Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and u...Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The common hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.展开更多
The continual growth in transportation fuels and more strict environmental legislations have led to immense interest in developing green biomass energy. In this work, a proposed catalytic transformation of oxygenated ...The continual growth in transportation fuels and more strict environmental legislations have led to immense interest in developing green biomass energy. In this work, a proposed catalytic transformation of oxygenated organic compounds (related to bio-oil) into pure hydrogen was desighed, involving the catalytic reforming of oxygenated organic compounds to hydrogen- rich mixture gas followed by the conversion of CO to CO2 via the water gas reaction and the removal of CO2. The optimization of the different reforming catalyst, the reaction conditions as well as various sources of oxygenated organic compounds were investigated in detail. The production of pure hydrogen, with the H2 content up to 99.96% and the conversion of 97.1%, was achieved by the integrated catalytic transformation. The reaction pathways were addressed based on the investigation of decomposition, catalytic reforming, and the water gas reaction.展开更多
The experiments were carried out at the Post Graduate Research Center, to study the influence of Gibberellic Acid (50 ppm) and Oxygenated Peptone (1% aqueous solution) on chick pea (Cicer arietinum L. cv. Vijay) durin...The experiments were carried out at the Post Graduate Research Center, to study the influence of Gibberellic Acid (50 ppm) and Oxygenated Peptone (1% aqueous solution) on chick pea (Cicer arietinum L. cv. Vijay) during germination by giving pre-sowing soaking treatment for 6 hours using petriplate method. Both the treatments enhanced the germination process. GA treatment was useful to increase shoot length, mobilization efficiency, emergence index, speed of germination and co-efficient of germination while oxygenated peptone showed an upper hand in root length, shoot/root ratio, biomass and vigour index. GA led to comparatively more synthesis of nucleic acids while oxygenated peptone showed more increase in total carbohydrates and soluble protein content. However, the activity of enzymes like amylase, catalase and protease showed upper hand with oxygenated peptone as compared to GA. In fact GA is costlier and can not be used in organic farming as it enters metabolic pathways of plant and alters them. Hence the use of oxygenated peptone is recommended being less expensive and usable under organic farming condition as it does not enter the plant metabolic pathways and yet brings about significant positive effect.展开更多
Based on Core GGC-6 from the South China Sea (SCS) and Core GGC-29 from the Sulu Sea,planktonic and benthic foraminifera and organic carbon measurements were used to evaluate the Water mass conditions in these sea are...Based on Core GGC-6 from the South China Sea (SCS) and Core GGC-29 from the Sulu Sea,planktonic and benthic foraminifera and organic carbon measurements were used to evaluate the Water mass conditions in these sea areas during the last glacial age. The results show that the higher organic carbon contents in the SCS and Sulu Sea during the last glacial period were mainly caused by low dissolved oxygen concentrations in bottom waters and that in the last glacial to Holocene, the fluctuation of dissolvd oxygen in the bottom weters was large in the SCS and reatively stable in the Sulu Sea. In addition, increased precipitation reduced surface water salinities, which at the water column to be more stratified in the SCS and Sulu Sea during the last glacial period. This process lowered dissolved oxygen concentrations in bottom waters, which resulted in better preservation of organic matter in both basins.展开更多
Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozz...Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozzle and an open tube. Mixtures were prepared using nano-aluminum(n-Al),potassium perchlorate(KClO_(4)), and different carbon nanomaterials(CNMs) including graphene-oxide(GO), reduced GO, carbon nanotubes(CNTs) and nanofibers(CNFs). The mixtures were packed at different densities and ignited by laser beam. Performance was measured using thrust measurement,high-speed imaging, and computational fluid dynamics modeling, respectively. Thrust, specific impulse(ISP), volumetric impulse(ISV), as well as normalized energy were found to increase notably with CNM content. Two distinctive reaction regimes(fast and slow) were observed in combustion of low and high packing densities(20% and 55%TMD), respectively. Total impulse(IFT) and ISPwere maximized in the 5%GO/Al/KClO_4 mixture, producing 7.95 m N·s and 135.20 s respectively at 20%TMD, an improvement of 57%compared to a GO-free sample(5.05 m N·s and 85.88 s). CFD analysis of the motors over predicts the thrust generated but trends in nozzle layout and packing density agree with those observed experimentally;peak force was maximized by reducing packing density and using an open tube. The numerical force profiles fit better for the nozzle cases than the open tube scenarios due to the rapid nature of combustion. This study reveals the potential of GO in improving oxygenated salt-based nanothermites,and further demonstrates their applicability for micro-propulsion and micro-energetic applications.展开更多
A new highly oxygenated iridoid,lamiophlomiol C,was isolated from the roots of Lamiophlomis rotata and its structure was elucidated by spectrosoopic techniques and X-ray diffraction.
