Nano-Ni-Induced Electronic Modulation of MoS_(2) Nanosheets Enables Energy-Saving H_(2) Production and Sulfide Degradation

Electrocatalytic hydrogen evolution and sulfion(S^(2-))recycling are promising strategies for boosting H_(2)production and removing environmental pollutants.Here,a nano-Ni-functionalized molybdenum disulfide(MoS_(2))nanosheet was assembled on steel mesh(Ni-MoS_(2)/SM)for use in sulfide oxidation reaction-assisted,energy-saving H_(2)production.Experimental and theoretical calculation results revealed that anchoring nano-Ni on high-surface-area slack MoS_(2)nanosheets not only optimized catalyst adsorption of polysulfides but also played an important role in promoting hydrogen evolution reaction kinetics by absorbing OH_(ad),thereby greatly enhancing the catalytic performance toward sulfide oxidation reaction and hydrogen evolution reaction.Meanwhile,the Ni/MoS^(2-)based hydrogen evolution reaction+sulfide oxidation reaction system achieved nearly 100%hydrogen production efficiency and only consumed 61%less power per kWh than the oxygen evolution reaction+hydrogen evolution reaction system,which suggested our proposed Ni-MoS_(2)and novel hydrogen production system are promising for sustainable energy production.

Lithium-ion and solvent co-intercalation enhancing the energy density of fluorinated graphene cathode

Fluorinated carbons CF_xhold the highest theoretical energy density(e.g.,2180 W h kg^(-1)when x=1)among all cathode materials of lithium primary batteries.However,the low conductivity and severe polarization limit it to achieve its theory.In this study,we design a new electrolyte,namely 1 M LiBF_(4)DMSO:DOL(1:9 vol.),achieving a high energy density in Li/CF_xprimary cells.The DMSO with a small molecular size and high donor number successfully solvates Li^(+)into a defined Li^(+)-solvation structure.Such solvated Li^(+)can intercalate into the large-spacing carbon layers and achieve an improved capacity.Consequently,when discharged to 1.0 V,the CF_(1.12)cathode demonstrates a specific capacity of 1944 m A h g^(-1)with a specific energy density of 3793 W h kg^(-1).This strategy demonstrates that designing the electrolyte is powerful in improving the electrochemical performance of CF_(x) cathode.

ZnO Additive Boosts Charging Speed and Cycling Stability of Electrolytic Zn–Mn Batteries

Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish deposition reaction kinetics of manganese oxide during the charge process and short cycle life. We show that, incorporating ZnO electrolyte additive can form a neutral and highly viscous gel-like electrolyte and render a new form of electrolytic Zn–Mn batteries with significantly improved charging capabilities. Specifically, the ZnO gel-like electrolyte activates the zinc sulfate hydroxide hydrate assisted Mn^(2+) deposition reaction and induces phase and structure change of the deposited manganese oxide(Zn_(2)Mn_(3)O_8·H_(2)O nanorods array), resulting in a significant enhancement of the charge capability and discharge efficiency. The charge capacity increases to 2.5 mAh cm^(-2) after 1 h constant-voltage charging at 2.0 V vs. Zn/Zn^(2+), and the capacity can retain for up to 2000 cycles with negligible attenuation. This research lays the foundation for the advancement of electrolytic Zn–Mn batteries with enhanced charging capability.

Interfacial Modification of NiO_(x)by Self-assembled Monolayer for Efficient and Stable Inverted Perovskite Solar Cells

NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.

Effects of Catalysis and Separator Functionalization on High-Energy Lithium–Sulfur Batteries:A Complete Review

Lithium–sulfur(Li-S)batteries have the advantages of high theoretical specific capacity(1675 mAh g^(−1)),rich sulfur resources,low production cost,and friendly environment,which makes it one of the most promising next-generation rechargeable energy storage devices.However,the“shuttle effect”of polysulfide results in the passivation of metal lithium anode,the decrease of battery capacity and coulombic efficiency,and the deterioration of cycle stability.To realize the commercialization of Li-S batteries,its serious“shuttle effect”needs to be suppress.The commercial separators are ineffective to suppress this effect because of its large pore size.Therefore,it is an effective strategy to modify the separator surface and introduce functional modified layer.In addition to the blocking strategy,the catalysis of polysulfide conversion reaction is also an important factor hindering the migration of polysulfides.In this review,the principles of separator modification,functionalization,and catalysis in Li-S batteries are reviewed.Furthermore,the research trend of separator functionalization and polysulfide catalysis in the future is prospected.

