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
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
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
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
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
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
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
The oxygen-containing functional groups in disordered carbon anodes have been widely reported to influence the Na storage performance.However,the effect of original oxygen-containing groups in the precursors on the fi...The oxygen-containing functional groups in disordered carbon anodes have been widely reported to influence the Na storage performance.However,the effect of original oxygen-containing groups in the precursors on the final structures and electrochemical performance is rarely studied.Herein,we used the anthraquinone derivatives with different oxygen-containing functional groups as precursors to make the disordered carbon anodes for Na-ion batteries(NIBs).Through comprehensive structural and electrochemical analyses,we found that the different types of functional groups in carbon precursors directly affect the cross-linking process during carbonization.The original precursors containing enough inter-chain oxygen or oxygen-containing functional groups with unsaturated bonds unattached to the ring are beneficial for the oxygen atoms to remain or cross-link in structure to result in more C–O–C group,forming nanovoids and disordered structure,which then determine the high performance of the carbon anodes in NIBs.This work highlights the importance of the type/content of functional groups in precursor and provides guidance for the future design of carbon anodes in NIBs from the perspective of precursor selection.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
An interfacially active cobalt complex,cobalt dodecylbenzenesulfonate,was synthesized.Elemental analysis,atomic absorption spectroscopy,Fourier transform infrared spectroscopy(FT-IR),thermogravimetric analysis,and s...An interfacially active cobalt complex,cobalt dodecylbenzenesulfonate,was synthesized.Elemental analysis,atomic absorption spectroscopy,Fourier transform infrared spectroscopy(FT-IR),thermogravimetric analysis,and surface/interfacial tension determination were performed to investigate the properties of the catalyst.Results showed that the synthesized catalyst showed active interfacial behavior,decreasing the surface tension and interfacial tension between heavy oil and liquid phase to below 30 and 1.5 mN/m,respectively.The catalyst was not thermally degraded at a temperature of 400 ℃,indicating its high thermal stability.Catalytic performance of the catalyst was evaluated by carrying out aquathermolysis.The viscosity determination showed that the viscosity of the heavy oil decreased by 38%.The average molecular weight,group compositions,and average molecular structure of various samples were analyzed using elemental analysis,FT-IR,electrospray ionization Fourier transform ion cyclotron resonance(ESI FT-ICR MS),and ~1H nuclear magnetic resonance.Results indicated that the catalyst could attack the sulfur- and O_2-type heteroatomic compounds in asphaltene and resin,especially the compounds with aromatic structure,leading to a decrease in the molecular weight and then the reduction in the viscosity of heavy oil.Therefore,the synthesized catalyst might find an application in catalytic aquathermolysis of heavy oil,especially for the high-aromaticity heavy oil with high oxygen content.展开更多
The systematical study about side reactions have revealed the formation mechanism of oxygen-containing groups of hypercrosslinked polymers. Surface chemistry and functionality of the polymers are characterized by Four...The systematical study about side reactions have revealed the formation mechanism of oxygen-containing groups of hypercrosslinked polymers. Surface chemistry and functionality of the polymers are characterized by Fourier-transform infrared spectroscopy (FT-IR), solid state nuclear magnetic resonance (NMR) and contact angle. The results showed that the ether groups were from chloromethylated reaction, and the alcohol groups arose from partial hydrolysis of chloromethyl groups during the post-crosslinking reaction, and the carbonyl functionality was formed by further oxidation of the alcohol groups. Catalyst and solvent used in the postcrosslinking reaction would greatly influence the surface chemistry of the polymer.展开更多
