Hongwei Liu

Overall artificial photosynthesis, as a promising approach for sunlight-driven CO₂ recycling, requires photocatalysts with efficient light adsorption and separate active sites for coupling with H₂O oxidation. Here we show a In-based metal–organic framework (MOF) heterostructure, i.e., In-porphyrin (In-TCPP) nanosheets enveloping an In-NH₂-MIL-68 (M68N) core, via a facile one-pot synthesis that utilises competitive nucleation and growth of two organic linkers with In nodes. The coherent interfaces of the core@shell MOFs assure the structural stability of heterostructure, which will function as heterojunctions to facilitate the efficient transfer of photogenerated charge for overall photosynthesis. The In-TCPP shell in MOFs heterostructure improves CO₂ adsorption capabilities and visible light absorption to enhance the photocatalytic CO₂ reduction. Simultaneously, In-O sites in M68N core efficiently catalyze H₂O oxidation, achieving high yields of HCOOH (397.5 μmol g⁻¹ h⁻¹) and H₂O₂ (321.2 μmol g⁻¹ h⁻¹) under focused sunlight irradiation. The superior performance of this heterostructure in overall photosynthesis, coupled with its straightforward synthesis, shows great potential for mitigating carbon emissions and producing valuable chemicals using solar energy.

In the past two decades, high entropy alloy (HEA) coatings have attracted great attention due to their superior mechanical properties, outstanding corrosion and oxidation resistance, and exceptionally high thermal stability. In comparison to HEA thin films, high entropy nitrides (HENs) exhibit higher mechanical strength and chemical inertness. In this work, AlCrFeCoNiCu0.5 HEA and HEN thin films were fabricated using a filtered cathodic arc. By regulating the deposition pressure from 0.0005 Pa (HEA thin film) to 0.05 Pa, the nitrogen concentration in each thin film was precisely controlled to tune the mechanical properties. Scanning transmission electron microscopy-energy dispersive spectroscopy revealed that the nitrogen concentration of the films was up to 21.2 at. % at the pressure of 0.05 Pa. The reduced effect of preferential sputtering increased aluminum concentration from 8.3 ± 1.5 to 12.9 ± 2.2 at. % as pressure increased up to 0.05 Pa. X-ray photoelectron spectroscopy further confirmed the formation of AlN and CrN at pressures of 0.01–0.05 Pa. The highest hardness and elastic modulus of the HEN film were 12.4 ± 0.6 and 347.3 ± 17.7 GPa, respectively, which were 84.8% and 131.4% higher than those of the HEA thin film.

Pair distribution function (PDF) analysis is a powerful technique to understand atomic scale structure in materials science. Unlike X-ray diffraction (XRD)-based PDF analysis, the PDF calculated from electron diffraction patterns (EDPs) using transmission electron microscopy can provide structural information from specific locations with high spatial resolution. The present work describes a new software tool for both periodic and amorphous structures that addresses several practical challenges in calculating the PDF from EDPs. The key features of this program include accurate background subtraction using a nonlinear iterative peak-clipping algorithm and automatic conversion of various types of diffraction intensity profiles into a PDF without requiring external software. The present study also evaluates the effect of background subtraction and the elliptical distortion of EDPs on PDF profiles. The EDP2PDF software is offered as a reliable tool to analyse the atomic structure of crystalline and non-crystalline materials.