An efficient catalytic system was developed to remove various organic pollutants by simultaneously using low-level cobalt ions,calcium carbonate micro-particles and peroxymonosulfate(PMS).A simple base-induced precipi...An efficient catalytic system was developed to remove various organic pollutants by simultaneously using low-level cobalt ions,calcium carbonate micro-particles and peroxymonosulfate(PMS).A simple base-induced precipitation was used to successfully loaded Co-centered reactive sites onto the surface of CaCO_(3)microparticles.Under optimal conditions at 25°C,10 mg/L methylene blue(MB)could be completely degraded within 10 min with 480μg/L Co^(2+),0.4 g/L CaCO_(3)microparticles(or 0.4 g/L Co@CaCO_(3))and 0.1 g/L PMS.The MB degradation followed the pseudo first order kinetics with a rate constant of 0.583 min^(−1),being 8.3,11.5 and 53.0 times that by using Co-OH(0.07 min^(−1)),Co^(2+)(0.044 min^(−1))and CaCO_(3)(0.011 min^(−1))as the catalyst,respectively.It was confirmed that there was a synergistic effect in the catalytic activity between Co species and the CaCO_(3)particles but the major contributor was the highly dispersed Co species.When Co^(2+)-containing simulated electroplating wastewater was used as the Co^(2+)source,not only the added MB was also completely degraded within 5 min in this catalytic system,but also the coexisting heavy metal ions were substantially removed.The presently developed method was applied to simultaneously treat organic wastewater and heavy metals wastewater.The present method was also successfully used to efficiently degrade other organic pollutants including bisphenol A,sulfamethoxazole,rhodamine B,tetrabromobisphenol A,ofloxacin and benzoic acid.A catalytic mechanism was proposed for the PMS activation by Co@CaCO_(3).The surface of CaCO_(3)particles favors the adsorption of Co^(2+).More importantly,the surface of CaCO_(3)particles provides plentiful surface-OH and-CO_(3)^(2+),and these surface groups complex with Co^(2+)to producemore catalytically active species such as surface[CoOH]^(−),resulting in rapid Co^(2+)/Co^(3+)cycling and electron transfer.These interactions cause the observed synergistic effect between Co species and CaCO_(3)particles in PMS activation.Due to good cycle stability,strong anti-interference ability and wide universality,the new method will have broad application prospects.展开更多
Magnetic Cu^0/Fe3O4 submicron composites were prepared using a hydrothermal method and used as heterogeneous catalysts for the activation of peroxymonosulfate(PMS) and the degradation of organic pollutants.The as-pr...Magnetic Cu^0/Fe3O4 submicron composites were prepared using a hydrothermal method and used as heterogeneous catalysts for the activation of peroxymonosulfate(PMS) and the degradation of organic pollutants.The as-prepared magnetic Cu^0/Fe3O4 submicron composites were composed of Cu^0 and Fe3O4 crystals and had an average size of approximately 220 nm.The Cu^0/Fe3O4 composites could efficiently catalyze the activation of PMS to generate singlet oxygen,and thus induced the rapid degradation of rhodamine B,methylene blue,orange Ⅱ,phenol and 4-chlorophenol.The use of0.1 g/L of the Cu^0/Fe3O4 composites induced the complete removal of rhodamine B(20 μmol/L) in15 min,methylene blue(20 μmol/L) in 5 min,orange Ⅱ(20 μmol/L) in 10 min,phenol(0.1mmol/L) in 30 min and 4-chlorophenol(0.1 mmol/L) in 15 min with an initial pH value of 7.0 and a PMS concentration of 0.5 mmol/L.The total organic carbon(TOC) removal higher than 85%for all of these five pollutants was obtained in 30 min when the PMS concentration was 2.5 mmol/L.The rate of degradation was considerably higher than that obtained with Cu^0 or Fe3O4 particles alone.The enhanced catalytic activity of the Cu^0/Fe3O4 composites in the activation of PMS was attributed to the synergistic effect of the Cu^0 and Fe3O4 crystals in the composites.Singlet oxygen was identified as the primary reactive oxygen species responsible for pollutant degradation by electron spin resonance and radical quenching experiments.A possible mechanism for the activation of PMS by Cu^0/Fe3O4 composites is proposed as electron transfer from the organic pollutants to PMS induces the activation of PMS to generate ^1O2,which induces the degradation of the organic pollutants.As a magnetic catalyst,the Cu^0/Fe3O4 composites were easily recovered by magnetic separation,and exhibited excellent stability over five successive degradation cycles.The present study provides a facile and green heterogeneous catalysis method for the oxidative removal of organic pollutants.展开更多
Phenol in waste water threatens human health and is difficultly to be decomposed by nature.Efficient degradation of high-loaded phenol in water under mild condition is still a great challenge.Herein,ionic liquids with...Phenol in waste water threatens human health and is difficultly to be decomposed by nature.Efficient degradation of high-loaded phenol in water under mild condition is still a great challenge.Herein,ionic liquids with tungstate anion were designed and prepared.It was found that dodecyltrimethylammonium tungstate could catalyzed degradation of phenol into gases and water thoroughly at 323 k in 8 h.Tungstate anion revealed good catalytic oxidative activity and long carbon chain group connecting with cation of ionic liquids enriched phenol around catalysts,which induced the complete degradation of phenol at mild conditions.Increasing the amounts of hydrogen peroxide benefited to the total degradation of phenol.In addition,the ionic liquid could be reused for its excellent thermal stability.Our work provided a different strategy to treat waste water containing phenol efficiently.展开更多
In this work,the gold nanoparticles(Au-NPs)were in-situ generated on the surface of MnO2nanosheets to form MnO2/Au-NPs nanocomposite in a simple and cost-effective way.Multiple experiments were carried out to optimi...In this work,the gold nanoparticles(Au-NPs)were in-situ generated on the surface of MnO2nanosheets to form MnO2/Au-NPs nanocomposite in a simple and cost-effective way.Multiple experiments were carried out to optimize the oxidation of basic dye(Methylene Blue(MB)),including the molar ratio of MnO2to chloroauric acid(HAu Cl4),the p H of the solution and the effect of initial material.Under the optimal condition,the highest degradation efficiency for MB achieved to 98.9%within 60 min,which was obviously better than commercial MnO2powders(4.3%)and MnO2nanosheets(74.2%).The enhanced oxidative degradation might attribute to the in-situ generation of ultra-small and highly-dispersed Au-NPs which enlarged the synergistic effect and/or interfacial effect between MnO2nanosheets and Au-NPs and facilitated the uptake of electrons by MnO2from MB during the oxidation,thus validating the application of MnO2/Au-NPs nanocomposite for direct removal of organic dyes from wastewater in a simple and convenient fashion.展开更多
