Construction of internal electric fields (IEFs) is crucial to realize efficient charge separation for charge-induced redox reactions, such as water splitting and CO2 reduction. However, a quantitative understanding of the charge transfer dynamics modulated by IEFs remains elusive. Here, electron microscopy study unveils that the non-equilibrium photo-excited electrons are collectively steered by two contiguous IEFs within binary (001)/(200) facet junctions of BiOBr platelets, and they exhibit characteristic Gaussian distribution profiles on reduction facets by using metal co-catalysts as probes. An analytical model justifies the Gaussian curve and allows us to measure the diffusion length and drift distance of electrons. The charge separation efficiency, as well as photocatalytic performances, are maximized when the platelet size is about twice the drift distance, either by tailoring particle dimensions or tuning IEF-dependent drift distances. The work offers great flexibility for precisely constructing high-performance particulate photocatalysts by understanding charge transfer dynamics.

The construction of heterojunctions is a promising manner to accelerate the separation and transfer of the charge carriers at the interface. Herein, a binary poly(heptazine‐triazine) imides (PHI/PTI) with semi‐coherent interfaces was fabricated via a facile two‐step salt‐melt synthetic process. The built‐in electric fields at the semi‐coherent interface endow prompt exciton splitting and charge carrier separation. Hence, the optimized PHI/PTI‐based copolymer presents a high apparent quantum yield (AQY=64 %) for visible‐light driven hydrogen production, by the aids of K2HPO4 as charge transfer mediator. This study provides physical insights for the rational promotion of the photocatalytic performance from the viewpoint of interfacial engineering of photocatalytic junctions on crystalline carbon nitride based semiconductors.

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Poly (triazine imide) (PTI/Li+Cl−), one of the crystalline versions of polymeric carbon nitrides, holds great promise for photocatalytic overall water splitting. In principle, the photocatalytic activity of PTI/Li+Cl− is closely related to the morphology, which could be reasonably tailored by the modulation of the polycondensation process. Herein, we demonstrate that the hexagonal prisms of PTI/Li+Cl− could be converted to hexagonal nanosheets by adjusting the binary eutectic salts from LiCl/KCl or NaCl/LiCl to ternary LiCl/KCl/NaCl. Results reveal that the extension of in‐plane conjugation is preferred, when the polymerisation was performed in the presence of ternary eutectic salts. The hexagonal nanosheets bears longer lifetimes of charge carriers than that of hexagonal prisms due to lower intensity of structure defects and shorter hopping distance of charge carriers along the stacking direction of triazine nanosheets. The optimized hexagonal nanosheets exhibits a record apparent quantum yield value of 25 % (λ=365 nm) for solar hydrogen production by one‐step excitation overall water splitting.

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Tunable crystalline defects endow WO 3−x catalysts with extended functionalities for a broad range of photo-and electric-related applications. However, direct visualization of the defect structures and their evolution mechanism is lacking. Herein, aberration-corrected and in situ transmission electron microscopy was complemented by theoretical calculations to investigate the effect of temperature on the defect evolution behavior during hydrogenation treatment. Low processing temperature (100−300 °C) leads to the occurrence of randomly distributed oxygen vacancies within WO 3−x nanosheets. At higher temperatures, oxygen vacancies become highly mobile and aggregate into stacking faults. Planar defects are prone to nucleate at the surface and develop in a zigzag form at 400 °C, while treating at 500 °C promotes the growth of {200}-type stacking faults. Our work clearly establishes that the atomic configuration of the defects in WO 3−x samples could be manipulated by regulating the hydrogenation temperature. This study not only expands our understanding of the structure−function relationships of sub-stoichiometric tungsten oxides but also unlocks their full potential as advanced catalysts by tuning stoichiometry in a controlled manner.

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