Modification conditions determine the surface topography and the active material phase composition of a catalyst.To study the influence of modification on a carbon-based sorbent,coconut husk activated carbon(AC)which ...Modification conditions determine the surface topography and the active material phase composition of a catalyst.To study the influence of modification on a carbon-based sorbent,coconut husk activated carbon(AC)which was activated using HNO3 and modified by FeSO4 and Fe(NO3)3 was examined.The pore textures and surface chemical characteristics of the carbon materials were examined by scanning electron microscopy(SEM),Brunner-Emmet-Teller(BET),X-ray diffraction(XRD)and Fourier transform infrared(FTIR)spectroscopy.The surface topography,the pore structure,active materials,and functional groups of AC,AC modificated by HNO3(HNO3/AC for short),and AC modificated by FeSO4 and Fe(NO3)3(Fe/AC for short)were systematically studied.Subsequently,the mechanism of modifying the conditions for the carbon materials was determined.Results showed that the surface micro topography of HNO3/AC became unsystematic and disordered.After modification with FeSO4,the ferriferous oxide was mainly present as a near-spherical crystal.Ferriferous oxides from Fe(NO3)3 modification mainly exhibited a plate shape.HNO3 modification could enlarge the pores but decrease the specific surface area of AC.FeSO4 modification resulted in a new net post structure in the pore canal of AC.Fe(NO3)3 modification caused the pore space structure to develop in the interior,and a higher calcination temperature was useful for ablation.The ash content of the AC was substantially reduced upon HNO3 modification.Upon FeSO4 modification,α-FeOOH,α-Fe2O3 andγ-Fe2O3 coexisted under the condition of a lower concentration of FeSO4 and a lower calcination temperature,and a higher FeSO4 concentration and calcination temperature generated moreα-Fe2O3.The same Fe(NO3)3 modification and a higher calcination temperature were beneficial to the minor chipping formation ofγ-Fe2O3.A higher Fe(NO3)3 loading produced a lower graphitization degree.HNO3 modification formed various new oxygen-containing functional groups and few nitrogen-containing groups.Based on the cover,FeSO4 and Fe(NO3)3 modification could decrease the oxygen-containing and nitrogen-containing functional groups.These results could optimize the modification condition and improve physical and chemical properties of carbon-based sorbents.展开更多
Activated carbon was prepared from cattail by H3PO4 activation. The effects influencing the surface area of the resulting activated carbon followed the sequence of activated temperature 〉 activated time 〉 impregnati...Activated carbon was prepared from cattail by H3PO4 activation. The effects influencing the surface area of the resulting activated carbon followed the sequence of activated temperature 〉 activated time 〉 impregnation ratio 〉 impregnation time. The optimum condition was found at an impregnation ratio of 2.5, an impregnation time of 9 hr, an activated temperature of 500℃, and an activated time of 80 min. The Brunauer-Emmett-Teller surface area and average pore size of the activated carbon were 1279 m^2/g and 5.585 nm, respectively. A heterogeneous structure in terms of both size and shape was highly developed and widely distributed on the carbon surface. Some groups containing oxygen and phosphorus were formed, and the carboxyl group was the major oxygen-containing functional group. An isotherm equilibrium study was carried out to investigate the adsorption capacity of the activated carbon. The data fit the Langmuir isotherm equation, with maximum monolayer adsorption capacities of 192.30 mg/g for Neutral Red and 196.08 mg/g for Malachite Green. Dye-exhausted carbon could be regenerated effectively by thermal treatment. The results indicated that cattail-derived activated carbon was a promising adsorbent for the removal of cationic dyes from aqueous solutions.展开更多
Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction(ORR)is extremely important for promoting the commercialized applicati...Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction(ORR)is extremely important for promoting the commercialized applications of such catalysts.In this work,the FeCl3-containing porphyrinato iron-based covalent porous polymer(FeCl3·FeP or-CPP)was fabricated in-situ onto porous corncob biomass supports via a simple one-pot method.Subsequent thermal-reduction pyrolysis at 700℃-900℃with CO2 gas as an activating agent resulted in Fe2O3-decorated and N-doped graphitic carbon composite Fe2O3@NC&bio-C with a high degree of graphitization of Fe-involved promotion during pyrolysis(Fe2O3=FeCl3·FePor-CPP derived Fe2O3;NC=N-doped graphene analog;bio-C=the corncob-derived hierarchically porous graphitic biomass carbon framework).The derivedα-Fe2O3 andγ-Fe2O3 nanocrystals(5-10 nm particle diameter)were all immobilized on the N-doped bio-C micro/nanofibers.Notably,the Fe2O3@NC&bio-C obtained at the pyrolysis temperature of 800℃(Fe2O3@NC&bio-C-800),exhibited unusual ORR catalytic efficiency via a 4-electron pathway with the onset and half-wave potentials of 0.96 V and 0.85 V vs.RHE,respectively.In addition,Fe2O3@NC&bio-C-800 also exhibited a high and stable limiting current density of-6.0 mA cm-2,remarkably stability(larger than 91%retention after 10000 s),and good methanol tolerance.The present work represents one of the best results for iron-based biomass material ORR catalysts reported to date.The high ORR activity is attributed to the uniformly distributedα-Fe2O3 andγ-Fe2O3 nanoparticles on the N-enriched carbon matrix with a large specific surface area of 772.6 m^2 g^-1.This facilitates favor faster electron movement and better adsorption of oxygen molecules on the surface of the catalyst.Nevertheless,comparative studies on the structure and ORR catalytic activity of Fe2O3@NC&bioC-800 with Fe2O3@bio-C-800 and NC&bio-C-800 clearly highlight the synergistic effect of the coexisting Fe2O3 nanocrystals,NC,and bio-C on the ORR performance.展开更多
Herein, Co_3O_4 nanoparticles/nitrogen-doped carbon(Co_3O_4/NPC) composites with different structures were prepared via a facile method. Structure control was achieved by the rational morphology design of ZIF-67 precu...Herein, Co_3O_4 nanoparticles/nitrogen-doped carbon(Co_3O_4/NPC) composites with different structures were prepared via a facile method. Structure control was achieved by the rational morphology design of ZIF-67 precursors, which were then pyrolyzed in air to obtain Co_3O_4/NPC composites. When applied as catalysts for the oxygen evolution reaction(OER), the M-Co_3O_4/NPC composites derived from the flower-like ZIF-67 showedsuperior catalytic activities than those derived from the rhombic dodecahedron and hollow spherical ZIF-67. The former M-Co_3O_4/NPC composite displayed a small overpotential of 0.3 V, low onset potential of 1.41 V, small Tafel slope of 83 m V dec^(-1), and a desirable stability.(94.7% OER activity was retained after 10 h.) The excellent performance of the flower-like M-Co_3O_4/NPC composite in the OER was attributed to its favorable structure.展开更多
To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstru...To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.展开更多
A novel flower-like hydrated magnesium carbonate hydroxide, Mg5 （CO3 ）4 （OH）2·4H2O, with micro-structure composed of individual thin nano-sheets was synthesized using a facile solution route without the use o...A novel flower-like hydrated magnesium carbonate hydroxide, Mg5 （CO3 ）4 （OH）2·4H2O, with micro-structure composed of individual thin nano-sheets was synthesized using a facile solution route without the use of template or organic surfactant. Reaction time has an important effect on the final morphology of the product. The micro-structure and morphology of Mg5 （CO3）4 （OH）2·4H2O were characterized by means of X-ray diffractometry （XRD）, fieldemission scanning electron microscopy（FE-SEM）. Brunauer-Emmett-Teller（BET） surface areas of the samples were also measured. The probable formation mechanism of flower-like micro-structure was discussed. It was found that Mg5 （CO3）4（ OH）2·4H2O with flower-like micro-structure was a novel and efficient catalyst for the synthesis of diphenyl carbonate （DPC） by transesterification of dimethyl carbonate （DMC） with phenol.展开更多