The natural attapulgite(NAPT)was disaggregated by high-pressure homogenization technology combined with extrusion process to prepare the attapulgite with disaggregated rod crystal bundles(DAPT)and large specific surfa...The natural attapulgite(NAPT)was disaggregated by high-pressure homogenization technology combined with extrusion process to prepare the attapulgite with disaggregated rod crystal bundles(DAPT)and large specific surface area of 133.7 m^(2)/g.NAPT and DAPT were incorporated into the silicone rubber to obtain the composite NAPTSR and DAPT-SR by mechanical blending method,respectively.After thermal oxidative ageing at 300℃ for 0.5 h,temperature for the 5%weight loss increased greatly from 385℃ of the neat silicone rubber to 396-399℃ with addition of NAPT and DAPT.NAPT and DAPT enhanced the interaction between the filler nanoparticles and rubber matrix thus inhibited the nanoparticle agglomeration.The conservation rate of the side methyl group in NAPT-SR and DAPT-SR was greatly improved after ageing.Therefore,the thermal oxidative degradation and ageing performance of the silicone rubber composites was significantly reinforced.Moreover,DAPT could greatly restrain the growth of nanoparticles after ageing.Therefore,DAPT-SR showed the better retention of tensile strength(40.6%),elongation at break(34.9%)and tear strength(30.1%)compared with the corresponding mechanical properties of the neat silicone rubber(10.6%,7.4%,and 5.0%)after ageing.展开更多
In order to evaluate the thermal oxidation degradation behavior of lubricant with different antioxidants,the thermal kinetics equation based on the anlyses of thermogravimetry(TG),differential thermal analysis(DTA),an...In order to evaluate the thermal oxidation degradation behavior of lubricant with different antioxidants,the thermal kinetics equation based on the anlyses of thermogravimetry(TG),differential thermal analysis(DTA),and differential scanning calorimetry(DSC)was established,respectively,to calculate the activation energy of lubricant thermal-oxidative reaction.The thermal analyses of TG and DTA were employed to determine the thermal decomposition properties of ester oils trimethylolpropane trioleate(TMPTO)with butyl-octyl-diphenylamine/octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propanoate/amine-phenol combination antioxidant.The activation energy of the lubricating oil adding antioxidant is increased relative to the TMPTO base oil,and the order of activation energy are Ec(93.732 kJ·mol^(-1))>Ed(88.71 kJ·mol^(-1))>Eb(58.41 kJ·mol^(-1))>Ea(46.32 kJ·mol^(-1)).The experimental results show that octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propanoate in TMPTO has favorable resistance to thermal oxidation and decomposition.The thermal analysis method of DSC accurately reflects the heat exchange of lubricant thermal-oxidative reaction.The order of activation energy is calculated to ED(144.385 kJ·mol^(-1))>EC(110.05 kJ·mol^(-1))>EB(97.187 kJ·mol^(-1))>EA(66.02 kJ·mol^(-1)).It is illustrated that the amine-phenol combination antioxidant has the best thermal oxidation resistance,which is the same as what the oxidation onset temperature effected.展开更多
Contact glow discharge electrolysis (CGDE) of o-chlorophenol (2-CP) was investigated under different pH, voltages and initial concentrations. And the mechanism of the oxidation was explored. The results suggested that...Contact glow discharge electrolysis (CGDE) of o-chlorophenol (2-CP) was investigated under different pH, voltages and initial concentrations. And the mechanism of the oxidation was explored. The results suggested that the degradation followed the first order kinetic law; Fe2+ had a remarkable catalytic effect on the removal rate of o-chloropenol. In the presence of Fe2+, 2-CP underwent an exhaustive degradation, from which the major intermediates included o-dihydroxybenze, p-hydroxybenze, p-benzoquione and carboxlic acids.展开更多
The factors and mechanisms of oxidative degradation of three organophosphorus pesticides (dichlorvos, methamidophos and phoxim) were studied with sodium percarbonate (SPC) as a solid oxidant. The result showed tha...The factors and mechanisms of oxidative degradation of three organophosphorus pesticides (dichlorvos, methamidophos and phoxim) were studied with sodium percarbonate (SPC) as a solid oxidant. The result showed that SPC has highly activity in degrading these organophosphous pesticides. The most efficient degradation of pesticides occurred under basic conditions and the degradation rates increased with time extension and high temperature. The degradation of organophosphorus pesticides was expected to get even better results at lower initial concentration. Furthermore, we analyzed the intermediate products by NMP, spectrometry. On the basis of the analytical result, the oxidative degradation mechanism was proposed for each organophosphous pesticide. It is significant to understand the environment chemistry of organophosphorus pesticides in environmental system.展开更多
A series of metal oxide catalysts for catalytic oxidative degradation of 2-chlorophenol (2-CP) and 4-chlorophenol (4-CP) were prepared, and the supported CuO catalysts were studied particularly. The supported CuO ...A series of metal oxide catalysts for catalytic oxidative degradation of 2-chlorophenol (2-CP) and 4-chlorophenol (4-CP) were prepared, and the supported CuO catalysts were studied particularly. The supported CuO catalysts were characterized by XRD and NH3-TPD techniques, in which CuO/γ-Al2O3 exhibited high degradation activity. The addition of Na2O or K2O into CuO/γ-Al2O3 improved the oxidative degradation of CPs remarkably, in which Na2O was more efficient than K2O. Over CuO/γ-Al2O3-Na2O, CPs were completely converted and the liberation of the inorganic chloride from 2-CP or 4-CP reached 97% or 100% respectively at 30 ?C for 2 h. The supported CuO catalysts with good dispersion of CuO particles and less acid sites were favorable for the efficient oxidative degradation of CPs. In addition, the initial pH of the reaction solution was found to be an important factor which influenced the catalytic oxidative degradation of CPs and the initial pH of 11.2 and 9.8 was preferred for the oxidative degradation of 2-CP and 4-CP respectively over CuO/γ-Al2O3 catalyst.展开更多
