Facile synthesis of accordion-like porous carbon from waste PET bottles-based MIL-53(Al)and its application for high-performance Zn-ion capacitor

It is of great scientific and economic value to recycle waste poly(ethylene terephthalate)(PET)into high-value PET-based metal organic frameworks(MOFs)and further convert it into porous carbon for green energy storage applications.In the present study,a facile and costeffective hydrothermal process was developed to direct recycle waste PET bottles into MIL-53(Al)with a 100% conversation,then the MOFderived porous carbon was assembled into electrodes for high-performance supercapacitors.The results indicated that the as-synthesized carbon exhibited high SSA of 1712 m^(2)g^(-1)and unique accordion-like structure with hierarchical porosity.Benefit to these advantageous characters,the assembled three-electrode supercapacitor displayed high specific capacitances of 391 F g^(-1)at the current density of 0.5 A g^(-1)and good rate capability of 73.6% capacitance retention at 20 A g^(-1)in 6 mol L^(-1)KOH electrolyte.Furthermore,the assembled zinc ion capacitor still revealed outstanding capacitance of 335 F g^(-1)at 0.1 A g^(-1),excellent cycling stability of 92.2% capacitance retention after 10000 cycles and ultra-high energy density of 150.3 Wh kg^(-1)at power density of 90 W kg^(-1)in 3 mol L^(-1)ZnSO_(4)electrolyte.It is believed that the current work provides a facile and effective strategy to recycle PET waste into high-valuable MOF,and further expands the applications of MOF-derived carbons for high-performance energy storage devices,so it is conducive to both pollution alleviation and sustainable economic development.

Unlocking the potential of ultra-thin two-dimensional antimony materials:Selective growth and carbon coating for efficient potassium-ion storage

Antimony-based anodes have attracted wide attention in potassium-ion batteries due to their high theoretical specific capacities(∼660 mA h g^(-1))and suitable voltage platforms.However,severe capacity fading caused by huge volume change and limited ion transportation hinders their practical applications.Recently,strategies for controlling the morphologies of Sb-based materials to improve the electrochemical performances have been proposed.Among these,the two-dimensional Sb(2D-Sb)materials present excellent properties due to shorted ion immigration paths and enhanced ion diffusion.Nevertheless,the synthetic methods are usually tedious,and even the mechanism of these strategies remains elusive,especially how to obtain large-scale 2D-Sb materials.Herein,a novel strategy to synthesize 2D-Sb material using a straightforward solvothermal method without the requirement of a complex nanostructure design is provided.This method leverages the selective adsorption of aldehyde groups in furfural to induce crystal growth,while concurrently reducing and coating a nitrogen-doped carbon layer.Compared to the reported methods,it is simpler,more efficient,and conducive to the production of composite nanosheets with uniform thickness(3–4 nm).The 2D-Sb@NC nanosheet anode delivers an extremely high capacity of 504.5 mA h g^(-1) at current densities of 100 mA g^(-1) and remains stable for more than 200 cycles.Through characterizations and molecular dynamic simulations,how potassium storage kinetics between 2D Sb-based materials and bulk Sb-based materials are explored,and detailed explanations are provided.These findings offer novel insights into the development of durable 2D alloy-based anodes for next-generation potassium-ion batteries.

Synergetic Control of Li^(+)Transport Ability and Solid Electrolyte Interphase by Boron-Rich Hexagonal Skeleton Structured All-Solid-State Polymer Electrolyte