<span style="font-family:Verdana;">The objective of this study was to evaluate the effect of blends of different oxygenated additives on gasoline in SI engine Otto cycle. The formulations analyzed were...<span style="font-family:Verdana;">The objective of this study was to evaluate the effect of blends of different oxygenated additives on gasoline in SI engine Otto cycle. The formulations analyzed were: pure gasoline (type A), common gasoline (type C), gasoline type A + 15% (v/v) oxygenated additives (ethanol, ethyl octanoate, ethyl oleate). The experiments were performed using engine Branco 4-stroke and 2-cylinder, electric dynamometer, exhaust system, control unit composed of Multi-K unit, variable selector and load cell, stroboscope tachometer, fuel supply system and stopwatch. The rotation was conserved at 4400 rpm and wheel power varied from 3 kW to 12 kW, with intervals of 3 kW to obtain hourly consumption curves and brake specific fuel consumption. Even esters and ethanol having lower heat of combustion, hourly consumption was similar to pure gasoline (type A). In relation to the brake specific fuel consumption, increasing the wheel power had a better conversion of the mass of fuel burned into energy. Thus, this study showed that the mixture of gasoline and esters (ethyl octanoate and ethyl oleate) presented good efficiency in terms of consumption. This research contributes to the needs and to the current studi</span><span style="font-family:Verdana;">es in which industries started to add renewable products to petroleum-</span><span style="font-family:Verdana;">derived fuels;in order to obtain more sustainable fuels at lower costs.</span>展开更多
Oxygenated organic molecules(OOMs)play an important role in the formation of secondary organic aerosols(SOAs),but the mixing states of OOMs are still unclear.This study investigates the mixing states of OOM-containing...Oxygenated organic molecules(OOMs)play an important role in the formation of secondary organic aerosols(SOAs),but the mixing states of OOMs are still unclear.This study investigates the mixing states of OOM-containing single particles from the measurements taken using a single particle aerosol mass spectrometer in Guangzhou,China in 2022.Generally,the particle counts of OOM particles and the mass concentration of secondary organic carbon(SOC)exhibited similar temporal trends throughout the entire year.The OOM particles were consistently enriched in secondary ions,including ^(16)O^(−),^(26)CN^(−),^(46)NO_(2)^(−),^(62)NO_(3)^(−),and ^(97)HSO_(4)^(−).In contrast,the number fractions and diurnal patterns of OOM particles among the total detected particles showed similar distributions in August and October;however,the SOC ratios in fine particulate matter were quite different,suggesting that there were different mixing states of single-particle oxygenated organics.In addition,further classification results indicated that the OOM particles were more aged in October than August,even though the SOC ratios were higher in August.Furthermore,the distribution of hydrocarbon fragments exhibited a notable decrease from January to October,emphasizing the more aged state of the organics in October.In addition,the sharp increase in elemental carbon(EC)-OOM particles in the afternoon in October suggests the potential role of EC in the aging process of organics.Overall,in contrast to the bulk analysis of SOC mass concentration,the mixing states of the OOM particles provide insights into the formation process of SOAs in field studies.展开更多
Lithium(Li)-metal batteries with polymer electrolytes are promising for high-energy-density and safe energy storage applications.However,current polymer electrolytes suffer either low ionic conductivity or inadequate ...Lithium(Li)-metal batteries with polymer electrolytes are promising for high-energy-density and safe energy storage applications.However,current polymer electrolytes suffer either low ionic conductivity or inadequate ability to suppress Li dendrite growth at high current densities.This study addresses both issues by incorporating two-dimensional oxygenated carbon nitride(2D OCN)into a polyvinylidene fluoride(PVDF)-based composite polymer electrolyte and modifying the Li anode with OCN.The OCN nanosheets incorporated PVDF electrolyte exhibits a high ionic conductivity(1.6×10^(-4)S cm^(-1)at 25℃)and Li+transference number(0.62),wide electrochemical window(5.3),and excellent fire resistance.Furthermore,the OCN-modified Li anode in situ generates a protective layer of Li_(3)N during cycling,preventing undesirable reactions with PVDF electrolyte and effectively suppressing Li dendrite growth.Symmetric cells using the upgraded PVDF polymer electrolyte and modified Li anode demonstrate long cycling stability over 2500 h at 0.1 mA cm^(-2).Full cells with a high-voltage LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode exhibit high energy density and long-term cycling stability,even at a high loading of 8.2 mg cm^(-2).Incorporating 2D OCN nanosheets into the PVDF-based electrolyte and Li-metal anode provides an effective strategy for achieving safe and high-energy-density Li-metal batteries.展开更多
Cardiac arrest can lead to severe neurological impairment as a result of inflammation,mitochondrial dysfunction,and post-cardiopulmonary resuscitation neurological damage.Hypoxic preconditioning has been shown to impr...Cardiac arrest can lead to severe neurological impairment as a result of inflammation,mitochondrial dysfunction,and post-cardiopulmonary resuscitation neurological damage.Hypoxic preconditioning has been shown to improve migration and survival of bone marrow–derived mesenchymal stem cells and reduce pyroptosis after cardiac arrest,but the specific mechanisms by which hypoxia-preconditioned bone marrow–derived mesenchymal stem cells protect against brain injury after cardiac arrest are unknown.To this end,we established an in vitro co-culture model of bone marrow–derived mesenchymal stem cells and oxygen–glucose deprived primary neurons and found that hypoxic preconditioning enhanced the protective effect of bone marrow stromal stem cells against neuronal pyroptosis,possibly through inhibition of the MAPK and nuclear factor κB pathways.Subsequently,we transplanted hypoxia-preconditioned bone marrow–derived mesenchymal stem cells into the lateral ventricle after the return of spontaneous circulation in an 8-minute cardiac arrest rat model induced by asphyxia.The results showed that hypoxia-preconditioned bone marrow–derived mesenchymal stem cells significantly reduced cardiac arrest–induced neuronal pyroptosis,oxidative stress,and mitochondrial damage,whereas knockdown of the liver isoform of phosphofructokinase in bone marrow–derived mesenchymal stem cells inhibited these effects.To conclude,hypoxia-preconditioned bone marrow–derived mesenchymal stem cells offer a promising therapeutic approach for neuronal injury following cardiac arrest,and their beneficial effects are potentially associated with increased expression of the liver isoform of phosphofructokinase following hypoxic preconditioning.展开更多