The current work deals with ZnO-Ag nanocomposites(in the wide range of x in the Zn1-x O-Ag x chemical composition) synthesized using microwave assisted solution combustion method.The structural, morphological and op...The current work deals with ZnO-Ag nanocomposites(in the wide range of x in the Zn1-x O-Ag x chemical composition) synthesized using microwave assisted solution combustion method.The structural, morphological and optical properties of the samples were characterized by XRD(X-ray diffraction), FTIR(Fourier transform infrared spectrometry), SEM(scanning electron microscopy technique), EDX(energy dispersive X-ray spectrum), ICP(inductively coupled plasma technique), TEM(transmission electron microscopy), BET(Brunauer–Emmett–Teller method), UV–Vis(ultraviolet–visible spectrophotometer) and photoluminescence spectrophotometer. The photocatalytic activity of the ZnO-Ag was investigated by photo-degradation of Acid Blue 113(AB 113) under UV illumination in a semi-batch reactor. This experiment showed that ZnO-Ag has much more excellent photocatalytic properties than ZnO synthesized by the same method. The enhanced photocatalytic activity was due to the decrease in recombination of photogenerated electron-holes. The results showed the improvement of ZnO photocatalytic activity and there is an optimum amount of Ag(3.5 mol%) that needs to be doped with ZnO.The effect of operating parameters such as p H, catalyst dose and dye concentration were investigated. The reaction byproducts were identified by LC/MS(liquid chromatography/mass spectrometry) analysis and a pathway was proposed as well. Kinetic studies indicated that the decolorization process follows the first order kinetics. Also, the degradation percentage of AB113 was determined using a total organic carbon(TOC) analyzer. Additionally, cost analysis of the process, the mechanism and the role of Ag were discussed.展开更多
Degradation of dyes is an important environmental issue. In order to avoid the carcinogenic risks in anaerobic-aerobic biological process for wastewater containing azo dyes, a hemin based biomimetic oxidative degradat...Degradation of dyes is an important environmental issue. In order to avoid the carcinogenic risks in anaerobic-aerobic biological process for wastewater containing azo dyes, a hemin based biomimetic oxidative degradation of azo dyes was developed. Acid orange 7 (AO7) was selected as the model for azo dye and the high efficient degradation was achieved in hemin/H2O2 system at pH 11.0. Degradation could be described by a pseudo-first-order kinetic model. The order of dependence on H2O2 concentration was significantly larger than that of hemin. Coexisting anions sulphate and chloride had little effect on the degradation, but reductive sulphite dramatically inhibited the degradation. The protic solvent 2-prophanol obviously promoted the degradation. Azo chromogenic group was destroyed quickly and some smaller intermediates formed. Active species oxoferryl porphyrin p-cation radical +PFeIV=O generated from heterolytic cleavage of O-O in H2O2 catalyzed by hemin play the main roles in degradation and reaction pathways were proposed.展开更多
2,4,6-trichlorophenol (TCP) was firstly treated with air ions generated by electric discharge, and high dechlorination (53%) was observed after 60 min treatment, indicating that air ions are an efficient dechlorinatio...2,4,6-trichlorophenol (TCP) was firstly treated with air ions generated by electric discharge, and high dechlorination (53%) was observed after 60 min treatment, indicating that air ions are an efficient dechlorination means and might have a future in the oxidative removal of chlorinated phenols. In addition, a stepwise degradation of TCP, beginning with the formation of a major product 2,6-dichloro-1,4-benzenediol via substitution, is proposed through a detailed analysis of gas chromatography/mass spectrometry.展开更多
In Fenton-like oxidation,the catalyst directly influences the reaction mechanism for the degradation of pollutants from water.Here,a α-MnO_(2)catalyst(OAm-1)was synthesized via a self-assembly method with the assista...In Fenton-like oxidation,the catalyst directly influences the reaction mechanism for the degradation of pollutants from water.Here,a α-MnO_(2)catalyst(OAm-1)was synthesized via a self-assembly method with the assistance of a surfactant.OAm-1 possessed a large specific surface area of_(2)21 m2/g,abundant mesoporous structures and a large proportion of Mn(III).Further characterization exhibited that OAm-1 had abundant oxygen vacancies and excellent reducibility and conductivity.The adsorption and catalytic ability of OAm-1 were studied in the degradation of oxytetracycline(OTC)via the activation of hydrogen peroxide(H_(2)O_(2)).Through the radical quenching experiments,electron resonance spectroscopy(EPR),X-ray photoelectron spectroscopy(XPS)and Fourier-transform infrared spectroscopy(FT-IR)analysis,Mn(III)of OAm-1 was proved to be the active sites for the chemisorption of OTC.Systematic electrochemical ex-periments and analysis have shown that a process of electron transfer mediated by OAm-1 occurred be-tween the pollutant and H_(2)O_(2)during a Fenton-like reaction.This work experimentally verifies the elec-tron transfer process dominated nonradical mechanism overα-MnO_(2),which is helpful for understanding the catalytic mechanism of the Fenton-like oxidation.展开更多
The oxidative degradation of aqueous carbofuran, a heavily used toxic carbamate insecticide by low temperature plasma, was investigated. The results show that the treatment efficiency increases with the increase in in...The oxidative degradation of aqueous carbofuran, a heavily used toxic carbamate insecticide by low temperature plasma, was investigated. The results show that the treatment efficiency increases with the increase in initial concentration. Raising the treatment temperature and changing the pH value can result in enhanced degradation of carbofuran in solution. The results also show that low temperature plasma treatment can effectively remove chemical oxygen demand (COD) of carbofuran in the solution.展开更多
Treatment of biliverdin IXα dimethyl ester(2)with silver nitrate in alkaline solution gave two violin-like tripyrrione carbaldehydes,one de- graded at C15-C16,other at C4-C5.Biliverdin IXα(1),bilirubin IXα(3)and it...Treatment of biliverdin IXα dimethyl ester(2)with silver nitrate in alkaline solution gave two violin-like tripyrrione carbaldehydes,one de- graded at C15-C16,other at C4-C5.Biliverdin IXα(1),bilirubin IXα(3)and its dimethyl ester(4)gave the same results.展开更多
In this work, the contribution of mediated oxidation mechanisms in the electrolytic degradation of cyanuric acid using boron-doped diamond(BDD) anodes was investigated in different electrolytes. A complete mineraliz...In this work, the contribution of mediated oxidation mechanisms in the electrolytic degradation of cyanuric acid using boron-doped diamond(BDD) anodes was investigated in different electrolytes. A complete mineralization of cyanuric acid was obtained in Na Cl;however lower degrees of mineralization of 70% and 40% were obtained in Na2SO4 and Na Cl O4, respectively. This can be explained by the nature of the oxidants electrogenerated in each electrolyte. It is clear that the contribution of active chlorine(Cl2, HCl O, Cl O-)electrogenerated from oxidation of chlorides on BDD is much more important in the electrolytic degradation of cyanuric acid than the persulfate and hydroxyl radicals produced by electro-oxidation of sulfate and water on BDD anodes. This could be explained by the high affinity of active chlorine towards nitrogen compounds. No organic intermediates were detected during the electrolytic degradation of cyanuric acid in any the electrolytes, which can be explained by their immediate depletion by hydroxyl radicals produced on the BDD surface. Nitrates and ammonium were the final products of electrolytic degradation of cyanuric acid on BDD anodes in all electrolytes. In addition, small amounts of chloramines were formed in the chloride medium. Low current density(≤ 10 m A/cm2) and neutral medium(p H in the range 6–9) should be used for high efficiency electrolytic degradation and negligible formation of hazardous chlorate and perchlorate.展开更多
