Latest ArticlesA 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.
Aprotic lithium-air batteries (LABs) have been known as the holy grail of energy storage systems due to their extremely high energy density. However, their real-world application is still hindered by the great challenges from the Li anode side, like dendrite growth and corrosion reactions, thus a pure oxygen atmosphere is usually adopted to prolong the lifetime of LABs, which is a major obstacle to fully liberate the energy density advantages of LABs. Here, a gel polymer electrolyte has been designed through in-situ polymerization of 1,3-dioxolane (DOL) by utilizing the unique semi-open nature of LABs to protect the Li anode to conquer its shortcomings, enabling the high-performance running of LABs in the ambient air. Unlike common liquid electrolytes, the in-situ formed gel polymer electrolyte could facilitate constructing a gradient SEI film with the gradual decrease of organic components from top to bottom, preventing the Li anode from dendrite growth and air-induced corrosion reactions and thus realizing durable Li repeated plating/stripping (2000 h). Benefiting from the anode protection effects of the gradient SEI film, the LABs display a long lifetime of 170 cycles, paving an avenue for practical, long-term, and high-efficiency operation of LABs.
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.
Single-atomic catalysts (SACs) caught considerable attention due to their unique structural properties, complete exposed active site, and 100% atom utilization efficiency with remarkable catalytic activity. Mesoporous single-atomic cobalt catalyst with Co-N4 active sites was synthesized by using nitrogen-doped graphene derived from acrylonitrile. Single-atomic cobalt was observed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) in Co@Nx-C-800. Notably, the density functional theory (DFT) calculation and the extended X-ray absorption fine structures (EXAFS) fitting results indicate that the coordination structure of Co-N is four-coordinated. In this work, the practical hydrogenation of nitroarenes to anilines enabled by Co@Nx-C-800 was established with excellent yields and selectivity, which proved its advantages and potential applications.
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.
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.
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.
P2-type layered oxides are receiving significant interest due to their superior structure and intrinsic performances. There are strenuous attempts to balance the structure stability, phase transition as well as desirable electrochemical performances by inducing anion/cation ions, changing morphology, adjusting valence, etc. In this work, several same-period elements of Sc, Ti, V, Cr, Fe, Cu and Zn are doped into Na0.50Li0.08Mn0.60Co0.16Ni0.16O2 cathodes, which are manipulated by ions radii and valence state, further studied by operando X-ray powder diffraction patterns (XRD). As a result, the Cu2+ doped cathode performed higher rate capacities (as high as 86 mAh/g even at 10 C) and more stable structures (capacity retention of ~89.4% for 100 cycles), which owing to the synergistic effect among the tightened TMO2 layer, enlarged d-spacing, reduce OO electrostatic repulsion, ameliorate lattice distortion as well as mitigate ordering of Na+/vacancy.
The design of pseudocapacitive materials by coupling transition metal compounds with a conductive carbon matrix is important for the high performance of supercapacitors. Herein, we construct the Prussian blue analogue derived nickel-cobalt selenides coupling with nitrogen-doped carbon nanofibers (NiCoSe4-NCNFs) by carbonization and selenization of polyacrylonitrile nanofibers. The effect of selenization and element N doping on the morphological structure and surface chemistry of NiCoSe4-NCNFs are evaluated. Due to the accelerated electrolyte ion diffusion, enlarged active surface area and the modified surface chemistry by the strong interaction at NiCoSe4/NCNFs interfaces, NiCoSe4-NCNFs show excellent capacitive behaviors in 1 mol/L KOH, and the specific capacitance is 1257 F/g at 1 A/g with a rate capability of 78% and cyclic stability of 82.9%. The Gibbs free energy of adsorption OH− is calculated by density functional theory to investigate the charge storage mechanism. This work offers a new strategy to construct the transition metal selenides/carbon nanofibers hybrids for high-performance supercapacitor devices.
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