Oxygenated volatile organic compounds(OVOCs) emitted from orange wastes during aerobic decomposition were investigated in a laboratory-controlled incubator for a period of two months. Emission of total OVOCs(TOVOCs...Oxygenated volatile organic compounds(OVOCs) emitted from orange wastes during aerobic decomposition were investigated in a laboratory-controlled incubator for a period of two months. Emission of total OVOCs(TOVOCs) from orange wastes reached 1714 mg/dry kg(330 mg/wet kg). Ethanol, methanol, ethyl acetate, methyl acetate, 2-butanone and acetaldehyde were the most abundant OVOC species with shares of 26.9%, 24.8%, 20.3%, 13.9%, 2.8%and 2.5%, respectively, in the TOVOCs released. The emission fluxes of the above top five OVOCs were quite trivial in the beginning but increased sharply to form one "peak emission window" with maximums at days 1-8 until leveling off after 10 days. This type of "peak emission window" was synchronized with the CO2 fluxes and incubation temperature of the orange wastes, indicating that released OVOCs were mainly derived from secondary metabolites of orange substrates through biotic processes rather than abiotic processes or primary volatilization of the inherent pool in oranges. Acetaldehyde instead had emission fluxes decreasing sharply from its initial maximum to nearly zero in about four days,suggesting that it was inherent rather than secondarily formed. For TOVOCs or all OVOC species except 2-butanone and acetone, over 80% of their emissions occurred during the first week, implying that organic wastes might give off a considerable amount of OVOCs during the early disposal period under aerobic conditions.展开更多
Biofuels have extensive available resources and have an immense potential as promising alternative fuels for automobile.The application advantages of biofuels are mainly reflected as particulate matter(PM)reduction,ca...Biofuels have extensive available resources and have an immense potential as promising alternative fuels for automobile.The application advantages of biofuels are mainly reflected as particulate matter(PM)reduction,carbon neutral,greenhouse gases reduction,waste utilization,energy and economic security,and fuel pluralism.Based on the understanding of molecular structure effects of biofuels on soot formation and particles morphology,the effects of alcohols,ethers,esters and biodiesel on spray and combustion process in constant volume bomb in recent years are retrospectively analyzed in this paper.For the mixture,macromolecular ester fuels and polyoxymethylene dimethyl ether(PODE)are conducive to the improvement of liquid spray,while biodiesel,small molecules,dimethyl ether(DME)and alcohols are reversed.Alcohols are advantageous to the extension of mixing time and the increasing of vapor-phase mixture.Through the influence integrated assessment,alcohols show the best performance on the spray,atomization and combustion,while biodiesels show the worst.But in terms of combustion,PODE is the best choice without considering spray and atomization.For binary alternative-diesel fuel blends,methanol or butanol is the best additive based on synthetically considerations on spray,atomization and combustion.To meet the requirements of the fuel application of diesel engine,ternary fuel or even quaternary fuel have been proposed and explored.This review can help to form a systematic understanding on fuel recombining and obtain the guide of clean and efficient fuel formulation for diesel engine.展开更多
The direct electrochemical synthesis of H_(2)O_(2)from O_(2)is currently the most promising alternative to energyintensive industrial anthraquinone oxidation/reduction methods. However, its widespread use is hampered ...The direct electrochemical synthesis of H_(2)O_(2)from O_(2)is currently the most promising alternative to energyintensive industrial anthraquinone oxidation/reduction methods. However, its widespread use is hampered by the lack of efficient low-cost electrocatalysts. In the current study,oxygenated boron-doped carbon(O-BC) materials were realized via a green synthetic strategy involving polymer dehalogenation and employed as electrode materials for the electrochemical synthesis of H_(2)O_(2)via a 2 e-oxygen reduction.The catalytic activity of the O-BC materials was optimized through systematic variation of the boron source(H_(2)BO_(2))dosage and annealing temperature. Electrochemical measurements revealed that the optimal sample(O-BC-2-650)exhibited a selectivity of 98% for the 2 e-oxygen reduction to H2 O_(2)and an average H_(2)O_(2)production rate of412.8 mmol g_(cat)^(-1) h^(-1)in an H-type alkaline electrolyzer. Density functional theory simulations indicated that the functionalization of active B sites with one oxygen atom provides the lowest Gibbs free energy change(ΔG) of 0.03 e V for the hydrogenation of*O_(2), while functionalization with zero or two O atoms results in much larger ΔG values(0.08 and 0.10 e V,respectively). Thus, this work details a new type of green, lowcost, and metal-free electrocatalyst for H_(2)O_(2)production.展开更多
In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for ...In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.展开更多
