A new approach,named production of aryl oxygen-containing compounds from the catalytic pyrolysis of bagasse lignin(BL) over perovskite oxide,was proposed,A series of LaTixFe1-xO3(LTF-x) samples were prepared by the so...A new approach,named production of aryl oxygen-containing compounds from the catalytic pyrolysis of bagasse lignin(BL) over perovskite oxide,was proposed,A series of LaTixFe1-xO3(LTF-x) samples were prepared by the solid state reaction method.The crystal phase and morphology of LTF-x were characterized by XRD and SEM respectively.Catalytic pyrolysis performance of LTF-x was performed by TG-DTG and the distribution patterns of gaseous,liquid and solid products from BL was investigated using a fixed-bed micro-reactor.The optimal reaction conditions were determined:the pyrolysis temperature was 600℃,the mass ratio of mBL:mLTF-0.2 was 3:1,the veloeity of earrier gas was 100 ml·min-1.The gaseous produets were mainly eomposed of CO2,CO,CH4 and CnHm(n=2-4,m=2 n+2 or m=2 n),The main aryl oxygen-containing compounds in liquid products were phenolics,guaiacols,syringols and phenylates,the rest were benzenes,furans,esters and carboxylic acid.The total contents of aryl oxygencontaining compounds were from 62% up to more than 72% under the action of the perovskite.Moreover,the LTF-0.2 sample had nice regenerability.展开更多
To realize the resource and high-value utilization,a new approach,named bagasse lignin(BL) used to produce aryl oxygen-containing compounds by catalytic pyrolysis over perovskite,was proposed,LaTi0.2Fe0.8O3(LTF) sampl...To realize the resource and high-value utilization,a new approach,named bagasse lignin(BL) used to produce aryl oxygen-containing compounds by catalytic pyrolysis over perovskite,was proposed,LaTi0.2Fe0.8O3(LTF) samples prepared by the sol-gel method(SG) and the solid-state reaction method(SS)were characterized.The catalytic action on BL pyrolysis was performed by the test of TG-DTG and the evaluation of the fixed bed micro-reactor,the components and contents of the products were determined.The results show that LTF samples have cubic perovskite phase,LTF prepared by SG(LTF-SG) is porous with larger specific surface area than LTF prepared by SS(LTF-SS).During the pyrolysis of BL,the addition of LTF lowers the pyrolysis temperature and the activation energy,the contents of CO2 and CO in gaseous products reduce by 4.6%-8.0% and 30.7%-34.3%,respectively,the total content of aryl oxygencontaining compounds(including phenolics,guaiacols,syringols and phenylates) in liquid products increases from 62 wt% to more than 72 wt%,and LTF-SG shows better catalytic performance.LTF samples have nice phase and catalytic stabilities for BL pyrolysis after five successive redox cycles.展开更多
New descriptors were constructed and structures of some oxygen-containing organic compounds were parameterized. The multiple linear regression（MLR） and partial least squares regression（PLS） methods were employed t...New descriptors were constructed and structures of some oxygen-containing organic compounds were parameterized. The multiple linear regression（MLR） and partial least squares regression（PLS） methods were employed to build two relationship models between the structures and octanol/water partition coefficients（LogP） of the compounds. The modeling correlation coefficients（R） were 0.976 and 0.922, and the ＂leave one out＂ cross validation correlation coefficients（R（CV）） were 0.973 and 0.909, respectively. The results showed that the structural descriptors could well characterize the molecular structures of the compounds; the stability and predictive power of the models were good.展开更多
The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) i...The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) ion adsorption onto AC-T.The modified activated carbon is characterized by scanning electron microscopy,Fourier transform infrared spectroscopy(FT-IR) and X-ray photoelectron spectroscopy(XPS).The results of batch experiments indicate that the maximal adsorption could be achieved over the broad pH range of 4.5 to 6.5.Adsorption isotherms and kinetic study suggest that the sorption of Cd(Ⅱ) onto AC-T produces monolayer coverage and that adsorption is controlled by chemical adsorption.And the adsorbent has a good reusability.According to the FT-IR and XPS analyses,electrostatic attraction and cation exchange between Cd(Ⅱ) and oxygen-containing functional groups on AC-T are dominant mechanisms for Cd(Ⅱ) adsorption.展开更多
Oxygen-containing functional groups were found to e ectively boost the K^(+)storage performance of carbonaceous materials,however,the mechanism behind the performance enhancement remains unclear.Herein,we report highe...Oxygen-containing functional groups were found to e ectively boost the K^(+)storage performance of carbonaceous materials,however,the mechanism behind the performance enhancement remains unclear.Herein,we report higher rate capability and better long-term cycle performance employing oxygen-doped graphite oxide(GO)as the anode material for potassium ion batteries(PIBs),compared to the raw graphite.The in situ Raman spectroscopy elucidates the adsorption-intercalation hybrid K^(+)storage mechanism,assigning the capacity enhancement to be mainly correlated with reversible K^(+)adsorption/desorption at the newly introduced oxygen sites.It is unraveled that the C=O and COOH rather than C-O-C and OH groups contribute to the capacity enhancement.Based on in situ Fourier transform infrared(FT-IR)spectra and in situ electrochemical impedance spectroscopy(EIS),it is found that the oxygen-containing functional groups regulate the components of solid electrolyte interphase(SEI),leading to the formation of highly conductive,intact and robust SEI.Through the systematic investigations,we hereby uncover the K^(+)storage mechanism of GO-based PIB,and establish a clear relationship between the types/contents of oxygen functional groups and the regulated composition of SEI.展开更多
Stable adsorption and direct electrochemistry of glucose oxidase （COx） occurred on nitric acid （HNO3）-treated multi-walled carbon nanotubcs （MWNTs） instead of as-received MWNTs, demonstrating the critical roles ...Stable adsorption and direct electrochemistry of glucose oxidase （COx） occurred on nitric acid （HNO3）-treated multi-walled carbon nanotubcs （MWNTs） instead of as-received MWNTs, demonstrating the critical roles of oxygen-containing groups in stable adsorption and direct electrochemistry of GOx on carbon nanotubcs （CNTs）.展开更多
