Latest ArticlesEnvironmental economics is accelerating the urgency to develop recycling technologies for the ever-growing quantity of discarded thermoset polymers. Herein, we developed a mild and energy-saving process for high-efficiency degradation and reuse of anhydride-cured epoxy thermoset with the aid of hydrazine hydrate. The degradation degree of the epoxy resin reached 99.6% at 120 ℃ within a short time of 60 min. During the reaction, the ester bonds in the cross-linked network were selectively cleaved by the amination of hydrazine hydrate, and the epoxy resin was fully converted to new monomers that contained hydrazide and hydroxyl groups, respectively. Moreover, the degradation mechanism of the epoxy resin in hydrazine hydrate was studied and a nucleation model was utilized to predict the actual degradation behavior of the system. Finally, the degradation products can be directly mixed with epoxy precursor to prepare a new waterborne epoxy coating with good comprehensive properties. This work not only demonstrates a new way to realize the efficient degradation of epoxy resins, but also provides a facile and efficient recycling protocol for thermosets.
The detection of cytokines plays an important role in clinical diagnosis and immune mechanism research of chicken diseases. In this work, a novel and ultrasensitive chemiluminescent (CL) imaging array immunosensor was proposed to detect multiple chicken cytokines based on DNAzyme@CuS nanoparticles (DNAzyme@CuSNPs) dual mimic enzyme signal amplification strategy. DNAzyme@CuSNPs owns excellent peroxidase property, which was modified with second antibody (Ab2) to prepare DNAzyme@CuSNPs detection probe, and demonstrated high catalysis CL imaging signal due to synergistic catalysis. Chicken interleukin-4 (ChIL-4) and chicken interferon-γ (ChIFN-γ) were used as model analysis samples, the DNAzyme@CuSNPs-based CL imaging immunosensor achieved simultaneous and high-throughput detection of ChIL-4 and ChIFN-γ with wide linear range of 10−3–102 ng/mL, and the detection limits are 0.41 pg/mL and 0.36 pg/mL, respectively. The multiplex chicken cytokines CL imaging array immunosensor shows a high sensitivity, wide linear range, excellent specificity and acceptable stability. This research opens dual mimic enzyme signal-amplified strategy to develop sensitive CL imaging immunoassay for chicken diseases detection application.
Artificial photocatalysis offers a promising strategy to sustainably produce hydrogen peroxide (H2O2) that is one of the most valuable multifunctional chemicals. Among various photocatalysts, polymeric carbon nitride (pCN) has drawn continuous attention in non-sacrificial H2O2 production. However, the poor activity of half reactions, i.e., the oxygen reduction reaction (ORR) and water oxidation reaction (WOR), greatly restricts the efficiency of photocatalytic H2O2 production. In this highlight, we discuss the significant advances in molecular engineering of carbon nitrides for H2O2 photosynthesis and the importance of the deep understanding of the photocatalysis process for rational design and reaction pathways of organic conjugated polymers to address the growing H2O2 demand. Furthermore, we summarize the emerging applications of photocatalytic H2O2 productions beyond energy and environment.
Emerging organic pollutants (EOPs) in water are of great concern due to their high environmental risk, so urgent technologies are needed for effective removal of those pollutants. Herein, a heterogeneous advanced oxidation process (AOP) of peroxymonosulfate (PMS) activation by functional material was developed for degradation of a typical antibiotic, gatifloxacin (GAT). The reactive species including sulfate radical (SO4•−) and singlet oxygen (1O2) in this AOP were regulated by interlayered ions (Na+/H+) of titanate nanotubes that supported on Co(OH)2 hollow microsphere. Both the Na-type (NaTi-CoHS) and H-type (HTi-CoHS) materials achieved efficient PMS activation for GAT degradation, and HTi-CoHS even exhibited a relatively high degradation efficiency of 96.6% within 5 min. Co(OH)2 was considered the key component for generation of SO4•− after PMS activation, while hydrogen titanate nanotubes (H-TNTs) promoted the transformation of peroxysulfate radical (SO5•−) to 1O2 by hydrogen bond interaction. Therefore, when the interlayer ion of TNTs transformed from Na+ to H+, more 1O2 was produced for organic pollutant degradation. H-TNTs with lower symmetry preferred to adsorb PMS molecules to achieve interlayer electron transport through hydrogen bonding, rather than electrostatic interaction of Na+ for Na-TNTs. In addition, the degradation pathway of GAT mainly proceeded by the cleavage of C–N bond at the 8 N site of the piperazine ring, which was confirmed by condensed Fukui index and mass spectrographic analysis. This work gives new sights into the regulation of reactive species in AOPs by the composition of material and promotes the understanding of pollutant degradation mechanisms in water treatment process.
