Latest ArticlesWater pollution caused by global population growth, urban expansion and industrialization development is one of the urgent issues that need to be addressed in the 21st century. Up to now, it was challenging for metal-organic frameworks (MOFs) to be used in the actual water treatment due to that the powder MOFs suffered from difficult reuse, poor water stability and easy corrosion. It is an effective strategy to immobilize MOFs powder onto porous sponge foam carriers for accomplishing large flux, facile recycling, easy processing water treatment setups. In this review article, the fabrication approaches and applications of different MOFs/sponge composites were highlighted, in which the fluorescence detection of pollutants, adsorption and separation of pollutants, catalytic reduction and oxidation of pollutants were included. Finally, the future challenges and opportunities of MOF/sponge for water treatment are proposed, aiming to provide in-depth guidance for the future design and manufacture of the immobilized MOFs onto sponge foams.
It is of great interest to make a degradable material widely tailorable to replace petroleum-derived products among diverse applications. Here, we report the construction of a new multi-purpose degradable material for the first time via a simple ternary copolymerization system comprising ε-caprolactone (ε-CL), cyclohexane oxide (CHO) and CO2. Under low pressure of 1 bar ~5 bar, the ring-opening polymerization (ROP) of ε-CL and ring-opening copolymerization (ROCOP) of CO2 and CHO can simultaneously proceed. The carbonate units are randomly distributed on the polymer chain. These random terpolymers have controllable molar mass (10–106 kDa) and compositions (4–33 mol% CO2). And the obtained materials show large-span tunability from tough plastic to elastomer and even adhesive.
Developing platinum-group-metal (PGM) catalysts possessing strong metal-support interaction and controllable PGM size is urgent for the sluggish oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells. Herein, we propose an in-situ self-assembled reduction strategy to successfully induce highly-dispersed sub-3 nm platinum nanoparticles (Pt NPs) to attach on resin-derived atomic Co coordinated by N-doped carbon substrate (Pt/CoSA-N-C) for ORR. To be specific, the interfacial electron interaction effect, along with a highly robust CoSA-N-C support endow the as-fabricated Pt/CoSA-N-C catalyst with significantly enhanced catalytic properties, i.e., a mass activity (MA) of 0.719 A/mgPt at 0.9 ViR‑free and a reduction of 24.2% in MA after a 20,000-cycles test. Density functional theory (DFT) calculations demonstrate that the enhanced electron interaction between Pt and CoSA-N-C support decreases the d-band center of Pt, which is in favor of lowering the desorption energy of *OH on Pt/CoSA-N-C surface and accelerating the formation of H2O, thus enhance the instinct activity of ORR. Furthermore, the higher binding energy between Pt and CoSA-N-C compared to Pt and C indicates that the migration of Pt has been suppressed, which theoretically explains the improved durability of Pt/CoSA-N-C. Our work offers an enlightenment on constructing composite Pt-based catalysts with multiple active sites.
Molecular weaving is a powerful approach to make molecularly woven materials that have showed unprecedented characteristics and properties intrinsically distinct to those of non-woven materials. We here report a facile and efficient approach for the synthesis of 2D woven supramolecular polymers by differentiated self-assembly through orthogonal noncovalent interactions. Importantly, the difference in binding strength of two orthogonal noncovalent interactions can be used to control the process of molecular weaving. Consequently, single-layered 2D woven supramolecular polymers were synthesized and fully characterized by various techniques. This study demonstrates a controllable method for molecular weaving, and will significantly hasten the development of molecularly woven materials.
Azulene is a promising building block for creating innovative polycyclic aromatic hydrocarbons. This study involved the construction of three nonalternant isomers of pentacene by fusing two azulene units, named Az-PH1/2/3. Az-PH1 was initially developed through the rhodium(II)-catalyzed cyclization of bis(N-tosylhydrazone)s. Intriguingly, Az-PH1 was also unexpectedly obtained during a nickel(0)-catalyzed one-step tandem reaction. We investigated the optical and electrochemical properties, aromaticity, and photo-oxidative stability of Az-PH1, comparing it with the well-known pentacene using density functional theory, electrochemical, and photophysical tests. Our results showed that the azulene-fusing strategy resulted in a molecule with narrow optical bandgaps (2.046 eV) and a long half-life time under ambient air conditions.