Oxygenated fuels are known to reduce particulate matter(PM)emissions from diesel engines.In this study,100%soy methyl ester(SME)biodiesel fuel(B100)and a blend of 10%acetal denoted by A-diesel with diesel fuel were te...Oxygenated fuels are known to reduce particulate matter(PM)emissions from diesel engines.In this study,100%soy methyl ester(SME)biodiesel fuel(B100)and a blend of 10%acetal denoted by A-diesel with diesel fuel were tested as oxygenated fuels.Particle size and number distributions from a diesel engine fueled with oxygenated fuels and base diesel fuel were measured using an Electrical Low Pressure Impactor(ELPI).Measurements were made at ten steady-state operational modes of various loads at two engine speeds.It was found that the geometric mean diameters of particles from SME and Adiesel were lower than that from base diesel fuel.Compared to diesel fuel,SME emitted more ultra-fine particles at rated speed while emitting less ultra-fine particles at maximum speed.Ultra-fine particle number concentrations of A-diesel were much higher than those of base diesel fuel at most test modes.展开更多
Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree c...Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere(NCS)decorated with dual-phase Co/Co_(7)Fe_(3)heterojunctions(CoFe@NCS).The phase composition of materials has been adjusted by controlling the alloying degree.The optimal CoFe_(0.08)@NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm^(-2)for OER in an alkaline electrolyte.The intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co_(7)Fe_(3)alloy and metallic Co species.When the CoFe_(0.08)@NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery(ZAB),the device shows a high peak power-density(157 mW·cm^(-2))and maintains a stable voltage gap over 150 h,outperforming those of the benchmark(Pt/C+RuO_(2))-based device.In particular,the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending conditions.Our work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.展开更多
Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3...Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.展开更多
Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by ...Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.展开更多
Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction.The surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has ...Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction.The surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity enhancement.Here,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is reported.The substituting Fe content influences both current change tendency and surface reconstruction degree.LaNi_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)series.The reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based catalysts.Besides,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term stability.Furthermore,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction degree.The effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface reconstruction.This finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.展开更多
Although poly(lactic acid)(PLA)is a good environmentally-friendly bio-degradable polymer which is used to substitute traditional petrochemical-based polymer packaging films,the barrier properties of PLA films are stil...Although poly(lactic acid)(PLA)is a good environmentally-friendly bio-degradable polymer which is used to substitute traditional petrochemical-based polymer packaging films,the barrier properties of PLA films are still insufficient for high-barrier packaging applications.In this study,oxygen scavenger hydroxyl-terminated polybutadiene(HTPB)and cobalt salt catalyst were incorporated into the PLA/poly(butylene adipate-co-terephthalate)(PLA/PBAT),followed by melting extrusion and three-layer co-extrusion blown film process to prepare the composite films.The oxygen permeability coefficient of the composite film combined with 6 wt%oxygen scavenger and 0.4 wt%catalyst was decreased significantly from 377.00 cc·mil·m^(-2)·day^(-1)·0.1 MPa^(-1) to 0.98 cc·mil·m^(-2)·day^(-1)·0.1 MPa^(-1),showing a remarkable enhancement of 384.69 times compared with the PLA/PBAT composite film.Meanwhile,the degradation behavior of the composite film was also accelerated,exhibiting a mass loss of nearly 60%of the original mass after seven days of degradation in an alkaline environment,whereas PLA/PBAT composite film only showed a mass loss of 32%.This work has successfully prepared PLA/PBAT composite films with simultaneously improved oxygen barrier property and degradation behavior,which has great potential for high-demanding green chemistry packaging industries,including food,agricultural,and military packaging.展开更多
基金supported by the National Natural Science Foundation of China(No.52171022,No.22105214)Zhejiang Provincial Natural Science Foundation of China(Grant No.LXR22B030001)+3 种基金Fujian Institute of Innovation and Chinese Academy of Sciences.K.C.Wong Education Foundation(GJTD-2019-13)the National Key Research and Development Program of China(2019YFB2203400)Ningbo Yongjiang Talent Introduction Programme(2021A-036-B)NingBo S&T Innovation 2025 Major Special Programme(No:2020z059)and the“111 Project”(B20030).
文摘Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The common hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.
文摘The continual growth in transportation fuels and more strict environmental legislations have led to immense interest in developing green biomass energy. In this work, a proposed catalytic transformation of oxygenated organic compounds (related to bio-oil) into pure hydrogen was desighed, involving the catalytic reforming of oxygenated organic compounds to hydrogen- rich mixture gas followed by the conversion of CO to CO2 via the water gas reaction and the removal of CO2. The optimization of the different reforming catalyst, the reaction conditions as well as various sources of oxygenated organic compounds were investigated in detail. The production of pure hydrogen, with the H2 content up to 99.96% and the conversion of 97.1%, was achieved by the integrated catalytic transformation. The reaction pathways were addressed based on the investigation of decomposition, catalytic reforming, and the water gas reaction.
