Charge generation and separation are regarded as the major constraints limiting the photocatalytic activity of polymeric photocatalysts. Herein, two new linear polyarylether‐based polymers (PAE–CPs) with distinct linking patterns between their donor and acceptor motifs were tailor‐made to investigate the influence of different linking patterns on the charge generation and separation process. Theoretical and experimental results revealed that compared to the traditional single‐stranded linker, the double‐stranded linking pattern strengthens donor–acceptor interactions in PAE–CPs and generates a coplanar structure, facilitating charge generation and separation, and enabling red‐shifted light absorption. With these prominent advantages, the PAE–CP interlinked with a double‐stranded linker exhibits markedly enhanced photocatalytic activity compared to that of its single‐strand‐linked analogue. Such findings can facilitate the rational design and modification of organic semiconductors for charge‐induced reactions.

Covalent triazine‐based frameworks (CTFs) are typically produced by the salt‐melt polycondensation of aromatic nitriles in the presence of ZnCl2. In this reaction, molten ZnCl2 salt acts as both a solvent and Lewis acid catalyst. However, when cyclotrimerization takes place at temperatures above 300 °C, undesired carbonization occurs. In this study, an ionothermal synthesis method for CTF‐based photocatalysts was developed using a ternary NaCl‐KCl‐ZnCl2 eutectic salt (ES) mixture with a melting point of approximately 200 °C. This temperature is lower than the melting point of pure ZnCl2 (318 °C), thus providing milder salt‐melt conditions. These conditions facilitated the polycondensation process, while avoiding carbonization of the polymeric backbone. The resulting CTF‐ES200 exhibited enhanced optical and electronic properties, and displayed remarkable photocatalytic performance in the hydrogen evolution reaction.

The industrial synthesis of NH 3 using Fe-or Ru-based catalysts usually requires harsh reaction conditions. It is desirable to develop catalysts that perform well at low temperature and pressure (250−400 °C, <2 MPa). The main challenge of low-temperature NH 3 synthesis is the dissociation of the extremely stable NN triple bond. Herein, we report the design of homogeneous single-atom Ru centers on an H-ZMS-5 (HZ) support with the Ru atoms individually anchored in the micropores of HZ, effectively boosting NH 3 synthesis under mild conditions via an associative pathway. Synchrotronbased near-edge X-ray absorption fine structure (NEXAFS) and in situ DRIFTS analyses show that N− groups are the primary intermediates, and DFT calculations further show that, unlike Ru nanoclusters, the cooperation of a single Ru atom and hydrogen species in HZ leads to N 2 hydrogenation rather than direct N 2 dissociation, and the indirect N−N bond dissociation occurs much more easily via the formation of the NHNH 3 * intermediate; the energy barrier for breaking the N−N bond keeps falling from 2.90 eV for *N 2 to 0.04 eV for *NHNH 3 , showing that N 2 hydrogenation is an effective way for sharp weakening of N−N bonds. Moreover, the rate-determining step is shifted from the dissociation of the NN triple bond to the formation of *N 2 H 2 . As a consequence, the single-atom 0.2 wt % Ru/H-ZSM-5 catalyst shows the highest NH 3 synthesis rate per gram of Ru (1.26 mol NH3 g Ru −1 h −1 at 300 °C and 1 MPa) among the Ru-based catalysts ever reported.

Three classical Fe-MOFs, viz., MIL-100­(Fe), MIL-101­(Fe), and MIL-53­(Fe), were synthesized to serve as platforms for the investigation of structure–activity relationship and catalytic mechanism in the selective conversion of H2S to sulfur. The physicochemical properties of the Fe-MOFs were characterized by various techniques. It was disclosed that the desulfurization performances of Fe-MOFs with well-defined microstructures are obviously different. Among these, MIL-100­(Fe) exhibits the highest catalytic performance (ca. 100% H2S conversion and 100% S selectivity at 100–180 °C) that is superior to that of commercial Fe2O3. Furthermore, the results of systematic characterization and DFT calculation reveal that the difference in catalytic performance is mainly because of discrepancy in the amount of Lewis acid sites. A plausible catalytic mechanism has been proposed for H2S selective conversion over Fe-MOFs. This work provides critical insights that are helpful for rational design of desulfurization catalysts.

Fully condensed poly(heptazine imide) (PHI) supported with highly dispersed Pt nanoparticles (PtNPs) achieves efficient and persistent H2 and CH4 production by photocatalytic reforming of biomass derived alcohols under visible light irradiation.