Microcystins (MCs), a family of cyclic heptapeptide cyanotoxins, exists in aquatic environment where cyanobacterial bloom happens, which will accumulate in aquatic organisms and transfer through the food chain to higher trophic levels, posing a health risk to both animals and human bodies. Among various MCs, Microcystin-LR (MC-LR) is worthiest studied for its strong toxicity, ubiquity and widespread. Here in this work, iminodiacetic acid (IDA) decorated magnetic mesoporous silica (mSiO2) nanocomposites (Fe3O4@mSiO2-IDA) were facilely synthesized which possessed the merits of large surface area (188.21 m2/g), accessible porosity (2.66 nm), excellent hydrophilicity and rapid responsiveness to magnetic field. Then the composites were successfully employed to the removal process of Microcystin-LR in real water samples followed by Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) analysis, achieving the removal efficiency above 92.5% even after ten recycles of the composites. It provided a potential method for removing MC-LR in aqueous environment with high effectiveness, lower costs and less secondary contamination.
Covalent adaptable networks (CANs), which share the properties of both thermosets and thermoplastics at the same time, are desirable for many applications. Introducing bulky substituents is a feasible way to design dynamic covalent bonds for constructing CANs, as evidenced by the successful implementation in CANs based on hindered urea bonds (HUBs). However, the dynamicity induced by introducing bulky substituents always come with low bond energy, resulting in low mechanical strength and poor stability of the CANs. Herein, we designed a novel hindered urethane bond, which is weak in thermodynamic (Keq = 1701.23 L/mol at 25 ℃) and inert in kinetic at low temperature, but stable in thermodynamic (Keq = 1.54 × 104 L/mol at 100 ℃) and active in kinetic at high temperature (k-1 = 0.105 h−1 at 80 ℃ and 0.315 h−1 at 120 ℃). As a result, the polyurethane based on it exhibits high mechanical properties (with Youngs' modulus of 1011 ± 29 MPa and flexible modulus reached 1833 ± 50 MPa) and excellent reversibility (can be reprocessed at 60 ℃ under 100 kPa in 30 min and completely healed at 40 ℃ in 10 min). Moreover, unlike to many CANs based on hindered urea bonds, our dynamic polyurethanes are highly stable in humid environment or even water solutions due to the slow hydrolysis kinetics. Such high-performance dynamic polyurethane polymers are attractive for many applications.
A water-soluble macrocycle that bears four carboxylate anions has been designed and prepared, which forms a rectangular cavity that can efficiently encapsulate discrete electron-deficient aromatic compounds, including berberine and palmatine. This macrocycle is revealed to be highly biocompatible and able to inhibit the bitter taste of the two drugs.
The 2-hydroxy-4-methoxybenzyl (Hmb) backbone modification can prevent amide bond-mediated side-reactions (e.g., aspartimide formation, peptide aggregation) by installing the removable Hmb group into a peptide bond, thus improving the synthesis of long and challenging peptides and proteins. However, its use is largely precluded by the limited Hmb's installation sites. In this report, an improved installation of Hmb (iHmb) method was developed to achieve the flexible installation and the convenient removal of Hmb. The iHmb method involves two critical steps: (1) oxidative diazotization of the readily installed 2-hydroxy-4-methoxy-5-amino-benzyl (Hmab) to give 2-hydroxy-4-methoxy-5-diazonium-benzyl (Hmdab) by combining soamyl nitrite (IAN)/HBF4, and (2) reductive elimination of Hmdab to give the desired Hmb by 1,2-ethanedithiol (EDT). The iHmb method enables the installation of Hmb at any primary amino acid including the highly sterically hindered amino acids (e.g., valine and isoleucine). The practicality and utility of the iHmb method was demonstrated by one-shot solid-phase synthesis of a challenging aspartimide-prone peptide, the mirror-image version of a hydrophobic peptide and a long-chain peptide up to 76-residue. Furthermore, the iHmb method can be utilized to facilitate chemical protein ligation, as exemplified by the synthesis of the single-spanning membrane protein sarcolipin. The iHmb method expands the toolkit for peptide synthesis and ligation and facilitates the preparation of peptides/proteins.
Protein recognition using host-guest recognition approach is of great interest but has been limited mainly to the protein N-terminal residues. Here, we site-specific incorporated two novel non-canonical amino acids containing supramolecular guest motifs into protein via an expanded genetic code. Through Staudinger reduction reactions, the encoded unnatural residues on protein becoming activated and can be specifically recognized by cucurbit[7]uril (CB[7]) and cucurbit[8]uril (CB[8]). We demonstrated that enzyme containing guest amino acid incorporated near the active site can be reversibly regulated by CB[7] recognition, and CB[8] recognition induces protein dimerization. These amino acids will make useful addition to the supramolecular toolbox for protein targeting using molecular recognition approaches.
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