文摘The experiments were carried out at the Post Graduate Research Center, to study the influence of Gibberellic Acid (50 ppm) and Oxygenated Peptone (1% aqueous solution) on chick pea (Cicer arietinum L. cv. Vijay) during germination by giving pre-sowing soaking treatment for 6 hours using petriplate method. Both the treatments enhanced the germination process. GA treatment was useful to increase shoot length, mobilization efficiency, emergence index, speed of germination and co-efficient of germination while oxygenated peptone showed an upper hand in root length, shoot/root ratio, biomass and vigour index. GA led to comparatively more synthesis of nucleic acids while oxygenated peptone showed more increase in total carbohydrates and soluble protein content. However, the activity of enzymes like amylase, catalase and protease showed upper hand with oxygenated peptone as compared to GA. In fact GA is costlier and can not be used in organic farming as it enters metabolic pathways of plant and alters them. Hence the use of oxygenated peptone is recommended being less expensive and usable under organic farming condition as it does not enter the plant metabolic pathways and yet brings about significant positive effect.
文摘Based on Core GGC-6 from the South China Sea (SCS) and Core GGC-29 from the Sulu Sea,planktonic and benthic foraminifera and organic carbon measurements were used to evaluate the Water mass conditions in these sea areas during the last glacial age. The results show that the higher organic carbon contents in the SCS and Sulu Sea during the last glacial period were mainly caused by low dissolved oxygen concentrations in bottom waters and that in the last glacial to Holocene, the fluctuation of dissolvd oxygen in the bottom weters was large in the SCS and reatively stable in the Sulu Sea. In addition, increased precipitation reduced surface water salinities, which at the water column to be more stratified in the SCS and Sulu Sea during the last glacial period. This process lowered dissolved oxygen concentrations in bottom waters, which resulted in better preservation of organic matter in both basins.
基金financial funding from the Egyptian governmentthe financial funding from the NSERC Discovery grant。
文摘Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozzle and an open tube. Mixtures were prepared using nano-aluminum(n-Al),potassium perchlorate(KClO_(4)), and different carbon nanomaterials(CNMs) including graphene-oxide(GO), reduced GO, carbon nanotubes(CNTs) and nanofibers(CNFs). The mixtures were packed at different densities and ignited by laser beam. Performance was measured using thrust measurement,high-speed imaging, and computational fluid dynamics modeling, respectively. Thrust, specific impulse(ISP), volumetric impulse(ISV), as well as normalized energy were found to increase notably with CNM content. Two distinctive reaction regimes(fast and slow) were observed in combustion of low and high packing densities(20% and 55%TMD), respectively. Total impulse(IFT) and ISPwere maximized in the 5%GO/Al/KClO_4 mixture, producing 7.95 m N·s and 135.20 s respectively at 20%TMD, an improvement of 57%compared to a GO-free sample(5.05 m N·s and 85.88 s). CFD analysis of the motors over predicts the thrust generated but trends in nozzle layout and packing density agree with those observed experimentally;peak force was maximized by reducing packing density and using an open tube. The numerical force profiles fit better for the nozzle cases than the open tube scenarios due to the rapid nature of combustion. This study reveals the potential of GO in improving oxygenated salt-based nanothermites,and further demonstrates their applicability for micro-propulsion and micro-energetic applications.
文摘A new highly oxygenated iridoid,lamiophlomiol C,was isolated from the roots of Lamiophlomis rotata and its structure was elucidated by spectrosoopic techniques and X-ray diffraction.
文摘<span style="font-family:Verdana;">The objective of this study was to evaluate the effect of blends of different oxygenated additives on gasoline in SI engine Otto cycle. The formulations analyzed were: pure gasoline (type A), common gasoline (type C), gasoline type A + 15% (v/v) oxygenated additives (ethanol, ethyl octanoate, ethyl oleate). The experiments were performed using engine Branco 4-stroke and 2-cylinder, electric dynamometer, exhaust system, control unit composed of Multi-K unit, variable selector and load cell, stroboscope tachometer, fuel supply system and stopwatch. The rotation was conserved at 4400 rpm and wheel power varied from 3 kW to 12 kW, with intervals of 3 kW to obtain hourly consumption curves and brake specific fuel consumption. Even esters and ethanol having lower heat of combustion, hourly consumption was similar to pure gasoline (type A). In relation to the brake specific fuel consumption, increasing the wheel power had a better conversion of the mass of fuel burned into energy. Thus, this study showed that the mixture of gasoline and esters (ethyl octanoate and ethyl oleate) presented good efficiency in terms of consumption. This research contributes to the needs and to the current studi</span><span style="font-family:Verdana;">es in which industries started to add renewable products to petroleum-</span><span style="font-family:Verdana;">derived fuels;in order to obtain more sustainable fuels at lower costs.</span>
基金supported by the National Natural Science Foundation of China(Grant Nos.41827804 and 41805093)the Natural Science Foundation of Guangdong Province(China)(No.2021A1515011206)+1 种基金the State Key Laboratory of Marine Resource Utilization in the South China Sea,Hainan University(China)(No.MRUKF2023009)the State Key Laboratory of Loess and Quaternary Geology,Institute of Earth Environment,CAS(No.SKLLQG2218).
