Mechanochemical synthesis of oxygenated alkynyl carbon materials with excellent Hg(Ⅱ) adsorption performance from CaC2 and carbonates

Adsorptive removal of heavy metal ions from wastewater is very important,and the key is the development of efficient sorbents.In this work,oxygenated alkynyl carbon materials(OACMs)were synthesized via mechanochemical reaction of CaC_(2) and a carbonate(CaCO_(3),Na2CO_(3),or NaHCO_(3))at ambient temperature.The resultant OACMs are micro mesoporous carbon nanomaterials with high specific area(>648 m2 g^(-1)),highly crosslinked texture,and rich alkynyl and oxygenated groups.The OACMs exhibit excellent Hg(Ⅱ)adsorption due to the soft acid-soft base interaction between alkynyl and Hg(Ⅱ),and OACM-3 derived from CaC_(2) and NaHCO_(3) has the saturated Hg(Ⅱ)adsorbance of 483.9 mg g^(-1)along with good selectivity and recyclability.The adsorption is mainly chemisorption following the Langmuir mode.OACM-3 also shows high adsorbance for other heavy metal ions,e.g.256.6 mg g^(-1)for Pb(II),232.4 mg g^(-1)for Zn(II),and 198.7 mg g^(-1)for Cu(II).This work expands the mechnochemical reaction of CaC_(2)with carbonates and possibly other oxyanionic salts,provides a new synthesis approach for functional alkynyl carbon materials with excellent adsorption performance for heavy metal ions,as well as a feasible approach for CO2 resource utilization.

Intelligent Small Sample Defect Detection of Concrete Surface Using Novel Deep Learning Integrating Improved YOLOv5

Dear Editor,This letter presents an intelligent small sample defect detection of concrete surface using novel deep learning integrating the improved YOLOv5 based on the Wasserstein GAN(WGAN)enhancement algorithm.The proposed method is capable of producing top-notch data sets to address the issues of insufficient samples and substandard quality.

High throughput screening of single atomic catalysts with optimized local structures for the electrochemical oxygen reduction by machine learning

Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utilization efficiency.However,there is still a lack of systematic screening and optimization of local structures surrounding active centers of SACs for ORR as the local coordination has an essential impact on their electronic structures and catalytic performance.Herein,we systematic study the ORR catalytic performance of M-NC SACs with different central metals and environmental atoms in the first and second coordination sphere by using density functional theory(DFT)calculation and machine learning(ML).The geometric and electronic informed overpotential model(GEIOM)based on random forest algorithm showed the highest accuracy,and its R^(2) and root mean square errors(RMSE)were 0.96 and 0.21,respectively.30 potential high-performance catalysts were screened out by GEIOM,and the RMSE of the predicted result was only 0.12 V.This work not only helps us fast screen high-performance catalysts,but also provides a low-cost way to improve the accuracy of ML models.

A novel calculation strategy for optimized prediction of the reduction of electrochemical window at anode

The reduction of the electrochemical window(EW)of electrolytes plays a significant role in assessing their compatibility with the anode in lithium-ion batteries.However,the accurate calculation of the reduction of EW is still challenging due to missing the solvation effects,condensation effects,kinetic factors,and the passivation on anodes.The theoretical prediction of the intrinsic and apparent EW is confirmed by a comprehensive experimental analysis of ethylene carbonatedimethyl carbonate(EC-DMC)electrolytes,combining linear sweep voltammetry(LSV)and gas chromatography-mass spectrometry(GC-MS).The proposed novel kinetic normal distribution theory model can quantitatively explain the current density from LSV and affirm acetaldehyde(MeCHO)as one of the primary reduction products of EC.The solvent effect restricts the intrinsic EW of EC-DMC without lithium salt to 2.6 V(vs.Li^(+)/Li)arising from the Marcus-Gerischer theory and the passivation of MeCHO on the anode broadens the apparent EW to 0.3 V(vs.Li^(+)/Li)arising from the normal distribution of the lowest unoccupied molecular orbital(LUMO)for MeCHO produced by thermal motion.In addition,the passivation on the anode depends intensively on the lithium salt,resulting in more complicated influences on the apparent EW.