Quantitative structure-retention relationship （QSRR） model for the estimation of retention indices （RIs） of 39 oxygen-containing compounds containing ketones and esters was established by our newly introduced dist...Quantitative structure-retention relationship （QSRR） model for the estimation of retention indices （RIs） of 39 oxygen-containing compounds containing ketones and esters was established by our newly introduced distance-based atom-type indices DAI. The useful application of the novel DAI indices has been demonstrated by developing accurate predictive equations for gas chromatographic retention indices. The statistical results of the multiple linear regression for the final model are τ=0.9973 and s=8.23. Furthermore, an external test set of 10 oxo-containing compounds can be accurately predicted with the final equation giving the following statistical results： τpred：0.9966 and spred=8.56.展开更多
This review focused on the recent reports related to the function, characterization and modification of oxygen-containing surface groups of activated carbon (AC). The Oxygen-containing surface groups were briefly desc...This review focused on the recent reports related to the function, characterization and modification of oxygen-containing surface groups of activated carbon (AC). The Oxygen-containing surface groups were briefly described, and the most frequently used techniques for characterization of the oxygen-containing surface groups on ACs were also briefly stated. A detailed discussion of the effects of the oxygen-containing surface groups on the adsorptive capacity of AC was given. The recent progresses in modification of the oxygen-containing surface groups of AC were also reviewed.展开更多
In this study,impurity-free porous graphene(PG) with intrinsic pore structure was synthesized through a facile acid-alkali etching-assisted sonication approach.The pore structure appears on the surface of graphene she...In this study,impurity-free porous graphene(PG) with intrinsic pore structure was synthesized through a facile acid-alkali etching-assisted sonication approach.The pore structure appears on the surface of graphene sheets due to intrinsic defects of graphene.The PG possessed an extremely high specific surface area of 2184 m^2/g,the size of^5 μm and layer numbers of 3-8.Additionally,PG contained micropores and mesopores simultaneously,with an average pore diameter of approximately 3 nm.The effects of acid,alkali,and ultrasound treatment on PG preparation were elucidated by transmission electron microscopy and fourier transform infrared spectroscopy.First,in an acidic solution,oxygen-containing functional groups(hydroxyls,carboxyl,and epoxides) were formed due to the hydrolysis of sulfate and continuous transformations of these functional groups on graphene oxide.Second,under the synergistic effects of alkali and ultrasound treatment,PG was obtained due to the loss of carboxyl and epoxide groups.A new route for preparing PG was provided by the proposed method.展开更多
The synthetic parameters were changed to explore the formation mechanism of the oxygen-containing groups on the surfaces of the hypercrosslinked polymers. The FT-IR spectra and the Boehm titration were used to charact...The synthetic parameters were changed to explore the formation mechanism of the oxygen-containing groups on the surfaces of the hypercrosslinked polymers. The FT-IR spectra and the Boehm titration were used to characterize the surface chemistry of the synthesized polymers. The GC-MS was applied to analyze nitrobenzene which was the solvent in the reaction. The functionalities such as carbonyls and phenols were formed through the oxidation of residual chloromethyl groups by nitrobenzene and the carboxylic groups were formed through further oxidation by oxygen. The nitrobenzene was deoxidized to nitrosobenzene and further to aniline.展开更多
Layered polymer suffers from a transfer barrier of photogenerated carriers resulting from the lack of interlamellar connection channels and intralayer disorder.Herein,a layer-stacked crystalline carbon nitride nanorod...Layered polymer suffers from a transfer barrier of photogenerated carriers resulting from the lack of interlamellar connection channels and intralayer disorder.Herein,a layer-stacked crystalline carbon nitride nanorod resembling an accordion(A-CNR)grafted abundant interlamellar oxygen-containing groups is ingeniously designed to break through the transfer barrier between layers without inserting any extra impurities.Density functional theory reveals that electrons are enriched near the oxygencontaining groups,promoting the extension and coupling of interlayer electron clouds.This reduces the interlamellar electrostatic potential barrier from 5.38 to 2.74 e V.Remarkably,the groups not only establish interlayer bridges but also guide carriers to the bridge entrance,further enhancing interlayer carrier transfer.Additionally,the intralayer carrier separation and transfer are also improved,profiting from the asymmetrical charge distribution and high crystallinity.A-CNR exhibits impressive photoelectric properties and photocatalytic water disinfection capability.Within 18 min irradiation,over 10~6 colony-forming units(CFU)/mL of bacteria are completely inactivated.Moreover,A-CNR can be dispersed in water over a long period benefiting from the introduced oxygen-containing groups,making it suitable for photocatalysis in the aqueous phase.The work provides a feasible and effective strategy to overcome the inherent barrier of layered polymeric photocatalysts.展开更多
Renewable-energy-powered electrochemical CO or CO_(2)reduction reactions(CO_(2)RR)provide one of the most promising strategies to upgrade CO_(2)to valuable products.In the past decade,the existence and the mechanistic...Renewable-energy-powered electrochemical CO or CO_(2)reduction reactions(CO_(2)RR)provide one of the most promising strategies to upgrade CO_(2)to valuable products.In the past decade,the existence and the mechanistic role of oxygen-containing species,such as(sub)surface oxide,hydroxide and oxyhydroxide species,at the electrode–electrolyte interface under reductive conditions have emerged as a topic of acute discussion within the CO_(2)RR field.Oxide-derived Cu attracted the most attention,while other surfaces,including Au,Ag and Sn,were also widely investigated.This review identifies likely causes for contrasting results and views in the literature,summarizes possible oxygen sources for the interfacial oxygen-containing species at the CO_(2)RR conditions,and discusses potential roles these species could play in affecting the rate and product distribution.Finally,perspectives on future efforts to reveal the identity and role of oxygen-containing species in the CO_(2)RR are presented.展开更多
