Latest ArticlesThe electricity-driven water splitting acts as a promising pathway for renewable energy conversion and storage, yet anodic oxygen evolution reaction (OER) largely hinders its efficiency. Seeking the alternatives to OER exhibits the competitive advance to address this predicament. In this work, we show a more thermodynamically and kinetically favorable reaction, electrochemical oxidative dehydrogenation (EODH) of benzylamine to replace the conventional OER, catalyzed by a cobalt cyclotetraphosphate (Co2P4O12) nanorods catalyst grown on nickel foam. This anodic reaction lowers the electricity input of 317 mV toward the desired current density of 100 mA/cm2, together with a highly selective benzonitrile product of more than 97%. More specifically, when coupling it with cathodic hydrogen evolution reaction (HER), the proposed HER||benzylamine-EODH configuration only requires a cell voltage of 1.47 V@100 mA/cm2, exhibiting an energy-saving up to 17% relative to conventional water splitting, as well as the near unit selectivity toward cathodic H2 and anodic benzonitrile products.
In this study, we proposed a novel method to investigate the advanced oxidation process of neonicotinoids (NNIs) from the perspective of concomitant chemiluminescence (CL) reaction. It was found that in the presence of cobalt ions with cyanoimino NNIs, acetamiprid (ACE) and thiacloprid (THI), could promote peroxymonosulfate and Ru(bpy)32+ to produce strong CL, but no CL occurred with nitro-involved NNIs as alternatives. Experimental dada from UV absorption spectra and chemiluminescence spectra suggested that new cyclic compounds might be formed during the reaction. Based on the results of free radical scavenging experiment and mass spectra, a new degradation and reaction mechanism of cyanoimino-containing NNIs was proposed. ACE or THI were first attacked by SO4•− to form benzyl radicals, which in turn reacted with the carbon atoms of cyano group through electrophilic addition reaction in the formation of intramolecular ring. Then a redox reaction between Ru(bpy)33+ and imino group immediately took place with CL emission (610 nm). The new mechanistic knowledge would be meaningful for other contaminants for their interactions with PMS.
Perovskite quantum dots (PQDs) possess remarkable optical properties, such as tunable photoluminescence (PL) emission spectra, narrow full width at half maximum (FWHM) and high PL quantum yield (QY), endowing the PQDs great application prospects. However, the inherent structural instability of PQDs has seriously hindered the application of PQDs in various photoelectric devices. In this work, a microfluidic electrospinning method was used to fabricate color-tunable fluorescent formamidinium lead halogen (FAPbX3, X = Cl, Br, I) PQDs/polymer core-shell nanofiber films. The core-shell spinning nanofiber not only supplies the interspace for the in-situ formation of PQDs, but also significantly reduces the permeability of moisture and oxygen in the air, which greatly improves the stability of PQDs. After adjusting the composition of precursors, the blue-emissive polystyrene (core) and polymethyl methacrylate (shell) coated FAPbCl3 QDs (abbreviated as PS/FAPbCl3/PMMA, hereinafter), green-emissive PS/FAPbBr3/PMMA and red-emissive PS/FAPbI3/PMMA nanofiber films were fabricated with the highest PL QY of 82.3%. Moreover, the PS/FAPbBr3/PMMA nanofiber film exhibits great PL stability under blue light irradiation, long-term storage in the air and water resistance test. Finally, the green- and red-emissive nanofiber films were directly applied as light conversion films to fabricate wide-color-gamut display with the color gamut of 125%, indicating their tremendous potentials in optoelectronic applications.
Compared with noble metals, improving the sensitivity of semiconducting surface-enhanced Raman scattering (SERS) substrates is of great significance to their fundamental research and practical application of Raman spectroscopy. Herein, a simple chemical method is developed to synthesize a rhenium trioxide (ReO3) microtubes assembled with highly crystalline nanoparticles. The ReO3 microtubes show a strong and well-defined surface plasmon resonance (SPR) behavior in visible region, which is rare for non-noble metals. As a low-cost SERS substrate, the plasmonic ReO3 microtubes exhibit a Raman enhancement factor of 8.9 × 105 and a lowest detection limit of 1.0 × 10−9 mol/L for phenolic pollutants. Moreover, these ReO3 microtubule SERS substrates show excellent chemical stability and can resist the corrosion of strong acids and bases.
