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Synthesis-oriented design led us to the discovery of a series of novel cyanine-borondifluoride curcuminoid hybrids called Nanchang Red (NCR) dyes that overcome the intrinsic low synthetic yields of symmetrical cyanine-difluoroboronate (BF 2 )-hybridized NIR dyes. The hybridization endows NCR dyes with high molar extinction coefficients, efficient red-to-NIR emission, and enlarged Stokes shifts. Quantum chemical calculations revealed that the asymmetrical layout of the three key electron-withdrawing and electron-donating fragments results in a special pattern of partial charge separation and inconsistent degrees of charge delocalization on their π-conjugated backbones. While the nature of the hemicyanine fragment exerts significant influence on the excitation modes of NCR dyes, the borondifluoride hemicurcuminoid fragment is the major contributor to the enlarged Stokes shifts. Cell imaging experiments illustrated that a subtle change in the N-heterocycle of the hemicyanine fragment has a remarkable effect on the subcellular localization of NCR dyes. Unlike other previously reported cyanine-BF 2 hybridized dyes, which mainly target mitochondria, the benzothiazole and indole-based NCR dyes accumulate in both the endoplasmic reticulum (ER) and lipid droplets of HeLa cells, whereas the benzoxazole and quinoline-based NCR dyes stain the ER specifically., (© 2023 Wiley-VCH GmbH.)

Plastic waste is an emerging environmental issue for our society. Critical action to tackle this problem is to upcycle plastic waste as valuable feedstock. Thermochemical conversion of plastic waste has received growing attention. Although thermochemical conversion is promising for handling mixed plastic waste, it typically occurs at high temperatures (300-800 °C). Catalysts can play a critical role in improving the energy efficiency of thermochemical conversion, promoting targeted reactions, and improving product selectivity. This Review aims to summarize the state-of-the-art of catalytic thermochemical conversions of various types of plastic waste. First, general trends and recent development of catalytic thermochemical conversions including pyrolysis, gasification, hydrothermal processes, and chemolysis of plastic waste into fuels, chemicals, and value-added materials were reviewed. Second, the status quo for the commercial implementation of thermochemical conversion of plastic waste was summarized. Finally, the current challenges and future perspectives of catalytic thermochemical conversion of plastic waste including the design of sustainable and robust catalysts were discussed., (© 2022 Wiley-VCH GmbH.)

Formamidinium lead triiodide (FAPbI 3 ) is attractive for photovoltaic devices due to its optimal bandgap at around 1.45 eV and improved thermal stability compared with methylammonium-based perovskites. Crystallization of phase-pure α-FAPbI 3 conventionally requires high-temperature thermal annealing at 150 °C whilst the obtained α-FAPbI 3 is metastable at room temperature. Here, aerosol-assisted crystallization (AAC) is reported, which converts yellow δ-FAPbI 3 into black α-FAPbI 3 at only 100 °C using precursor solutions containing only lead iodide and formamidinium iodide with no chemical additives. The obtained α-FAPbI 3 exhibits remarkably enhanced stability compared to the 150 °C annealed counterparts, in combination with improvements in film crystallinity and photoluminescence yield. Using X-ray diffraction, X-ray scattering, and density functional theory simulation, it is identified that relaxation of residual tensile strains, achieved through the lower annealing temperature and post-crystallization crystal growth during AAC, is the key factor that facilitates the formation of phase-stable α-FAPbI 3 . This overcomes the strain-induced lattice expansion that is known to cause the metastability of α-FAPbI 3 . Accordingly, pure FAPbI 3 p-i-n solar cells are reported, facilitated by the low-temperature (≤100 °C) AAC processing, which demonstrates increases of both power conversion efficiency and operational stability compared to devices fabricated using 150 °C annealed films., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Purposefully designing the well-defined catalysts for the selective electroreduction of CO 2 to C 2 H 4 is an extremely important but challenging work. In this work, three crystalline trinuclear copper clusters (Cu 3 -X, X=Cl - , Br - , NO 3 - ) have been designed, containing three active Cu sites with the identical coordination environment and appropriate spatial distance, delivering high selectivity for the electrocatalytic reduction of CO 2 to C 2 H 4 . The highest faradaic efficiency of Cu 3 -X for CO 2 -to-C 2 H 4 conversion can be adjusted from 31.90 % to 55.01 % by simply replacing the counter anions (NO 3 - , Cl - , Br - ). The DFT calculation results verify that Cu 3 -X can facilitate the C-C coupling of identical *CHO intermediates, subsequently forming molecular symmetrical C 2 H 4 product. This work provides an important molecular model system and a new design perspective for electroreduction of CO 2 to C 2 products with symmetrical molecular structure., (© 2021 Wiley-VCH GmbH.)