High Li^(+)transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li^(+).However,such electrolytes with immobilized anions would result in incomplete solid electrolyte interphase(SEI)formation on the Li anode because it suffers from the absence of appropriate inorganic components entirely derived from anions decomposition.Herein,a boron-rich hexagonal polymer structured all-solid-state polymer electrolyte(BSPE+10%LiBOB)with regulated intermolecular interaction is proposed to trade off a high Li^(+)transference number against stable SEI properties.The Li^(+)transference number of the as-prepared electrolyte is increased from 0.23 to 0.83 owing to the boron-rich cross-linker(BC)addition.More intriguingly,for the first time,the experiments combined with theoretical calculation results reveal that BOB^(-)anions have stronger interaction with B atoms in polymer chain than TFSI^(-),which significantly induce the TFSI^(-)decomposition and consequently increase the amount of LiF and Li3N in the SEI layer.Eventually,a LiFePO_(4)|BSPE+10%LiBOBlLi cell retains 96.7%after 400 cycles while the cell without BC-resisted electrolyte only retains 40.8%.BSPE+10%LiBOB also facilitates stable electrochemical cycling of solid-state Li-S cells.This study blazes a new trail in controlling the Li^(+)transport ability and SEI properties,synergistically.

Interface defect induced upgrade of K-storage properties in KFeSO4Fcathode: From lowered Fe-3d orbital energy level to advancedpotassium-ion batteries

KFeSO_(4)F(KFSF)is considered a potential cathode due to the large capacity and low cost.However,the inferior electronic conductivity leads to poor electrochemical performance.Defect engineering can facilitate the electron/ion transfer by tuning electronic structure,thus providing favorable electrochemical performance.Herein,through the regulation of surface defect engineering in reduced graphene oxide(rGO),the Fe–C bonds were formed between KFSF and rGO.The Fe–C bonds formed work in regulating the Fe-3d orbital as well as promoting the migration ability of K ions and increasing the electronic conductivity of KFSF.Thus,the KFSF@rGO delivers a high capacity of 119.6 mAh g^(-1).When matched with a graphite@pitch-derived S-doped carbon anode,the full cell delivers an energy density of 250.5 Wh kg^(-1) and a capacity retention of 81.5%after 400 cycles.This work offers a simple and valid method to develop high-performance cathodes by tuning defect sites.

The corrosion characteristic and mechanism of Mg-5Y-1.5Nd-xZn-0.5Zr(x=0,2,4,6 wt.%)alloys in marine atmospheric environment

The microstructure and precipitated phases of as-cast Mg-5Y-1.5Nd-x Zn-0.5Zr(x=0,2,4,6 wt.%)alloys were investigated by optical microscopy,scanning electron microscopy,energy-dispersive spectrometry and X-ray Diffraction.The exposure corrosion experiment of these magnesium alloys was tested in South China Sea and KEXUE vessel atmospheric environment.The corrosion characteristic and mechanism of magnesium alloys of Mg-5Y-1.5Nd-x Zn-0.5Zr(x=0,2,4,6 wt.%)alloys were analyzed by weight loss rate,corrosion depth,corrosion products and corrosion morphologies.The electrochemical corrosion tests were also measured in the natural seawater.The comprehensive results showed that Mg-5Y-1.5Nd-4Zn-0.5Zr magnesium alloy existed the best corrosion resistance whether in the marine atmospheric environment and natural seawater environment.That depended on the microstructure,type and distribution of precipitated phases in Mg-5Y-1.5Nd-4Zn-0.5Zr magnesium alloy.Sufficient quantity anodic precipitated phases in the microstructure of Mg-5Y-1.5Nd-4Zn-0.5Zr alloy played the key role in the corrosion resistance.

In-Situ Microscopic FTIR Spectroelectrochemistry of Ascorbic Acid in Poly(ethylene glycol)/LiClO_4 Electrolyte Paste and in the Presence of Dispersed Cobalt Hexacyanoferrate Microcrystalline Powder

In-situ microscopic FTIR spectroelectrochemical technique(MFTIRs) was applied to studying the electrochemical oxidation of ascorbic acid(AA) in poly(ethylene glycol)(PEG) paste at a 100 μm diameter Pt disk electrode. Using this technique, the catalytic ability of cobalt hexacyanoferrate(CoHCF) microcrystalline toward AA oxidation was also studied. It was found that the dispersed CoHCF powder in the PEG paste can generate well shaped thin layer cyclic voltammetric waves with the peak height proportional to the scan rate, corresponding to the Fe centered redox reactions. This oxidation step catalyzed the AA oxidation. Also, this pasted CoHCF powder generated well resolved in situ MFTIRs spectra, by which a chemical interaction between CC bond of AA ring and CoHCF lattice was revealed. A corresponding surface docking mechanism for the catalytic reaction has been proposed.