Effects of Additives on the Microstructure and Tribology Performance of Ta-12W Alloy Micro-Arc Oxidation Coating

Oxide ceramic coatings were fabricated on tantalum alloys by micro-arc oxidation (MAO) to improve their hardness and tribological properties. The MAO coatings were manufactured in a mixed silicatephosphate electrolyte containing NaF and/or EDTA (ethylene diamine tetraacetic acid). The surface morphology,cross-sectional view, chemical composition, hardness, and wear performance of the coatings were analysed. As revealed by the scanning electron microscopy, silica-rich nodules appear on the MAO coating obtained in the silicate-phosphate electrolyte, but the formation of nodules is inhibited with NaF and/or EDTA in the electrolyte.Also, they reduce the roughness and improve the compactness of the coatings, which are composed of Ta_(2)O_(5),(Ta, O), and TaO. A thick and hard coating is obtained in the NaF-containing electrolyte, and the tribology performance is effectively improved. With additives, the nodule structure is detached from the coating surface and dissolved in the electrolyte. By using NaF as an electrolyte additive, the abrasion performance of the MAO coating is enhanced by decreasing the nodule structure, increasing the size of micropores, and improving the coating hardness.

Regulation of the quantum barrier and carrier transport toward high-efficiency quasi-2D Dion-Jacobson tin perovskite solar cells

Quasi-2D Dion-Jacobson(DJ)tin halide perovskite has attracted much attention due to its elimination of Van der Waals gap and enhanced environmental stability.However,the bulky organic spacers usually form a natural quantum well structure,which brings a large quantum barrier and poor film quality,further limiting the carrier transport and device performance.Here,we designed three organic spacers with different chain lengths(ethylenediamine(EDA),1,3-propanediamine(PDA),and 1,4-butanediamine(BDA))to investigate the quantum barrier dependence.Theoretical and experimental characterizations indicate that EDA with short chain can reduce the lattice distortion and dielectric confinement effect,which is beneficial to the effective dissociation of excitons and the inhibition of trap-free non-radiative relaxation.In addition,EDA cation shows strong interaction with the inorganic octahedron,realizing large aggregates in precursor solution and high-quality films with improved structural stability.Furthermore,femtosecond transient absorption proves that EDA cations can also weaken the formation of small n-phases with large quantum barrier to achieve effective carrier transport between different nphases.Finally,the quasi-2D DJ(EDA)FA_(9)Sn_(10)I_(31)solar cells achieves a 7.07%power conversion efficiency with good environment stability.Therefore,this work sheds light on the regulation of the quantum barrier and carrier transport through the chain length of organic spacer for qua si-2D DJ lead-free perovskites.

The rise of supercapacitor diodes:Current progresses and future challenges

Supercapacitor has been widely known as a representative electrochemical energy storage device with high power density and long lifespan.Recently,with the deeper understanding of its charge storage mechanism,unidirectional-charging supercapacitor,also called supercapacitor diode(CAPode),is successfully developed based on the ion-sieving effect of its working electrode towards electrolyte ions.Because CAPode integrates mobile ion and mobile electron in one hybrid circuit,it has a great potential in the emerging fields of ion/electron coupling logic operations,human–machine interface,neural network interaction,and in vivo diagnosis and treatment.Accordingly,we herein elucidate the working mechanism and design philosophy of CAPode,and summarize the electrode materials that are suitable for constructing CAPode.Meanwhile,some other supercapacitor-based devices beyond CAPode are also introduced,and their potential applications are instructively presented.Finally,we outline the challenges and chances of CAPode-related techniques.

Progress and prospects of Mg-based amorphous alloys in azo dye wastewater treatment

Mg-based amorphous alloys exhibit efficient catalytic performance and excellent biocompatibility with a promising application probability,specifically in the field of azo dye wastewater degradation.However,the problems like difficulty in preparation and poor cycling stability need to be solved.At present,Mg-based amorphous alloys applied in wastewater degradation are available in powder and ribbon.The amorphous alloy powder fabricated by ball milling has a high specific surface area,and its reactivity is thousands of times better than that of gas atomized alloy powder.But the development is limited due to the high energy consumption,difficult and costly process of powder recycling.The single roller melt-spinning method is a new manufacturing process of amorphous alloy ribbon.Compared to amorphous powder,the specific surface area of amorphous ribbon is relatively lower,therefore,it is necessary to carry out surface modification to enhance it.Dealloying is a way that can form a pore structure on the surface of the amorphous alloys,increasing the specific surface area and providing more reactive sites,which all contribute to the catalytic performance.Exploring the optimal conditions for Mg-based amorphous alloys in wastewater degradation by adjusting amorphous alloy composition,choosing suitable method to preparation and surface modification,reducing cost,expanding the pH range will advance the steps to put Mg-based amorphous alloys in industrial environments into practice.