Fe2O3/active carbon（Fe2O3/AC） nanocomposites were readily fabricated by pyrolyzing Fe3＋ impregnated active carbon in a nitrogen atmosphere. The as-prepared composites were studied by X-ray powder diffraction（XRD）...Fe2O3/active carbon（Fe2O3/AC） nanocomposites were readily fabricated by pyrolyzing Fe3＋ impregnated active carbon in a nitrogen atmosphere. The as-prepared composites were studied by X-ray powder diffraction（XRD）, X-ray photoelectron spectroscopy（XPS） and transmission electron microscopy（TEM）. The capacitive property of the composites was investigated by cyclic voltammetry（CV） and galvanostatic charge-discharge test. Physical characterizations show that the γ-Fe2O3 fine grains dispersed in the AC well, with a mean size of 21.24 nm. Electrochemical tests in 6 mol/L KOH solutions indicate that the as-prepared nanocomposites exhibited improved capacitive properties. The specific capacitance（SC） of Fe2O3/AC nanocomposites was up to 188.4 F/g that was derived from both electrochemical double-layer capacitance and pseudo-capacitance, which was 78% larger than that of pristine AC. A symmetric capacitor with Fe2O3/AC nanocomposites as electrode showed an excellent cycling stability. The SC was only reduced by a factor of 9.2% after 2000 cycles at a current density of 1 A/g.展开更多
This article shows main principles and presents ideas described in the scientific and technical literature, on the mechanism of interaction of microwave radiation with a solid phase materials, which were used as a bas...This article shows main principles and presents ideas described in the scientific and technical literature, on the mechanism of interaction of microwave radiation with a solid phase materials, which were used as a basis of creation of new perspective, energy efficient and environmentally safe technologies of preparation of heterogeneous catalysts for the reactions which were carried out under the influence of electro-magnetic radiation of microwave radiation. Author’s research results confirm possibilities of practical use of proposed method of hydrothermal oxidation of industrial low-dispersing of aluminum powders with presence of bulk phase of Al(ОН)<sub>3</sub>·nH<sub>2</sub>O, with further thermal treatment in microwave field for acquisition of armored А1/А1<sub>2</sub>О3<sub>3</sub> compositions, which effectively consume energy of microwave radiation. Due to the textured characteristics and thermo-transforming ability, synthesized components can be used as potential universal bearings of catalysts for reactions stimulated by electromagnetic radiation of (2.45 GHz) microwave frequency.展开更多
杨梅素是一种主要用于抗炎的多酚类黄酮化合物,为改善其水溶性和稳定性,合成了杨梅素-3-O-β-D-乳糖,并开发了一条高效的合成路线。首先以杨梅苷为起始原料,对杨梅苷的5位、7位、3′位、4′位和5′位酚羟基进行保护,形成五苄基保护的杨...杨梅素是一种主要用于抗炎的多酚类黄酮化合物,为改善其水溶性和稳定性,合成了杨梅素-3-O-β-D-乳糖,并开发了一条高效的合成路线。首先以杨梅苷为起始原料,对杨梅苷的5位、7位、3′位、4′位和5′位酚羟基进行保护,形成五苄基保护的杨梅苷。然后脱除3位鼠李糖,再与乙酰基保护的乳糖溴苷反应,最后通过依次脱去乙酰基和苄基得到目标化合物。经过路径优化,最终以更高效的方法合成了杨梅素-3-O-β-D-乳糖,减少了副产物的生成,提高了原合成路线总收率,此方法的总产率为44.5%。该路径得到了2个新型的杨梅素衍生物中间体。目标化合物的结构均经过1 H NMR,13 C NMR和HR-MS(ESI)确证。展开更多
Conversion-type reaction anode materials with high specific capacity are attractive candidates to improve lithium ion batteries(LIBs), yet the rapid capacity fading and poor rate capability caused by drastic volume ch...Conversion-type reaction anode materials with high specific capacity are attractive candidates to improve lithium ion batteries(LIBs), yet the rapid capacity fading and poor rate capability caused by drastic volume change and low electronic conductivity greatly hinder their practical applications. To circumvent these issues, the successful design of yolk@shell Fe2 O3@C hybrid composed of a columnar-like Fe2O3 core within a hollow cavity completely surrounded by a thin, self-supported carbon(C) shell is presented as an anode for high-performance LIBs. This yolk@shell structure allows each Fe2O3 core to swell upon lithiation without deforming the carbon shell. This preserves the structural and electrical integrity against pulverization, as revealed by in situ transmission electron microscopy(TEM) measurement. Benefiting from these structural advantages, the resulting electrode exhibits a high reversible capacity(1013 m Ah g-1 after80 cycles at 0.2 A g-1), outstanding rate capability(710 m Ah g-1 at 8 A g-1) and superior cycling stability(800 m Ah g-1 after 300 cycles at 4 A g-1). A Li-ion full cell using prelithiated yolk@shell Fe2 O3@C hybrid as the anode and commercial Li CoO2(LCO) as the cathode demonstrates impressive cycling stability with a capacity retention of 84.5% after 100 cycles at 1 C rate, holding great promise for future practical applications.展开更多