Metal-free electrocatalysts for the oxygen evolution reaction(OER)are gaining attention for their low cost,high conductivity,and moderate catalytic performance.While trace metal interference in assynthesized catalysts...Metal-free electrocatalysts for the oxygen evolution reaction(OER)are gaining attention for their low cost,high conductivity,and moderate catalytic performance.While trace metal interference in assynthesized catalysts has been ruled out,the impact of trace metal contamination during electrochemical activation remains unexplored.This study demonstrates that anodic pretreatment in alkaline electrolytes enhances the catalytic performance of carbon cloth.Specifically,carbon cloth activated in 8 mol/L Na OH achieves a current density of 10 m A/cm^(2)with an overpotential of only 338 m V,comparable to metalbased OER catalysts.Electrochemical and spectroscopic analyses show the deposition of Fe Ni O_(x)H_(y)oxyhydroxides(0.19±0.06μg/cm^(2))on specific sites of the carbon substrate during activation.These nanoparticles contribute significantly to the catalytic activity,with a synergistic effect between Fe Ni O_(x)H_(y)and the carbon substrate.The turnover frequency(TOF)for Fe correlates with the amount of C=O groups on the carbon substrate,providing evidence for an interfacial synergistic effect.This work emphasizes the importance of considering trace metal effects in metal-free catalyst evaluation and offers insights for the design of more efficient carbon-based hybrid OER catalysts.展开更多
Lignin-derived hard carbon shows potential as an anode material for sodium-ion batteries(SIBs)due to its high carbon content and aromatic structure,but its limited reversible adsorption sites and low conductivity hind...Lignin-derived hard carbon shows potential as an anode material for sodium-ion batteries(SIBs)due to its high carbon content and aromatic structure,but its limited reversible adsorption sites and low conductivity hinder performance.This study introduces a self-activation strategy to optimize carbon layer stacking and surface functional groups in microporous carbon,significantly enhancing sodium storage capacity and rate performance.By utilizing oxygen-containing functional groups in organic solvent lignin,we induce micropore formation during pyrolysis,effectively regulating graphite domains and closed pores structures without disrupting carbon layer growth.Unstacked graphene layers serve as efficient electron transport channels and expose additional adsorption sites,simultaneously increasing sodium storage capacity and intrinsic conductivity.The resultant S-OLHC demonstrates a remarkable sodium storage capacity of 358 mA h/g at 0.05 A/g after 200 cycles and maintains 231 mA h/g after 1000 cycles at 2 A/g.This strategy eliminates the need for additional pore-forming agents,offering a simpler,more efficient,and environmentally friendly approach compared to traditional activation methods.This work advances the rational design of high-performance biomass-derived hard carbon for SIBs by leveraging inherent structural characteristics and provides a sustainable low-carbon strategy for lignin valorization in renewable energy storage.展开更多
An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide （GO） at -0.8 V, which shows unique electrocatalytic activity toward tetracycline （TTC） det...An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide （GO） at -0.8 V, which shows unique electrocatalytic activity toward tetracycline （TTC） detection compared to the ERGO-12v （GO applied to a negative potential of-1.2 V）, GO, chemically reduced GO （CRGO）-modified glassy carbon electrode （GC） and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode （GC/ERGO-0.8v） were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared （FT-IR）, Raman, and X-ray photoelectron spectroscopies （XPS） demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.展开更多
LaTi(0.2)Fe(0.8)O3(LTF)was prepared by the sol-gel method,and the effects of calcination temperature on the structure and properties were investigated,A new method of preparing aryl oxygen-containing compounds from ba...LaTi(0.2)Fe(0.8)O3(LTF)was prepared by the sol-gel method,and the effects of calcination temperature on the structure and properties were investigated,A new method of preparing aryl oxygen-containing compounds from bagasse lignin(BL)by the catalytic pyrolysis over LTF was proposed.The results show that LTF has cubic crystal phase and porous structure and its optimal calcination temperature is 800℃(LTF-800).In the test for catalytic pyrolysis of BL,with the addition of LTF-800,the yield of liquid product reaches the maximum;the contents of phenolics,guaiacols,syringols,phenylates and furans increase obviously,while those of benzenes,esters and carboxylic acid decrease.The total content of aryl oxygencompounds(including phenolics,guaiacols,syringols and phenylates)in liquid product is more than 74 wt%with the addition of LTF-800,larger than that obtained by single BL pyrolysis(62 wt%).LTF could avoid oxygen-containing functional groups from being excessively destroyed.It has nice regeneration performance by controlled combustion of char even after 5 cycles.展开更多
Oxygen and nitrogen-functionalized carbon nanotubes （OCNTs and NCNTs） were applied as metal-free catalysts in selective olefin hydro- genation. A series of NCNTs was synthesized by NH3 post-treatment of OCNTs. Tempe...Oxygen and nitrogen-functionalized carbon nanotubes （OCNTs and NCNTs） were applied as metal-free catalysts in selective olefin hydro- genation. A series of NCNTs was synthesized by NH3 post-treatment of OCNTs. Temperature-programmed desorption, N2 physisorption, Raman spectroscopy, high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy were employed to characterize the surface properties of OCNTs and NCNTs, aiming at a detailed analysis of the type and amount of oxygen- and nitrogen-containing groups as well as surface defects. The gas-phase treatments applied for oxygen and nitrogen functionalization at elevated temperatures up to 600 ℃ led to the increase of surface defects, but did not cause structural damages in the bulk. NCNTs showed a clearly higher activity than the pristine CNTs and OCNTs in the hydrogenation of 1,5-cyclooctadiene, and also the selectivity to cyclooctene was higher. The favorable catalytic properties are ascribed to the nitrogen-containing surface functional groups as well as surface defects related to nitrogen species. In contrast, oxygen-containing surface groups and the surface defects caused by oxygen species did not show clear contribution to the hydrogenation catalysis.展开更多