Water pollution caused by dye is a serious challenge.Herein,we use a novel discharge process to functionalize carbon nanotube(CNT)by COOH groups to form CNT30 for removing methyl red(MR)from water.By pristine CNT,75%M...Water pollution caused by dye is a serious challenge.Herein,we use a novel discharge process to functionalize carbon nanotube(CNT)by COOH groups to form CNT30 for removing methyl red(MR)from water.By pristine CNT,75%MR is removed in 60 min,with an adsorption capacity of 68.44 mg g-1.By CNT30,85%MR is fast removed in only 5 min,and the removal efficiency reaches to 95%after 30 min,with an adsorption capacity of80.33 mg g-1.Thus,a higher MR removal efficiency is achieved in a much shorter time on CNT30.Moreover,CNT30 has an outstanding reusability,with the MR removal efficiency decreasing by only 7%after ten cycles.The COOH groups on CNT30 improve the hydrophilicity of CNT30,thus promoting the interaction of MR in water with CNT30.The hydrogen bonding and electrostatic interaction of MR with the COOH groups on CNT30 could be the force to drive MR adsorption on CNT30.The higher COOH content could be the origin for the better performance of CNT30 in removing dye from water.The discharge process developed herein is operated in O2,without using harmful substances,and the COOH content on CNT can be efficiently tuned by simply changing discharge time.This is different from the chemical modification widely used to functionalize CNT by strong oxidants,e.g.,HNO_(3).The present work is of great significance to realize green construction of materials for more efficiently removing dye from water.展开更多
The evolution of pore structure and functional groups of coal char in different stages of Shenhua coal combustion process in O_(2)/CO_(2)atmosphere was studied by the low temperature nitrogen adsorption method,the sca...The evolution of pore structure and functional groups of coal char in different stages of Shenhua coal combustion process in O_(2)/CO_(2)atmosphere was studied by the low temperature nitrogen adsorption method,the scanning electron microscopy and the FTIR method.The relationship between the pore structure,oxygen-containing functional groups and NO generation characteristics of coal char under different inlet oxygen concentrations was analyzed.The result shows that the overall pore structure and shape of pulverized coal particles change continuously with the combustion;and the oxygen-containing functional groups on the surface of coal char indicate multi-peak changes and are related to NO generation.The oxygen concentration poses a larger impact on the change in coal particle size,oxygen-containing functional groups and NO generation;and there is an oxygen concentration that optimizes the reduction effect of the oxygen-containing functional group on NO.展开更多
Many types of sustainably-prepared functional biochar catalysts are needed to transform biomass substrates into platform chemicals.In this work,weak-acid biochar catalysts were prepared by mix ball-milled(10 min,isoth...Many types of sustainably-prepared functional biochar catalysts are needed to transform biomass substrates into platform chemicals.In this work,weak-acid biochar catalysts were prepared by mix ball-milled(10 min,isothermal,room temperature)cherry blossom tree leaf biomass(BM)with humic acid(H)prior to carbonization of samples for 1 h under nitrogen gas.Characterization of the as-prepared materials(HBM-carbonization temperature in℃)showed that humic acid activated the biochars and increased their number of oxygen-containing functional(-COOH,OH)groups.The weak-acid biochars were applied as heterogeneous catalysts for dehydration of fructose to 5-hydroxymethylfurfural(5-HMF),where it was found that biochar catalyst,HBM-400,gave 100%fructose conversion and 77.5%5-HMF yields in an ionic liquid(1-butyl-3-methylimidazolium chloride)reaction system(140℃,60 min reaction time).As-prepared HBM-400 biochars exhibited constant catalytic activity for fructose dehydration with repeated use without any type of reactivation treatment and were stable for 5 cycles.Humic acid is an effective additive for preparing weak-acid catalytic materials from waste biomass.展开更多
Electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))through two-electron oxygen reduction represents an attractive alternative for on-site H_(2)O_(2) generation.Here,we develop a facile thermally activatedpersul...Electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))through two-electron oxygen reduction represents an attractive alternative for on-site H_(2)O_(2) generation.Here,we develop a facile thermally activatedpersulfate approach to obtain oxidized carbon nanotubes(O-CNTs-x,x represents oxidation time)with enhanced H_(2)O_(2) electrosynthesis performance.Electrochemical studies have demonstrated that the optimized O-CNTs-6(i.e.,oxidation time is 6 h)could deliver a sustained high selectivity of around 92%for H_(2)O_(2) over a wide voltage window in 0.1 mol/L KOH and a high H_(2)O_(2) production rate of 296.84 mmol/L g^(-1) cat h^(-1).Compared with pristine CNTs,the enhanced catalytic activity primarily stems from the newly-generated oxygen-containing functional groups and some defects created on the surface of O-CNTs-x.Importantly,the proposed oxidation process is proved to be valid for promoting H_(2)O_(2) electrosynthesis performance of the Ketjen black.This study provides an universal oxidation method to obtain highly active carbon-based catalysts and initiates new opportunities for the exploration of highperformance electrosynthesis H_(2)O_(2) catalysts.展开更多
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).
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.
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.