Efficient and selective upcycling of waste polylactic acid into acetate using nickel selenide

The conversion of waste polylactic acid(PLA)plastics into high-value-added chemicals through electrochemical methods is a promising and sustainable approach.However,developing efficient and highly selective catalysts for lactic acid oxidation reaction(LAOR)and understanding the reaction process are challenging.Here,we report the electrooxidation of waste PLA to acetate at a high current density of 100 mA cm-2 with high Faraday efficiency(~95%)and excellent stability(>100 h)over a nickel selenide nanosheet catalyst.In addition,a total Faraday efficiency of up to 190%was achieved for carboxylic acids,including acetic acid and formic acid,by coupling with the cathodic CO_(2) reduction reaction.In situ experimental results and theoretical simulations revealed that the catalytic activity center of LAOR was dynamically formed NiOOH species,and the surface-adsorbed SeO_(x) species accelerated the formation of Ni~(3+)species,thus promoting catalytic activity.The mechanism of lactic acid electrooxidation was further elucidated.Lactic acid was dehydrogenated to produce pyruvate first and then formed CH_3CO due to preferential C-C bond cleavage,resulting in the presence of acetate.This work demonstrated a sustainable method for recycling waste PLA and CO_(2) into high-value-added products.

Effects of cooling rate on microstructure and microhardness of directionally solidified Galvalume alloy

The influences of cooling rate on the phase constitution,microstructural length scale,and microhardness of directionally solidified Galvalume(Zn-55Al-1.6Si)alloy were investigated by directional solidification experiments at different withdrawal speeds(5,10,20,50,100,200,and 400μm·s^(-1)).The results show that the microstructure of directionally solidified Galvalume alloys is composed of primary Al dendrites,Si-rich phase and(Zn-Al-Si)ternary eutectics at the withdrawal speed ranging from 5 to 400μm·s^(-1).As the withdrawal speed increases,the segregation of Si element intensifies,resulting in an increase in the area fraction of the Si-rich phase.In addition,the primary Al dendrites show significant refinement with an increase in the withdrawal speed.The relationship between the primary dendrite arm spacing(λ_(1))and the thermal parameters of solidification is obtained:λ_(1)=127.3V^(-0.31).Moreover,as the withdrawal speed increases from 5 to 400μm·s^(-1),the microhardness of the alloy increases from 90 HV to 151 HV.This is a combined effect of grain refinement and second-phase strengthening.

Efficient Polytelluride Anchoring for Ultralong-Life Potassium Storage: Combined Physical Barrier and Chemisorption in Nanogrid-in-Nanofiber

Metal tellurides(MTes) are highly attractive as promising anodes for high-performance potassium-ion batteries. The capacity attenuation of most reported MTe anodes is attributed to their poor electrical conductivity and large volume variation. The evolution mechanisms, dissolution properties, and corresponding manipulation strategies of intermediates(K-polytellurides, K-pTe_(x)) are rarely mentioned. Herein,we propose a novel structural engineering strategy to confine ultrafine CoTe_(2) nanodots in hierarchical nanogrid-in-nanofiber carbon substrates(CoTe_(2)@NC@NSPCNFs) for smooth immobilization of K-pTe_(x) and highly reversible conversion of CoTe_(2) by manipulating the intense electrochemical reaction process. Various in situ/ex situ techniques and density functional theory calculations have been performed to clarify the formation, transformation, and dissolution of K-pTe_(x)(K_(5)Te_(3) and K_(2)Te), as well as verifying the robust physical barrier and the strong chemisorption of K_(5)Te_(3) and K_(2)Te on S, N co-doped dual-type carbon substrates. Additionally, the hierarchical nanogrid-in-nanofiber nanostructure increases the chemical anchoring sites for K-pTe_(x), provides sufficient volume buffer space, and constructs highly interconnected conductive microcircuits, further propelling the battery reaction to new heights(3500 cycles at 2.0 A g^(-1)). Furthermore, the full cells further demonstrate the potential for practical applications. This work provides new insights into manipulating K-pTe_(x) in the design of ultralong-cycling MTe anodes for advanced PIBs.