Regenerated activated carbon(RAC)samples were prepared by carbon activation using waste activated carbon from solid waste resources as the carbon source precursor coupled with adding alkaline additives,and then were f...Regenerated activated carbon(RAC)samples were prepared by carbon activation using waste activated carbon from solid waste resources as the carbon source precursor coupled with adding alkaline additives,and then were further modified by potassium ferrate to finally prepare high-performance carbon for VOCs adsorption.At the same time,the samples before and after modification were systematically studied through characterization techniques such as SEM,Raman spectrometry,FT-IR,XPS,and dynamic/static adsorption.The results showed that the specific surface area and pore volume of the RAC after modification by the strong oxidant potassium ferrate increased by 1.4 times;the degree of defects was enhanced and the content of oxygen-containing functional groups on the surface increased significantly.Among them,the sample modified with potassium ferrate for 24 h had the best dynamic toluene adsorption performance(375.5 mg/g),and the dynamic adsorption capacity was twice that of the original sample(192.8 mg/g).The static adsorption test found that the maximum adsorption capacity of RAC-6%K_(2)FeO_(4)+H_(2)SO_(4)-24h was 796 mg/g,which indicated that the potassium ferrate modification treatment could significantly increase the VOCs adsorption performance of RAC.In addition,through consecutive toluene adsorption-desorption cycle tests,it was found that the RAC-6%K_(2)FeO_(4)+H_(2)SO_(4)-24h sample still retained 91%of adsorption activity after the fifth regeneration cycle.This indicates that RAC-6%K_(2)FeO_(4)+H_(2)SO_(4)-24h has good cycle stability and great application value for the efficient purification of industrial waste VOCs gas.展开更多
The low-temperature coal tar contains a considerable number of oxygen-containing compounds,which results in poor quality.The catalytic hydrodeoxygenation of oxygen-containing compound to an added-value chemical compou...The low-temperature coal tar contains a considerable number of oxygen-containing compounds,which results in poor quality.The catalytic hydrodeoxygenation of oxygen-containing compound to an added-value chemical compound is one of the most efficient methods to upgrade coal tar.In this study,density functional theory calculations are employed to assess and analyze in detail the hydrodeoxygenation of dibenzofuran,as a model compound of coal tar,on the Ni(111)surface.The obtained results indicate that dibenzofuran can be firstly hydrogenated to tetra hy d rod i be nzofura n and hexahydfodibenzofufan.The five-membered-ring opening reaction of tetrahydrodibenzofuran is more straightforward than that of hexahydrodibenzofuran(Ea=0.71 eV vs.1.66 eV).Then,both pathways generate an intermediate 2-cyclohexylphenoxy compound.One part of 2-cyclohexylphenoxy is hydrogenated to 2-cyclohexylphenol and consecutively hydrogenated to cyclohexylcyclohexanol,and another part is directly hydrogenated to cyclohexylcyclohexanone.The hydrogenated intermediates of2-cyclohexylphenol have higher deoxygenation barriers than 2-cyclohexylphenol and cyclohexylcy clohexanol.During the hydrogenation process of cyclohexylcyclohexanone to cyclohexylcyclohexanol,the intermediate 26,formed by adding H to O atom of cyclohexylcyclohexanone,exhibits the lowest deoxygenation barrier of 1.08 eV.High hydrogen coverage may promote the hydrogenation of tetrahydrodibenzofuran,hexahydrodibenzofuran,and intermediate 26 to generate dodecahydrodibenzofuran and cyclohexylcyclohexanol.This dibenzofuran hydrodeoxygenation reaction mechanism corroborates well with previous experimental results and provides a theoretical basis for further optimization of the design of nickel-based catalysts.展开更多
The positive-and negative-ion electrospray ionization(ESI)coupled with Fourier transform-ion cyclotron resonance mass spectrometry(FT-ICR MS)was employed to identify the chemical composition of heteroatomic compounds ...The positive-and negative-ion electrospray ionization(ESI)coupled with Fourier transform-ion cyclotron resonance mass spectrometry(FT-ICR MS)was employed to identify the chemical composition of heteroatomic compounds in four distillates of Fushun shale oil,and their catalytic cracking performance was investigated.There are nine classes of basic nitrogen compounds(BNCs)and eleven classes of non-basic heteroatomic compounds(NBHCs)in the different distillates.The dominant BNCs are mainly basic N1 class species.The dominant NBHCs are mainly acidic O2 and O1 class species in the300-350℃,350-400℃,and 400-450℃distillates,while the neutral N1,N1 O1 and N2 compounds become relatively abundant in the>450℃fraction.The basic N1 compounds and acidic O1 and O2 compounds are separated into different distillates by the degree of alkylation(different carbon number)but not by aromaticity(different double-bond equivalent values).The basic N1 O1 and N2 class species and neutral N1 and N2 class species are separated into different distillates by the degrees of both alkylation and aromaticity.After the catalytic cracking of Fushun shale oil,the classes of BNCs in the liquid products remain unchanged,while the classes and relative abundances of NBHCs vary significantly.展开更多
基金Supported by the National Natural Science Foundation of China,China(51674089)Heilongjiang Provincial Science Fund for Distinguished Youth Scholar(JC2018002)+2 种基金Heilongjiang Postdoctoral Scientific Research Development Fund of China(LBH-Q16037)the Youth Fund of Northeast Petroleum University(2018QNL-17)Postgraduate Innovative Research Projects of Northeast Petroleum University(YJSCX2017-014NEPU)
文摘A new approach,named production of aryl oxygen-containing compounds from the catalytic pyrolysis of bagasse lignin(BL) over perovskite oxide,was proposed,A series of LaTixFe1-xO3(LTF-x) samples were prepared by the solid state reaction method.The crystal phase and morphology of LTF-x were characterized by XRD and SEM respectively.Catalytic pyrolysis performance of LTF-x was performed by TG-DTG and the distribution patterns of gaseous,liquid and solid products from BL was investigated using a fixed-bed micro-reactor.The optimal reaction conditions were determined:the pyrolysis temperature was 600℃,the mass ratio of mBL:mLTF-0.2 was 3:1,the veloeity of earrier gas was 100 ml·min-1.The gaseous produets were mainly eomposed of CO2,CO,CH4 and CnHm(n=2-4,m=2 n+2 or m=2 n),The main aryl oxygen-containing compounds in liquid products were phenolics,guaiacols,syringols and phenylates,the rest were benzenes,furans,esters and carboxylic acid.The total contents of aryl oxygencontaining compounds were from 62% up to more than 72% under the action of the perovskite.Moreover,the LTF-0.2 sample had nice regenerability.