High-efficient rubber antioxidants for enhanced heat resistance without compromising mechanical properties remain an enormous and long-term challenge for the rubber industry.Herein,we employed the in-situ growth of Ce...High-efficient rubber antioxidants for enhanced heat resistance without compromising mechanical properties remain an enormous and long-term challenge for the rubber industry.Herein,we employed the in-situ growth of Ce-doped Co-metal-organic framework(Ce Co-MOF)in dendritic mesoporous organosilica nanoparticles(DMONs@Ce Co-MOF,denoted as DCCM)to prepare a novel antioxidant that exhibit outstanding thermal stability.Dendritic mesoporous organosilica nanoparticles(DMONs)effectively alleviated the incompatibility of Ce Co-MOF in the polymer matrix,and the effective scavenging of free radicals was attributed to the various oxidation states of metal ions in Ce Co-MOF.Surprising,by adding only0.5 phr(parts per hundred of rubber)of DMONs@Ce Co-MOF to silicone rubber,(SR),the retention rate of tensile strength increased from 37.3%to 61.6%after aging 72 h at 250℃,and the retention rate of elongation at break of DCCM/SR1 composites reached 68%,which was 5.43 times of SR.The strategy of anchoring MOFs on the surface of silica also provides a viable method for preparing effective compound functionalized rubber antioxidant.展开更多
Harnessing photocatalyzed hydrogen atom transfer(HAT)for the precise activation of C–H/O–H bonds is a pivotal yet challenging strategy to selectively drive oxidative C–C bond scission in renewable lignin,yielding v...Harnessing photocatalyzed hydrogen atom transfer(HAT)for the precise activation of C–H/O–H bonds is a pivotal yet challenging strategy to selectively drive oxidative C–C bond scission in renewable lignin,yielding value-added chemicals with exceptional selectivity.Herein,we present a metal-free photochemical strategy that enables selective C–C bond scission in lignin via a unique synergistic HAT pathway driven by triplet-excited 2-ethylanthraquinone(EAQ^(*))and hydroxyl radicals(•OH)generated in situ from EAQH_(2) and O_(2).Under simulated natural conditions,this process achieves a benzaldehyde yield of 146.6 mol%from a lignin-derived phenolic dimer.Mechanistic investigations reveal that preferential activation of the Cα-OH in lignin facilitates a tandem HAT process,forming alkoxy radical intermediates that undergoβ–scission to produce benzaldehyde,as corroborated by extensive control reactions and density functional theory calculations.Furthermore,this straightforward protocol efficiently cleaves the C–C bonds of technical kraft lignins,providing a rapid,scalable,and metal-free protocol for lignin valorization under mild conditions.展开更多
Although supported solid amine adsorbents have attracted great attention for CO_(2) capture,critical chemical deactivation problems including oxidative degradation and urea formation have severely restricted their pra...Although supported solid amine adsorbents have attracted great attention for CO_(2) capture,critical chemical deactivation problems including oxidative degradation and urea formation have severely restricted their practical applications for flue gas CO_(2) capture.In this work,we reveal that the nature of surface hydroxyl groups(metal hydroxyl Al–OH and nonmetal hydroxyl Si–OH)plays a key role in the deactivation mechanisms.The polyethyleneimine(PEI)supported on Al–OH-containing substrates suffers from severe oxidative degradation during the CO_(2) capture step due to the breakage of amine-support hydrogen bonding networks,but exhibits an excellent anti-urea formation feature by preventing dehydration of carbamate products under a pure CO_(2) regeneration atmosphere.In contrast,PEI supported on Si–OHcontaining substrates exhibits excellent anti-oxidative stability under simulated flue gas conditions by forming a robust hydrogen bonding protective network with Si–OH,but suffers from obvious urea formation during the pure CO_(2) regeneration step.We also reveal that the urea formation problem for PEI-SBA-15 can be avoided by the incorporation of an OH-containing PEG additive.Based on the intrinsic understanding of degradation mechanisms,we successfully synthesized an adsorbent 40PEI-20PEG-SBA-15 that demonstrates outstanding stability and retention of a high CO_(2) capacity of 2.45 mmol g^(−1) over 1000 adsorption–desorption cycles,together with negligible capacity loss during aging in simulated flue gas(10%CO_(2)+5%O_(2)+3%H_(2)O)for one month at 60–70℃.We believe this work makes great contribution to the advancement in the field of ultra-stable solid amine-based CO_(2) capture materials.展开更多
High-temperature proton exchange membrane fuel cells(HT-PEMFCs)are pursued worldwide as efficient energy conversion devices.Great efforts have been made in the area of designing and developing phosphoric acid(PA)-base...High-temperature proton exchange membrane fuel cells(HT-PEMFCs)are pursued worldwide as efficient energy conversion devices.Great efforts have been made in the area of designing and developing phosphoric acid(PA)-based proton exchange membrane(PEM)of HT-PEMFCs.This review focuses on recent advances in the limitations of acid-based PEM(acid leaching,oxidative degradation,and mechanical degradation)and the approaches mitigating the membrane degradation.Preparing multilayer or polymers with continuous network,adding hygroscopic inorganic materials,and introducing PA doping sites or covalent interactions with PA can effectively reduce acid leaching.Membrane oxidative degradation can be alleviated by synthesizing crosslinked or branched polymers,and introducing antioxidative groups or highly oxidative stable materials.Crosslinking to get a compact structure,blending with stable polymers and inorganic materials,preparing polymer with high molecular weight,and fabricating the polymer with PA doping sites away from backbones,are recommended to improve the membrane mechanical strength.Also,by comparing the running hours and decay rate,three current approaches,1.crosslinking via thermally curing or polymeric crosslinker,2.incorporating hygroscopic inorganic materials,3.increasing membrane layers or introducing strong basic groups and electron-withdrawing groups,have been concluded to be promising approaches to improve the durability of HT-PEMFCs.The overall aim of this review is to explore the existing degradation challenges and opportunities to serve as a solid basis for the deployment in the fuel cell market.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22076052 and 21976063)China Postdoctoral Science Foundation(No.2018M642850)the Research Funding of Wuhan Polytechnic University(No.2023RZ017).