Photosynthesis [6CO2 + 12H2O → (CH2O)6 + 6O2 + 6H2O] in nature contains a light reaction process for oxygen evolution and a dark reaction process for carbon dioxide (CO2) reduction to carbohydrates, which is of great significance for the survival of living matter. Therefore, for simulating photosynthesis, it is desirable to design and fabricate a bifunctional catalyst for promoting photocatalytic water oxidation and CO2 reduction performances. Herein, a molecular confined synthesis strategy is reasonably proposed and applied, that is the bifunctional CoOx/Co/C-T (T = 700, 800 and 900 ℃) photocatalysts prepared by the pyrolysis of molecular Co-EDTA under N2 and air atmosphere in turn. Among the prepared photocatalysts, the CoOx/Co/C-800 shows the best photocatalytic water oxidation activity with an oxygen yield of 51.2%. In addition, for CO2 reduction reaction, the CO evolution rate of 12.6 µmol/h and selectivity of 75% can be achieved over this catalyst. The improved photocatalytic activities are attributed to the rapid electron transfer between the photosensitizer and the catalyst, which is strongly supported by the current density-voltage (j-V), steady-state and time-resolved photoluminescence spectra (PL). Overall, this work provides a reference for the preparation and optimization of photocatalysts with the capacity for water oxidation and CO2 reduction reactions.
A double-cable conjugated polymer DCPIC-BO is designed via introducing a long-branched alkyl chains 2-buthyloctyl into the acceptor side unit. Compared with the double-cable polymer (DCPIC-EH) with the 2-ethylhexyl alkyl chains, the solubility of the DCPIC-BO in non-halogen solvents is substantially improved. Therefore, a power conversion efficiency (PCE) of 9.77% can be obtained by the devices processed from o-xylene at 40 ℃, while the DCPIC-EH cannot be processed due to its poor solubility under this condition. Moreover, PCEs of 10.10% for small-area (0.04 cm2) devices and nearly 9% for devices with an area of 1 cm2 are achieved using a non-halogenated solid additive in o-xylene, realizing the "absolutely halogen-free" OSC fabrication.
Electrochemical nitrogen reduction reaction (NRR) is a mild and sustainable method for ammonia synthesis. Therefore, developing high activity, selectivity, and economic efficiency catalysts with considering the synergistic effects between catalysts and carriers to design novel structural models is very important. Considering the non-noble metal NRR catalyst, Mo3, we tried to find a suitable carrier which is stable and economical. Herein, we used the largest atomically precise aluminum-pyrazole ring (AlOC-69) to date (diameter up to 2.3 nm). The larger ring cavities and the presence of abundant hydroxy groups make AlOC-69 an ideal molecular carrier model and provide a basis for studying its structure-activity relationship. The formation energy (−0.76 eV) and stable Mo-O bonds indicate that Mo3 can be stabilized on the Al10O10 surface. Additionally, N2 has fully activated due to the strong interaction between the p-orbital of N and the d-orbital of Mo. The low limiting potential (−0.28 V) emerges that Mo3@Al10O10 has ideal catalytic activity and selectivity. This research provides a promising catalyst model and an understanding of its catalytic process at the atomic level, providing a new approach for the co-design of catalyst and carrier in NRR.