基金Project supported by National Natural Science Foundation of China(51674089)Heilongjiang Provincial Science Fund for Distinguished Youth Scholar(JC2018002)+2 种基金Postdoctoral Scientific Research Development Fund of Heilongjiang Province(LBH-Q16037)Postgraduate Innovative Research Project of Northeast Petroleum University(YJSCX2017-014NEPU)Youth Fund of Northeast Petroleum University(2018QNL-17)
文摘To realize the resource and high-value utilization,a new approach,named bagasse lignin(BL) used to produce aryl oxygen-containing compounds by catalytic pyrolysis over perovskite,was proposed,LaTi0.2Fe0.8O3(LTF) samples prepared by the sol-gel method(SG) and the solid-state reaction method(SS)were characterized.The catalytic action on BL pyrolysis was performed by the test of TG-DTG and the evaluation of the fixed bed micro-reactor,the components and contents of the products were determined.The results show that LTF samples have cubic perovskite phase,LTF prepared by SG(LTF-SG) is porous with larger specific surface area than LTF prepared by SS(LTF-SS).During the pyrolysis of BL,the addition of LTF lowers the pyrolysis temperature and the activation energy,the contents of CO2 and CO in gaseous products reduce by 4.6%-8.0% and 30.7%-34.3%,respectively,the total content of aryl oxygencontaining compounds(including phenolics,guaiacols,syringols and phenylates) in liquid products increases from 62 wt% to more than 72 wt%,and LTF-SG shows better catalytic performance.LTF samples have nice phase and catalytic stabilities for BL pyrolysis after five successive redox cycles.
基金supported by the Youth Foundation of Education Bureau,Sichuan Province(13ZB0003)
文摘New descriptors were constructed and structures of some oxygen-containing organic compounds were parameterized. The multiple linear regression（MLR） and partial least squares regression（PLS） methods were employed to build two relationship models between the structures and octanol/water partition coefficients（LogP） of the compounds. The modeling correlation coefficients（R） were 0.976 and 0.922, and the ＂leave one out＂ cross validation correlation coefficients（R（CV）） were 0.973 and 0.909, respectively. The results showed that the structural descriptors could well characterize the molecular structures of the compounds; the stability and predictive power of the models were good.
基金Supported by the Fundamental Research Funds for the Central Universities(TD2013-2,2012LYB33)the National Natural Science Foundation of China(51278053,21373032)grant-in-aid from Kochi University of Technology and China Scholarship Council
文摘The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) ion adsorption onto AC-T.The modified activated carbon is characterized by scanning electron microscopy,Fourier transform infrared spectroscopy(FT-IR) and X-ray photoelectron spectroscopy(XPS).The results of batch experiments indicate that the maximal adsorption could be achieved over the broad pH range of 4.5 to 6.5.Adsorption isotherms and kinetic study suggest that the sorption of Cd(Ⅱ) onto AC-T produces monolayer coverage and that adsorption is controlled by chemical adsorption.And the adsorbent has a good reusability.According to the FT-IR and XPS analyses,electrostatic attraction and cation exchange between Cd(Ⅱ) and oxygen-containing functional groups on AC-T are dominant mechanisms for Cd(Ⅱ) adsorption.
基金financially supported by the National Natural Science Foundation of China(51802091,51902102,22075074)Outstanding Young Scientists Research Funds from Hunan Province(2020JJ2004)+2 种基金Major Science and Technology Program of Hunan Province(2020WK2013)Creative Research Funds from Hunan Province(2018RS3046)Natural Science Foundation of Hunan Province(2020JJ5035)。
文摘Oxygen-containing functional groups were found to e ectively boost the K^(+)storage performance of carbonaceous materials,however,the mechanism behind the performance enhancement remains unclear.Herein,we report higher rate capability and better long-term cycle performance employing oxygen-doped graphite oxide(GO)as the anode material for potassium ion batteries(PIBs),compared to the raw graphite.The in situ Raman spectroscopy elucidates the adsorption-intercalation hybrid K^(+)storage mechanism,assigning the capacity enhancement to be mainly correlated with reversible K^(+)adsorption/desorption at the newly introduced oxygen sites.It is unraveled that the C=O and COOH rather than C-O-C and OH groups contribute to the capacity enhancement.Based on in situ Fourier transform infrared(FT-IR)spectra and in situ electrochemical impedance spectroscopy(EIS),it is found that the oxygen-containing functional groups regulate the components of solid electrolyte interphase(SEI),leading to the formation of highly conductive,intact and robust SEI.Through the systematic investigations,we hereby uncover the K^(+)storage mechanism of GO-based PIB,and establish a clear relationship between the types/contents of oxygen functional groups and the regulated composition of SEI.