文摘Oxygenated organic molecules(OOMs)play an important role in the formation of secondary organic aerosols(SOAs),but the mixing states of OOMs are still unclear.This study investigates the mixing states of OOM-containing single particles from the measurements taken using a single particle aerosol mass spectrometer in Guangzhou,China in 2022.Generally,the particle counts of OOM particles and the mass concentration of secondary organic carbon(SOC)exhibited similar temporal trends throughout the entire year.The OOM particles were consistently enriched in secondary ions,including ^(16)O^(−),^(26)CN^(−),^(46)NO_(2)^(−),^(62)NO_(3)^(−),and ^(97)HSO_(4)^(−).In contrast,the number fractions and diurnal patterns of OOM particles among the total detected particles showed similar distributions in August and October;however,the SOC ratios in fine particulate matter were quite different,suggesting that there were different mixing states of single-particle oxygenated organics.In addition,further classification results indicated that the OOM particles were more aged in October than August,even though the SOC ratios were higher in August.Furthermore,the distribution of hydrocarbon fragments exhibited a notable decrease from January to October,emphasizing the more aged state of the organics in October.In addition,the sharp increase in elemental carbon(EC)-OOM particles in the afternoon in October suggests the potential role of EC in the aging process of organics.Overall,in contrast to the bulk analysis of SOC mass concentration,the mixing states of the OOM particles provide insights into the formation process of SOAs in field studies.
基金National Key Research and Development Program of China,Grant/Award Number:2023YFB2503801National Natural Science Foundation of China,Grant/Award Numbers:52302253,5202780089+2 种基金Fundamental Research Funds for the Central Universities,Grant/Award Number:HUST:2172020kfyXJJS089Key R&D Program of Hubei Province,Grant/Award Number:2023BAB028Key Program of the National Natural Science Foundation of China,Grant/Award Number:52231009。
文摘Lithium(Li)-metal batteries with polymer electrolytes are promising for high-energy-density and safe energy storage applications.However,current polymer electrolytes suffer either low ionic conductivity or inadequate ability to suppress Li dendrite growth at high current densities.This study addresses both issues by incorporating two-dimensional oxygenated carbon nitride(2D OCN)into a polyvinylidene fluoride(PVDF)-based composite polymer electrolyte and modifying the Li anode with OCN.The OCN nanosheets incorporated PVDF electrolyte exhibits a high ionic conductivity(1.6×10^(-4)S cm^(-1)at 25℃)and Li+transference number(0.62),wide electrochemical window(5.3),and excellent fire resistance.Furthermore,the OCN-modified Li anode in situ generates a protective layer of Li_(3)N during cycling,preventing undesirable reactions with PVDF electrolyte and effectively suppressing Li dendrite growth.Symmetric cells using the upgraded PVDF polymer electrolyte and modified Li anode demonstrate long cycling stability over 2500 h at 0.1 mA cm^(-2).Full cells with a high-voltage LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)cathode exhibit high energy density and long-term cycling stability,even at a high loading of 8.2 mg cm^(-2).Incorporating 2D OCN nanosheets into the PVDF-based electrolyte and Li-metal anode provides an effective strategy for achieving safe and high-energy-density Li-metal batteries.
基金supported by the Natural Science Fund of Fujian Province,No.2020J011058(to JK)the Project of Fujian Provincial Hospital for High-level Hospital Construction,No.2020HSJJ12(to JK)+1 种基金the Fujian Provincial Finance Department Special Fund,No.(2021)848(to FC)the Fujian Provincial Major Scientific and Technological Special Projects on Health,No.2022ZD01008(to FC).
文摘Cardiac arrest can lead to severe neurological impairment as a result of inflammation,mitochondrial dysfunction,and post-cardiopulmonary resuscitation neurological damage.Hypoxic preconditioning has been shown to improve migration and survival of bone marrow–derived mesenchymal stem cells and reduce pyroptosis after cardiac arrest,but the specific mechanisms by which hypoxia-preconditioned bone marrow–derived mesenchymal stem cells protect against brain injury after cardiac arrest are unknown.To this end,we established an in vitro co-culture model of bone marrow–derived mesenchymal stem cells and oxygen–glucose deprived primary neurons and found that hypoxic preconditioning enhanced the protective effect of bone marrow stromal stem cells against neuronal pyroptosis,possibly through inhibition of the MAPK and nuclear factor κB pathways.Subsequently,we transplanted hypoxia-preconditioned bone marrow–derived mesenchymal stem cells into the lateral ventricle after the return of spontaneous circulation in an 8-minute cardiac arrest rat model induced by asphyxia.The results showed that hypoxia-preconditioned bone marrow–derived mesenchymal stem cells significantly reduced cardiac arrest–induced neuronal pyroptosis,oxidative stress,and mitochondrial damage,whereas knockdown of the liver isoform of phosphofructokinase in bone marrow–derived mesenchymal stem cells inhibited these effects.To conclude,hypoxia-preconditioned bone marrow–derived mesenchymal stem cells offer a promising therapeutic approach for neuronal injury following cardiac arrest,and their beneficial effects are potentially associated with increased expression of the liver isoform of phosphofructokinase following hypoxic preconditioning.