文摘An efficient catalytic system was developed to remove various organic pollutants by simultaneously using low-level cobalt ions,calcium carbonate micro-particles and peroxymonosulfate(PMS).A simple base-induced precipitation was used to successfully loaded Co-centered reactive sites onto the surface of CaCO_(3)microparticles.Under optimal conditions at 25°C,10 mg/L methylene blue(MB)could be completely degraded within 10 min with 480μg/L Co^(2+),0.4 g/L CaCO_(3)microparticles(or 0.4 g/L Co@CaCO_(3))and 0.1 g/L PMS.The MB degradation followed the pseudo first order kinetics with a rate constant of 0.583 min^(−1),being 8.3,11.5 and 53.0 times that by using Co-OH(0.07 min^(−1)),Co^(2+)(0.044 min^(−1))and CaCO_(3)(0.011 min^(−1))as the catalyst,respectively.It was confirmed that there was a synergistic effect in the catalytic activity between Co species and the CaCO_(3)particles but the major contributor was the highly dispersed Co species.When Co^(2+)-containing simulated electroplating wastewater was used as the Co^(2+)source,not only the added MB was also completely degraded within 5 min in this catalytic system,but also the coexisting heavy metal ions were substantially removed.The presently developed method was applied to simultaneously treat organic wastewater and heavy metals wastewater.The present method was also successfully used to efficiently degrade other organic pollutants including bisphenol A,sulfamethoxazole,rhodamine B,tetrabromobisphenol A,ofloxacin and benzoic acid.A catalytic mechanism was proposed for the PMS activation by Co@CaCO_(3).The surface of CaCO_(3)particles favors the adsorption of Co^(2+).More importantly,the surface of CaCO_(3)particles provides plentiful surface-OH and-CO_(3)^(2+),and these surface groups complex with Co^(2+)to producemore catalytically active species such as surface[CoOH]^(−),resulting in rapid Co^(2+)/Co^(3+)cycling and electron transfer.These interactions cause the observed synergistic effect between Co species and CaCO_(3)particles in PMS activation.Due to good cycle stability,strong anti-interference ability and wide universality,the new method will have broad application prospects.
基金supported by the National Natural Science Foundation of China (21377169, 21507168)the Fundamental Research Funds for the Central Universities (CZW15078)the Natural Science Foundation of Hubei Province of China (2014CFC1119, 2015CFB505)~~
文摘Magnetic Cu^0/Fe3O4 submicron composites were prepared using a hydrothermal method and used as heterogeneous catalysts for the activation of peroxymonosulfate(PMS) and the degradation of organic pollutants.The as-prepared magnetic Cu^0/Fe3O4 submicron composites were composed of Cu^0 and Fe3O4 crystals and had an average size of approximately 220 nm.The Cu^0/Fe3O4 composites could efficiently catalyze the activation of PMS to generate singlet oxygen,and thus induced the rapid degradation of rhodamine B,methylene blue,orange Ⅱ,phenol and 4-chlorophenol.The use of0.1 g/L of the Cu^0/Fe3O4 composites induced the complete removal of rhodamine B(20 μmol/L) in15 min,methylene blue(20 μmol/L) in 5 min,orange Ⅱ(20 μmol/L) in 10 min,phenol(0.1mmol/L) in 30 min and 4-chlorophenol(0.1 mmol/L) in 15 min with an initial pH value of 7.0 and a PMS concentration of 0.5 mmol/L.The total organic carbon(TOC) removal higher than 85%for all of these five pollutants was obtained in 30 min when the PMS concentration was 2.5 mmol/L.The rate of degradation was considerably higher than that obtained with Cu^0 or Fe3O4 particles alone.The enhanced catalytic activity of the Cu^0/Fe3O4 composites in the activation of PMS was attributed to the synergistic effect of the Cu^0 and Fe3O4 crystals in the composites.Singlet oxygen was identified as the primary reactive oxygen species responsible for pollutant degradation by electron spin resonance and radical quenching experiments.A possible mechanism for the activation of PMS by Cu^0/Fe3O4 composites is proposed as electron transfer from the organic pollutants to PMS induces the activation of PMS to generate ^1O2,which induces the degradation of the organic pollutants.As a magnetic catalyst,the Cu^0/Fe3O4 composites were easily recovered by magnetic separation,and exhibited excellent stability over five successive degradation cycles.The present study provides a facile and green heterogeneous catalysis method for the oxidative removal of organic pollutants.
基金financially supported by the National Natural Science Foundation of China(21875265,22293015,22121002)。
文摘Phenol in waste water threatens human health and is difficultly to be decomposed by nature.Efficient degradation of high-loaded phenol in water under mild condition is still a great challenge.Herein,ionic liquids with tungstate anion were designed and prepared.It was found that dodecyltrimethylammonium tungstate could catalyzed degradation of phenol into gases and water thoroughly at 323 k in 8 h.Tungstate anion revealed good catalytic oxidative activity and long carbon chain group connecting with cation of ionic liquids enriched phenol around catalysts,which induced the complete degradation of phenol at mild conditions.Increasing the amounts of hydrogen peroxide benefited to the total degradation of phenol.In addition,the ionic liquid could be reused for its excellent thermal stability.Our work provided a different strategy to treat waste water containing phenol efficiently.