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supported by the National Key Research and Development Program of China(No.2022YFB3807800)the National Natural Science Foundation(NSFC)of China(Nos.52122214 and 52072403)+1 种基金Youth Innovation Promotion Association of the Chinese Academy of Sciences(CAS)(No.2020006)One Hundred Talent Project of Institute of Physics,CAS.
文摘The oxygen-containing functional groups in disordered carbon anodes have been widely reported to influence the Na storage performance.However,the effect of original oxygen-containing groups in the precursors on the final structures and electrochemical performance is rarely studied.Herein,we used the anthraquinone derivatives with different oxygen-containing functional groups as precursors to make the disordered carbon anodes for Na-ion batteries(NIBs).Through comprehensive structural and electrochemical analyses,we found that the different types of functional groups in carbon precursors directly affect the cross-linking process during carbonization.The original precursors containing enough inter-chain oxygen or oxygen-containing functional groups with unsaturated bonds unattached to the ring are beneficial for the oxygen atoms to remain or cross-link in structure to result in more C–O–C group,forming nanovoids and disordered structure,which then determine the high performance of the carbon anodes in NIBs.This work highlights the importance of the type/content of functional groups in precursor and provides guidance for the future design of carbon anodes in NIBs from the perspective of precursor selection.
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the financial support from the Key Programs of Science and Technology of SINPOEC (Grant No. P11093)
文摘An interfacially active cobalt complex,cobalt dodecylbenzenesulfonate,was synthesized.Elemental analysis,atomic absorption spectroscopy,Fourier transform infrared spectroscopy(FT-IR),thermogravimetric analysis,and surface/interfacial tension determination were performed to investigate the properties of the catalyst.Results showed that the synthesized catalyst showed active interfacial behavior,decreasing the surface tension and interfacial tension between heavy oil and liquid phase to below 30 and 1.5 mN/m,respectively.The catalyst was not thermally degraded at a temperature of 400 ℃,indicating its high thermal stability.Catalytic performance of the catalyst was evaluated by carrying out aquathermolysis.The viscosity determination showed that the viscosity of the heavy oil decreased by 38%.The average molecular weight,group compositions,and average molecular structure of various samples were analyzed using elemental analysis,FT-IR,electrospray ionization Fourier transform ion cyclotron resonance(ESI FT-ICR MS),and ~1H nuclear magnetic resonance.Results indicated that the catalyst could attack the sulfur- and O_2-type heteroatomic compounds in asphaltene and resin,especially the compounds with aromatic structure,leading to a decrease in the molecular weight and then the reduction in the viscosity of heavy oil.Therefore,the synthesized catalyst might find an application in catalytic aquathermolysis of heavy oil,especially for the high-aromaticity heavy oil with high oxygen content.
基金The Project Supported by:NSFC of PR China (50778088)National "863 Resource and Environment" Funding of PR China (2006AA06Z383)National Excellent Young Scientists (50825802).
文摘The systematical study about side reactions have revealed the formation mechanism of oxygen-containing groups of hypercrosslinked polymers. Surface chemistry and functionality of the polymers are characterized by Fourier-transform infrared spectroscopy (FT-IR), solid state nuclear magnetic resonance (NMR) and contact angle. The results showed that the ether groups were from chloromethylated reaction, and the alcohol groups arose from partial hydrolysis of chloromethyl groups during the post-crosslinking reaction, and the carbonyl functionality was formed by further oxidation of the alcohol groups. Catalyst and solvent used in the postcrosslinking reaction would greatly influence the surface chemistry of the polymer.
基金supported by the National Natural Science Foundation of China(Grant Nos.21922807 and 22078193)Double Thousand Plan of Jiangxi Province(461654,jxsq2019102052)Shaanxi Provincial Key Research and Development Program(Grant No.2020ZDLGY11-06)。
文摘Water pollution caused by dye is a serious challenge.Herein,we use a novel discharge process to functionalize carbon nanotube(CNT)by COOH groups to form CNT30 for removing methyl red(MR)from water.By pristine CNT,75%MR is removed in 60 min,with an adsorption capacity of 68.44 mg g-1.By CNT30,85%MR is fast removed in only 5 min,and the removal efficiency reaches to 95%after 30 min,with an adsorption capacity of80.33 mg g-1.Thus,a higher MR removal efficiency is achieved in a much shorter time on CNT30.Moreover,CNT30 has an outstanding reusability,with the MR removal efficiency decreasing by only 7%after ten cycles.The COOH groups on CNT30 improve the hydrophilicity of CNT30,thus promoting the interaction of MR in water with CNT30.The hydrogen bonding and electrostatic interaction of MR with the COOH groups on CNT30 could be the force to drive MR adsorption on CNT30.The higher COOH content could be the origin for the better performance of CNT30 in removing dye from water.The discharge process developed herein is operated in O2,without using harmful substances,and the COOH content on CNT can be efficiently tuned by simply changing discharge time.This is different from the chemical modification widely used to functionalize CNT by strong oxidants,e.g.,HNO_(3).The present work is of great significance to realize green construction of materials for more efficiently removing dye from water.