基金This research is supported by the National Natural Science Foundation of China(Nos.30370397 and 60571042).
文摘Stable adsorption and direct electrochemistry of glucose oxidase （COx） occurred on nitric acid （HNO3）-treated multi-walled carbon nanotubcs （MWNTs） instead of as-received MWNTs, demonstrating the critical roles of oxygen-containing groups in stable adsorption and direct electrochemistry of GOx on carbon nanotubcs （CNTs）.
文摘Quantitative structure-retention relationship （QSRR） model for the estimation of retention indices （RIs） of 39 oxygen-containing compounds containing ketones and esters was established by our newly introduced distance-based atom-type indices DAI. The useful application of the novel DAI indices has been demonstrated by developing accurate predictive equations for gas chromatographic retention indices. The statistical results of the multiple linear regression for the final model are τ=0.9973 and s=8.23. Furthermore, an external test set of 10 oxo-containing compounds can be accurately predicted with the final equation giving the following statistical results： τpred：0.9966 and spred=8.56.
基金National Natural Science Foundation of China (No. 20336020) and Science Foundation of Guangdong Province of China (2002C32103).
文摘This review focused on the recent reports related to the function, characterization and modification of oxygen-containing surface groups of activated carbon (AC). The Oxygen-containing surface groups were briefly described, and the most frequently used techniques for characterization of the oxygen-containing surface groups on ACs were also briefly stated. A detailed discussion of the effects of the oxygen-containing surface groups on the adsorptive capacity of AC was given. The recent progresses in modification of the oxygen-containing surface groups of AC were also reviewed.
基金financially supported by the National Natural Science Foundation of China (Nos.11765010,51704136)the Applied Basic Research Programs of Yunnan Provincial Science and Technology Department (No.2016FB087)the Freely Exploring Fund for Academicians in Yunnan Province (No.2018HA006)
文摘In this study,impurity-free porous graphene(PG) with intrinsic pore structure was synthesized through a facile acid-alkali etching-assisted sonication approach.The pore structure appears on the surface of graphene sheets due to intrinsic defects of graphene.The PG possessed an extremely high specific surface area of 2184 m^2/g,the size of^5 μm and layer numbers of 3-8.Additionally,PG contained micropores and mesopores simultaneously,with an average pore diameter of approximately 3 nm.The effects of acid,alkali,and ultrasound treatment on PG preparation were elucidated by transmission electron microscopy and fourier transform infrared spectroscopy.First,in an acidic solution,oxygen-containing functional groups(hydroxyls,carboxyl,and epoxides) were formed due to the hydrolysis of sulfate and continuous transformations of these functional groups on graphene oxide.Second,under the synergistic effects of alkali and ultrasound treatment,PG was obtained due to the loss of carboxyl and epoxide groups.A new route for preparing PG was provided by the proposed method.
文摘The synthetic parameters were changed to explore the formation mechanism of the oxygen-containing groups on the surfaces of the hypercrosslinked polymers. The FT-IR spectra and the Boehm titration were used to characterize the surface chemistry of the synthesized polymers. The GC-MS was applied to analyze nitrobenzene which was the solvent in the reaction. The functionalities such as carbonyls and phenols were formed through the oxidation of residual chloromethyl groups by nitrobenzene and the carboxylic groups were formed through further oxidation by oxygen. The nitrobenzene was deoxidized to nitrosobenzene and further to aniline.
基金supported by the National Natural Science Foundation of China(52103315)the Natural Science Foundation of Jiangsu(BK20221270)+3 种基金the Science and Technology Program of Suzhou(SS202113)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_0703)the Open Project of Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province(CSPC202310)the Industrial Guided Development Project of Suzhou Yangcheng Lake。
文摘Layered polymer suffers from a transfer barrier of photogenerated carriers resulting from the lack of interlamellar connection channels and intralayer disorder.Herein,a layer-stacked crystalline carbon nitride nanorod resembling an accordion(A-CNR)grafted abundant interlamellar oxygen-containing groups is ingeniously designed to break through the transfer barrier between layers without inserting any extra impurities.Density functional theory reveals that electrons are enriched near the oxygencontaining groups,promoting the extension and coupling of interlayer electron clouds.This reduces the interlamellar electrostatic potential barrier from 5.38 to 2.74 e V.Remarkably,the groups not only establish interlayer bridges but also guide carriers to the bridge entrance,further enhancing interlayer carrier transfer.Additionally,the intralayer carrier separation and transfer are also improved,profiting from the asymmetrical charge distribution and high crystallinity.A-CNR exhibits impressive photoelectric properties and photocatalytic water disinfection capability.Within 18 min irradiation,over 10~6 colony-forming units(CFU)/mL of bacteria are completely inactivated.Moreover,A-CNR can be dispersed in water over a long period benefiting from the introduced oxygen-containing groups,making it suitable for photocatalysis in the aqueous phase.The work provides a feasible and effective strategy to overcome the inherent barrier of layered polymeric photocatalysts.
