To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and ...To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and waste plastic(HDPE),into a blended coal sample and carried out pyrolysis experiments.The pyrolysis process and the microstructure of char were systematically characterized using various analytical techniques,including thermogravimetric analysis(TGA),X-ray diffraction(XRD)and Raman spectroscopy.Data correlation analysis was performed to reveal the mechanism of carbon structural ordering evolution within the critical temperature range(350−600℃)from colloidal layer formation to semi-coke conversion in coking coal,and to elucidate the regulatory effects of different additives on coal pyrolysis pathways.The results indicate that HDPE releases free radicals during high-temperature pyrolysis,accelerating the pyrolysis reaction and increase the yield of volatile components.Conversely,CTP facilitates pyrolysis at low temperatures through its light components,thereby delaying high-temperature reactions due to the colloidal layer’s effect.XRD results indicate that during the process of pyrolysis,there is a progressive decrease in the interlayer spacing of aromatic layers(d002),while the aromatic ring stacking height(L_(c))and lateral size(L_(a))undergo significant of carbon skeleton ordering.Further comparative reveals that CTP partially suppresses structural ordering at low temperatures,whereas HDPE promotes the condensation and alignment of aromatic clusters via a free radical mechanism.Raman spectroscopy reveals a two-stage reorganization mechanism in the microstructure of the coal char:the decrease in the I_(D)/I_(G)ratio between 350 and 550℃is primarily attributed to the cleavage of aliphatic side chains and cross-linking bonds,leading to a reduction in defective structures;whereas the increase in ID/IG between 550 and 600℃is closely associated with enhanced condensation reactions of aromatic structures.Correlation analysis further demonstrates progressive graphitization during pyrolysis,with a significant positive correlation(R^(2)>0.85)observed between d002 and the full width at half maximum of the G-band(FWHM-G).展开更多
The accelerated shift toward high efficiency and sustainability of the iron and steel is driving the advancement of green,low-carbon and high-quality carbon-containing refractories used for ladles.It is undoubtedly a ...The accelerated shift toward high efficiency and sustainability of the iron and steel is driving the advancement of green,low-carbon and high-quality carbon-containing refractories used for ladles.It is undoubtedly a significant challenge,since the addition of graphite enables refractories to possess superior thermal shock resistance and slag corrosion resistance.To develop low carbon-containing refractories with excellent properties,researchers over the past decades have endeavored to seek additives which can mitigate the adverse effects associated with the decrease in carbon in refractories.These additives can promote the occurrence of various mechanisms about toughening,which depends on inherent properties of additives or reacting with refractories to in situ form different ceramic phases,thereby responding the challenge of low-carbonization in refractories.The latest advances in additives used for low carbon-containing refractories from metal/alloys,oxide,non-oxide and composite powders four aspects were comprehensively overviewed in this review.Oxide additives exhibit a moderate effect on improving thermal shock resistance of refractories but show limited efficacy in improving oxidation resistance.In contrast,non-oxide additives demonstrate remarkable advantages in enhancing both oxidation and slag corrosion resistance.Composite powders combine the advantageous properties of their individual components.These additives often require combination with antioxidants such as Al,Si,or B4C not only to reduce costs but also to achieve optimal properties.Furthermore,future perspectives of these additives are discussed,with the aim of providing useful insights for the continuous progress and practical application of low carbon-containing refractories.展开更多
Background Dietary protein level and amino acid(AA)balance are crucial determinants of animal health and productivity.Supplementing rumen-protected AAs in low-protein diets was considered as an efficient strategy to i...Background Dietary protein level and amino acid(AA)balance are crucial determinants of animal health and productivity.Supplementing rumen-protected AAs in low-protein diets was considered as an efficient strategy to improve the growth performance of ruminants.The colon serves as a crucial conduit for nutrient metabolism during rumen-protected methionine(RPMet)and rumen-protected lysine(RPLys)supplementation,however,it has been challenging to clarify which specific microbiota and their metabolites play a pivotal role in this process.Here,we applied metagenomic and metabolomic approaches to compare the characteristic microbiome and metabolic strategies in the colon of lambs fed a control diet(CON),a low-protein diet(LP)or a LP diet supplemented with RPMet and RPLys(LR).Results The LP treatment decreased the average daily weight gain(ADG)in lambs,while the LR treatment tended to elicit a remission in ADG.The butyrate molar concentration was greater(P<0.05),while acetate molar concentration(P<0.05)was lower for lambs fed the LP and LR diets compared to those fed the CON diet.Moreover,the LP treatment remarkably decreased total AA concentration(P<0.05),while LR treatment showed an improvement in the concentrations of methionine,lysine,leucine,glutamate,and tryptophan.Metagenomic insights proved that the microbial metabolic potentials referring to biosynthesis of volatile fatty acids(VFAs)and AAs in the colon were remarkably altered by three dietary treatments.Metagenomic binning identified distinct microbial markers for the CON group(Alistipes spp.,Phocaeicola spp.,and Ruminococcus spp.),LP group(Fibrobacter spp.,Prevotella spp.,Ruminococcus spp.,and Escherichia coli),and LR group(Akkermansia muciniphila and RUG099 spp.).Conclusions Our findings suggest that RPMet and RPLys supplementation to the low-protein diet could enhance the microbial biosynthesis of butyrate and amino acids,enriche the beneficial bacteria in the colon,and thereby improve the growth performance of lambs.展开更多
Aqueous-electrolyte-based zinc-ion batteries(ZIBs),which have significant advantages over other batteries,including low cost,high safety,high ionic conductivity,and a natural abundance of zinc,have been regarded as a ...Aqueous-electrolyte-based zinc-ion batteries(ZIBs),which have significant advantages over other batteries,including low cost,high safety,high ionic conductivity,and a natural abundance of zinc,have been regarded as a potential alternative to lithium-ion batteries(LIBs).ZIBs still face some critical challenges,however,especially for building a reversible zinc anode.To address the reversibility of zinc anode,great efforts have been made on intrinsic anode engineering and anode interface modification.Less attention has been devoted to the electrolyte additives,however,which could not only significantly improve the reversibility of zinc anode,but also determine the viability and overall performance of ZIBs.This review aims to provide an overview of the two main functions of electrolyte additives,followed by details on six reasons why additives might improve the performance of ZIBs from the perspectives of creating new layers and regulating current plating/stripping processes.Furthermore,the remaining difficulties and potential directions for additives in aqueous ZIBs are also highlighted.展开更多
Increasing environmental concerns about limiting harmful emissions has necessitated sulfur-and phosphorus-free green lubricant additives.Although boron-containing compounds have been widely investigated as green lubri...Increasing environmental concerns about limiting harmful emissions has necessitated sulfur-and phosphorus-free green lubricant additives.Although boron-containing compounds have been widely investigated as green lubricant additives,their macromolecular analogs have been rarely considered yet to develop environmentally friendly lubricant additives.In this work,a series of boron-containing copolymers have been synthesized by free-radical copolymerization of stearyl methacrylate and isopropenyl boronic acid pinacol ester with different feeding ratios(S_(n)-r-B_(m),n=1,m=1/3,1,2,3,5,9).The resulting copolymers of S_(n)-r-B_(m)(n=1,m=1/3,1,2,3,5)are readily dispersed in the PAO-10 base oil and form micelle-like aggregates with hydrodynamic diameters ranging from 9.7 to 52 nm.SRV-IV oscillating reciprocating tribological tests on ball-on-flat steel pairs show that compared with the base oil of PAO-10,the friction coefficients and wear volumes of the base oil solutions of S_(n)-r-B_(m)decrease considerably up to 62%and 97%,respectively.Moreover,the base oil solution of S_(1)-r-B_(1)exhibits an excellent load-bearing capacity of(850±100)N.These superior lubricating properties are due to the formation of protective tribofilms comprising S_(n)-r-B_(m),boron oxide,and iron oxide compounds on the lubricated steel surface.Therefore,the boron-containing copolymers can be regarded as a novel class of environmentally friendly lubricating oil macroadditives for efficient friction and wear reduction without sulfur and phosphorus elements.展开更多
