Latest ArticlesEmerging 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.
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.
Anode SnO2 in lithium-ion batteries suffers from volume expansion and agglomeration. Here, the SnO2 nanoparticles are hybrided with ZrO2 particles by the support of carbon nanotube networks. The obtained SnO2/C/ZrO2 composite shows improved electrochemical performances. Investigations reveal that the carbon nanotubes shorten the transmission path of electrons and Li+ ions. Ball milling with ZrO2 promotes the formation of nanosized SnO2 to weaken the internal strain change, being beneficial to buffering volume change during electrochemical cycling afterwards. High-resolution 6, 7Li NMR investigations indicate that conversion and alloying reactions are stepwise involved for SnO2/C/ZrO2 anode. The strategy of designing SnO2/C/ZrO2 composite from the morphology-controlled metal-organic frameworks for energy storage widens the possibility to fabricate promising materials with enhanced performances.
Optimal bulk-heterojunction (BHJ) morphology is crucial for efficient charge transport and good photovoltaic performance in organic solar cells (OSCs). Yet, the correlation between chemical structures of nonfullerene acceptors (NFAs) and molecular interaction in the BHJ blends remains opaque. Herein, we study three isomeric NFAs referred to as MQ1-x (x = β, γ, or δ) that shared an asymmetric selenophene-fused heteroheptacene backbone end-capped by two monochlorinated end groups. Remarkably, miscibility between the polymer donor of PM6 and MQ1-x successively elevates as the chlorine atoms move from β-, to γ-, to δ-position of terminals. Combined with the varied molecular crystallinity of these NFAs, diverse BHJ morphologies are observed in their blend films. As a result, the MQ1-δ-based devices present the highest PCE of 12.08% owing to the efficient charge dissociation and transport induced by the compact molecular packing and optimal BHJ morphology. Our investigation provides a new insight in the material design that has a good balance in molecular packing and film morphology for high-performance OSCs.
“Rocking chair” type lithium-ion batteries with lithium metal-free anodes have been successfully commercialized over the past few decades. Zinc-ion batteries (ZIBs) have gained increasing attention in recent years given their safety, greenness, ease of manufacture, and cost-efficiency. Nevertheless, the practical application of ZIBs is largely hindered by the dendritic growth of the Zn metal anode, low Coulombic efficiency, great harm, and existence of various side reactions. Herein, this review provides a systematic overview of emerging “rocking chair” type ZIBs with zinc metal-free anodes. Firstly, the basic fundamentals, advantages, and challenges of “rocking chair” type ZIBs are introduced. Subsequently, an overview of the design principles and recent progress of “rocking chair” type ZIBs with zinc metal-free anodes are presented. Finally, the key challenges and perspectives for future advancement of “rocking chair” type ZIBs with zinc metal-free anodes are proposed. This review is anticipated to attracted increased focus to metal-free anodes “rocking chair” type metal-ion battery and provide new inspirations for the development of high-energy metal-ion batteries.
Persulfate-based advanced oxidation processes (AOPs) have obtained increasing attention due to the generation of sulfate radical (SO4•‒) with high reactivity for organic contaminants degradation. Numerous activation methods have been used to activate two common persulfates: peroxymonosulfate (PMS) and peroxydisulfate (PDS). However, the comparisons of activation methods and two oxidants in the comprehensive degradation performance of the target contaminant are still limited. Thus, taking norfloxacin (NOR) as the target contaminant, we proposed five key parameters (the observed pseudo-first-order rate constant, kobs; average mineralization rate, rm; utilization efficiency of catalyst, Ucat; utilization efficiency of oxidant, Uox; and net utilization efficiency of oxidant, Uox') to quantify the comprehensive degradation performance of NOR. The irradiation affected target pollutants, catalysts, and oxidants, leading to an improved degradation performance of NOR. Various heterogeneous catalysts were compared in terms of the key elements contained. Fe, Co, and Mn-based materials performed better, while carbon-based catalysts performed poorly on NOR degradation. The overall degradation performance of NOR was different for PMS and PDS, which can be ascribed to their varied reaction pathways towards NOR, but stemmed from different properties of PMS and PDS. Besides, the effect of pH on the degradation efficiency of NOR was investigated. A neutral solution was optimal for PMS system, while an acidic solution worked better for PDS system. Finally, we analyzed the molecule structure of NOR by density functional theory (DFT) calculation to study the sites easy to attack. Then, we summarized four typical degradation pathways of NOR in SO4•‒-based AOP systems, including defluorination, piperazine ring cleavage, piperazine ring oxidation, and quinoline group transformation.
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.
A facile and efficient electrochemical method for sustainable constructing both selanyl phenanthrenes and selanyl polycyclic heteroaromatics (32 examples, 71%-97% yields) through the radical annulation of 2-alkynyl biaryls and 2-heteroaryl-substituted alkynyl benzenes with diselenides at ambient temperature under additive-, chemical oxidant-, catalyst-free and mild conditions was established.
Aging-related diseases are gradually becoming a major problem with the rapid development of aged population in human society. Although many fluorescent probes have been employed to diagnosis senescence via imaging senescence-associated β-galactosidase (SA-β-Gal), which is proved to be closely associated with senescent cells, the similar catalytic effectiveness of enzymatic reaction of ovarian cancer-associated β-Gal (OA-β-Gal) will interfere with imaging accuracy. Herein, a near-infrared (NIR) hemicyanine based fluorescent probe HCyXA-βGal was designed for light-up imaging of live cells containing β-Gal. With the organelle-targeting morpholinyl and positive charge moieties, HCyXA-βGal was successfully applicated to image the difference of enzymatic location in senescent cells and ovarian cancer cells. Furthermore, inspired by the fast response performance, fast and precise imaging of the two cell lines was realized via covering another dimension of fluorescence signal: time-dependent intensity.
Highly enantioselective sulfa-Michael additions (SMA) between 2-alkenyl quinoxalines and aromatic thiols are accomplished using a low loading of chiral phosphoric acid catalyst (1 mol%). It was confirmed by an investigation of a lot of azaarenes that the two C=N units of quinoxalines are indispensable for controlling the reaction enantioselectivities. A series of non-terminal 2-alkenes substituted with aryls or alkyls, even other electro-withdrawing groups such as ketones, esters, or amides, selectively reacted and afforded the desired SMA products (48 examples) in good regioselectivities with high yields (up to 99%) and good ee values (up to 97%).
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