基金supported by the National Natural Science Foundation of China (Nos. 21277048 and 21505046)the China Postdoctoral Science Foundation (No. 2016 M590336)+1 种基金the "Chenguang Program" funded by Shanghai Education Development FoundationShanghai Municipal Education Commission (No. 15CG21)
文摘In this work,the gold nanoparticles(Au-NPs)were in-situ generated on the surface of MnO2nanosheets to form MnO2/Au-NPs nanocomposite in a simple and cost-effective way.Multiple experiments were carried out to optimize the oxidation of basic dye(Methylene Blue(MB)),including the molar ratio of MnO2to chloroauric acid(HAu Cl4),the p H of the solution and the effect of initial material.Under the optimal condition,the highest degradation efficiency for MB achieved to 98.9%within 60 min,which was obviously better than commercial MnO2powders(4.3%)and MnO2nanosheets(74.2%).The enhanced oxidative degradation might attribute to the in-situ generation of ultra-small and highly-dispersed Au-NPs which enlarged the synergistic effect and/or interfacial effect between MnO2nanosheets and Au-NPs and facilitated the uptake of electrons by MnO2from MB during the oxidation,thus validating the application of MnO2/Au-NPs nanocomposite for direct removal of organic dyes from wastewater in a simple and convenient fashion.
基金supported by the Key Special Program on the S&T for the Pollution Control and Treatment of Water Bodies (No.2017ZX07603-003)。
文摘The natural attapulgite(NAPT)was disaggregated by high-pressure homogenization technology combined with extrusion process to prepare the attapulgite with disaggregated rod crystal bundles(DAPT)and large specific surface area of 133.7 m^(2)/g.NAPT and DAPT were incorporated into the silicone rubber to obtain the composite NAPTSR and DAPT-SR by mechanical blending method,respectively.After thermal oxidative ageing at 300℃ for 0.5 h,temperature for the 5%weight loss increased greatly from 385℃ of the neat silicone rubber to 396-399℃ with addition of NAPT and DAPT.NAPT and DAPT enhanced the interaction between the filler nanoparticles and rubber matrix thus inhibited the nanoparticle agglomeration.The conservation rate of the side methyl group in NAPT-SR and DAPT-SR was greatly improved after ageing.Therefore,the thermal oxidative degradation and ageing performance of the silicone rubber composites was significantly reinforced.Moreover,DAPT could greatly restrain the growth of nanoparticles after ageing.Therefore,DAPT-SR showed the better retention of tensile strength(40.6%),elongation at break(34.9%)and tear strength(30.1%)compared with the corresponding mechanical properties of the neat silicone rubber(10.6%,7.4%,and 5.0%)after ageing.
基金Funded by the National Natural Science Foundation of China(52075391)the China Postdoctoral Science Foundation(2019M660596)。
文摘In order to evaluate the thermal oxidation degradation behavior of lubricant with different antioxidants,the thermal kinetics equation based on the anlyses of thermogravimetry(TG),differential thermal analysis(DTA),and differential scanning calorimetry(DSC)was established,respectively,to calculate the activation energy of lubricant thermal-oxidative reaction.The thermal analyses of TG and DTA were employed to determine the thermal decomposition properties of ester oils trimethylolpropane trioleate(TMPTO)with butyl-octyl-diphenylamine/octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propanoate/amine-phenol combination antioxidant.The activation energy of the lubricating oil adding antioxidant is increased relative to the TMPTO base oil,and the order of activation energy are Ec(93.732 kJ·mol^(-1))>Ed(88.71 kJ·mol^(-1))>Eb(58.41 kJ·mol^(-1))>Ea(46.32 kJ·mol^(-1)).The experimental results show that octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propanoate in TMPTO has favorable resistance to thermal oxidation and decomposition.The thermal analysis method of DSC accurately reflects the heat exchange of lubricant thermal-oxidative reaction.The order of activation energy is calculated to ED(144.385 kJ·mol^(-1))>EC(110.05 kJ·mol^(-1))>EB(97.187 kJ·mol^(-1))>EA(66.02 kJ·mol^(-1)).It is illustrated that the amine-phenol combination antioxidant has the best thermal oxidation resistance,which is the same as what the oxidation onset temperature effected.
基金The project supported by the Key Project of Science and Technology from the Ministry of Education China (No. 00250) the project of KJCXGC-01 of Northwest Normal University, China
文摘Contact glow discharge electrolysis (CGDE) of o-chlorophenol (2-CP) was investigated under different pH, voltages and initial concentrations. And the mechanism of the oxidation was explored. The results suggested that the degradation followed the first order kinetic law; Fe2+ had a remarkable catalytic effect on the removal rate of o-chloropenol. In the presence of Fe2+, 2-CP underwent an exhaustive degradation, from which the major intermediates included o-dihydroxybenze, p-hydroxybenze, p-benzoquione and carboxlic acids.
文摘The factors and mechanisms of oxidative degradation of three organophosphorus pesticides (dichlorvos, methamidophos and phoxim) were studied with sodium percarbonate (SPC) as a solid oxidant. The result showed that SPC has highly activity in degrading these organophosphous pesticides. The most efficient degradation of pesticides occurred under basic conditions and the degradation rates increased with time extension and high temperature. The degradation of organophosphorus pesticides was expected to get even better results at lower initial concentration. Furthermore, we analyzed the intermediate products by NMP, spectrometry. On the basis of the analytical result, the oxidative degradation mechanism was proposed for each organophosphous pesticide. It is significant to understand the environment chemistry of organophosphorus pesticides in environmental system.
基金financially supported by the Education Department of Liaoning Province(No.2009A421)
文摘A series of metal oxide catalysts for catalytic oxidative degradation of 2-chlorophenol (2-CP) and 4-chlorophenol (4-CP) were prepared, and the supported CuO catalysts were studied particularly. The supported CuO catalysts were characterized by XRD and NH3-TPD techniques, in which CuO/γ-Al2O3 exhibited high degradation activity. The addition of Na2O or K2O into CuO/γ-Al2O3 improved the oxidative degradation of CPs remarkably, in which Na2O was more efficient than K2O. Over CuO/γ-Al2O3-Na2O, CPs were completely converted and the liberation of the inorganic chloride from 2-CP or 4-CP reached 97% or 100% respectively at 30 ?C for 2 h. The supported CuO catalysts with good dispersion of CuO particles and less acid sites were favorable for the efficient oxidative degradation of CPs. In addition, the initial pH of the reaction solution was found to be an important factor which influenced the catalytic oxidative degradation of CPs and the initial pH of 11.2 and 9.8 was preferred for the oxidative degradation of 2-CP and 4-CP respectively over CuO/γ-Al2O3 catalyst.
