract

Photocatalytic hydrogen (H2) evolution provides a sustainable pathway for clean energy production. However, conventional photocatalysts suffer from wide bandgaps and rapid charge recombination, leading to low photocatalytic efficiency. Herein, we construct an asymmetric N─Pd─O coordination environment by anchoring Pd single atoms (SAs) onto N‑doped MIL‑125‑derived TiO2. The optimized 1%PdN‑TiO2 catalyst achieves a high H2 evolution rate up to 185.8 mmol g-1 h-1 and an apparent quantum efficiency of 67.4% both measured under 365 nm monochromatic light irradiation. Synchrotron X‑ray absorption fine structure spectroscopy, ultrafast spectroscopy, and density functional theory calculations reveal that the asymmetric N─Pd─O coordination promotes directional charge transfer and lowers the H2 evolution reaction (HER) barrier. This work offers insights into the rational design of heteroatom‑modulated asymmetric coordination microenvironments toward high‑efficiency MOF‑derived single‑atom photocatalysts for sacrificial‑agent‑assisted photocatalytic H2 production.

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