Xinlei Zhang

Creating ordered two-dimensional (2D) metal-organic framework (MOF) nanosheets has attracted extensive interest. However, it still remains a great challenge to synthesize ultrathin 2D MOF nanosheets with controlled thickness in high yields. In this work, we demonstrate a novel intercalation and chemical exfoliation approach to obtain MOF nanosheets from intrinsically layered MOF crystals. This approach involves two steps: first, layered porphyrinic MOF crystals are intercalated with 4,4'-dipyridyl disulfide through coordination bonding with the metal nodes; subsequently, selective cleavage of the disulfide bond induces exfoliation of the intercalated MOF crystals, leading to individual freestanding MOF nanosheets. This chemical exfoliation process can proceed efficiently at room temperature to produce ultrathin (∼1 nm) 2D MOF nanosheets in ∼57% overall yield. The obtained ultrathin nanosheets exhibit efficient and far superior heterogeneous photocatalysis performance compared with the corresponding bulk MOF.

Direct water splitting into H 2 and O 2 using photocatalysts by harnessing sunlight is very appealing to produce storable chemical fuels. Conjugated polymers, which have tunable molecular structures and optoelectronic properties, are promising alternatives to inorganic semiconductors for water splitting. Unfortunately, conjugated polymers that are able to efficiently split pure water under visible light (400 nm) via a four‐electron pathway have not been previously reported. This study demonstrates that 1,3‐diyne‐linked conjugated microporous polymer nanosheets (CMPNs) prepared by oxidative coupling of terminal alkynes such as 1,3,5‐tris‐(4‐ethynylphenyl)‐benzene (TEPB) and 1,3,5‐triethynylbenzene (TEB) can act as highly efficient photocatalysts for splitting pure water (pH ≈ 7) into stoichiometric amounts of H 2 and O 2 under visible light. The apparent quantum efficiencies at 420 nm are 10.3% and 7.6% for CMPNs synthesized from TEPB and TEB, respectively; the measured solar‐to‐hydrogen conversion efficiency using the full solar spectrum can reach 0.6%, surpassing photosynthetic plants in converting solar energy to biomass (globally average ≈0.10%). First‐principles calculations reveal that photocatalytic H 2 and O 2 evolution reactions are energetically feasible for CMPNs under visible light irradiation. The findings suggest that organic polymers hold great potential for stable and scalable solar‐fuel generation.

The ultra-stable highly efficient HER over a wide pH range on defect-rich MoN nanosheets synthesized using a modified salt-template process.

Abstract Scintillators are critical in medical imaging, non‐destructive security screening, and space exploration applications. However, it still remains a challenge to achieve large‐area and high‐transparency scintillators by a low‐cost and easy‐to‐implement way. Herein, a large transparent medium with a diameter over 10 cm is prepared via a facile melt‐quenching strategy using a stoichiometric mixture of ethyltriphenylphosphonium bromide (ETPBr) and MnBr 2 as raw materials. Benefiting from the crystallization behavior of high‐efficiency green‐emitting (ETP) 2 MnBr 4 nanocrystals hybridized with amorphous phase in the transparent wafer, the (ETP) 2 MnBr 4 ‐based transparent medium as a scintillator evidences a high transparency (over 80%, ranging from 500 to 800 nm), a high light yield of ≈35 000 ± 2000 photon per MeV, a low detection limit of 103 nGy S –1 , and a competitive spatial resolution of 13.4 lp mm –1 for X‐ray imaging. This work offers a distinctive simple and fast melt‐quenching methodology to fabricate (ETP) 2 MnBr 4 metal halide X‐ray scintillator wafer with large‐area and shape flexibility, excellent transparency, and high scintillation performance for the medical or industrial X‐ray imaging application.