Deactivation mechanism of Cr-Al2O3catalyst and the interaction of Cr-A1 in the dehydrogenation of isobutane, as well as the nature of the catalytic active center, were studied using XRD, SEM, XPS, H2-TPR, isobutane-TP...Deactivation mechanism of Cr-Al2O3catalyst and the interaction of Cr-A1 in the dehydrogenation of isobutane, as well as the nature of the catalytic active center, were studied using XRD, SEM, XPS, H2-TPR, isobutane-TPR and TPO techniques. The results revealed that the deactivation of Cr-Al2O3 catalyst was mainly caused by carbon deposition on its surface. The Cr3＋ ion could not be reduced by hydrogen but could be reduced to Cr2＋ by hydrocarbons and monoxide carbon. The active center for isobutane dehydrogenation could be Cr2＋/Cr3＋ produced from Cr6＋ by the on line reduction of hydrocarbon and carbon monoxide. The binding energy of Al3＋ was strongly affected by the state of chromium cations in the catalysts.展开更多
Ammonia borane(AB)is an excellent candidate for the chemical storage of hydrogen.However,its practical utilization for hydrogen production is hindered by the need for expensive noble-metal-based catalysts.Herein,we re...Ammonia borane(AB)is an excellent candidate for the chemical storage of hydrogen.However,its practical utilization for hydrogen production is hindered by the need for expensive noble-metal-based catalysts.Herein,we report Co-Co3O4 nanoparticles(NPs)facilely deposited on carbon dots(CDs)as a highly efficient,robust,and noble-metal-free catalyst for the hydrolysis of AB.The incorporation of the multiinterfaces between Co,Co3O4 NPs,and CDs endows this hybrid material with excellent catalytic activity(rB=6816 mLH2 min^-1 gCo^-1)exceeding that of previous non-noble-metal NP systems and even that of some noble-metal NP systems.A further mechanistic study suggests that these interfacial interactions can affect the electronic structures of interfacial atoms and provide abundant adsorption sites for AB and water molecules,resulting in a low energy barrier for the activation of reactive molecules and thus substantial improvement of the catalytic rate.展开更多
In this work, a CoNxC active sites-rich three-dimensional porous carbon nanofibers network derived from bacterial cellulose and bimetal-ZIFs is prepared via a nucleation growth strategy and a pyrolysis process.The mat...In this work, a CoNxC active sites-rich three-dimensional porous carbon nanofibers network derived from bacterial cellulose and bimetal-ZIFs is prepared via a nucleation growth strategy and a pyrolysis process.The material displays excellent electrocatalytic activity for the oxygen reduction reaction, reaching a high limiting diffusion current density of -7.8 mA cm^(-2), outperforming metal–organic frameworks derived multifunctional electrocatalysts, and oxygen evolution reaction and hydrogen evolution reaction with low overpotentials of 380 and 107 mV, respectively. When the electrochemical properties are further evaluated, the electrocatalyst as an air cathode for Zn-air batteries exhibits a high cycling stability for63 h as well as a maximum power density of 308 mW cm^(-2), which is better than those for most Zn-air batteries reported to date. In addition, a power density of 152 mW cm^(-2) is provided by the solid-state Zn-air batteries, and the cycling stability is outstanding for 24 h. The remarkable electrocatalytic properties are attributed to the synergistic effect of the 3 D porous carbon nanofibers network and abundant inserted CoNxC active sites, which enable the fast transmission of ions and mass and simultaneously provide a large contact area for the electrode/electrolyte.展开更多