Synthesis, Fluorescence and Electrochemistry of Three New Ruthenium(Ⅱ) Complexes

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Electrochemistry of Hydroquinone Derivatives at Metal and Iodine-modified Metal Electrodes

The difference in the electrochemical behavior of hydroquinone and pyrocatechol at platinum and gold surfaces was analyzed using voltammetry and attenuated total reflection Fourier transform infrared spectroscopy. The results show that the hydroquinone derivatives are adsorbed on a gold surface with vertical orientation, which makes the electron transfer between the bulk species and the electrode surface easier than that in the case of flat adsorption of hydroquinone derivatives that occurs at a platinum electrode. The formation of the vertical conformation and the rapid process of electron transfer were also confirmed by quantum chemistry calculations. In addition, the pre-adsorbed iodine on the electrodes played a key role on the adsorbed configuration and electron transfer of redox species.

Facet Engineering of Advanced Electrocatalysts Toward Hydrogen/Oxygen Evolution Reactions

The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed.

Hardening effect and precipitation evolution of an isothermal aged Mg-Sm based alloy

The age-hardening behavior and precipitation evolution of an isothermal aged Mg-5Sm-0.6Zn-0.5Zr(wt.%) alloy have been systematically investigated by means of transmission electron microscopy(TEM) and atomic-resolution high-angle annular dark field scanning transmission electron microscopy(HAADF-STEM). The Vickers hardness of the present alloy increases first and then decreases with ageing time. The sample aged at 200 ℃ for 10 h exhibits a peak-hardness of 90.5 HV. In addition to the dominant β_(0)’ precipitate(orthorhombic,a = 0.642 nm, b = 3.336 nm and c = 0.521 nm) formed on {11-20}α planes, a certain number of γ’’ precipitate(hexagonal, a = 0.556 nm and c = 0.431 nm) formed on basal planes are also observed in the peak-aged alloy. Significantly, the basal γ’’ precipitate is more thermostable than prismatic β_(0)’ precipitate in the present alloy. β_(0)’ precipitates gradually coarsened and were even likely to transform into β_(1) phase(face centered cubic, a = 0.73 nm) with the increase of ageing time, which accordingly led to a gradual decrease in number density of precipitates and finally resulted in the decreased hardness and mechanical property in the over-aged alloys.

The decisive role of adsorbed OH^(*)in low‐potential CO electro‐oxidation on single‐atom catalytic sites

CO impurity-induced catalyst deactivation has long been one of the biggest challenges in proton-exchange membrane fuel cells,with the poisoning phenomenon mainly attributed to the overly strong adsorption on the catalytic site.Here,we present a mechanistic study that overturns this understanding by using Rh-based single-atom catalysis centers as model catalysts.We precisely modulated the chelation structure of the Rh catalyst by coordinating Rh with C or N atoms,and probed the reaction mechanism by surface-enhanced Raman spectroscopy.Direct spectroscopic evidence for intermediates indicates that the reactivity of adsorbed OH^(*),rather than the adsorption strength of CO^(*),dictates the CO electrocatalytic oxidation behavior.The RhN_(4)sites,which adsorb the OH^(*)intermediate more weakly than RhC4 sites,showed prominent CO oxidation activity that not only far exceeded the traditional Pt/C but also the RhC4 sites with similar CO adsorption strength.From this study,it is clear that a paradigm shift in future research should be considered to rationally design high-performance CO electro-oxidation reaction catalysts by sufficiently considering the water-related reaction intermediate during catalysis.