文摘The current work deals with ZnO-Ag nanocomposites(in the wide range of x in the Zn1-x O-Ag x chemical composition) synthesized using microwave assisted solution combustion method.The structural, morphological and optical properties of the samples were characterized by XRD(X-ray diffraction), FTIR(Fourier transform infrared spectrometry), SEM(scanning electron microscopy technique), EDX(energy dispersive X-ray spectrum), ICP(inductively coupled plasma technique), TEM(transmission electron microscopy), BET(Brunauer–Emmett–Teller method), UV–Vis(ultraviolet–visible spectrophotometer) and photoluminescence spectrophotometer. The photocatalytic activity of the ZnO-Ag was investigated by photo-degradation of Acid Blue 113(AB 113) under UV illumination in a semi-batch reactor. This experiment showed that ZnO-Ag has much more excellent photocatalytic properties than ZnO synthesized by the same method. The enhanced photocatalytic activity was due to the decrease in recombination of photogenerated electron-holes. The results showed the improvement of ZnO photocatalytic activity and there is an optimum amount of Ag(3.5 mol%) that needs to be doped with ZnO.The effect of operating parameters such as p H, catalyst dose and dye concentration were investigated. The reaction byproducts were identified by LC/MS(liquid chromatography/mass spectrometry) analysis and a pathway was proposed as well. Kinetic studies indicated that the decolorization process follows the first order kinetics. Also, the degradation percentage of AB113 was determined using a total organic carbon(TOC) analyzer. Additionally, cost analysis of the process, the mechanism and the role of Ag were discussed.
文摘Degradation of dyes is an important environmental issue. In order to avoid the carcinogenic risks in anaerobic-aerobic biological process for wastewater containing azo dyes, a hemin based biomimetic oxidative degradation of azo dyes was developed. Acid orange 7 (AO7) was selected as the model for azo dye and the high efficient degradation was achieved in hemin/H2O2 system at pH 11.0. Degradation could be described by a pseudo-first-order kinetic model. The order of dependence on H2O2 concentration was significantly larger than that of hemin. Coexisting anions sulphate and chloride had little effect on the degradation, but reductive sulphite dramatically inhibited the degradation. The protic solvent 2-prophanol obviously promoted the degradation. Azo chromogenic group was destroyed quickly and some smaller intermediates formed. Active species oxoferryl porphyrin p-cation radical +PFeIV=O generated from heterolytic cleavage of O-O in H2O2 catalyzed by hemin play the main roles in degradation and reaction pathways were proposed.
基金the Alexander von Humboldt Foundation of Germany, and partly by the CAS and the NNSF of China.
文摘2,4,6-trichlorophenol (TCP) was firstly treated with air ions generated by electric discharge, and high dechlorination (53%) was observed after 60 min treatment, indicating that air ions are an efficient dechlorination means and might have a future in the oxidative removal of chlorinated phenols. In addition, a stepwise degradation of TCP, beginning with the formation of a major product 2,6-dichloro-1,4-benzenediol via substitution, is proposed through a detailed analysis of gas chromatography/mass spectrometry.
基金supported by the Youth Innovation Promotion Association,CAS(No.2018456)Major Program of Lanzhou Institute of Chemical Physics,CAS(No.ZYFZFX-10)State Key Laboratory Program of the Lanzhou Institute of Chemical Physics,CAS(No.CHGZ-202211).
文摘In Fenton-like oxidation,the catalyst directly influences the reaction mechanism for the degradation of pollutants from water.Here,a α-MnO_(2)catalyst(OAm-1)was synthesized via a self-assembly method with the assistance of a surfactant.OAm-1 possessed a large specific surface area of_(2)21 m2/g,abundant mesoporous structures and a large proportion of Mn(III).Further characterization exhibited that OAm-1 had abundant oxygen vacancies and excellent reducibility and conductivity.The adsorption and catalytic ability of OAm-1 were studied in the degradation of oxytetracycline(OTC)via the activation of hydrogen peroxide(H_(2)O_(2)).Through the radical quenching experiments,electron resonance spectroscopy(EPR),X-ray photoelectron spectroscopy(XPS)and Fourier-transform infrared spectroscopy(FT-IR)analysis,Mn(III)of OAm-1 was proved to be the active sites for the chemisorption of OTC.Systematic electrochemical ex-periments and analysis have shown that a process of electron transfer mediated by OAm-1 occurred be-tween the pollutant and H_(2)O_(2)during a Fenton-like reaction.This work experimentally verifies the elec-tron transfer process dominated nonradical mechanism overα-MnO_(2),which is helpful for understanding the catalytic mechanism of the Fenton-like oxidation.
基金the Invention Foundation of Science and Technology,Gansu Agriculture University of China(No.GAU-CX0527)the Young and Middle-aged Foundation of Science and Technology,Gansu Province of China(No.3YS061-A25-020)
文摘The oxidative degradation of aqueous carbofuran, a heavily used toxic carbamate insecticide by low temperature plasma, was investigated. The results show that the treatment efficiency increases with the increase in initial concentration. Raising the treatment temperature and changing the pH value can result in enhanced degradation of carbofuran in solution. The results also show that low temperature plasma treatment can effectively remove chemical oxygen demand (COD) of carbofuran in the solution.
文摘Treatment of biliverdin IXα dimethyl ester(2)with silver nitrate in alkaline solution gave two violin-like tripyrrione carbaldehydes,one de- graded at C15-C16,other at C4-C5.Biliverdin IXα(1),bilirubin IXα(3)and its dimethyl ester(4)gave the same results.