Tailoring the microstructure of Mg-Al-Sn-RE alloy via friction stir processing and the impact on its electrochemical discharge behaviour as the anode for Mg-air battery

Constructing the magnesium alloy with fine grains,low density of dislocations,and weak crystal orientation is of crucial importance to enhance its comprehensive performance as the anode for Mg-air battery.However,this unique microstructure can hardly be achieved with conventional plastic deformation such as rolling or extrusion.Herein,we tailor the microstructure of Mg-Al-Sn-RE alloy by using the friction stir processing,which obviously refines the grains without increasing dislocation density or strengthening crystal orientation.The Mg-air battery with the processed Mg-Al-Sn-RE alloy as the anode exhibits higher discharge voltages and capacities than that employing the untreated anode.Furthermore,the impact of friction stir processing on the electrochemical discharge behaviour of Mg-Al-Sn-RE anode and the corresponding mechanism are also analysed according to microstructure characterization and electrochemical response.

A layered multifunctional framework based on polyacrylonitrile and MOF derivatives for stable lithium metal anode

Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.

Generation and regulation of electromagnetic pulses generated by femtosecond lasers interacting with multitargets

Ultrashort and powerful laser interactions with a target generate intense wideband electromagnetic pulses(EMPs).In this study,we report EMPs generated by the interactions between petawatt(30 fs,1.4×10^(20) W/cm^(2))femtosecond(fs)lasers with metal flat,plastic flat,and plastic nanowire-array(NWA)targets.Detailed analyses are conducted on the EMPs in terms of their spatial distribution,time and frequency domains,radiation energy,and protection.The results indicate that EMPs from metal targets exhibit larger amplitudes at varying angles than those generated by other types of targets and are enhanced significantly for NWA targets.Using a plastic target holder and increasing the laser focal spot can significantly decrease the radiation energy of the EMPs.Moreover,the composite shielding materials indicate an effective shielding effect against EMPs.The simulation results show that the NWA targets exert a collimating effect on thermal electrons,which directly affects the distribution of EMPs.This study provides guidance for regulating EMPs by controlling the laser focal spot,target parameters,and target rod material and is beneficial for electromagnetic-shielding design.

Spatial and temporal evolution of electromagnetic pulses from solid target irradiated with multi-hundred-terawatt laser pulse inside target chamber

Giant electromagnetic pulses(EMPs) induced by high-power laser irradiating solid targets interfere with various experimental diagnoses and even damage equipment,so unveiling the evolution of EMPs inside the laser chamber is crucial for designing effective EMP shielding.In this work,the transmission characteristics of EMPs as a function of distances from the target chamber center(TCC) are studied using B-dot probes.The mean EMP amplitude generated by picosecond laser-target interaction reaches 561 kV m^(-1),357 kV m^(-1),395 kV m^(-1),and 341 kV m^(-1)at 0.32 m,0.53 m,0.76 m,and 1 m from TCC,which decreases dramatically from 0.32 m to 0.53 m.However,it shows a fluctuation from 0.53 m to 1 m.The temporal features of EMPs indicate that time-domain EMP signals near the target chamber wall have a wider full width at half maximum compared to that close to TCC,mainly due to the echo oscillation of electromagnetic waves inside the target chamber based on simulation and experimentation.The conclusions of this study will provide a new approach to mitigate strong electromagnetic pulses by decreasing the echo oscillation of electromagnetic waves inside the target chamber during laser coupling with targets.

