Suppression of Auger Cross Relaxation in Mn-Doped Core-Shell Perovskite Nanocrystals via Wave Function Engineering.

Mn-doped perovskite nanocrystals (NCs) exhibit great application potential because of their unique optical properties. However, the long-lived nature of excited Mn easily leads to the coexistence of excited Mn and host excitons in a single NC, which inevitably induces an Auger cross relaxation between them, thus significantly limiting the luminescent efficiency of Mn due to its competition with internal energy transfer. Herein, we design and prepare a kind of Mn-doped core-shell CsPbCl@CsPbCl perovskite NC with Mn doped only in the shell layer, which is expected to suppress this Auger process by spatially separating the electronic wave functions.

Photocatalytic asymmetric C-C coupling for CO reduction on dynamically reconstructed Ru-O/Ru-O sites.

Solar-driven CO reduction to value-added C chemicals is thermodynamically challenging due to multiple complicated steps. The design of active sites and structures for photocatalysts is necessary to improve solar energy efficiency. In this work, atomically dispersed Ru-O sites in RuInO are constructed by interior lattice anchoring of Ru.

Insight into the Rate-Determining Step in Photocatalytic Z-Scheme Overall Water Splitting by Employing A Series of Perovskite RTaON (R = Pr, Nd, Sm, and Gd) as Model Photocatalysts.

Photocatalysis is an intricate process that involves a multitude of physical and chemical factors operating across diverse temporal and spatial scales. Identifying the dominant factors that influence photocatalyst performance is one of the central challenges in the field. Here, we synthesized a series of perovskite RTaON semiconductors with different A-site rare earth atoms (R = Pr, Nd, Sm, and Gd) as model photocatalysts to discuss the influence of the A-site modulation on their local structures as well as both physical and chemical properties and to get insight into the rate-determining step in photocatalytic Z-scheme overall water splitting (OWS).

Time-Resolved Spectroscopy for Dynamic Investigation of Photoresponsive Metal-Organic Frameworks.

Photoresponsive MOFs with precise and adjustable reticular structures are attractive for light conversion applications. Uncovering the photoinduced carrier dynamics lays the essential foundation for the further development and optimization of the MOF material. With the application of time-resolved spectroscopy, photophysical processes including excimer formation, energy transfer/migration, and charge transfer/separation have been widely investigated.

Insight into the Key Restriction of BiVO Photoanodes Prepared by Pyrolysis Method for Scalable Preparation.

Bismuth Vanadate (BiVO ) photoanode has been popularly investigated for promising solar water oxidation, but its intrinsic performance has been greatly retarded by the direct pyrolysis method. Here we insight the key restriction of BiVO prepared by metal-organic decomposition (MOD) method. It is found that the evaporation of vanadium during the pyrolysis tends to cause a substantial phase impurity, and the unexpected few tetragonal phase inhibits the charge separation evidently.

Water-Stable Nickel Metal-Organic Framework Nanobelts for Cocatalyst-Free Photocatalytic Water Splitting to Produce Hydrogen.

Development of water-stable metal-organic frameworks (MOFs) for promising visible-light-driven photocatalytic water splitting is highly desirable but still challenging. Here we report a novel p-type nickel-based MOF single crystal (Ni-TBAPy-SC) and its exfoliated nanobelts (Ni-TBAPy-NB) that can bear a wide range of pH environment in aqueous solution. Both experimental and theoretical results indicate a feasible electron transfer from the HTBAPy ligand (light-harvesting center) to the Ni-O cluster node (catalytic center), on which water splitting to produce hydrogen can be efficiently driven free of cocatalyst.

Water-Stable Cobalt-Based MOF for Water Oxidation in Neutral Aqueous Solution: A Case of Mimicking the Photosystem II.

Inspired by the highly efficient water oxidation of MnCaO in natural photosynthesis, development of novel artificial water oxidation catalysts (WOCs) with structure and function mimicked has inspired extensive interests. A novel 3D cobalt-based MOF (GXY-L8-Co) was synthesized for promising artificial water oxidation by employing the CoO quasi-cubane motifs with a similar structure as the MnCaO as the core. The GXY-L8-Co not only shows good chemical stability in common organic solvents or water for up to 10 days but also exhibits oxygen evolution performance.

Engineered Electronic Structure and Carrier Dynamics in Emerging CsAgNaFeCl Perovskite Single Crystals.

Lead-free double perovskites have attracted noteworthy attention due to their compositional flexibility and electronic diversity. In this study, we hydrothermally grow a new class of CsAgNaFeCl (0 ≤ ≤ 1) perovskite single crystals with high thermal stability. The substitution of B-site cation allows to regulate the crystallographic and band structure, which gives rise to enlarged band absorbance close to the near-infrared region (∼800 nm) via composition engineering.

Visible-Light-Responsive 2D Cadmium-Organic Framework Single Crystals with Dual Functions of Water Reduction and Oxidation.

The development of new metal-organic frameworks (MOFs) with dual functions of both water reduction and oxidation under visible-light irradiation is highly desirable for promising solar water splitting, but is not yet reported. Herein, a cadmium-based MOF (denoted as "Cd-TBAPy") single crystal with a 2D layered framework by employing 1,3,6,8-tetrakis(p-benzoic acid)pyrene (H TBAPy) as an organic linker is reported, which exhibits good visible-light absorption with edge of ≈600 nm. The Mott-Schottky (M-S) measurement and UV-vis analysis integrally reveal that the Cd-TBAPy is an n-type semiconductor with a bandgap of ≈2.

Synthesis of BaTaON oxynitride from Ba-rich oxide precursor for construction of visible-light-driven Z-scheme overall water splitting.

Barium tantalum oxynitride (BaTaON) with an absorption edge of ca. 660 nm is one of the most promising photocatalysts for solar water splitting, and is usually synthesized by nitriding a mixture of Ba and Ta-containing compounds with a Ba/Ta molar ratio of unity under ammonia flow at high temperature, usually causing a high density of defect sites. Herein, we introduce a novel synthesis method for BaTaON (BTON) by employing Ba-rich LiBaTaO, prepared by a flux method, as a precursor of nitridation.