基金General Project of Science and Technology Plan of Yunnan Science and Technology Department,China(No.2019FB077)Open Fund of Key Laboratory of Ministry of Education for Metallurgical Emission Reduction and Comprehensive Utilization of Resources,China(No.JKF19-08)。
文摘Modification conditions determine the surface topography and the active material phase composition of a catalyst.To study the influence of modification on a carbon-based sorbent,coconut husk activated carbon(AC)which was activated using HNO3 and modified by FeSO4 and Fe(NO3)3 was examined.The pore textures and surface chemical characteristics of the carbon materials were examined by scanning electron microscopy(SEM),Brunner-Emmet-Teller(BET),X-ray diffraction(XRD)and Fourier transform infrared(FTIR)spectroscopy.The surface topography,the pore structure,active materials,and functional groups of AC,AC modificated by HNO3(HNO3/AC for short),and AC modificated by FeSO4 and Fe(NO3)3(Fe/AC for short)were systematically studied.Subsequently,the mechanism of modifying the conditions for the carbon materials was determined.Results showed that the surface micro topography of HNO3/AC became unsystematic and disordered.After modification with FeSO4,the ferriferous oxide was mainly present as a near-spherical crystal.Ferriferous oxides from Fe(NO3)3 modification mainly exhibited a plate shape.HNO3 modification could enlarge the pores but decrease the specific surface area of AC.FeSO4 modification resulted in a new net post structure in the pore canal of AC.Fe(NO3)3 modification caused the pore space structure to develop in the interior,and a higher calcination temperature was useful for ablation.The ash content of the AC was substantially reduced upon HNO3 modification.Upon FeSO4 modification,α-FeOOH,α-Fe2O3 andγ-Fe2O3 coexisted under the condition of a lower concentration of FeSO4 and a lower calcination temperature,and a higher FeSO4 concentration and calcination temperature generated moreα-Fe2O3.The same Fe(NO3)3 modification and a higher calcination temperature were beneficial to the minor chipping formation ofγ-Fe2O3.A higher Fe(NO3)3 loading produced a lower graphitization degree.HNO3 modification formed various new oxygen-containing functional groups and few nitrogen-containing groups.Based on the cover,FeSO4 and Fe(NO3)3 modification could decrease the oxygen-containing and nitrogen-containing functional groups.These results could optimize the modification condition and improve physical and chemical properties of carbon-based sorbents.
基金supported by the National Key Technology R&D Program for the 11th Five-year Plan of China (No.2006BAC10B03)the National Natural Science Foundation of China-Japan Science and Technology Agency (NSFC-JST) Strategic Joint Research Project (No.50721140017)the National Natural Science Foundation of China (No.50508019)
文摘Activated carbon was prepared from cattail by H3PO4 activation. The effects influencing the surface area of the resulting activated carbon followed the sequence of activated temperature 〉 activated time 〉 impregnation ratio 〉 impregnation time. The optimum condition was found at an impregnation ratio of 2.5, an impregnation time of 9 hr, an activated temperature of 500℃, and an activated time of 80 min. The Brunauer-Emmett-Teller surface area and average pore size of the activated carbon were 1279 m^2/g and 5.585 nm, respectively. A heterogeneous structure in terms of both size and shape was highly developed and widely distributed on the carbon surface. Some groups containing oxygen and phosphorus were formed, and the carboxyl group was the major oxygen-containing functional group. An isotherm equilibrium study was carried out to investigate the adsorption capacity of the activated carbon. The data fit the Langmuir isotherm equation, with maximum monolayer adsorption capacities of 192.30 mg/g for Neutral Red and 196.08 mg/g for Malachite Green. Dye-exhausted carbon could be regenerated effectively by thermal treatment. The results indicated that cattail-derived activated carbon was a promising adsorbent for the removal of cationic dyes from aqueous solutions.