ELECTROCHEMISTRY OF OI-μ-OXO-DIMANGANESE COMPLEX AT THIOURACIL MODIFIED GOLD ELECTRODE

The electrochemistry of di-μ-oxo-dimanganese complex was investigated. It was found that no redox peak was observed in the cyclic voltammogram (CV) of the complex at the bare gold electrode, but at thiouracil-modified gold electrode, a pair of redox peaks were observed showing that thiouracil can promote the proton-coupled electron transfer reaction of the complex.

Intratympanic injection of hydrogel nanodrug for the prevention and treatment of sensorineural hearing loss

Safe and efficient drug delivery to the inner ear has always been the focus of prevention and treatment of sensorineural deafness.The rapid development of nanodrug delivery systems based on hydrogel has provided a new opportunity.Among them,thermo-sensitive hydrogels promote the development of new dosage form for intratympanic injection.This smart biomaterial could transform to semisolid phase when the temperature increased.Thermo-sensitive hydrogel nanodrug delivery system is expected to achieve safe,efficient,and sustained inner ear drug administration.This article introduces the key techniques and the latest progress in this field.

Control of Phase Separation and Crystallization for High-Efficiency and Mechanically Deformable Organic Solar Cells

Stretchable organic solar cells(OSCs)have great potential as power sources for the next-generation wearable electronics.Although blending rigid photovoltaic components with soft insulating materials can easily endow the mechanical ductility of active layers,the photovoltaic efficiencies usually drops in the resulting OSCs.Herein,a high photovoltaic efficiency of 15.03%and a large crack-onset strain of 15.70%is simultaneously achieved based on a ternary blend consisting of polymer donor poly[(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione))](PM6),non-fullerene accepter 2,2'-((2Z,2'Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2",3":4',5']thieno[2',3':4,5]pyrrolo[3,2-g]thieno[2',3':4,5]thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(Y6),and soft elastomer polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene(SEBS)through the control of phase separation and crystallization.By employing a high-boiling point solvent additive 1-chloronaphthalene(CN)with different solubilities for PM6 and Y6,the aggregation dynamics of PM6 and Y6 as well as the film solidification process are dramatically altered,allowing for the different molecular rearrangement and liquid-liquid phase separation evolution.Consequently,the ternary film with optimal CN content presents decreased SEBS domains and moderately improved molecular ordering of PM6 and Y6,enabling effective mechanical deformation and charge generation/transport.The revealed corrections between the film-formation process,film microstructure,and photovoltaic/mechanical characteristics in the ternary blend provide deep understanding of the morphology control toward high-performance stretchable OSCs.

Next-generation vaccines for substance use disorders

Substance use disorders(SUDs)impact an estimated 300 million people worldwide,significantly impairing both health and social functioning.These disorders are marked by an inability to regulate substance use,despite the harmful consequences.Addiction affects various neurotransmitter systems,including dopamine,serotonin,γ-aminobutyric acid(GABA),and glutamate,each of which plays a role in the reward,stress,and self-control pathways of the brain(Koob&Volkow,2016).While significant advances have been made in neuroscience,our understanding of how these neurotransmitter systems interact and contribute to addiction is still evolving.This knowledge gap represents a significant challenge in the formulation of effective treatments for SUDs.At present,the US Food and Drug Administration(FDA)has approved pharmacological treatments for alcohol,nicotine,and opioid use disorders(Vasiliu,2022);however,no such treatments have been authorized for SUDs in general,or specifically for stimulant use disorders,such as cocaine and methamphetamine addiction.Notably,the FDA has not approved any new drugs for SUD treatment in the past 40 years.

Microglia in drug addiction:A perspective from neuroimmunopharmacology

Drug addiction refers to a state of dependence that arises from habitual drug intake and can result in specific withdrawal symptoms upon cessation.The most commonly abused substances include psychostimulants,cannabinoids,and opioids.When drugs are consumed,they stimulate the release of dopamine,a neurotransmitter crucial for the pleasure and reward centers of the brain.With repeated drug use,the brain undergoes various changes,leading to tolerance,dependence,and addiction(Lüscher et al.,2020).The mechanisms involved in drug addiction are highly complex and involve diverse cell types within the brain.