The textile industry has long relied on various additives to enhance the properties of fabrics,making them more durable,resistant to stains,and even antimicrobial.These additives include dyes,coatings,flame retardants...The textile industry has long relied on various additives to enhance the properties of fabrics,making them more durable,resistant to stains,and even antimicrobial.These additives include dyes,coatings,flame retardants,and water-repellent finishes.While they offer significant functional benefits,they pose a serious challenge when it comes to recycling textiles.Since many of these additives are chemically bonded to fibres,they make the separation and recovery of pure materials incredibly difficult.展开更多
Chemical looping oxidative dehydrogenation(CL‐ODH)is a promising novel method to convert ethane into higher value‐added ethylene.In this study,perovskite‐type Co_(2)O_(3)/LaCoO_(3) was prepared by the one‐step cit...Chemical looping oxidative dehydrogenation(CL‐ODH)is a promising novel method to convert ethane into higher value‐added ethylene.In this study,perovskite‐type Co_(2)O_(3)/LaCoO_(3) was prepared by the one‐step citric acid‐gel method and applied as an oxygen carrier in the CL‐ODH process of ethane to ethylene;moreover,the effects of CuO,ZnO,and MgO as additives were investigated.The properties of the oxygen carriers were characterized using XRD,BET,XPS,H_(2)‐TPR,O_(2)‐TPD,and EPR.Characterization results showed that the addition of additives into Co_(2)O_(3)/LaCoO_(3) increased the amounts of surface chemisorbed oxygen and lattice oxygen.Co_(2)O_(3)/LaCoO_(3) had a strong ability to absorb and release oxygen after adding CuO,ZnO,and MgO,respectively.The performances of the oxygen carriers for CL‐ODH of ethane to ethylene were studied at a reaction temperature of 650℃,atmospheric pressure,and GHSV of 15,000 mL/g·h in eight redox cycles.All the oxygen carriers had 100%ethane conversion,and ZnO‐Co_(2)O_(3)/LaCoO_(3) exhibited the best ethylene selectivity of more than 70%in all the oxygen carriers.It was confirmed that lattice oxygen was mainly responsible for the selectivity of ethylene,and oxygen vacancies were conducive to the migration of lattice oxygen.Most of Zn^(2+) entered into the bulk phase of Co_(2)O_(3)/LaCoO_(3),and formed lots of oxygen vacancies.展开更多
Lubricating greases are widely used in mechanical engineering,especially in rolling bearing.Carbon-based materials show promise as lubricant additive for formulating high-performance grease.However,the enhancement of ...Lubricating greases are widely used in mechanical engineering,especially in rolling bearing.Carbon-based materials show promise as lubricant additive for formulating high-performance grease.However,the enhancement of lubrication performance of carbon-based materials limits by the simple lubricating mechanism.This work demonstrates that nanocomposite of metal-organic frameworks(MOFs)-derived carbon as a grease additive can improve the tribological properties of bentone grease.HKUST-1 was synthesized by a solvent method and converted into HKUST-1 derived carbon(HDC) via one-step pyrolysis sacrifice template method.After pyrolysis of HKUST-1 at 350℃,Cu_(2+)was reduced to zero-valence copper.With increasing pyrolysis temperature from 350 to 950℃,both the particle size of copper in HDC and the degree of graphite defect increased gradually.Types of HDCs as base grease additives significantly improved friction-reduction and anti-wear performance of bentone grease.Compared with the base grease,HDC-950 ℃ with the amount of 2 wt% addition reduced friction coefficient and wear volume loss by 35.5% and 97.0%,respectively.The superior tribological performance of the HDC-950℃is attributed to the synergistic effect of carbon and copper nanoparticles to induce tribochemical reaction,which form a stable protective film on the friction surfaces.This study highlights the potential of MOFs-derived carbon for developing high-performance grease additives.展开更多
Zwitterionic materials with covalently tethered cations and anions have great potential as electrolyte additives for aqueous Znion batteries(AZIBs)owing to their appealing intrinsic characteristics and merits.However,...Zwitterionic materials with covalently tethered cations and anions have great potential as electrolyte additives for aqueous Znion batteries(AZIBs)owing to their appealing intrinsic characteristics and merits.However,the impact of cationic and anionic moieties within zwitterions on enhancing the performance of AZIBs remains poorly understood.Herein,three zwitterions,namely carboxybetaine methacrylate(CBMA),sulfobetaine methacrylate(SBMA),and 2-methacryloyloxyethyl phosphorylcholine(MPC),were selected as additives to investigate their different action mechanisms in AZIBs.All three zwitterions have the same quaternary ammonium as the positively charged group,but having different negatively charged segments,i.e.,carboxylate,sulfonate,and phosphate for CBMA,SBMA,and MPC,respectively.By systematical electrochemical analysis,these zwitterions all contribute to enhanced cycling life of Zn anode,with MPC having the most pronounced effect,which can be attributed to the synergistic effect of positively quaternary ammonium group and unique negatively phosphate groups.As a result,the Zn//Zn cell with MPC as additive in ZnSO_(4)electrolyte exhibits an ultralong lifespan over 5000 h.This work proposes new insights to the future development of multifunctional zwitterionic additives for remarkably stable AZIBs.展开更多
The fine control of active blend morphologies is crucial to achieve efficient and stable organic solar cells(OSCs).Herein,by introducing structurally simple,non-halogenated volatile solid additives,we have demonstrate...The fine control of active blend morphologies is crucial to achieve efficient and stable organic solar cells(OSCs).Herein,by introducing structurally simple,non-halogenated volatile solid additives,we have demonstrated that the polar 2-naphthonitrile(2-CAN)additives help modulate the kinetics of blend morphological evolution during film drying.It is revealed that 2-CAN favorably interacted with acceptor moieties,and the transition from presence to absence of additives triggered the arrangement and aggregation of acceptors,hence yielding the ordered molecular stacks in the bulk heterojunction(BHJ)blends.Optimal blend morphologies with fibril networks were established to improve the excitonic and charge dynamics of active blends,enabling PM6:L8-BO binary OSCs with the promising efficiency of 19.08%(with 2-CAN),which outperformed that of devices with non-polar naphthalene(NA)additives(18.18%)or without additive treatments(17.43%).Meanwhile,non-halogenated 2-CAN exhibited excellent processing features of reproducibility and versatility toward different active blends for fabricating efficient devices.Such 2-CAN-assisted devices with robust transport layers allowed maintaining decent thermal stabilities under continuous 85℃ of thermal annealing.Overall,this work provides an effective strategy on tuning blend morphologies for efficient organic photovoltaics.展开更多
In the quest to develop high-performance lubrication additives,a novel nanocomposite comprising biodiesel soot modified by silver(Ag/BDS)was synthesized.The tribological behavior of Ag/BDS nanocomposite as an additive...In the quest to develop high-performance lubrication additives,a novel nanocomposite comprising biodiesel soot modified by silver(Ag/BDS)was synthesized.The tribological behavior of Ag/BDS nanocomposite as an additive for liquid paraffin(LP)were systematically investigated using response surface methodology.To elucidate the friction and wear mechanisms associated with the Ag/BDS nanocomposite,various analytical techniques were employed,including scanning electron microscopy with energy-dispersive spectroscopy(SEM/EDS),Raman spectroscopy,and molecular dynamics simulations.The results show that the concentration of Ag/BDS has a significant impact on the tribological properties of LP under different applied loads and sliding speeds.Notably,LP containing 0.25%Ag/BDS shows the most favorable tribological performance and in comparison,to pure LP,the average friction coefficient and average wear volume have been reduced by 42.7%and 21.2%,respectively.The mechanisms underlying the reduction in friction and anti-wear mechanism of Ag/BDS have been attributed to the excellent synergies of Ag and BDS.Specifically,the Ag particles facilitate the incorporation of BDS particles in the formation of uniform boundary lubrication films.展开更多