The exploration of novel systems for the electrochemical CO 2 reduction reaction (CO 2 RR) for the production of hydrocarbons like CH 4 remains a giant challenge. Well-designed electrocatalysts with advantages like proton generation/transferring and intermediate-fixating for efficient CO 2 RR are much preferred yet largely unexplored. In this work, a kind of Cu-porphyrin-based large-scale (≈1.5 μm) and ultrathin nanosheet (≈5 nm) has been successfully applied in electrochemical CO 2 RR. It exhibits a superior FE CH 4 of 70 % with a high current density (-183.0 mA cm -2 ) at -1.6 V under rarely reported neutral conditions and maintains FE CH 4 >51 % over a wide potential range (-1.5 to -1.7 V) in a flow cell. The high performance can be attributed to the construction of numerous hydrogen-bonding networks through the integration of diaminotriazine with Cu-porphyrin, which is beneficial for proton migration and intermediate stabilization, as supported by DFT calculations. This work paves a new way in exploring hydrogen-bonding-based materials as efficient CO 2 RR catalysts., (© 2021 Wiley-VCH GmbH.)

Multidimensional fabrication of metal-organic frameworks (MOFs) into multilevel channel integrated devices are in high demanded for Li-S separators. Such separators have advantages in pore-engineering that might fulfill requirements such as intercepting the diffusing polysulfides and improving the Li + /electrolyte transfer in Li-S batteries. However, most reported works focus on the roles of MOFs as ionic sieves for polysulfides while offering limited investigation on the tuning of Li + transfer across the separators. A photoinduced heat-assisted processing strategy is proposed to fabricate MOFs into multidimensional devices (e.g., hollow/Janus fibers, double-or triple-layer membranes). For the first time, a triple-layer separator with stepped-channels has been designed and demonstrated as a powerful separator with outstanding specific capacity (1365.0 mAh g -1 ) and cycling performance (0.03 % fading per cycle from 100 th to 700 th cycle), which is superior to single/double-layer and commercial separators. The findings may expedite the development of MOF-based membranes and extend the scope of MOFs in energy-storage technologies., (© 2021 Wiley-VCH GmbH.)

Metal-organic framework (MOF) based mixed matrix membranes (MMMs) have received significant attention in applications such as gas separation, sensing, and energy storage. However, the mass production of MOF-based MMMs with retained porosity remains a longstanding challenge. Herein, an in situ heat-assisted solvent-evaporation method is described to facilely produce MOF-based MMMs. This method can be extended into various MOFs and polymers with minimum reaction time of 5 min. Thus-obtained MMMs with high uniformity, excellent robustness, well-tuned loading, and thickness can be massively produced in industrial-level efficiency (≈4 m in a batch experiment). Furthermore, they can be readily applied as powerful separators for Li-S cell with high specific capacity (1163.7 mAh g -1 ) and a capacity retention of 500.7 mAh g -1 after 700 cycles at 0.5 C (0.08% fading per cycle). This work may overcome the longstanding challenge of processing MOFs into MMMs and largely facilitate the industrialization process of MOFs., Competing Interests: The authors declare no conflict of interest., (© 2020 The Authors. Published by Wiley‐VCH GmbH.)

Hydrogen storage is a primary challenge for using hydrogen as a fuel. With ideal hydrogen storage kinetics, the weak binding strength of hydrogen to sorbents is the key barrier to obtain decent hydrogen storage performance. Here, we reported the rational synthesis of a methyllithium-doped naphthyl-containing conjugated microporous polymer with exceptional binding strength of hydrogen to the polymer guided by theoretical simulations. Meanwhile, the experimental results showed that isosteric heat can reach up to 8.4 kJ mol(-1) and the methyllithium-doped naphthyl-containing conjugated microporous polymer exhibited an enhanced hydrogen storage performance with 150 % enhancement compared with its counterpart naphthyl-containing conjugated microporous polymer. These results indicate that this strategy provides a direction for design and synthesis of new materials that meet the US Department of Energy (DOE) hydrogen storage target., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Zinc-coordinated conjugated microporous polymers (Zn-CMPs), prepared by linking salen zinc and 1,3,5-triethynylbenzene, exhibit extraordinary activities (turnover frequencies of up to 11600 h(-1) ), broad substrate scope, and group tolerance for the synthesis of functional organic carbonates by coupling epoxides with CO2 at 120 °C and 3.0 MPa without the use of additional solvents. The catalytic activity of Zn-CMP is comparable to those of homogeneous catalysts and superior to those of other heterogeneous catalysts. This catalyst could be reused more than ten times without a significant decrease in performance., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)