文摘In this work, the contribution of mediated oxidation mechanisms in the electrolytic degradation of cyanuric acid using boron-doped diamond(BDD) anodes was investigated in different electrolytes. A complete mineralization of cyanuric acid was obtained in Na Cl;however lower degrees of mineralization of 70% and 40% were obtained in Na2SO4 and Na Cl O4, respectively. This can be explained by the nature of the oxidants electrogenerated in each electrolyte. It is clear that the contribution of active chlorine(Cl2, HCl O, Cl O-)electrogenerated from oxidation of chlorides on BDD is much more important in the electrolytic degradation of cyanuric acid than the persulfate and hydroxyl radicals produced by electro-oxidation of sulfate and water on BDD anodes. This could be explained by the high affinity of active chlorine towards nitrogen compounds. No organic intermediates were detected during the electrolytic degradation of cyanuric acid in any the electrolytes, which can be explained by their immediate depletion by hydroxyl radicals produced on the BDD surface. Nitrates and ammonium were the final products of electrolytic degradation of cyanuric acid on BDD anodes in all electrolytes. In addition, small amounts of chloramines were formed in the chloride medium. Low current density(≤ 10 m A/cm2) and neutral medium(p H in the range 6–9) should be used for high efficiency electrolytic degradation and negligible formation of hazardous chlorate and perchlorate.
基金support from the Beijing Natural Science Foundation(No.JQ23035)。
文摘High-efficient rubber antioxidants for enhanced heat resistance without compromising mechanical properties remain an enormous and long-term challenge for the rubber industry.Herein,we employed the in-situ growth of Ce-doped Co-metal-organic framework(Ce Co-MOF)in dendritic mesoporous organosilica nanoparticles(DMONs@Ce Co-MOF,denoted as DCCM)to prepare a novel antioxidant that exhibit outstanding thermal stability.Dendritic mesoporous organosilica nanoparticles(DMONs)effectively alleviated the incompatibility of Ce Co-MOF in the polymer matrix,and the effective scavenging of free radicals was attributed to the various oxidation states of metal ions in Ce Co-MOF.Surprising,by adding only0.5 phr(parts per hundred of rubber)of DMONs@Ce Co-MOF to silicone rubber,(SR),the retention rate of tensile strength increased from 37.3%to 61.6%after aging 72 h at 250℃,and the retention rate of elongation at break of DCCM/SR1 composites reached 68%,which was 5.43 times of SR.The strategy of anchoring MOFs on the surface of silica also provides a viable method for preparing effective compound functionalized rubber antioxidant.
文摘Harnessing photocatalyzed hydrogen atom transfer(HAT)for the precise activation of C–H/O–H bonds is a pivotal yet challenging strategy to selectively drive oxidative C–C bond scission in renewable lignin,yielding value-added chemicals with exceptional selectivity.Herein,we present a metal-free photochemical strategy that enables selective C–C bond scission in lignin via a unique synergistic HAT pathway driven by triplet-excited 2-ethylanthraquinone(EAQ^(*))and hydroxyl radicals(•OH)generated in situ from EAQH_(2) and O_(2).Under simulated natural conditions,this process achieves a benzaldehyde yield of 146.6 mol%from a lignin-derived phenolic dimer.Mechanistic investigations reveal that preferential activation of the Cα-OH in lignin facilitates a tandem HAT process,forming alkoxy radical intermediates that undergoβ–scission to produce benzaldehyde,as corroborated by extensive control reactions and density functional theory calculations.Furthermore,this straightforward protocol efficiently cleaves the C–C bonds of technical kraft lignins,providing a rapid,scalable,and metal-free protocol for lignin valorization under mild conditions.
基金supported by the Fundamental Research Funds for the National Natural Science Foundation of China 52225003,22208021,22109004the National Key R&D Program of China 2022YFB4101702.
文摘Although supported solid amine adsorbents have attracted great attention for CO_(2) capture,critical chemical deactivation problems including oxidative degradation and urea formation have severely restricted their practical applications for flue gas CO_(2) capture.In this work,we reveal that the nature of surface hydroxyl groups(metal hydroxyl Al–OH and nonmetal hydroxyl Si–OH)plays a key role in the deactivation mechanisms.The polyethyleneimine(PEI)supported on Al–OH-containing substrates suffers from severe oxidative degradation during the CO_(2) capture step due to the breakage of amine-support hydrogen bonding networks,but exhibits an excellent anti-urea formation feature by preventing dehydration of carbamate products under a pure CO_(2) regeneration atmosphere.In contrast,PEI supported on Si–OHcontaining substrates exhibits excellent anti-oxidative stability under simulated flue gas conditions by forming a robust hydrogen bonding protective network with Si–OH,but suffers from obvious urea formation during the pure CO_(2) regeneration step.We also reveal that the urea formation problem for PEI-SBA-15 can be avoided by the incorporation of an OH-containing PEG additive.Based on the intrinsic understanding of degradation mechanisms,we successfully synthesized an adsorbent 40PEI-20PEG-SBA-15 that demonstrates outstanding stability and retention of a high CO_(2) capacity of 2.45 mmol g^(−1) over 1000 adsorption–desorption cycles,together with negligible capacity loss during aging in simulated flue gas(10%CO_(2)+5%O_(2)+3%H_(2)O)for one month at 60–70℃.We believe this work makes great contribution to the advancement in the field of ultra-stable solid amine-based CO_(2) capture materials.
基金funded by the UK Research Council EPSRC EP/009050/1。
文摘High-temperature proton exchange membrane fuel cells(HT-PEMFCs)are pursued worldwide as efficient energy conversion devices.Great efforts have been made in the area of designing and developing phosphoric acid(PA)-based proton exchange membrane(PEM)of HT-PEMFCs.This review focuses on recent advances in the limitations of acid-based PEM(acid leaching,oxidative degradation,and mechanical degradation)and the approaches mitigating the membrane degradation.Preparing multilayer or polymers with continuous network,adding hygroscopic inorganic materials,and introducing PA doping sites or covalent interactions with PA can effectively reduce acid leaching.Membrane oxidative degradation can be alleviated by synthesizing crosslinked or branched polymers,and introducing antioxidative groups or highly oxidative stable materials.Crosslinking to get a compact structure,blending with stable polymers and inorganic materials,preparing polymer with high molecular weight,and fabricating the polymer with PA doping sites away from backbones,are recommended to improve the membrane mechanical strength.Also,by comparing the running hours and decay rate,three current approaches,1.crosslinking via thermally curing or polymeric crosslinker,2.incorporating hygroscopic inorganic materials,3.increasing membrane layers or introducing strong basic groups and electron-withdrawing groups,have been concluded to be promising approaches to improve the durability of HT-PEMFCs.The overall aim of this review is to explore the existing degradation challenges and opportunities to serve as a solid basis for the deployment in the fuel cell market.