The performance of organic solar cells is significantly influenced by the acceptor molecular packing properties within the active layers,which is essential for optimizing charge dynamics and photovoltaic performance.H...The performance of organic solar cells is significantly influenced by the acceptor molecular packing properties within the active layers,which is essential for optimizing charge dynamics and photovoltaic performance.However,achieving precise control over this packaging structure presents a considerable challenge.Herein,we propose a dual additive strategy utilizing dibenzofuran and halogenated naphthalene to systematically manipulate molecular packing orientation and enhance the long-range molecular packing order of the acceptors.Dibenzofuran is crucial in promoting crystallinity within the material,facilitating the formation of an ordered structure,while halogenated naphthalene regulates the orientation of the molecules,ensuring proper alignment.Specifically,the combination of dibenzofuran and 1-chloronaphthalene promotes edge-on molecular packing and enhances the formation of nanofibrillar structures with improved order,leading to improved charge transport and device performance.Implementing this strategy in devices composed of PM6 and L8-BO has yielded a power conversion efficiency of 19.58%,accompanied by long-term stability.Similarly,1-fluoronaphthalene has also demonstrated effectiveness in improving molecular orientation and overall device efficiency,demonstrating the robustness of this dual additive strategy.By addressing the challenges associated with molecular packing and orientation in active layers,our result contributes valuable insights into optimizing organic solar cells for practical applications.展开更多
The performance of lithium metal batteries(LMBs)is greatly hampered by the unstable solid electrolyte interphase(SEI)and uncontrollable growth of Li dendrites.To address this question,we developed a weak polar additiv...The performance of lithium metal batteries(LMBs)is greatly hampered by the unstable solid electrolyte interphase(SEI)and uncontrollable growth of Li dendrites.To address this question,we developed a weak polar additive strategy to develop stable and dendrite-free electrolyte for LMBs.In this paper,the effects of additives on the Li^(+)solvation kinetics and the electrode-electrolyte interphases(EEI)formation are discussed.The function of synergistically boosting the superior Li^(+)kinetics and alleviating solvent decomposition on the electrodes is confirmed.From the thermodynamic view,the exothermic process of defluorination reaction for 3,5-difluoropyridine(3,5-DFPy)results in the formation of LiF-rich SEI layer for promoting the uniform Li nucleation and deposition.From the dynamic view,the weakened Li^(+)solvation structure induced by weak polar 3,5-DFPy contributes to better Li^(+)kinetics through the easier Li^(+)desolvation.As expected,Li||Li cell with 1.0 wt%3,5-DFPy exhibits 400 cycles at 1.0 mA cm^(-2)with a deposition capacity of 0.5 mAh cm^(-2),and the Li||LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)batteries delivers the highly reversible capacity after 200 cycles.展开更多
The addition of complexing agents to the electrolyte has been shown to be an effective method to enhance the discharge performance of magnesium-air batteries.In this work,four complexing agents:citric acid(CIT),salicy...The addition of complexing agents to the electrolyte has been shown to be an effective method to enhance the discharge performance of magnesium-air batteries.In this work,four complexing agents:citric acid(CIT),salicylic acid(SAL),2,6-dihydroxybenzoic acid(2,6-DHB),and 5-sulfoisophthalic acid(5-sulfoSAL)were selected as potential candidates.Through electrochemical tests,full-cell discharge experiments,and physicochemical characterization,the impact of these complexing agents on the discharge performance of magnesium-air batteries using AZ31 alloy as the anode material was investigated.The results demonstrated that the four complexing agents increased the discharge voltage of the batteries.Notably,SAL could significantly improve the anodic efficiency and the discharge specific capacity,achieving an anodic efficiency of 60.3%and a specific capacity of 1358.3 mA·h/g at a discharge current density of 10 mA/cm^(2).展开更多
Organic additives with multiple functional groups have shown great promise in improving the performance and stability of perovskite solar cells.The functional groups can passivate undercoordinated ions to reduce nonra...Organic additives with multiple functional groups have shown great promise in improving the performance and stability of perovskite solar cells.The functional groups can passivate undercoordinated ions to reduce nonradiative recombination losses.However,how these groups synergistically affect the enhancement beyond passivation is still unclear.Specifically,isomeric molecules with different substitution patterns or molecular shapes remain elusive in designing new organic additives.Here,we report two isomeric carbazolyl bisphosphonate additives,2,7-Cz BP and 3,6-Cz BP.The isomerism effect on passivation and charge transport process was studied.The two molecules have similar passivation effects through multiple interactions,e.g.,P=O···Pb,P=O···H–N and N–H···I.2,7-CzBP can further bridge the perovskite crystallites to facilitates charge transport.Power conversion efficiencies(PCEs)of 25.88%and 21.04%were achieved for 0.09 cm^(2)devices and 14 cm^(2)modules after 2,7-Cz BP treatment,respectively.The devices exhibited enhanced operational stability maintaining 95%of initial PCE after 1000 h of continuous maximum power point tracking.This study of isomerism effect hints at the importance of tuning substitution positions and molecular shapes for organic additives,which paves the way for innovation of next-generation multifunctional aromatic additives.展开更多
Unstable Zn interface caused by rampant dendrite growth and parasitic side reactions always hinders the practical application of aqueous zinc metal batteries(AZMBs),Herein,tyrosine(Tyr)with high molecular polarity was...Unstable Zn interface caused by rampant dendrite growth and parasitic side reactions always hinders the practical application of aqueous zinc metal batteries(AZMBs),Herein,tyrosine(Tyr)with high molecular polarity was introduced into aqueous electrolyte to modulate the interfacial electrochemistry of Zn anode.In AZMBs,the positively charged side of Tyr can be well adsorbed on the surface of Zn anode to form a water-poor layer,and the exposed carboxylate side can be easily coordinated with Zn^(2+),favoring inducing uniform plating of Zn^(2+)and inhibiting the occurrence of water-induced side reactions.These in turn enable the achievement of highly stable Zn anode.Accordingly,the Zn anodes achieve outstanding cyclic stability(3000 h at 2 mA cm^(-2),2 mA h cm^(-2)and 1300 h at 5 mA cm^(-2),5 mA h cm^(-2)),high average Coulombic efficiency(99.4%over 3200 cycles),and high depth of discharge(80%for 500 h).Besides,the assembled Zn‖NaV_(3)O_(8)·1.5H_(2)O full cells deliver remarkable capacity retention and ultra-long lifetime(61.8%over 6650 cycles at 5 A g^(-1))and enhanced rate capability(169 mA h g^(-1)at 5 A g^(-1)).The work may promote the design and deep understanding of electrolyte additives with high molecular polarity for high-performance AZMBs.展开更多