基金the National Natural Science Foundation of China(Nos.21771192,21631003,21871024)the Major Program of Shandong Province Natural Science Foundation(No.ZR2017ZB0315)+2 种基金Fundamental Research Funds for the Central Universities(Nos.18CX06001A,19CX05001A)Research Foundation from China University of Petroleum(East China)(No.Y1510051)Taishan Scholar Program of Shandong Province(ts201712019,ts201511019).
文摘Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction(ORR)is extremely important for promoting the commercialized applications of such catalysts.In this work,the FeCl3-containing porphyrinato iron-based covalent porous polymer(FeCl3·FeP or-CPP)was fabricated in-situ onto porous corncob biomass supports via a simple one-pot method.Subsequent thermal-reduction pyrolysis at 700℃-900℃with CO2 gas as an activating agent resulted in Fe2O3-decorated and N-doped graphitic carbon composite Fe2O3@NC&bio-C with a high degree of graphitization of Fe-involved promotion during pyrolysis(Fe2O3=FeCl3·FePor-CPP derived Fe2O3;NC=N-doped graphene analog;bio-C=the corncob-derived hierarchically porous graphitic biomass carbon framework).The derivedα-Fe2O3 andγ-Fe2O3 nanocrystals(5-10 nm particle diameter)were all immobilized on the N-doped bio-C micro/nanofibers.Notably,the Fe2O3@NC&bio-C obtained at the pyrolysis temperature of 800℃(Fe2O3@NC&bio-C-800),exhibited unusual ORR catalytic efficiency via a 4-electron pathway with the onset and half-wave potentials of 0.96 V and 0.85 V vs.RHE,respectively.In addition,Fe2O3@NC&bio-C-800 also exhibited a high and stable limiting current density of-6.0 mA cm-2,remarkably stability(larger than 91%retention after 10000 s),and good methanol tolerance.The present work represents one of the best results for iron-based biomass material ORR catalysts reported to date.The high ORR activity is attributed to the uniformly distributedα-Fe2O3 andγ-Fe2O3 nanoparticles on the N-enriched carbon matrix with a large specific surface area of 772.6 m^2 g^-1.This facilitates favor faster electron movement and better adsorption of oxygen molecules on the surface of the catalyst.Nevertheless,comparative studies on the structure and ORR catalytic activity of Fe2O3@NC&bioC-800 with Fe2O3@bio-C-800 and NC&bio-C-800 clearly highlight the synergistic effect of the coexisting Fe2O3 nanocrystals,NC,and bio-C on the ORR performance.
基金supported by the Scientific and Technological Innovation Platform of Fujian Province(2006L2003)Scientific Research Project of Wuyi University(YJ201706)
文摘Herein, Co_3O_4 nanoparticles/nitrogen-doped carbon(Co_3O_4/NPC) composites with different structures were prepared via a facile method. Structure control was achieved by the rational morphology design of ZIF-67 precursors, which were then pyrolyzed in air to obtain Co_3O_4/NPC composites. When applied as catalysts for the oxygen evolution reaction(OER), the M-Co_3O_4/NPC composites derived from the flower-like ZIF-67 showedsuperior catalytic activities than those derived from the rhombic dodecahedron and hollow spherical ZIF-67. The former M-Co_3O_4/NPC composite displayed a small overpotential of 0.3 V, low onset potential of 1.41 V, small Tafel slope of 83 m V dec^(-1), and a desirable stability.(94.7% OER activity was retained after 10 h.) The excellent performance of the flower-like M-Co_3O_4/NPC composite in the OER was attributed to its favorable structure.
基金Open Fund of Key Laboratory of Ministry of Education for Metallurgical Emission Reduction and Comprehensive Utilization of Resources,China(No.JKF19-08)General Project of Science and Technology Plan of Yunnan Science and Technology Department,China(No.2019FB077)+1 种基金Industrialization Cultivation Project of Scientific Research Fund of Yunnan Provincial Department of Education,China(No.2016CYH07)Top Young Talents of Yunnan Ten Thousand Talents Plan,China(No.YNWR-QNBJ-2019-263)。
文摘To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.
基金Supported by the National Natural Science Foundation of China(Nos.20671011,20331010,90406002and90406024)the 111 Project(No.B07012)the Key Laboratory of Structural Chemistry Foundation(No.060017).