基金supported by the Ministry of Science and Technology of China (No. 2012IM030700)the National Natural Science Foundation of China (Nos. 41025012, U0833003, 41273095 and 41103067)
文摘Oxygenated volatile organic compounds(OVOCs) emitted from orange wastes during aerobic decomposition were investigated in a laboratory-controlled incubator for a period of two months. Emission of total OVOCs(TOVOCs) from orange wastes reached 1714 mg/dry kg(330 mg/wet kg). Ethanol, methanol, ethyl acetate, methyl acetate, 2-butanone and acetaldehyde were the most abundant OVOC species with shares of 26.9%, 24.8%, 20.3%, 13.9%, 2.8%and 2.5%, respectively, in the TOVOCs released. The emission fluxes of the above top five OVOCs were quite trivial in the beginning but increased sharply to form one "peak emission window" with maximums at days 1-8 until leveling off after 10 days. This type of "peak emission window" was synchronized with the CO2 fluxes and incubation temperature of the orange wastes, indicating that released OVOCs were mainly derived from secondary metabolites of orange substrates through biotic processes rather than abiotic processes or primary volatilization of the inherent pool in oranges. Acetaldehyde instead had emission fluxes decreasing sharply from its initial maximum to nearly zero in about four days,suggesting that it was inherent rather than secondarily formed. For TOVOCs or all OVOC species except 2-butanone and acetone, over 80% of their emissions occurred during the first week, implying that organic wastes might give off a considerable amount of OVOCs during the early disposal period under aerobic conditions.
基金supported by the Key Research and Development Program of Shaanxi Province(2019ZDLGY15-07)the National Natural Science Foundation of China(51806020)+1 种基金the Youth Innovation Team of Shaanxi Universities(Energy Saving and New Energy Vehicles)the Special Fund for Basic Scientific Research of Central Colleges,Chang’an University(300102229104)。
文摘Biofuels have extensive available resources and have an immense potential as promising alternative fuels for automobile.The application advantages of biofuels are mainly reflected as particulate matter(PM)reduction,carbon neutral,greenhouse gases reduction,waste utilization,energy and economic security,and fuel pluralism.Based on the understanding of molecular structure effects of biofuels on soot formation and particles morphology,the effects of alcohols,ethers,esters and biodiesel on spray and combustion process in constant volume bomb in recent years are retrospectively analyzed in this paper.For the mixture,macromolecular ester fuels and polyoxymethylene dimethyl ether(PODE)are conducive to the improvement of liquid spray,while biodiesel,small molecules,dimethyl ether(DME)and alcohols are reversed.Alcohols are advantageous to the extension of mixing time and the increasing of vapor-phase mixture.Through the influence integrated assessment,alcohols show the best performance on the spray,atomization and combustion,while biodiesels show the worst.But in terms of combustion,PODE is the best choice without considering spray and atomization.For binary alternative-diesel fuel blends,methanol or butanol is the best additive based on synthetically considerations on spray,atomization and combustion.To meet the requirements of the fuel application of diesel engine,ternary fuel or even quaternary fuel have been proposed and explored.This review can help to form a systematic understanding on fuel recombining and obtain the guide of clean and efficient fuel formulation for diesel engine.
基金financially supported by the National Natural Science Foundation of China (22071137)the Program for Tsingtao Al-ion Power and Energy-storage Battery Research Team in the University (17-2-1-1-zhc)。
文摘The direct electrochemical synthesis of H_(2)O_(2)from O_(2)is currently the most promising alternative to energyintensive industrial anthraquinone oxidation/reduction methods. However, its widespread use is hampered by the lack of efficient low-cost electrocatalysts. In the current study,oxygenated boron-doped carbon(O-BC) materials were realized via a green synthetic strategy involving polymer dehalogenation and employed as electrode materials for the electrochemical synthesis of H_(2)O_(2)via a 2 e-oxygen reduction.The catalytic activity of the O-BC materials was optimized through systematic variation of the boron source(H_(2)BO_(2))dosage and annealing temperature. Electrochemical measurements revealed that the optimal sample(O-BC-2-650)exhibited a selectivity of 98% for the 2 e-oxygen reduction to H2 O_(2)and an average H_(2)O_(2)production rate of412.8 mmol g_(cat)^(-1) h^(-1)in an H-type alkaline electrolyzer. Density functional theory simulations indicated that the functionalization of active B sites with one oxygen atom provides the lowest Gibbs free energy change(ΔG) of 0.03 e V for the hydrogenation of*O_(2), while functionalization with zero or two O atoms results in much larger ΔG values(0.08 and 0.10 e V,respectively). Thus, this work details a new type of green, lowcost, and metal-free electrocatalyst for H_(2)O_(2)production.
基金the National Natural Science Foundation of China(No.21978183)。
文摘In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.
基金the National High Technology Research and Development Program of China(863 Program)(Grant No.2006AA06A305)the National Natural Science Foundation of China(Grant No.20807025)。
文摘Oxygenated fuels are known to reduce particulate matter(PM)emissions from diesel engines.In this study,100%soy methyl ester(SME)biodiesel fuel(B100)and a blend of 10%acetal denoted by A-diesel with diesel fuel were tested as oxygenated fuels.Particle size and number distributions from a diesel engine fueled with oxygenated fuels and base diesel fuel were measured using an Electrical Low Pressure Impactor(ELPI).Measurements were made at ten steady-state operational modes of various loads at two engine speeds.It was found that the geometric mean diameters of particles from SME and Adiesel were lower than that from base diesel fuel.Compared to diesel fuel,SME emitted more ultra-fine particles at rated speed while emitting less ultra-fine particles at maximum speed.Ultra-fine particle number concentrations of A-diesel were much higher than those of base diesel fuel at most test modes.