The manipulation of crystallization and healing defects by introducing additives to prepare high-quality perovskite(PVK)films is crucial for achieving efficient and stable perovskite solar cells(PSCs).However,the inte...The manipulation of crystallization and healing defects by introducing additives to prepare high-quality perovskite(PVK)films is crucial for achieving efficient and stable perovskite solar cells(PSCs).However,the intermolecular interactions of the additives,which may affect their modulation of the quality of the PVK films as well as the performance of PSCs,are neglected.In this work,two benzimidazole-based additives with different intermolecular interactions,5-chloro-1-[1-[3-(2,3-dihydro-2-oxo-1H-benzimidazol-1-yl)propyl]piperidin-4-yl]-1,3-dihydro-2H-benzimidazol-2-one(DOM)and 5-chloro-1-(4-piperidinyl)-2-benzimidazolinone(CPBI),are introduced into the PVK precursor to explore the impact of the own intermolecular interactions of additives on their functions.After a detailed investigation,the results demonstrate that the weaker interactions between DOM molecules than those between CPBI molecules enable the stronger binding of DOM with PbI_(2) precursor and(110)plane of PVK than that of CPBI,which induces a significantly slow crystallization of PVK with preferentially oriented growth and a high passivation effect on defects after DOM introduction.The PVK films with DOM additives also exhibit a distinctly enhanced residual strain release compared with the CPBI-treated films and energy level matching that of the carbon electrode.Consequently,the DOM-treated carbon-based PSCs without encapsulation prepared in air achieve a remarkable power conversion efficiency of 17.30%and excellent stability with 86%efficiency retention after 1000 h storage in air.This work provides an insight into understanding the effect of the intermolecular interactions of additives on affecting the quality regulation and defect passivation of PVK films.展开更多
Organic solar cells(OSCs)have emerged as promising candidates for next‐generation photovoltaics,yet traditional bulk heterojunction(BHJ)devices face inherent limitations in morphology control and phase separation.La...Organic solar cells(OSCs)have emerged as promising candidates for next‐generation photovoltaics,yet traditional bulk heterojunction(BHJ)devices face inherent limitations in morphology control and phase separation.Layer‐by‐layer(LbL)processing with a p–i–n configuration offers an innovative solution by enabling precise control over donor–acceptor distribution and interfacial characteristics.Here,we systematically investigate nine halogen‐functionalized additives across three categories—methyl halides,thiophene halides,and benzene halides—for optimizing LbL device performance.These additives,distinguished by their diverse thermal properties and solid–liquid transformation capabilities below 100°C,are functionalized as both nucleation centers and morphology‐modulating plasticizers during thermal treatment.Among them,2‐bromo‐5‐iodothiophene(BIT)demonstrates superior performance through synergistic effects of its bromine–iodine combination and thiophene core in mediating donor–acceptor interactions.LbL devices processed with BIT achieve exceptional metrics in the PM6/L8‐BO system,including a open‐circuit voltage of 0.916 V,a short‐circuit current density of 27.12 mA cm−2,and an fill factor of 80.97%,resulting in an impressive power conversion efficiency of 20.12%.This study establishes a molecular design strategy for halogen‐functionalized additives that simultaneously optimizes both donor and acceptor layers while maintaining processing simplicity for potential industrial applications.展开更多
Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prep...Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prepared,and the influence mechanism of additives on the structure-performance relationship of the catalysts was systematically explored.Through a variety of characterization methods such as XRD,N2 physical adsorption-desorption,TEM,H_(2)-TPR,CO_(2)-TPD and XPS,combined with catalytic performance evaluation experiments,the correlation between the microstructure of catalysts and the reaction performance of CO_(2)hydrogenation to methanol was analyzed in depth.The results show that metal additives significantly improve the performance of catalysts.After the introduction of additives,the specific surface area and pore volume of the catalysts increase,the grain size of Cu decreases,and its dispersion improves.The Ce-modified CZC catalyst exhibited the best performance,with the grain size of CuO as small as 11.41 nm,and the surface oxygen vacancy concentration(OⅡ/OⅠ=3.15)was significantly higher than that of other samples.The reaction performance test shows that under the conditions of 2.8 MPa,8000 h−1 and 280℃,the CO_(2)conversion of the CZC catalyst reached 18.83%,the methanol selectivity was 68.40%,and the methanol yield was 12.88%,all of which are superior to other catalysts.Its excellent performance can be attributed to the fact that CeO_(2)enhances the metal-support interaction,increases the surface basicity,promotes the adsorption and activation of CO_(2),and simultaneously inhibits the reverse water-gas shift side reaction.This study clarifies the structure-activity regulation mechanism of additive modification on Cu-ZnO catalysts,providing a theoretical basis and technical reference for the development of efficient catalysts for CO_(2)hydrogenation to methanol.展开更多
Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-li...Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-lithiation additives is a challenging research hotspot.Herein,interfacial engineered multifunctional Li_(13)Si_(4)@perfluoropolyether(PFPE)/LiF micro/nanoparticles are proposed as anode pre-lithiation additives,successfully constructed with the hybrid interface on the surface of Li_(13)Si_(4)through PFPE-induced nucleophilic substitution.The synthesized multifunctional Li_(13)Si_(4)@PFPE/LiF realizes the integration of active Li compensation,long-term chemical structural stability in air,and solid electrolyte interface(SEI)optimization.In particular,the Li_(13)Si_(4)@PFPE/LiF with a high pre-lithiation capacity(1102.4 mAh g^(-1))is employed in the pre-lithiation Si-based anode,which exhibits a superior initial Coulombic efficiency of 102.6%.Additionally,in situ X-ray diffraction/Raman,density functional theory calculation,and finite element analysis jointly illustrate that PFPE-predominant hybrid interface with modulated abundant highly electronegative F atoms distribution reduces the water adsorption energy and oxidation kinetics of Li_(13)Si_(4)@PFPE/LiF,which delivers a high pre-lithiation capacity retention of 84.39%after exposure to extremely moist air(60%relative humidity).Intriguingly,a LiF-rich mechanically stable bilayer SEI is constructed on anodes through a pre-lithiation-driven regulation for the behavior of electrolyte decomposition.Benefitting from pre-lithiation via multifunctional Li_(13)Si_(4)@PFPE/LiF,the full cell and pouch cell assembled with pre-lithiated anodes operate with long-time stability of 86.5%capacity retention over 200 cycles and superior energy density of 549.9 Wh kg^(-1),respectively.The universal multifunctional pre-lithiation additives provide enlightenment on promoting large-scale applications of pre-lithiation on commercial high-energy-density and long-cycle-life lithium-ion batteries.展开更多
基金Supported by National Natural Science Foundation of China(22378180,22078141)Education Department Foundation of Liaoning Province(JYTMS20230960)。
文摘To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and waste plastic(HDPE),into a blended coal sample and carried out pyrolysis experiments.The pyrolysis process and the microstructure of char were systematically characterized using various analytical techniques,including thermogravimetric analysis(TGA),X-ray diffraction(XRD)and Raman spectroscopy.Data correlation analysis was performed to reveal the mechanism of carbon structural ordering evolution within the critical temperature range(350−600℃)from colloidal layer formation to semi-coke conversion in coking coal,and to elucidate the regulatory effects of different additives on coal pyrolysis pathways.The results indicate that HDPE releases free radicals during high-temperature pyrolysis,accelerating the pyrolysis reaction and increase the yield of volatile components.Conversely,CTP facilitates pyrolysis at low temperatures through its light components,thereby delaying high-temperature reactions due to the colloidal layer’s effect.XRD results indicate that during the process of pyrolysis,there is a progressive decrease in the interlayer spacing of aromatic layers(d002),while the aromatic ring stacking height(L_(c))and lateral size(L_(a))undergo significant of carbon skeleton ordering.Further comparative reveals that CTP partially suppresses structural ordering at low temperatures,whereas HDPE promotes the condensation and alignment of aromatic clusters via a free radical mechanism.Raman spectroscopy reveals a two-stage reorganization mechanism in the microstructure of the coal char:the decrease in the I_(D)/I_(G)ratio between 350 and 550℃is primarily attributed to the cleavage of aliphatic side chains and cross-linking bonds,leading to a reduction in defective structures;whereas the increase in ID/IG between 550 and 600℃is closely associated with enhanced condensation reactions of aromatic structures.Correlation analysis further demonstrates progressive graphitization during pyrolysis,with a significant positive correlation(R^(2)>0.85)observed between d002 and the full width at half maximum of the G-band(FWHM-G).