文摘A novel flower-like hydrated magnesium carbonate hydroxide, Mg5 （CO3 ）4 （OH）2·4H2O, with micro-structure composed of individual thin nano-sheets was synthesized using a facile solution route without the use of template or organic surfactant. Reaction time has an important effect on the final morphology of the product. The micro-structure and morphology of Mg5 （CO3）4 （OH）2·4H2O were characterized by means of X-ray diffractometry （XRD）, fieldemission scanning electron microscopy（FE-SEM）. Brunauer-Emmett-Teller（BET） surface areas of the samples were also measured. The probable formation mechanism of flower-like micro-structure was discussed. It was found that Mg5 （CO3）4（ OH）2·4H2O with flower-like micro-structure was a novel and efficient catalyst for the synthesis of diphenyl carbonate （DPC） by transesterification of dimethyl carbonate （DMC） with phenol.
基金Supported by the National Natural Science Foundation of China(No.21271138)the Natural Science Foundation of Tianjin City, China(No.10JCZDJC21500)
文摘Fe2O3/active carbon（Fe2O3/AC） nanocomposites were readily fabricated by pyrolyzing Fe3＋ impregnated active carbon in a nitrogen atmosphere. The as-prepared composites were studied by X-ray powder diffraction（XRD）, X-ray photoelectron spectroscopy（XPS） and transmission electron microscopy（TEM）. The capacitive property of the composites was investigated by cyclic voltammetry（CV） and galvanostatic charge-discharge test. Physical characterizations show that the γ-Fe2O3 fine grains dispersed in the AC well, with a mean size of 21.24 nm. Electrochemical tests in 6 mol/L KOH solutions indicate that the as-prepared nanocomposites exhibited improved capacitive properties. The specific capacitance（SC） of Fe2O3/AC nanocomposites was up to 188.4 F/g that was derived from both electrochemical double-layer capacitance and pseudo-capacitance, which was 78% larger than that of pristine AC. A symmetric capacitor with Fe2O3/AC nanocomposites as electrode showed an excellent cycling stability. The SC was only reduced by a factor of 9.2% after 2000 cycles at a current density of 1 A/g.
文摘This article shows main principles and presents ideas described in the scientific and technical literature, on the mechanism of interaction of microwave radiation with a solid phase materials, which were used as a basis of creation of new perspective, energy efficient and environmentally safe technologies of preparation of heterogeneous catalysts for the reactions which were carried out under the influence of electro-magnetic radiation of microwave radiation. Author’s research results confirm possibilities of practical use of proposed method of hydrothermal oxidation of industrial low-dispersing of aluminum powders with presence of bulk phase of Al(ОН)<sub>3</sub>·nH<sub>2</sub>O, with further thermal treatment in microwave field for acquisition of armored А1/А1<sub>2</sub>О3<sub>3</sub> compositions, which effectively consume energy of microwave radiation. Due to the textured characteristics and thermo-transforming ability, synthesized components can be used as potential universal bearings of catalysts for reactions stimulated by electromagnetic radiation of (2.45 GHz) microwave frequency.
