The freshwater scarcity and inadequate access to clean water globally have rallied tremendous efforts in developing robust technologies for water purification and decontamination, and heterogeneous catalysis is a highly-promising solution. Sub-nanometer-confined reaction is the ultimate frontier of catalytic chemistry, yet it is challenging to form the angstrom channels with distributed atomic catalytic centers within, and to match the internal mass transfer and the reactive species’ lifetimes. Here, we resolve these issues by applying the concept of the angstrom-confined catalytic water contaminant degradation to achieve unprecedented reaction rates within 4.6 Å channels of two-dimensional laminate membrane assembled from monolayer cobalt-doped titanium oxide nanosheets. The demonstrated degradation rate constant of the target pollutant ranitidine (1.06 ms−1) is 5–7 orders of magnitude faster compared with the state-of-the-art, achieving the 100% degradation over 100 h continuous operation. This approach is also ~100% effective against diverse water contaminates with a retention time of <30 ms, and the strategy developed can be also extended to other two-dimensional material-assembled membranes. This work paves the way towards the generic angstrom-confined catalysis and unravels the importance of utilizing angstrom-confinement strategy in the design of efficient catalysts for water purification.
Deep eutectic solvents (DESs) based on 1-ethyl-3-methylimidazolium chloride (EmimCl) and triethylene glycol (TEG) with different molar ratios (from 6 : 1 to 1 : 1) were prepared. FTIR and theoretical calculation indicated that the C2-H on the imidazolium ring form hydrogen bonds with the hydroxyl group rather than the ether O atom of the TEG. The EmimCl-TEG DESs can efficiently capture SO2; in particular, EmimCl-TEG (6 : 1) can capture 0.54 g SO2 per gram of solvent at 0.10 atm and 20 °C, the highest absorption amount for DESs under the same conditions. Theoretical calculation showed that the high SO2 absorption capacity was mainly due to the strong charge-transfer interaction between SO2 and the anion Cl-. Moreover, SO2 desorption in the DESs can be controlled by tuning the interaction between EmimCl and TEG, and the DESs can be cycled many times.
High-fidelity trapping of mitochondrial dynamic activity is critical to value cellular functions and forecast disease but lack of spatial-temporal probes. Given that commercial mitochondria probes suffering from low photostability, aggregation-caused quenching effect, and limited signal-to-noise ratio from fluorescence "always on" in the process of targeting mitochondria, here, the rational design strategy of a novel aggregation-induced emission (AIE) molecular motif and unique insight into the high-fidelity targeting of mitochondria is reported, thereby illustrating the relationship between tailoring molecular aggregation state and mitochondrial targeting ability. This study focuses on how to exactly modulate the hydrophilicity and the aggregated state for realizing "off-on" fluorescence, as well as matching the charge density to go across the cell membrane for mitochondrial targeting. Probe tricyano-methylene-pyridine (TCM-1) exhibits an unprecedented high-fidelity feedback on spatial-temporal mitochondrial information with several advantages such as "off-on" near-infrared characteristic, high targeting capacity, favorable biocompatibility, as well as excellent photostability. TCM-1 also produces reactive oxygen species in situ for image-guided photodynamic anticancer therapy. Through unraveling the relationship between tuning molecular aggregation behavior and organelle-specific targeting ability, for the first time, a unique guide is provided in designing AIE-active probes to explore the hydrophilicity and membrane potential for targeting subcellular organelles.
Membrane technology for carbon capture is a critical avenue in mitigating the CO 2 emissions to the atmosphere, particularly for existing fossil fuel-fired power plants. Herein, we designed highly oxygen-rich polymers with strong CO 2 -philicity and high CO 2 /N 2 solubility selectivity. These polar groups are incorporated in short branches with flexible ethoxy chain end groups, resulting in amorphous nature and high CO 2 permeability. Such polymers show superior CO 2 /N 2 separation properties better than state-of-the-art materials and above Robeson's 2008 upper bound.
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