Ammonia is the feedstock chemical for most fertilizers and the alternative of renewable energy carriers. Environmentally benign electrochemical nitrogen reduction reaction (NRR) under mild conditions has been recognized as one of the most attractive strategies for N2 fixation. Herein, inspired by Mo-based nitrogenase, W/Mo-doping electrocatalysts were developed with mixed-metal polyoxometalate H3PW6Mo6O40 as the precursor for high performance electrocatalytic NRR. Trace amount of Pt was transplanted on the surface of W/Mo@rGO via in situ electroplating treatment to further improve the NRR performance. The resulting Pt-W/Mo@rGO-6 achieves excellent performance for NRR with a high NH3 yield of 79.2 µg h−1 mgcat−1 due to the multicomponent synergistic effect in the composite catalyst. The Pt-W/Mo@rGO-6 represents the first example of highly efficient NRR electraocatalyst derived from mixed-metal polyoxometalate, which exhibits outstanding stability confirmed by the constant catalytic performance over 24 h chronoamperometric test. This finding opens a new avenue to construct highly efficient NRR electrocatalyst by employing mixed metal polyoxometalate as the precursor under ambient conditions.
The Z-scheme heterostructure for photocatalyst can effectively prolong the lifetime of photogenerated carriers and retain a higher conduction/valence band position, promoting the synergistic coupling of photocatalysis and peroxymonosulfate (PMS) activation. In order to fully utilize the luminous energy and realize the efficient activation of PMS, this work achieved successful construction of NiCo2O4/BiOCl/Bi24O31Br10 ternary Z-scheme heterojunction by simultaneously synthesizing BiOCl and NiCo2O4 with NiCl2 and CoCl2 as the precursors. The intercalated BiOCl could serve as a carrier migration ladder to further achieve the spatial separation of electron-hole pairs, so that the oxidation and reduction processes separately occurred in different regions. Compared with the reported catalysts, the as-prepared composites exhibited the enhanced removal efficiency for tetracycline hydrochloride (TCH) in the visible light/PMS system, with a degradation efficiency of 85.30% in 2 min, and possessed good stability. Z-scheme heterojunction was shown to be beneficial for maximizing the superiority of photo-assisted Fenton-like reaction system. The experimental and characterization results confirmed that both non-radicals (1O2) and radicals (SO5•− and SO4•−) were involved in the reaction process and the SO5•− generated by the oxidation of PMS played a crucial role in the TCH degradation. The possible reaction mechanism was finally proposed. This study provided new insight into the Z-scheme heterostructure to promote the photo-assisted Fenton-like reaction.
Na-CO2 batteries have attracted extensive attention due to their high theoretical energy density (1125 Wh/kg), efficient utilization of CO2, and abundant sodium resources. However, they are trapped by the sluggish decomposition kinetic of discharge products (mainly Na2CO3) on cathode side during the charging process. Here we prepared a series of nano-composites composed of RuO2 nanoparticles in situ loaded on activated multi-walled carbon nanotubes (RuO2@a-MWCNTs) through hydrolyzing reaction followed by calcination method and used them as cathode catalysts to accelerate the decomposition of Na2CO3. Among all catalysts, the RuO2@a-MWCNTs with appropriate ratio of RuO2 (49.7 wt%) demonstrated best stability and rate performance in Na-CO2 batteries, benefiting from both high specific surface area (160.3 m2/g) and highly dispersed RuO2 with ultrafine nanostructures (~2 nm). At a limited capacity of 500 mAh/g, Na-CO2 batteries could afford the operation of over 120 cycles at 100 mA/g, and even at the current density to 500 mA/g, the charge voltage was still lower than 4.0 V after 40 cycles. Further theoretical calculations proved that RuO2 was the catalytically active center and contributed to the decomposition of Na2CO3 by weakening the C=O bond. The synergetic functions of high specific surface (CNTs) and high catalytic activity (RuO2) will inspire more progress on metal-CO2 batteries.