基金support of the National Natural Science Foundation of China(Grant/Project Nos.52272027,52372034 and 52502016)the China Postdoctoral Science Foundation(Grant No.2025T180025)Postdoctoral Fellowship Program(Grant No.GZC20252393).
文摘The accelerated shift toward high efficiency and sustainability of the iron and steel is driving the advancement of green,low-carbon and high-quality carbon-containing refractories used for ladles.It is undoubtedly a significant challenge,since the addition of graphite enables refractories to possess superior thermal shock resistance and slag corrosion resistance.To develop low carbon-containing refractories with excellent properties,researchers over the past decades have endeavored to seek additives which can mitigate the adverse effects associated with the decrease in carbon in refractories.These additives can promote the occurrence of various mechanisms about toughening,which depends on inherent properties of additives or reacting with refractories to in situ form different ceramic phases,thereby responding the challenge of low-carbonization in refractories.The latest advances in additives used for low carbon-containing refractories from metal/alloys,oxide,non-oxide and composite powders four aspects were comprehensively overviewed in this review.Oxide additives exhibit a moderate effect on improving thermal shock resistance of refractories but show limited efficacy in improving oxidation resistance.In contrast,non-oxide additives demonstrate remarkable advantages in enhancing both oxidation and slag corrosion resistance.Composite powders combine the advantageous properties of their individual components.These additives often require combination with antioxidants such as Al,Si,or B4C not only to reduce costs but also to achieve optimal properties.Furthermore,future perspectives of these additives are discussed,with the aim of providing useful insights for the continuous progress and practical application of low carbon-containing refractories.
基金jointly supported by the International Partnership Program of Chinese Academy of Sciences(161343KYSB20200015)Guangxi Provincial Natural Science Foundation of China(2023GXNSFAA026107)+1 种基金the Science and Technology Innovation Program of Hunan Province(2022RC1158)Youth Innovation Promotion Association CAS(2023382)。
文摘Background Dietary protein level and amino acid(AA)balance are crucial determinants of animal health and productivity.Supplementing rumen-protected AAs in low-protein diets was considered as an efficient strategy to improve the growth performance of ruminants.The colon serves as a crucial conduit for nutrient metabolism during rumen-protected methionine(RPMet)and rumen-protected lysine(RPLys)supplementation,however,it has been challenging to clarify which specific microbiota and their metabolites play a pivotal role in this process.Here,we applied metagenomic and metabolomic approaches to compare the characteristic microbiome and metabolic strategies in the colon of lambs fed a control diet(CON),a low-protein diet(LP)or a LP diet supplemented with RPMet and RPLys(LR).Results The LP treatment decreased the average daily weight gain(ADG)in lambs,while the LR treatment tended to elicit a remission in ADG.The butyrate molar concentration was greater(P<0.05),while acetate molar concentration(P<0.05)was lower for lambs fed the LP and LR diets compared to those fed the CON diet.Moreover,the LP treatment remarkably decreased total AA concentration(P<0.05),while LR treatment showed an improvement in the concentrations of methionine,lysine,leucine,glutamate,and tryptophan.Metagenomic insights proved that the microbial metabolic potentials referring to biosynthesis of volatile fatty acids(VFAs)and AAs in the colon were remarkably altered by three dietary treatments.Metagenomic binning identified distinct microbial markers for the CON group(Alistipes spp.,Phocaeicola spp.,and Ruminococcus spp.),LP group(Fibrobacter spp.,Prevotella spp.,Ruminococcus spp.,and Escherichia coli),and LR group(Akkermansia muciniphila and RUG099 spp.).Conclusions Our findings suggest that RPMet and RPLys supplementation to the low-protein diet could enhance the microbial biosynthesis of butyrate and amino acids,enriche the beneficial bacteria in the colon,and thereby improve the growth performance of lambs.
基金supported by a Discovery Early Career Researcher Award (DECRA,No.DE180101478) of the Australian Research CouncilNational Natural Science Foundation of China (Youth Program,No.52204378).
文摘Aqueous-electrolyte-based zinc-ion batteries(ZIBs),which have significant advantages over other batteries,including low cost,high safety,high ionic conductivity,and a natural abundance of zinc,have been regarded as a potential alternative to lithium-ion batteries(LIBs).ZIBs still face some critical challenges,however,especially for building a reversible zinc anode.To address the reversibility of zinc anode,great efforts have been made on intrinsic anode engineering and anode interface modification.Less attention has been devoted to the electrolyte additives,however,which could not only significantly improve the reversibility of zinc anode,but also determine the viability and overall performance of ZIBs.This review aims to provide an overview of the two main functions of electrolyte additives,followed by details on six reasons why additives might improve the performance of ZIBs from the perspectives of creating new layers and regulating current plating/stripping processes.Furthermore,the remaining difficulties and potential directions for additives in aqueous ZIBs are also highlighted.
文摘Increasing environmental concerns about limiting harmful emissions has necessitated sulfur-and phosphorus-free green lubricant additives.Although boron-containing compounds have been widely investigated as green lubricant additives,their macromolecular analogs have been rarely considered yet to develop environmentally friendly lubricant additives.In this work,a series of boron-containing copolymers have been synthesized by free-radical copolymerization of stearyl methacrylate and isopropenyl boronic acid pinacol ester with different feeding ratios(S_(n)-r-B_(m),n=1,m=1/3,1,2,3,5,9).The resulting copolymers of S_(n)-r-B_(m)(n=1,m=1/3,1,2,3,5)are readily dispersed in the PAO-10 base oil and form micelle-like aggregates with hydrodynamic diameters ranging from 9.7 to 52 nm.SRV-IV oscillating reciprocating tribological tests on ball-on-flat steel pairs show that compared with the base oil of PAO-10,the friction coefficients and wear volumes of the base oil solutions of S_(n)-r-B_(m)decrease considerably up to 62%and 97%,respectively.Moreover,the base oil solution of S_(1)-r-B_(1)exhibits an excellent load-bearing capacity of(850±100)N.These superior lubricating properties are due to the formation of protective tribofilms comprising S_(n)-r-B_(m),boron oxide,and iron oxide compounds on the lubricated steel surface.Therefore,the boron-containing copolymers can be regarded as a novel class of environmentally friendly lubricating oil macroadditives for efficient friction and wear reduction without sulfur and phosphorus elements.
文摘The textile industry has long relied on various additives to enhance the properties of fabrics,making them more durable,resistant to stains,and even antimicrobial.These additives include dyes,coatings,flame retardants,and water-repellent finishes.While they offer significant functional benefits,they pose a serious challenge when it comes to recycling textiles.Since many of these additives are chemically bonded to fibres,they make the separation and recovery of pure materials incredibly difficult.