基金the National Key R&D Program of China(2017YFB0601805)support from the Natural Science Foundation of China(51376008)。
文摘The evolution of pore structure and functional groups of coal char in different stages of Shenhua coal combustion process in O_(2)/CO_(2)atmosphere was studied by the low temperature nitrogen adsorption method,the scanning electron microscopy and the FTIR method.The relationship between the pore structure,oxygen-containing functional groups and NO generation characteristics of coal char under different inlet oxygen concentrations was analyzed.The result shows that the overall pore structure and shape of pulverized coal particles change continuously with the combustion;and the oxygen-containing functional groups on the surface of coal char indicate multi-peak changes and are related to NO generation.The oxygen concentration poses a larger impact on the change in coal particle size,oxygen-containing functional groups and NO generation;and there is an oxygen concentration that optimizes the reduction effect of the oxygen-containing functional group on NO.
基金Iwatani Naoji Foundation,Basic Frontier Project of Agro-Environmental Protection Institute,Ministry of Agriculture and Rural Affairs of China,Central Public-interest Scientific Institution Basal Research Fund(No.Y2022QC30)the Materials Processing Science project(“Materealize”)of the Ministry of Education,Culture,Sports,Science and Technology(MEXT),Grant Number JPMXP0219192801.
文摘Many types of sustainably-prepared functional biochar catalysts are needed to transform biomass substrates into platform chemicals.In this work,weak-acid biochar catalysts were prepared by mix ball-milled(10 min,isothermal,room temperature)cherry blossom tree leaf biomass(BM)with humic acid(H)prior to carbonization of samples for 1 h under nitrogen gas.Characterization of the as-prepared materials(HBM-carbonization temperature in℃)showed that humic acid activated the biochars and increased their number of oxygen-containing functional(-COOH,OH)groups.The weak-acid biochars were applied as heterogeneous catalysts for dehydration of fructose to 5-hydroxymethylfurfural(5-HMF),where it was found that biochar catalyst,HBM-400,gave 100%fructose conversion and 77.5%5-HMF yields in an ionic liquid(1-butyl-3-methylimidazolium chloride)reaction system(140℃,60 min reaction time).As-prepared HBM-400 biochars exhibited constant catalytic activity for fructose dehydration with repeated use without any type of reactivation treatment and were stable for 5 cycles.Humic acid is an effective additive for preparing weak-acid catalytic materials from waste biomass.
基金supported by the National Natural Science Foundation of China(21902062 and 21705056)the Young Taishan Scholars Program(tsqn201812080)the Natural Science Foundation of Shandong Province(ZR2019YQ10).
文摘Electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))through two-electron oxygen reduction represents an attractive alternative for on-site H_(2)O_(2) generation.Here,we develop a facile thermally activatedpersulfate approach to obtain oxidized carbon nanotubes(O-CNTs-x,x represents oxidation time)with enhanced H_(2)O_(2) electrosynthesis performance.Electrochemical studies have demonstrated that the optimized O-CNTs-6(i.e.,oxidation time is 6 h)could deliver a sustained high selectivity of around 92%for H_(2)O_(2) over a wide voltage window in 0.1 mol/L KOH and a high H_(2)O_(2) production rate of 296.84 mmol/L g^(-1) cat h^(-1).Compared with pristine CNTs,the enhanced catalytic activity primarily stems from the newly-generated oxygen-containing functional groups and some defects created on the surface of O-CNTs-x.Importantly,the proposed oxidation process is proved to be valid for promoting H_(2)O_(2) electrosynthesis performance of the Ketjen black.This study provides an universal oxidation method to obtain highly active carbon-based catalysts and initiates new opportunities for the exploration of highperformance electrosynthesis H_(2)O_(2) catalysts.