Hydrophilic interaction liquid chromatography (HILIC) has been recognized as an effective strategy for glycopeptide enrichment. Hydrophilic materials pave the way to solve the limit of low enrichment capacity and poor selectivity. The present study is the first attempt to combine chitosan (CS) and L-cysteine (L-Cys) to design a novel hydrophilic material focusing on glycopeptide enrichment. CS containing a large number of hydrophilic amino and hydroxyl groups has unique chemical properties, which makes it a very attractive biomaterial for glycopeptide enrichment. The excellent hydrophilicity of zwitterionic molecule L-Cys inspires the idea of anchoring L-Cys onto CS to design a novel hydrophilic material (named as Fe3O4@CS@Au-L-Cys) for the capture of low abundance glycopeptides. To be specific, Au nanoparticles (Au NPs) was introduced into CS-coated Fe3O4 via electrostatic interaction and served as bridges to anchor L-Cys onto the surface of CS through strong Au-S bond interaction. The prepared Fe3O4@CS@Au-L-Cys exhibited strong affinity, low detection limit (0.5 fmol/µL HRP), high selectivity (HRP/BSA with a molar ratio of 1:1000) for glycopeptides. Moreover, successful application of glycopeptide enrichment in human serum and saliva by Fe3O4@CS@Au-L-Cys was achieved. A satisfactory data set indicates that Fe3O4@CS@Au-L-Cys has promising potential in the application of glycopeptide enrichment in real complex bio-samples and for related glycoproteome research.
Potassium ion batteries (PIBs) have been regarded as promising alternatives to lithium ion batteries (LIBs) on account of their abundant resource and low cost in large scale energy storage applications. However, it still remains great challenges to explore suitable electrode materials that can reversibly accommodate large size of potassium ions. Here, we construct oxygen-deficient V2O3 nanoparticles encapsulated in amorphous carbon shell (Od-V2O3@C) as anode materials for PIBs by subtly combining the strategies of morphology and deficiency engineering. The MOF derived nanostructure along with uniform carbon coating layer can not only enables fast K+ migration and charge transfer kinetics, but also accommodate volume change and maintain structural stability. Besides, the introduction of oxygen deficiency intrinsically tunes the electronic structure of materials according to DFT calculation, and thus lead to improved electrochemical performance. When utilized as anode for PIBs, Od-V2O3@C electrode exhibits superior rate capability (reversible capacities of 262.8, 227.8, 201.5, 179.8, 156.9 mAh/g at 100, 200, 500, 1000 and 2000 mA/g, respectively), and ultralong cycle life (127.4 mAh/g after 1000 cycles at 2 A/g). This study demonstrates a feasible way to realize high performance PIBs through morphology and deficiency engineering.
Angiotensin-converting enzyme 2 (ACE2) is not only an enzyme but also a functional receptor on cell membrane for severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). Here, the activity of ACE2 in single living cell is firstly determined using a nanokit coupled electrospray ionization mass spectrometry (nanokit-ESI-MS). Upon the insertion of a micro-capillary into the living hACE2-CHO cell and the electrochemical sorting of the cytosol, the target ACE2 enzyme hydrolyses angiotensin II inside the capillary to generate angiotensin 1–7. After the electrospray of the mixture at the tip of the capillary, the product is differentiated from the substrate in molecular weight to achieve the detection of ACE2 activity in single cells. The further measurement illustrates that the inflammatory state of cells does not lead to the significant change of ACE2 catalytic activity, which elucidates the relationship between intracellular ACE2 activity and inflammation at single cell level. The established strategy will provide a specific analytical method for further studying the role of ACE2 in the process of virus infection, and extend the application of nanokit based single cell analysis.
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