基金The funding of this submission came from our laboratory sponsored by the college
文摘Chemical looping oxidative dehydrogenation(CL‐ODH)is a promising novel method to convert ethane into higher value‐added ethylene.In this study,perovskite‐type Co_(2)O_(3)/LaCoO_(3) was prepared by the one‐step citric acid‐gel method and applied as an oxygen carrier in the CL‐ODH process of ethane to ethylene;moreover,the effects of CuO,ZnO,and MgO as additives were investigated.The properties of the oxygen carriers were characterized using XRD,BET,XPS,H_(2)‐TPR,O_(2)‐TPD,and EPR.Characterization results showed that the addition of additives into Co_(2)O_(3)/LaCoO_(3) increased the amounts of surface chemisorbed oxygen and lattice oxygen.Co_(2)O_(3)/LaCoO_(3) had a strong ability to absorb and release oxygen after adding CuO,ZnO,and MgO,respectively.The performances of the oxygen carriers for CL‐ODH of ethane to ethylene were studied at a reaction temperature of 650℃,atmospheric pressure,and GHSV of 15,000 mL/g·h in eight redox cycles.All the oxygen carriers had 100%ethane conversion,and ZnO‐Co_(2)O_(3)/LaCoO_(3) exhibited the best ethylene selectivity of more than 70%in all the oxygen carriers.It was confirmed that lattice oxygen was mainly responsible for the selectivity of ethylene,and oxygen vacancies were conducive to the migration of lattice oxygen.Most of Zn^(2+) entered into the bulk phase of Co_(2)O_(3)/LaCoO_(3),and formed lots of oxygen vacancies.
基金financially supported by National Natural Science Foundations of China(No.52475216)the National Key Research and Development Program of China(No.2023YFE0206300)+1 种基金the Natural Science Foundation of Shaanxi Province(No.2024RS-CXTD-62)the Research Fund of the State Key Laboratory of Solidification Processing(NPU)(No.2022-QZ04)
文摘Lubricating greases are widely used in mechanical engineering,especially in rolling bearing.Carbon-based materials show promise as lubricant additive for formulating high-performance grease.However,the enhancement of lubrication performance of carbon-based materials limits by the simple lubricating mechanism.This work demonstrates that nanocomposite of metal-organic frameworks(MOFs)-derived carbon as a grease additive can improve the tribological properties of bentone grease.HKUST-1 was synthesized by a solvent method and converted into HKUST-1 derived carbon(HDC) via one-step pyrolysis sacrifice template method.After pyrolysis of HKUST-1 at 350℃,Cu_(2+)was reduced to zero-valence copper.With increasing pyrolysis temperature from 350 to 950℃,both the particle size of copper in HDC and the degree of graphite defect increased gradually.Types of HDCs as base grease additives significantly improved friction-reduction and anti-wear performance of bentone grease.Compared with the base grease,HDC-950 ℃ with the amount of 2 wt% addition reduced friction coefficient and wear volume loss by 35.5% and 97.0%,respectively.The superior tribological performance of the HDC-950℃is attributed to the synergistic effect of carbon and copper nanoparticles to induce tribochemical reaction,which form a stable protective film on the friction surfaces.This study highlights the potential of MOFs-derived carbon for developing high-performance grease additives.
基金supported by the Australian Research Council(LP220100036)the National Key Research and Development Program(2022YFB2502104 and 2022YFA1602700)+3 种基金the Key Research and Development Program of Jiangsu Provincial Department of Science and Technology of China(BE2022332)the Jiangsu Carbon Peak Carbon Neutralization Science and Technology Innovation Special Fund(BE2022605)the Australian Research Council for his Discovery Early Career Researcher Award fellowship(DE230101105)the China Scholarship Council(CSC,grant no.202306190185)for funding a scholarship。
文摘Zwitterionic materials with covalently tethered cations and anions have great potential as electrolyte additives for aqueous Znion batteries(AZIBs)owing to their appealing intrinsic characteristics and merits.However,the impact of cationic and anionic moieties within zwitterions on enhancing the performance of AZIBs remains poorly understood.Herein,three zwitterions,namely carboxybetaine methacrylate(CBMA),sulfobetaine methacrylate(SBMA),and 2-methacryloyloxyethyl phosphorylcholine(MPC),were selected as additives to investigate their different action mechanisms in AZIBs.All three zwitterions have the same quaternary ammonium as the positively charged group,but having different negatively charged segments,i.e.,carboxylate,sulfonate,and phosphate for CBMA,SBMA,and MPC,respectively.By systematical electrochemical analysis,these zwitterions all contribute to enhanced cycling life of Zn anode,with MPC having the most pronounced effect,which can be attributed to the synergistic effect of positively quaternary ammonium group and unique negatively phosphate groups.As a result,the Zn//Zn cell with MPC as additive in ZnSO_(4)electrolyte exhibits an ultralong lifespan over 5000 h.This work proposes new insights to the future development of multifunctional zwitterionic additives for remarkably stable AZIBs.
基金funded by the National Natural Science Foundation of China(No.22125901)the National Key Research and Development Program of China(No.2019YFA0705900)+1 种基金the Fundamental Research Funds for the Central Universities(226-2024-00005)the Scientific Research Project of China Three Gorges Corporation(202303014)。
文摘The fine control of active blend morphologies is crucial to achieve efficient and stable organic solar cells(OSCs).Herein,by introducing structurally simple,non-halogenated volatile solid additives,we have demonstrated that the polar 2-naphthonitrile(2-CAN)additives help modulate the kinetics of blend morphological evolution during film drying.It is revealed that 2-CAN favorably interacted with acceptor moieties,and the transition from presence to absence of additives triggered the arrangement and aggregation of acceptors,hence yielding the ordered molecular stacks in the bulk heterojunction(BHJ)blends.Optimal blend morphologies with fibril networks were established to improve the excitonic and charge dynamics of active blends,enabling PM6:L8-BO binary OSCs with the promising efficiency of 19.08%(with 2-CAN),which outperformed that of devices with non-polar naphthalene(NA)additives(18.18%)or without additive treatments(17.43%).Meanwhile,non-halogenated 2-CAN exhibited excellent processing features of reproducibility and versatility toward different active blends for fabricating efficient devices.Such 2-CAN-assisted devices with robust transport layers allowed maintaining decent thermal stabilities under continuous 85℃ of thermal annealing.Overall,this work provides an effective strategy on tuning blend morphologies for efficient organic photovoltaics.
基金funded by the National Natural Science Foundation of China(52075141)the Open Project of Anhui Province Key Laboratory of Critical Friction Pair for Advanced Equipment(LCFP-2408)+9 种基金Key Research&Development(R&D)Plan of Anhui Province under Grant(2022a05020019)Support Program for Outstanding Young Talents in Anhui Province Colleges and Universities(gxyq2022079)Excellent Research and Innovation Teams Project of Anhui Province's Universities(2022AH010092)Discipline Construction Quality Improvement Project of Chaohu University(kj22fdzy03,XLZ202307,XLZ202301)School-level Scientific Research Project of Chaohu University(XLY-202112)Scientific Research Planning Project of Anhui Provincial(2022AH051726)Anhui Province University Science and Engineering Teachers'Internship Program in Enterprises(2024jsqygz89)Anhui Province College Students'Innovation and Entrepreneurship Training Program(S202410380020)Anhui Province Postdoctoral Research Project(2024A773)Horizontal Research Project of Chaohu University(hxkt20230006).
文摘In the quest to develop high-performance lubrication additives,a novel nanocomposite comprising biodiesel soot modified by silver(Ag/BDS)was synthesized.The tribological behavior of Ag/BDS nanocomposite as an additive for liquid paraffin(LP)were systematically investigated using response surface methodology.To elucidate the friction and wear mechanisms associated with the Ag/BDS nanocomposite,various analytical techniques were employed,including scanning electron microscopy with energy-dispersive spectroscopy(SEM/EDS),Raman spectroscopy,and molecular dynamics simulations.The results show that the concentration of Ag/BDS has a significant impact on the tribological properties of LP under different applied loads and sliding speeds.Notably,LP containing 0.25%Ag/BDS shows the most favorable tribological performance and in comparison,to pure LP,the average friction coefficient and average wear volume have been reduced by 42.7%and 21.2%,respectively.The mechanisms underlying the reduction in friction and anti-wear mechanism of Ag/BDS have been attributed to the excellent synergies of Ag and BDS.Specifically,the Ag particles facilitate the incorporation of BDS particles in the formation of uniform boundary lubrication films.