基金supported by Beijing National Laboratory for Molecular Sciences and the National Natural Science Foundation of China(21872079)。
文摘Renewable-energy-powered electrochemical CO or CO_(2)reduction reactions(CO_(2)RR)provide one of the most promising strategies to upgrade CO_(2)to valuable products.In the past decade,the existence and the mechanistic role of oxygen-containing species,such as(sub)surface oxide,hydroxide and oxyhydroxide species,at the electrode–electrolyte interface under reductive conditions have emerged as a topic of acute discussion within the CO_(2)RR field.Oxide-derived Cu attracted the most attention,while other surfaces,including Au,Ag and Sn,were also widely investigated.This review identifies likely causes for contrasting results and views in the literature,summarizes possible oxygen sources for the interfacial oxygen-containing species at the CO_(2)RR conditions,and discusses potential roles these species could play in affecting the rate and product distribution.Finally,perspectives on future efforts to reveal the identity and role of oxygen-containing species in the CO_(2)RR are presented.
基金financially supported by the National Natural Science Foundation of China(No.22479097)the Shanghai Science and Technology Committee(Nos.23ZR1433000 and 22511100400)+1 种基金the National High-Level Talent Program for Young Scholarsthe Start-up Fund(F.Song)from Shanghai Jiao Tong University。
文摘Metal-free electrocatalysts for the oxygen evolution reaction(OER)are gaining attention for their low cost,high conductivity,and moderate catalytic performance.While trace metal interference in assynthesized catalysts has been ruled out,the impact of trace metal contamination during electrochemical activation remains unexplored.This study demonstrates that anodic pretreatment in alkaline electrolytes enhances the catalytic performance of carbon cloth.Specifically,carbon cloth activated in 8 mol/L Na OH achieves a current density of 10 m A/cm^(2)with an overpotential of only 338 m V,comparable to metalbased OER catalysts.Electrochemical and spectroscopic analyses show the deposition of Fe Ni O_(x)H_(y)oxyhydroxides(0.19±0.06μg/cm^(2))on specific sites of the carbon substrate during activation.These nanoparticles contribute significantly to the catalytic activity,with a synergistic effect between Fe Ni O_(x)H_(y)and the carbon substrate.The turnover frequency(TOF)for Fe correlates with the amount of C=O groups on the carbon substrate,providing evidence for an interfacial synergistic effect.This work emphasizes the importance of considering trace metal effects in metal-free catalyst evaluation and offers insights for the design of more efficient carbon-based hybrid OER catalysts.
基金supported by the National Natural Science Foundation of China(22278155,U23A6005)。
文摘Lignin-derived hard carbon shows potential as an anode material for sodium-ion batteries(SIBs)due to its high carbon content and aromatic structure,but its limited reversible adsorption sites and low conductivity hinder performance.This study introduces a self-activation strategy to optimize carbon layer stacking and surface functional groups in microporous carbon,significantly enhancing sodium storage capacity and rate performance.By utilizing oxygen-containing functional groups in organic solvent lignin,we induce micropore formation during pyrolysis,effectively regulating graphite domains and closed pores structures without disrupting carbon layer growth.Unstacked graphene layers serve as efficient electron transport channels and expose additional adsorption sites,simultaneously increasing sodium storage capacity and intrinsic conductivity.The resultant S-OLHC demonstrates a remarkable sodium storage capacity of 358 mA h/g at 0.05 A/g after 200 cycles and maintains 231 mA h/g after 1000 cycles at 2 A/g.This strategy eliminates the need for additional pore-forming agents,offering a simpler,more efficient,and environmentally friendly approach compared to traditional activation methods.This work advances the rational design of high-performance biomass-derived hard carbon for SIBs by leveraging inherent structural characteristics and provides a sustainable low-carbon strategy for lignin valorization in renewable energy storage.
基金supported by the National Natural Science Foundation of China(21007033)the Fundamental Research Funds of Shandong University(2015JC017)~~
文摘An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide （GO） at -0.8 V, which shows unique electrocatalytic activity toward tetracycline （TTC） detection compared to the ERGO-12v （GO applied to a negative potential of-1.2 V）, GO, chemically reduced GO （CRGO）-modified glassy carbon electrode （GC） and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode （GC/ERGO-0.8v） were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared （FT-IR）, Raman, and X-ray photoelectron spectroscopies （XPS） demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.
基金Project supported by the National Natural Science Foundation of China(51674089)Heilongjiang Provincial Science Fund for Distinguished Youth Scholar(JC2018002)+1 种基金Postdoctoral Scientific Research Development Fund of Heilongjiang Province(LBH-Q16037)Postgraduate Innovative Research Projects of Northeast Petroleum University(YJSCX2017-014NEPU)
文摘LaTi(0.2)Fe(0.8)O3(LTF)was prepared by the sol-gel method,and the effects of calcination temperature on the structure and properties were investigated,A new method of preparing aryl oxygen-containing compounds from bagasse lignin(BL)by the catalytic pyrolysis over LTF was proposed.The results show that LTF has cubic crystal phase and porous structure and its optimal calcination temperature is 800℃(LTF-800).In the test for catalytic pyrolysis of BL,with the addition of LTF-800,the yield of liquid product reaches the maximum;the contents of phenolics,guaiacols,syringols,phenylates and furans increase obviously,while those of benzenes,esters and carboxylic acid decrease.The total content of aryl oxygencompounds(including phenolics,guaiacols,syringols and phenylates)in liquid product is more than 74 wt%with the addition of LTF-800,larger than that obtained by single BL pyrolysis(62 wt%).LTF could avoid oxygen-containing functional groups from being excessively destroyed.It has nice regeneration performance by controlled combustion of char even after 5 cycles.