基金financially supported by the National Natural Science Foundation of China(No.22279047)the Instrumental Analysis Center of Jiangsu University of Science and Technology。
文摘Exploring efficient and nonprecious metal electrocatalysts of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is crucial for developing rechargeable zinc-air batteries(ZABs).Herein,an alloying-degree control strategy was employed to fabricate nitrogen-doped carbon sphere(NCS)decorated with dual-phase Co/Co_(7)Fe_(3)heterojunctions(CoFe@NCS).The phase composition of materials has been adjusted by controlling the alloying degree.The optimal CoFe_(0.08)@NCS electrocatalyst displays a half-wave potential of 0.80 V for ORR and an overpotential of 283 mV at 10 mA·cm^(-2)for OER in an alkaline electrolyte.The intriguing bifunctional electrocatalytic activity and durability is attributed to the hierarchically porous structure and interfacial electron coupling of highly-active Co_(7)Fe_(3)alloy and metallic Co species.When the CoFe_(0.08)@NCS material is used as air-cathode catalyst of rechargeable liquid-state zinc-air battery(ZAB),the device shows a high peak power-density(157 mW·cm^(-2))and maintains a stable voltage gap over 150 h,outperforming those of the benchmark(Pt/C+RuO_(2))-based device.In particular,the as-fabricated solid-state flexible ZAB delivers a reliable compatibility under different bending conditions.Our work provides a promising strategy to develop metal/alloy-based electrocatalysts for the application in renewable energy conversion technologies.
基金Research Institute for Smart Energy(CDB2)the grant from the Research Institute for Advanced Manufacturing(CD8Z)+4 种基金the grant from the Carbon Neutrality Funding Scheme(WZ2R)at The Hong Kong Polytechnic Universitysupport from the Hong Kong Polytechnic University(CD9B,CDBZ and WZ4Q)the National Natural Science Foundation of China(22205187)Shenzhen Municipal Science and Technology Innovation Commission(JCYJ20230807140402006)Start-up Foundation for Introducing Talent of NUIST and Natural Science Foundation of Jiangsu Province of China(BK20230426).
文摘Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.
基金support from the Czech Science Foundation,project EXPRO,No 19-27454Xsupport by the European Union under the REFRESH—Research Excellence For Region Sustainability and High-tech Industries project number CZ.10.03.01/00/22_003/0000048 via the Operational Programme Just Transition from the Ministry of the Environment of the Czech Republic+1 种基金Horizon Europe project EIC Pathfinder Open 2023,“GlaS-A-Fuels”(No.101130717)supported from ERDF/ESF,project TECHSCALE No.CZ.02.01.01/00/22_008/0004587).
文摘Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.
基金funded by the National Key R&D Program of China(2021YFA1501101)the National Natural Science Foundation of China(No.22471103,22425105,22201111,21931001,22221001,and 22271124)+5 种基金Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province(2019ZX-04)the 111 Project(B20027)as well as the National Natural Science Foundation of Gansu Province(22JR5RA470)the Fundamental Research Funds for the Central Universities(lzujbky-2023-eyt03)supported by the Agency for Science,Technology and Research(A*STAR)MTC Individual Research Grants(IRG)M22K2c0078.
文摘Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction.The surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity enhancement.Here,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is reported.The substituting Fe content influences both current change tendency and surface reconstruction degree.LaNi_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)series.The reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based catalysts.Besides,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term stability.Furthermore,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction degree.The effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface reconstruction.This finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.
基金financial support of this work by the National Natural Science Foundation of China(Nos.22378332,52003219)the Open Fund of Zhejiang Key Laboratory of Flexible Electronics(No.2022FE008)+1 种基金the Natural Science Foundation of Ningbo(NO.2022J058)Ministry of Industry and Information Technology high quality development project(TC220A04A-206).
文摘Although poly(lactic acid)(PLA)is a good environmentally-friendly bio-degradable polymer which is used to substitute traditional petrochemical-based polymer packaging films,the barrier properties of PLA films are still insufficient for high-barrier packaging applications.In this study,oxygen scavenger hydroxyl-terminated polybutadiene(HTPB)and cobalt salt catalyst were incorporated into the PLA/poly(butylene adipate-co-terephthalate)(PLA/PBAT),followed by melting extrusion and three-layer co-extrusion blown film process to prepare the composite films.The oxygen permeability coefficient of the composite film combined with 6 wt%oxygen scavenger and 0.4 wt%catalyst was decreased significantly from 377.00 cc·mil·m^(-2)·day^(-1)·0.1 MPa^(-1) to 0.98 cc·mil·m^(-2)·day^(-1)·0.1 MPa^(-1),showing a remarkable enhancement of 384.69 times compared with the PLA/PBAT composite film.Meanwhile,the degradation behavior of the composite film was also accelerated,exhibiting a mass loss of nearly 60%of the original mass after seven days of degradation in an alkaline environment,whereas PLA/PBAT composite film only showed a mass loss of 32%.This work has successfully prepared PLA/PBAT composite films with simultaneously improved oxygen barrier property and degradation behavior,which has great potential for high-demanding green chemistry packaging industries,including food,agricultural,and military packaging.