THE NONLINEAR STABILITY OF PLANE PARALLEL SHEAR FLOWS WITH RESPECT TO TILTED

The nonlinear stability of plane parallel shear flows with respect to tilted perturbations is studied by energy methods.Tilted perturbation refers to the fact that perturbations form an angleθ∈(0,π/2)with the direction of the basic flows.By defining an energy functional,it is proven that plane parallel shear flows are unconditionally nonlinearly exponentially stable for tilted streamwise perturbation when the Reynolds number is below a certain critical value and the boundary conditions are either rigid or stress-free.In the case of stress-free boundaries,by taking advantage of the poloidal-toroidal decomposition of a solenoidal field to define energy functionals,it can be even shown that plane parallel shear flows are unconditionally nonlinearly exponentially stable for all Reynolds numbers,where the tilted perturbation can be either spanwise or streamwise.

Constructing high-toughness polyimide binder with robust polarity and ion-conductive mechanisms ensuring long-term operational stability of silicon-based anodes

Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH) groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.

Highly selective extraction of aromatics from aliphatics by using metal chloride-based ionic liquids

The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry.In this study,a series of metal chloride-based ionic liquids were prepared and their performances in the separation of 1,2,3,4-tetrahydronaphthalene(tetralin)/dodecane and tetralin/decalin systems were studied.Among these ionic liquids,1-ethyl-3-methylimidazolium tetrachloroferrate([EMIM][FeCl_(4)])with the highest selectivity was used as the extractant.Density functional theory calculations showed that[EMIM][FeCl_(4)]interacted more strongly with tetralin than with dodecane and decalin.Energy decomposition analysis of[EMIM][FeCl_(4)]-tetralin indicated that electrostatics and dispersion played essential roles,and induction cannot be neglected.The van der Waals forces was a main effect in[EMIM][FeCl_(4)]-tetralin by independent gradient model analysis.The tetralin distribution coefficient and selectivity were 0.8 and 110,respectively,with 10%(mol)tetralin in the initial tetralin/dodecane system,and 0.67 and 19.5,respectively,with 10%(mol)tetralin in the initial tetralin/decalin system.The selectivity increased with decreasing alkyl chain length of the extractant.The influence of the extraction temperature,extractant dosage,and initial concentrations of the system components on the separation performance were studied.Recycling experiments showed that the regenerated[EMIM][FeCl_(4)]could be used repeatedly.

Polymer engineering for electrodes of aqueous zinc ion batteries

With the increasing demand for scalable and cost-effective electrochemical energy storage,aqueous zinc ion batteries(AZIBs)have a broad application prospect as an inexpensive,efficient,and naturally secure energy storage device.However,the limitations suffered by AZIBs,including volume expansion and active materials dissolution of the cathode,electrochemical corrosion,irreversible side reactions,zinc dendrites of the anode,have seriously decelerated the civilianization process of AZIBs.Currently,polymers have tremendous superiority for application in AZIBs attributed to their exceptional chemical stability,tunable structure,high energy density and outstanding mechanical properties.Considering the expanding applications of AZIBs and the superiority of polymers,this comprehensive paper meticulously reviews the benefits of utilizing polymeric applied to cathodes and anodes,respectively.To begin with,with adjustable structure as an entry point,the correlation between polymer structure and the function of energy storage as well as optimization is deeply investigated in respect to the mechanism.Then,depending on the diversity of properties and structures,the development of polymers in AZIBs is summarized,including conductive polymers,redox polymers as well as carbon composite polymers for cathode and polyvinylidene fluoride-,carbonyl-,amino-,nitrile-based polymers for anode,and a comprehensive evaluation of the shortcomings of these strategies is provided.Finally,an outlook highlights some of the challenges posed by the application of polymers and offers insights into the potential future direction of polymers in AZIBs.It is designed to provide a thorough reference for researchers and developers working on polymer for AZIBs.

THE GLOBAL EXISTENCE OF STRONG SOLUTIONS TO THERMOMECHANICAL CUCKER-SMALE-STOKES EQUATIONS IN THE WHOLE DOMAIN

We study the global existence and uniqueness of a strong solution to the kinetic thermomechanical Cucker-Smale(for short,TCS) model coupled with Stokes equations in the whole space.The coupled system consists of the kinetic TCS equation for a particle ensemble and the Stokes equations for a fluid via a drag force.In this paper,we present a complete analysis of the existence of global-in-time strong solutions to the coupled model without any smallness restrictions on the initial data.

Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance electro-catalysts.Currently,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications.Compared to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic activity.Of these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal atoms.DACs have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active sites.In this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related applications.The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction reaction.The future research challenges and opportunities are also raised in prospective section.

Analysis of the Erosion-Corrosion Mechanism of the Air Cooler in a Hydrocracking Unit:A Numerical and Experimental Study

Corrosion leakages often occur in the air cooler of a hydrocracking unit,with the failure sites mainly located in the entrance area of the tubes.An analysis of the macroscopic morphology and corrosion products confirmed that the damage was caused by erosion-corrosion(E-C).Numerical and experimental methods were applied to investigate the E-C mechanism in the air cooler.Computational fluid dynamics(CFD)was used to calculate the hydrodynamic parameters of the air cooler.The results showed that there was a biased flow in the air cooler,which led to a significant increase in velocity,turbulent kinetic energy and wall shear within 0.2 m of the tube entrance.A visualization experiment was then performed to determine the principles of migration and transformation of multiphase flow in the air cooler tubes.Various flow patterns(pure droplet flow,mist flow,and annular flow)and their evolutionary processes were clearly depicted experimentally.The initiation mechanism and processes leading to the development of E-C in the air cooler were also determined.This study provided a comprehensive explanation for the E-C failures that occur in air coolers during operation.

Potential industrial applications of photo/electrocatalysis: Recent progress and future challenges

Nowadays,the rapid development of the social economy inevitably leads to global energy and environmental crisis.For this reason,more and more scholars focus on the development of photocatalysis and/or electrocatalysis technology for the advantage in the sustainable production of high-value-added products,and the high efficiency in pollutants remediation.Although there is plenty of outstanding research has been put forward continuously,most of them focuses on catalysis performance and reaction mechanisms in laboratory conditions.Realizing industrial application of photo/electrocatalytic processes is still a challenge that needs to be overcome by social demand.In this regard,this review comprehensively summarized several explorations in thefield of photo/electrocatalytic reduction towards potential industrial applications in recent years.Special attention is paid to the successful attempts and the current status of photo/electrocatalytic water splitting,carbon dioxide conversion,resource utilization from waste,etc.,by using advanced reactors.The key problems and challenges of photo/electrocatalysis in future industrial practice are also discussed,and the possible development directions are also pointed out from the industry view.

Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO_(2) into carboxylic acids

The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.

The Journey/DAO/TAO of Embodied Intelligence: From Large Models to Foundation Intelligence and Parallel Intelligence

THE tremendous impact of large models represented by ChatGPT[1]-[3]makes it necessary to con-sider the practical applications of such models[4].However,for an artificial intelligence(AI)to truly evolve,it needs to possess a physical“body”to transition from the virtual world to the real world and evolve through interaction with the real environments.In this context,“embodied intelligence”has sparked a new wave of research and technology,leading AI beyond the digital realm into a new paradigm that can actively act and perceive in a physical environment through tangible entities such as robots and automated devices[5].

Synthesis of Petroleum Sulfonate Surfactant by Different Sulfonating Agent with Application of HIGEE Technology

With the application of HIGEE process intensification technology, petroleum sulfonate surfactant used for enhanced oil recovery was synthesized from petroleum fraction of Shengli crude oil with three sulfonating agents, including diluted liquid sulfur trioxide, diluted gaseous sulfur trioxide and fuming sulfuric acid. For each sulfonating agent, different operation modes (liquid-liquid or gas-liquid reaction with semi-continuous or continuous operation) were applied. The effects of various experimental conditions, such as solvent/oil mass ratio, sulfonating agent/oil mass ratio, gas/liquid ratio, gas concentration, reaction temperature, rotating speed, circulation ratio, reaction time and aging time, on the content of active matter and unsulfonated oil were investigated. Under relatively optimal reaction conditions, the target product was prepared with high mass content of active matter (up to 45.3%) and extremely low oil/water interfacial tension (4.5×10 –3 mN·m –1 ). The product quality and process efficiency are higher compared with traditional sulfonation technology.