Compared with the widespread exploitation of hot electrons in plasmonic nanoparticles (NPs), hot holes generated from plasmonic metal interband transitions, are often overlooked in photoelectrochemistry, including photoelectrochemical sensing. Motivated by the subtle spectral overlap between the characteristic plasmonic bands of Ag NPs and interband transitions of Au, herein, we construct unusual core-shell Ag@Au NPs via an anti-galvanic reaction to promote the generation of hot holes. Benefiting from the unique plasmon resonances of Ag cores in specific wavelength regimes, Ag@Au can excite multiplied hot holes while Au cannot under the same conditions. With satisfactory accuracy and good practicability, the photoelectrochemical sensing platform based on Ag@Au NPs possesses a detection limit of 77 nmol/L for glucose, exhibiting significantly higher sensitivity compared to that using Au NPs. This work exemplifies the applications of interband hot-hole accumulation initiated by plasmons and may inspire more strategies to explore the utilization of hot holes in photoelectrochemistry.
Lithium metal batteries (LMBs) are considered to be one of the most promising high-energy-density battery systems. However, their practical application in carbonate electrolytes is hampered by lithium dendrite growth, resulting in short cycle life. Herein, an electrolyte regulation strategy is developed to improve the cyclability of LMBs in carbonate electrolytes by introducing LiNO3 using trimethyl phosphate with a slightly higher donor number compared to NO3− as a solubilizer. This not only allows the formaion of Li+-coordinated NO3− but also achieves the regulation of electrolyte solvation structures, leading to the formation of robust and ion-conductive solid-electrolyte interphase films with inorganic-rich inner and organic-rich outer layers on the Li metal anodes. As a result, high Coulombic efficiency of 99.1% and stable plating/stripping cycling of Li metal anode in Li||Cu cells were realized. Furthermore, excellent performance was also demonstrated in Li||LiNi0.83Co0.11Mn0.06O2 (NCM83) full cells and Cu||NCM83 anode-free cells using high mass-loading cathodes. This work provides a simple interphase engineering strategy through regulating the electrolyte solvation structures for high-energy-density LMBs.
Metal-organic frameworks (MOFs) received considerable attention to adsorption and removal of various environmental pollutants because of some inherent advantages. However, it is challenging but meaningful to design and fabricate hierarchical mixed-dimensional MOFs with synergistic effects to enhance the performance for removal and preconcentration of environmental pollutants. Herein, a new hierarchical two-dimensional (2D)-three-dimensional (3D) mixed-dimensional cactus‐like MOF@MOF hybrid material (PCN-134@Zr-BTB) was prepared by in-situ growth of 2D MOF nanosheets (Zr-BTB) on the surface of 3D MOF (PCN-134). The PCN-134@Zr-BTB composites combine the advantages of 2D and 3D MOFs with extensive mesoporous structures and large surface area for effective removal and enrichment of bisphenols (BPs). In comparison with pristine PCN-134 and Zr-BTB materials, the PCN-134@Zr-BTB hybrid material presented excellent adsorption performance for BPs. The adsorption isotherms are consistent with the Langmuir model, and the maximum adsorption capacity of four bisphenols (BPs) ranged from 135.1 mg/g to 628.9 mg/g. The adsorption kinetics are in accordance with the pseudo-second-order model. The recoveries ranged from 72.8% to 108%. The limits of detection were calculated at 0.02–0.03 ng/mL. The enrichment factors were calculated in the range of 310–374. According to FT-IR and XPS analysis, the main adsorption mechanisms are hydrogen bonding and π-π stacking. Nevertheless, this work provides a new and convenient strategy for the preparation of new hierarchical mixed-dimensional MOF@MOF (PCN-134@Zr-BTB) hybrid material for extraction and enrichment of BPs from aqueous matrix.
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