基金the financial support from the National Natural Science Foundation of China(62275057)the Guangxi Natural Science Foundation(2023GXNSFFA026004)+2 种基金the Guangxi Talent Program("Highland of Innovation Talents")the Shenzhen High-tech Development Special Plan-Pingshan Districts Innovation Platform Project(29853M-KCJ-2023-002-04)Industry and Energy(MOTIE),Republic of Korea(Project No.:RS-2025-02413058)。
文摘The performance of organic solar cells is significantly influenced by the acceptor molecular packing properties within the active layers,which is essential for optimizing charge dynamics and photovoltaic performance.However,achieving precise control over this packaging structure presents a considerable challenge.Herein,we propose a dual additive strategy utilizing dibenzofuran and halogenated naphthalene to systematically manipulate molecular packing orientation and enhance the long-range molecular packing order of the acceptors.Dibenzofuran is crucial in promoting crystallinity within the material,facilitating the formation of an ordered structure,while halogenated naphthalene regulates the orientation of the molecules,ensuring proper alignment.Specifically,the combination of dibenzofuran and 1-chloronaphthalene promotes edge-on molecular packing and enhances the formation of nanofibrillar structures with improved order,leading to improved charge transport and device performance.Implementing this strategy in devices composed of PM6 and L8-BO has yielded a power conversion efficiency of 19.58%,accompanied by long-term stability.Similarly,1-fluoronaphthalene has also demonstrated effectiveness in improving molecular orientation and overall device efficiency,demonstrating the robustness of this dual additive strategy.By addressing the challenges associated with molecular packing and orientation in active layers,our result contributes valuable insights into optimizing organic solar cells for practical applications.
基金supported by the National Natural Science Foundation of China(U21A20311)Researchers Supporting Project Number(RSP2025R304),King Saud University,Riyadh,Saudi Arabia。
文摘The performance of lithium metal batteries(LMBs)is greatly hampered by the unstable solid electrolyte interphase(SEI)and uncontrollable growth of Li dendrites.To address this question,we developed a weak polar additive strategy to develop stable and dendrite-free electrolyte for LMBs.In this paper,the effects of additives on the Li^(+)solvation kinetics and the electrode-electrolyte interphases(EEI)formation are discussed.The function of synergistically boosting the superior Li^(+)kinetics and alleviating solvent decomposition on the electrodes is confirmed.From the thermodynamic view,the exothermic process of defluorination reaction for 3,5-difluoropyridine(3,5-DFPy)results in the formation of LiF-rich SEI layer for promoting the uniform Li nucleation and deposition.From the dynamic view,the weakened Li^(+)solvation structure induced by weak polar 3,5-DFPy contributes to better Li^(+)kinetics through the easier Li^(+)desolvation.As expected,Li||Li cell with 1.0 wt%3,5-DFPy exhibits 400 cycles at 1.0 mA cm^(-2)with a deposition capacity of 0.5 mAh cm^(-2),and the Li||LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)batteries delivers the highly reversible capacity after 200 cycles.
基金supported by the National Natural Science Foundation of China(No.52001015)the Urban Carbon Neutral Science Innovation Foundation of Beijing University of Technology,China(No.053000514124601)the Science and Technology Program of Beijing Municipal Education Commission,China(No.KM201810005007).
文摘The addition of complexing agents to the electrolyte has been shown to be an effective method to enhance the discharge performance of magnesium-air batteries.In this work,four complexing agents:citric acid(CIT),salicylic acid(SAL),2,6-dihydroxybenzoic acid(2,6-DHB),and 5-sulfoisophthalic acid(5-sulfoSAL)were selected as potential candidates.Through electrochemical tests,full-cell discharge experiments,and physicochemical characterization,the impact of these complexing agents on the discharge performance of magnesium-air batteries using AZ31 alloy as the anode material was investigated.The results demonstrated that the four complexing agents increased the discharge voltage of the batteries.Notably,SAL could significantly improve the anodic efficiency and the discharge specific capacity,achieving an anodic efficiency of 60.3%and a specific capacity of 1358.3 mA·h/g at a discharge current density of 10 mA/cm^(2).
基金financially supported by the National Science Foundation of China(62474142)Natural Science Foundation of Shandong Province(No.ZR2024YQ070)。
文摘Organic additives with multiple functional groups have shown great promise in improving the performance and stability of perovskite solar cells.The functional groups can passivate undercoordinated ions to reduce nonradiative recombination losses.However,how these groups synergistically affect the enhancement beyond passivation is still unclear.Specifically,isomeric molecules with different substitution patterns or molecular shapes remain elusive in designing new organic additives.Here,we report two isomeric carbazolyl bisphosphonate additives,2,7-Cz BP and 3,6-Cz BP.The isomerism effect on passivation and charge transport process was studied.The two molecules have similar passivation effects through multiple interactions,e.g.,P=O···Pb,P=O···H–N and N–H···I.2,7-CzBP can further bridge the perovskite crystallites to facilitates charge transport.Power conversion efficiencies(PCEs)of 25.88%and 21.04%were achieved for 0.09 cm^(2)devices and 14 cm^(2)modules after 2,7-Cz BP treatment,respectively.The devices exhibited enhanced operational stability maintaining 95%of initial PCE after 1000 h of continuous maximum power point tracking.This study of isomerism effect hints at the importance of tuning substitution positions and molecular shapes for organic additives,which paves the way for innovation of next-generation multifunctional aromatic additives.
基金the financial support from the Foshan Talents Special Foundation(BKBS202003).
文摘Unstable Zn interface caused by rampant dendrite growth and parasitic side reactions always hinders the practical application of aqueous zinc metal batteries(AZMBs),Herein,tyrosine(Tyr)with high molecular polarity was introduced into aqueous electrolyte to modulate the interfacial electrochemistry of Zn anode.In AZMBs,the positively charged side of Tyr can be well adsorbed on the surface of Zn anode to form a water-poor layer,and the exposed carboxylate side can be easily coordinated with Zn^(2+),favoring inducing uniform plating of Zn^(2+)and inhibiting the occurrence of water-induced side reactions.These in turn enable the achievement of highly stable Zn anode.Accordingly,the Zn anodes achieve outstanding cyclic stability(3000 h at 2 mA cm^(-2),2 mA h cm^(-2)and 1300 h at 5 mA cm^(-2),5 mA h cm^(-2)),high average Coulombic efficiency(99.4%over 3200 cycles),and high depth of discharge(80%for 500 h).Besides,the assembled Zn‖NaV_(3)O_(8)·1.5H_(2)O full cells deliver remarkable capacity retention and ultra-long lifetime(61.8%over 6650 cycles at 5 A g^(-1))and enhanced rate capability(169 mA h g^(-1)at 5 A g^(-1)).The work may promote the design and deep understanding of electrolyte additives with high molecular polarity for high-performance AZMBs.