Electrolytic Preparation,Structure Characterization and Electro-chemical Performance of NiOOH

NiOOH was prepared by one-step electrolysis of spherical Ni(OH)2 and the effects of electrolysis pa-rameters were examined.The highly pure NiOOH was obtained after electrolysis at a current density of 60mA·g-1 and 30℃ with anodic potential controlled in the range of 1.73—1.85V(vs.Zn/ZnO)for 360min.The NiOOH sam-ples were characterized by X-ray powder diffraction(XRD)and scanning electron microscope(SEM)analysis.Re-sults indicate that the electrolysis product is spherical NiOOH doped with graphite.Charge and discharge tests show that the prepared NiOOH offers a discharge capacity of over 270mAh·g-1 at current density of 30mA·g-1 and can be directly used as cathode material of alkaline Zn/NiOOH batteries.Galvanostatic charge/discharge and cyclic volt-ammetry(CV)tests reveal good cycling reversibility of the NiOOH electrode.

Electrochemical dechlorination of chloroform in neutral aqueous solution on palladium/foam-nickel and palladium/polymeric pyrrole film/foam-nickel electrodes

Electrochemical dechlorination of chloroform in neutral aqueous solution was investigated using palladium-loaded electrodes at ambient temperature. Palladium/foam-nickel （Pd/foam-Ni） and palladium/polymeric pyrrole film/foam-nickel （Pd/PPy/foam-Ni） composite electrodes which provided catalytic surface for reductive dechlorination of chloroform in aqueous solution were prepared using an electrodepositing method. Scanning electron microscope （SEM） micrographs showed that polymeric pyrrole film modified the electrode-surface characteristics and resulted in the uniform dispersion of needle-shaped palladium particles on foam-Ni supporting electrode. The experimental results of dechlorination indicated that the removal efficiency of chloroform and current efficiency in neutral aqueous solution on Pd/PPy/foam-Ni electrode could be up to 36.8% and 33.0% at dechlorination current of 0.1 mA and dechlorination time of 180 min, which is much higher than that of Pd/foam-Ni electrode.

Improving physicochemical characteristics and anaerobic digestion performance of rice straw via ammonia pretreatment at varying concentrations and moisture levels

Rice straw physicochemical characteristics and anaerobic digestion(AD)performance via ammonia pretreatment at varying ammonia concentrations(2%,4%,and 6%)and moisture contents(30%,50%,70%,and 90%)under a mild condition were investigated.The results showed that the ammonia pretreatment effectively damaged the rice straw structure,increased the soluble organic concentration,and improved rice straw hydrolysis and AD performance.After pretreatment,the ester bond and ether bond were ruptured in lignocellulose and the volatile fatty acids(VFAs)were within the range of 1457.81–1823.67 mg·L-1.In addition,ammonia pretreatment had high selectivity on lignin removal,resulting in a maximum lignin removal rate of 50.80%.The highest methane yield of rice straw was 250.34 ml·(g VS)-1 at a 4%ammonia concentration coupled with a 70%moisture content,which was 28.55%higher than that of the control.The result showed that ammonia pretreatment of rice straw is technically suitable to enhance AD performance for further application.

Ozonation of o-phenylenediamine in the presence of hydrogen peroxide by high-gravity technology

The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was employed to create a high-gravity environment in order to enhance ozone-liquid mass transfer rate and possibly improve the degradation rate of o-PDA. The degradation efficiency of o-PDA(η) as well as the overall gas-phase volumetric mass transfer coefficient(KGa) were determined under different operating conditions of H_2O_2 concentration, initial o-PDA concentration, temperature of reaction, initial p H and rotation speed of RSR in attempt to establish the optimal conditions. Chemical oxygen demand reduction rate(rCOD) of wastewater treated at a particular set of conditions was also analyzed. Additionally, the intermediate products of degradation were identified using a gas chromatography-mass spectrometer(GC/MS) to further evaluate the extent of o-PDA degradation as well as establish its possible degradation pathway. Results were validated by comparison with those of sole use of ozone(O_3 process), and it was noted that η, KGa and rCODachieved by O_3/H_2O_2 process was 24.4%,31.6% and 25.2% respectively higher than those of O_3 process, indicating that H_2O_2 can greatly enhance ozonation of o-PDA. This work further demonstrates that an RSR can significantly intensify ozone-liquid mass transfer rate and thus provides a feasible intensification means for the ozonation of o-PDA as well as other recalcitrant organics.