基金supported by the German Federal Ministry of Education and Research (BMBF) for the CarboKat Project (03X0204D) within the scope of the Inno.CNT Alliance
文摘Oxygen and nitrogen-functionalized carbon nanotubes （OCNTs and NCNTs） were applied as metal-free catalysts in selective olefin hydro- genation. A series of NCNTs was synthesized by NH3 post-treatment of OCNTs. Temperature-programmed desorption, N2 physisorption, Raman spectroscopy, high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy were employed to characterize the surface properties of OCNTs and NCNTs, aiming at a detailed analysis of the type and amount of oxygen- and nitrogen-containing groups as well as surface defects. The gas-phase treatments applied for oxygen and nitrogen functionalization at elevated temperatures up to 600 ℃ led to the increase of surface defects, but did not cause structural damages in the bulk. NCNTs showed a clearly higher activity than the pristine CNTs and OCNTs in the hydrogenation of 1,5-cyclooctadiene, and also the selectivity to cyclooctene was higher. The favorable catalytic properties are ascribed to the nitrogen-containing surface functional groups as well as surface defects related to nitrogen species. In contrast, oxygen-containing surface groups and the surface defects caused by oxygen species did not show clear contribution to the hydrogenation catalysis.
基金financialy supported by the National Natural Science Foundation of China (No.21936005,52070114,21876093)the Postdoctoral Science Program of China (No.2019M660061)
文摘Regenerated activated carbon(RAC)samples were prepared by carbon activation using waste activated carbon from solid waste resources as the carbon source precursor coupled with adding alkaline additives,and then were further modified by potassium ferrate to finally prepare high-performance carbon for VOCs adsorption.At the same time,the samples before and after modification were systematically studied through characterization techniques such as SEM,Raman spectrometry,FT-IR,XPS,and dynamic/static adsorption.The results showed that the specific surface area and pore volume of the RAC after modification by the strong oxidant potassium ferrate increased by 1.4 times;the degree of defects was enhanced and the content of oxygen-containing functional groups on the surface increased significantly.Among them,the sample modified with potassium ferrate for 24 h had the best dynamic toluene adsorption performance(375.5 mg/g),and the dynamic adsorption capacity was twice that of the original sample(192.8 mg/g).The static adsorption test found that the maximum adsorption capacity of RAC-6%K_(2)FeO_(4)+H_(2)SO_(4)-24h was 796 mg/g,which indicated that the potassium ferrate modification treatment could significantly increase the VOCs adsorption performance of RAC.In addition,through consecutive toluene adsorption-desorption cycle tests,it was found that the RAC-6%K_(2)FeO_(4)+H_(2)SO_(4)-24h sample still retained 91%of adsorption activity after the fifth regeneration cycle.This indicates that RAC-6%K_(2)FeO_(4)+H_(2)SO_(4)-24h has good cycle stability and great application value for the efficient purification of industrial waste VOCs gas.
基金financial support from the National Key Research and Development Program of China(2016YFB0600305)National Natural Science Foundation of China(21808153,22078220)。
文摘The low-temperature coal tar contains a considerable number of oxygen-containing compounds,which results in poor quality.The catalytic hydrodeoxygenation of oxygen-containing compound to an added-value chemical compound is one of the most efficient methods to upgrade coal tar.In this study,density functional theory calculations are employed to assess and analyze in detail the hydrodeoxygenation of dibenzofuran,as a model compound of coal tar,on the Ni(111)surface.The obtained results indicate that dibenzofuran can be firstly hydrogenated to tetra hy d rod i be nzofura n and hexahydfodibenzofufan.The five-membered-ring opening reaction of tetrahydrodibenzofuran is more straightforward than that of hexahydrodibenzofuran(Ea=0.71 eV vs.1.66 eV).Then,both pathways generate an intermediate 2-cyclohexylphenoxy compound.One part of 2-cyclohexylphenoxy is hydrogenated to 2-cyclohexylphenol and consecutively hydrogenated to cyclohexylcyclohexanol,and another part is directly hydrogenated to cyclohexylcyclohexanone.The hydrogenated intermediates of2-cyclohexylphenol have higher deoxygenation barriers than 2-cyclohexylphenol and cyclohexylcy clohexanol.During the hydrogenation process of cyclohexylcyclohexanone to cyclohexylcyclohexanol,the intermediate 26,formed by adding H to O atom of cyclohexylcyclohexanone,exhibits the lowest deoxygenation barrier of 1.08 eV.High hydrogen coverage may promote the hydrogenation of tetrahydrodibenzofuran,hexahydrodibenzofuran,and intermediate 26 to generate dodecahydrodibenzofuran and cyclohexylcyclohexanol.This dibenzofuran hydrodeoxygenation reaction mechanism corroborates well with previous experimental results and provides a theoretical basis for further optimization of the design of nickel-based catalysts.
基金supported by the National Natural Science Foundation of China(21776312)。
文摘The positive-and negative-ion electrospray ionization(ESI)coupled with Fourier transform-ion cyclotron resonance mass spectrometry(FT-ICR MS)was employed to identify the chemical composition of heteroatomic compounds in four distillates of Fushun shale oil,and their catalytic cracking performance was investigated.There are nine classes of basic nitrogen compounds(BNCs)and eleven classes of non-basic heteroatomic compounds(NBHCs)in the different distillates.The dominant BNCs are mainly basic N1 class species.The dominant NBHCs are mainly acidic O2 and O1 class species in the300-350℃,350-400℃,and 400-450℃distillates,while the neutral N1,N1 O1 and N2 compounds become relatively abundant in the>450℃fraction.The basic N1 compounds and acidic O1 and O2 compounds are separated into different distillates by the degree of alkylation(different carbon number)but not by aromaticity(different double-bond equivalent values).The basic N1 O1 and N2 class species and neutral N1 and N2 class species are separated into different distillates by the degrees of both alkylation and aromaticity.After the catalytic cracking of Fushun shale oil,the classes of BNCs in the liquid products remain unchanged,while the classes and relative abundances of NBHCs vary significantly.