Applications of Metal–Organic Frameworks and Their Derivatives in Electrochemical CO_(2)Reduction

Electrochemically reducing CO_(2)to more reduced chemical species is a promising way that not only enables the conversion of intermittent energy resources to stable fuels,but also helps to build a closed-loop anthropogenic carbon cycle.Among various electrocatalysts for electrochemical CO_(2)reduction,multifunctional metal–organic frameworks(MOFs)have been employed as highly efficient and selective heterogeneous electrocatalysts due to their ultrahigh porosity and topologically diverse structures.Up to now,great progress has been achieved in the design and synthesis of highly active and selective MOF-related catalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR),and their corresponding reaction mechanisms have been thoroughly studied.In this review,we summarize the recent progress of applying MOFs and their derivatives in CO_(2)RR,with a focus on the design strategies for electrocatalysts and electrolyzers.We first discussed the reaction mechanisms for different CO_(2)RR products and introduced the commonly applied electrolyzer configurations in the current CO_(2)RR system.Then,an overview of several categories of products(CO,HCOOH,CH_(4),CH_(3)OH,and multi-carbon chemicals)generated from MOFs or their derivatives via CO_(2)RR was discussed.Finally,we offer some insights and perspectives for the future development of MOFs and their derivatives in electrochemical CO_(2)reduction.We aim to provide new insights into this field and further guide future research for large-scale applications.

Additive manufacturing of Ni-based superalloys: Residual stress, mechanisms of crack formation and strategies for crack inhibition

The additive manufacturing(AM)of Ni-based superalloys has attracted extensive interest from both academia and industry due to its unique capabilities to fabricate complex and high-performance components for use in high-end industrial systems.However,the intense temperature gradient induced by the rapid heating and cooling processes of AM can generate high levels of residual stress and metastable chemical and structural states,inevitably leading to severe metallurgical defects in Ni-based superalloys.Cracks are the greatest threat to these materials’integrity as they can rapidly propagate and thereby cause sudden and non-predictable failure.Consequently,there is a need for a deeper understanding of residual stress and cracking mechanisms in additively manufactured Ni-based superalloys and ways to potentially prevent cracking,as this knowledge will enable the wider application of these unique materials.To this end,this paper comprehensively reviews the residual stress and the various mechanisms of crack formation in Ni-based superalloys during AM.In addition,several common methods for inhibiting crack formation are presented to assist the research community to develop methods for the fabrication of crack-free additively manufactured components.

COF-based single Li^(+)solid electrolyte accelerates the ion diffusionandrestrains dendritegrowthin quasi-solid-state organic batteries

A solid-state electrolyte(SSE),which is a solid ionic conductor and electroninsulating material,is known to play a crucial role in adapting a lithium metal anode to a high-capacity cathode in a solid-state battery.Among the various SSEs,the single Li-ion conductor has advantages in terms of enhancing the ion conductivity,eliminating interfacial side reactions,and broadening the electrochemical window.Covalent organic frameworks(COFs)are optimal platforms for achieving single Li-ion conduction behavior because of wellordered one-dimensional channels and precise chemical modification features.Herein,we study in depth three types of Li-carboxylate COFs(denoted LiOOC-COFn,n=1,2,and 3)as single Li-ion conducting SSEs.Benefiting from well-ordered directional ion channels,the single Li-ion conductor LiOOC-COF3 shows an exceptional ion conductivity of 1.36×10^(-5) S cm^(-1) at room temperature and a high transference number of 0.91.Moreover,it shows excellent electrochemical performance with long-term cycling,high-capacity output,and no dendrites in the quasi-solid-state organic battery,with the organic small molecule cyclohexanehexone(C_(6)O_(6))as the cathode and the Li metal as the anode,and enables effectively avoiding dissolution of the organic electrode by the liquid electrolyte.

Understanding Dual-Polar Group Functionalized COFs for Accelerating Li-Ion Transport and Dendrite-Free Deposition in Lithium Metal Anodes

Lithium metal batteries(LMBs)have attracted wide attentions because of their high theoretical specific capacity and low electrochemical potential.However,the growth of lithium dendrites seriously affects the practical application of LMBs.Thus,the lithium-philic carbonyl and carboxy dualgroup-modified covalent organic framework(COF-COOH)is designed to coat the polypropylene(PP)separator(COF-COOH@PP separator),realizing the regulation of ion transport and uniform lithium deposition.The plentiful and negative charge sites in the COF-COOH can suppress the diffusion of the freely movable lithium salt anion by the electrostatic interaction.Density functional theory(DFT)calculations demonstrate that the COF-COOH possesses the function of anchoring anion and desolvation.Consequently,the Li^(+)transference number(0.7),ion conductivity(0.64 mS cm^(-1)),and desolvating of Li^(+)are obviously improved by using the COF-COOH@PP separator.The modified Li-Li symmetric battery delivers stable cycle for more than 1000 h and lower voltage hysteresis(0.02 V).This dendrite-free deposition strategy holds great promise for practical application of Li metal anodes.