基金financial supports from the National Natural Science Foundation of China(52472259,22179051)the Natural Science Foundation of Shandong Province(ZR2021ME037)+1 种基金the Special Fund of Taishan Scholar Program of Shandong Province(tsqnz20221141)the Foundation of Key Laboratory of Advanced Technique&Preparation for Renewable Energy Materials,Ministry of Education,Yunnan Normal University(OF2022-02)。
文摘The manipulation of crystallization and healing defects by introducing additives to prepare high-quality perovskite(PVK)films is crucial for achieving efficient and stable perovskite solar cells(PSCs).However,the intermolecular interactions of the additives,which may affect their modulation of the quality of the PVK films as well as the performance of PSCs,are neglected.In this work,two benzimidazole-based additives with different intermolecular interactions,5-chloro-1-[1-[3-(2,3-dihydro-2-oxo-1H-benzimidazol-1-yl)propyl]piperidin-4-yl]-1,3-dihydro-2H-benzimidazol-2-one(DOM)and 5-chloro-1-(4-piperidinyl)-2-benzimidazolinone(CPBI),are introduced into the PVK precursor to explore the impact of the own intermolecular interactions of additives on their functions.After a detailed investigation,the results demonstrate that the weaker interactions between DOM molecules than those between CPBI molecules enable the stronger binding of DOM with PbI_(2) precursor and(110)plane of PVK than that of CPBI,which induces a significantly slow crystallization of PVK with preferentially oriented growth and a high passivation effect on defects after DOM introduction.The PVK films with DOM additives also exhibit a distinctly enhanced residual strain release compared with the CPBI-treated films and energy level matching that of the carbon electrode.Consequently,the DOM-treated carbon-based PSCs without encapsulation prepared in air achieve a remarkable power conversion efficiency of 17.30%and excellent stability with 86%efficiency retention after 1000 h storage in air.This work provides an insight into understanding the effect of the intermolecular interactions of additives on affecting the quality regulation and defect passivation of PVK films.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFB4200500)National Natural Science Foundation of China(NSFC,22379101 and 22422904)Sichuan Natural Science Foundation(2024NSFSC0001 and 2025ZNSFSC0960).
文摘Organic solar cells(OSCs)have emerged as promising candidates for next‐generation photovoltaics,yet traditional bulk heterojunction(BHJ)devices face inherent limitations in morphology control and phase separation.Layer‐by‐layer(LbL)processing with a p–i–n configuration offers an innovative solution by enabling precise control over donor–acceptor distribution and interfacial characteristics.Here,we systematically investigate nine halogen‐functionalized additives across three categories—methyl halides,thiophene halides,and benzene halides—for optimizing LbL device performance.These additives,distinguished by their diverse thermal properties and solid–liquid transformation capabilities below 100°C,are functionalized as both nucleation centers and morphology‐modulating plasticizers during thermal treatment.Among them,2‐bromo‐5‐iodothiophene(BIT)demonstrates superior performance through synergistic effects of its bromine–iodine combination and thiophene core in mediating donor–acceptor interactions.LbL devices processed with BIT achieve exceptional metrics in the PM6/L8‐BO system,including a open‐circuit voltage of 0.916 V,a short‐circuit current density of 27.12 mA cm−2,and an fill factor of 80.97%,resulting in an impressive power conversion efficiency of 20.12%.This study establishes a molecular design strategy for halogen‐functionalized additives that simultaneously optimizes both donor and acceptor layers while maintaining processing simplicity for potential industrial applications.
基金Supported by National Key R&D Program of China(2022YFA1503400)。
文摘Aiming at the problems of insufficient activity and selectivity of Cu-based catalysts in CO_(2)hydrogenation to methanol,Al_(2)O_(3),ZrO_(2)and CeO_(2)modified Cu-ZnO catalysts by the co-precipitation method were prepared,and the influence mechanism of additives on the structure-performance relationship of the catalysts was systematically explored.Through a variety of characterization methods such as XRD,N2 physical adsorption-desorption,TEM,H_(2)-TPR,CO_(2)-TPD and XPS,combined with catalytic performance evaluation experiments,the correlation between the microstructure of catalysts and the reaction performance of CO_(2)hydrogenation to methanol was analyzed in depth.The results show that metal additives significantly improve the performance of catalysts.After the introduction of additives,the specific surface area and pore volume of the catalysts increase,the grain size of Cu decreases,and its dispersion improves.The Ce-modified CZC catalyst exhibited the best performance,with the grain size of CuO as small as 11.41 nm,and the surface oxygen vacancy concentration(OⅡ/OⅠ=3.15)was significantly higher than that of other samples.The reaction performance test shows that under the conditions of 2.8 MPa,8000 h−1 and 280℃,the CO_(2)conversion of the CZC catalyst reached 18.83%,the methanol selectivity was 68.40%,and the methanol yield was 12.88%,all of which are superior to other catalysts.Its excellent performance can be attributed to the fact that CeO_(2)enhances the metal-support interaction,increases the surface basicity,promotes the adsorption and activation of CO_(2),and simultaneously inhibits the reverse water-gas shift side reaction.This study clarifies the structure-activity regulation mechanism of additive modification on Cu-ZnO catalysts,providing a theoretical basis and technical reference for the development of efficient catalysts for CO_(2)hydrogenation to methanol.
基金Huaiyu Shao acknowledges the Shenzhen-Hong Kong-Macao Science and Technology Plan Project(Category C)(Grant No.SGDX20220530111004028)the Macao Science and Technology Development Fund(FDCT)for funding(FDCT No.0013/2024/RIB1,FDCT-MOST joint project No.0026/2022/AMJ and No.006/2022/ALC of the Macao Centre for Research and Development in Advanced Materials[2022–2024])+2 种基金the Multi-Year Research Grant(MYRG)from University of Macao(project No.MYRG-GRG2023-00140-IAPME-UMDF and No.MYRG-GRG2024-00206-IAPME)Natural Science Foundation of Guangdong Province(Grant No.2023A1515010765)Science and Technology Program of Guangdong Province of China(Grant No.2023A0505030001)。
文摘Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment,developing effective and environmentally stable pre-lithiation additives is a challenging research hotspot.Herein,interfacial engineered multifunctional Li_(13)Si_(4)@perfluoropolyether(PFPE)/LiF micro/nanoparticles are proposed as anode pre-lithiation additives,successfully constructed with the hybrid interface on the surface of Li_(13)Si_(4)through PFPE-induced nucleophilic substitution.The synthesized multifunctional Li_(13)Si_(4)@PFPE/LiF realizes the integration of active Li compensation,long-term chemical structural stability in air,and solid electrolyte interface(SEI)optimization.In particular,the Li_(13)Si_(4)@PFPE/LiF with a high pre-lithiation capacity(1102.4 mAh g^(-1))is employed in the pre-lithiation Si-based anode,which exhibits a superior initial Coulombic efficiency of 102.6%.Additionally,in situ X-ray diffraction/Raman,density functional theory calculation,and finite element analysis jointly illustrate that PFPE-predominant hybrid interface with modulated abundant highly electronegative F atoms distribution reduces the water adsorption energy and oxidation kinetics of Li_(13)Si_(4)@PFPE/LiF,which delivers a high pre-lithiation capacity retention of 84.39%after exposure to extremely moist air(60%relative humidity).Intriguingly,a LiF-rich mechanically stable bilayer SEI is constructed on anodes through a pre-lithiation-driven regulation for the behavior of electrolyte decomposition.Benefitting from pre-lithiation via multifunctional Li_(13)Si_(4)@PFPE/LiF,the full cell and pouch cell assembled with pre-lithiated anodes operate with long-time stability of 86.5%capacity retention over 200 cycles and superior energy density of 549.9 Wh kg^(-1),respectively.The universal multifunctional pre-lithiation additives provide enlightenment on promoting large-scale applications of pre-lithiation on commercial high-energy-density and long-cycle-life lithium-ion batteries.