A universal multifunctional dual cation doping strategy towards stabilized ultra-high nickel cobalt-free lithium layered oxide cathode

Ultra-high nickel cobalt-free lithium layered oxides are promising cathode material for lithium-ion batteries(LIBs)because of their relatively high capacity and low cost.Nevertheless,the high nickel content would induce bulk structure degradation and interfacial environment deterioration,and the absence of Co element reduces the lithium diffusion kinetics,severely limiting the performance liberation of this kind of cathodes.Herein,a multifunctional Ti/Zr dual cation co-doping strategy has been employed to improve the lithium storage performance of LiNi_(0.9)Mn_(0.1)O_(2)(NM91)cathode.On the one hand,the Ti/Zr co-doping weakens the Li^(+)/Ni^(2+)mixing through magnetic interactions due to the inexistence of unpaired electrons for Ti^(4+)and Zr^(4+),increasing the lithium diffusion rate and suppressing the harmful coexistence of H1 and H2 phases.On the other hand,they enhance the lattice oxygen stability because of the strong Ti-O and Zr-O bonds,inhibiting the undesired H3 phase transition and lattice oxygen loss,improving the bulk structure and cathode-electrolyte interface stability.As a result,the Ti/Zr co-doped NM91(NMTZ)exhibits a 91.2%capacity retention rate after 100 cycles,while that of NM91 is only82.9%.Also,the NMTZ displays better rate performance than NM91 with output capacities of 115 and93 mA h g^(-1)at a high current density of 5 C,respectively.Moreover,the designed NMTZ could enable the full battery to deliver an energy density up to 263 W h kg^(-1),making the ultra-high nickel cobaltfree lithium layered oxide cathode closer to practical applications.

Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

Exceptional reversed yield strength asymmetry in a rare-earth free Mg alloy containing quasicrystal precipitates

This work reports an exceptional reversed yield strength asymmetry at room temperature for a rare-earth free magnesium alloy containing a mass of fine dispersed quasicrystal(I-phase)precipitates.Although exhibiting traditional basal texture,it owns an exceptional CYS/TYS as high as~1.17.Electron back-scattered diffraction(EBSD)and transmission electron microscopy(TEM)examinations indicate pyramidal and prismatic dislocations plus tensile twinning being activated after immediate yielding in compression while basal and non-basal dislocations in tension.I-phase particles transferred the concentrated stress by self-twinning to provide the driving force for tensile twin initiating in neighboring grains,thereby significantly increasing the critical resolved shear stress of tensile twinning to possibly the level of pyramidal slip,finally leading to the dominance of pyramidal slip plus tensile twinning in texture grains.This results in a higher contribution on yield strength by~55 MPa in compression than in tension,which reasonably agrees with the experimental yield strength difference(~38 MPa).It can be concluded that I-phase particles influence deformation modes in tension and in compression,finally result in reversed yield strength asymmetry.

Recent advances in living cell nucleic acid probes based on nanomaterials for early cancer diagnosis

The early diagnosis of cancer is vital for effective treatment and improved prognosis. Tumor biomarkers, which can be used for the early diagnosis, treatment, and prognostic evaluation of cancer, have emerged as a topic of intense research interest in recent years. Nucleic acid, as a type of tumor biomarker, contains vital genetic information, which is of great significance for the occurrence and development of cancer. Currently, living cell nucleic acid probes, which enable the in situ imaging and dynamic monitoring of nucleic acids, have become a rapidly developing field. This review focuses on living cell nucleic acid probes that can be used for the early diagnosis of tumors. We describe the fundamental design of the probe in terms of three units and focus on the roles of different nanomaterials in probe delivery.