文摘杨梅素是一种主要用于抗炎的多酚类黄酮化合物,为改善其水溶性和稳定性,合成了杨梅素-3-O-β-D-乳糖,并开发了一条高效的合成路线。首先以杨梅苷为起始原料,对杨梅苷的5位、7位、3′位、4′位和5′位酚羟基进行保护,形成五苄基保护的杨梅苷。然后脱除3位鼠李糖,再与乙酰基保护的乳糖溴苷反应,最后通过依次脱去乙酰基和苄基得到目标化合物。经过路径优化,最终以更高效的方法合成了杨梅素-3-O-β-D-乳糖,减少了副产物的生成,提高了原合成路线总收率,此方法的总产率为44.5%。该路径得到了2个新型的杨梅素衍生物中间体。目标化合物的结构均经过1 H NMR,13 C NMR和HR-MS(ESI)确证。
基金supported by the National Natural Science Foundation of China(Grants No.21703185)the leading Project Foundation of Science Department of Fujian Province(Grants No.2018H0034)+1 种基金Fundamental Research Funds for the Central Universities(Xiamen University:20720170042)the“Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen University。
文摘Conversion-type reaction anode materials with high specific capacity are attractive candidates to improve lithium ion batteries(LIBs), yet the rapid capacity fading and poor rate capability caused by drastic volume change and low electronic conductivity greatly hinder their practical applications. To circumvent these issues, the successful design of yolk@shell Fe2 O3@C hybrid composed of a columnar-like Fe2O3 core within a hollow cavity completely surrounded by a thin, self-supported carbon(C) shell is presented as an anode for high-performance LIBs. This yolk@shell structure allows each Fe2O3 core to swell upon lithiation without deforming the carbon shell. This preserves the structural and electrical integrity against pulverization, as revealed by in situ transmission electron microscopy(TEM) measurement. Benefiting from these structural advantages, the resulting electrode exhibits a high reversible capacity(1013 m Ah g-1 after80 cycles at 0.2 A g-1), outstanding rate capability(710 m Ah g-1 at 8 A g-1) and superior cycling stability(800 m Ah g-1 after 300 cycles at 4 A g-1). A Li-ion full cell using prelithiated yolk@shell Fe2 O3@C hybrid as the anode and commercial Li CoO2(LCO) as the cathode demonstrates impressive cycling stability with a capacity retention of 84.5% after 100 cycles at 1 C rate, holding great promise for future practical applications.
基金supported by the Natural Science Foundation of Shandong Provence of China(ZR2013BM008)
文摘Deactivation mechanism of Cr-Al2O3catalyst and the interaction of Cr-A1 in the dehydrogenation of isobutane, as well as the nature of the catalytic active center, were studied using XRD, SEM, XPS, H2-TPR, isobutane-TPR and TPO techniques. The results revealed that the deactivation of Cr-Al2O3 catalyst was mainly caused by carbon deposition on its surface. The Cr3＋ ion could not be reduced by hydrogen but could be reduced to Cr2＋ by hydrocarbons and monoxide carbon. The active center for isobutane dehydrogenation could be Cr2＋/Cr3＋ produced from Cr6＋ by the on line reduction of hydrocarbon and carbon monoxide. The binding energy of Al3＋ was strongly affected by the state of chromium cations in the catalysts.
基金financially supported by the National Natural Science Foundation of China(21774041 and 51433003)the China Postdoctoral Science Foundation(2018M640681 and 2019T120632)。
文摘Ammonia borane(AB)is an excellent candidate for the chemical storage of hydrogen.However,its practical utilization for hydrogen production is hindered by the need for expensive noble-metal-based catalysts.Herein,we report Co-Co3O4 nanoparticles(NPs)facilely deposited on carbon dots(CDs)as a highly efficient,robust,and noble-metal-free catalyst for the hydrolysis of AB.The incorporation of the multiinterfaces between Co,Co3O4 NPs,and CDs endows this hybrid material with excellent catalytic activity(rB=6816 mLH2 min^-1 gCo^-1)exceeding that of previous non-noble-metal NP systems and even that of some noble-metal NP systems.A further mechanistic study suggests that these interfacial interactions can affect the electronic structures of interfacial atoms and provide abundant adsorption sites for AB and water molecules,resulting in a low energy barrier for the activation of reactive molecules and thus substantial improvement of the catalytic rate.
基金financial support from the following sources: the National Natural Science Foundation of China (NSFC) (Grants 51607054, 51772073)Young Talent of Hebei Province (Nos. 70280011808, 70280016160250)+1 种基金Hebei Province Outstanding Youth Fund (A2018201019, A2017201082)Hebei Province Natural Science Fund (A2015201050)。
文摘In this work, a CoNxC active sites-rich three-dimensional porous carbon nanofibers network derived from bacterial cellulose and bimetal-ZIFs is prepared via a nucleation growth strategy and a pyrolysis process.The material displays excellent electrocatalytic activity for the oxygen reduction reaction, reaching a high limiting diffusion current density of -7.8 mA cm^(-2), outperforming metal–organic frameworks derived multifunctional electrocatalysts, and oxygen evolution reaction and hydrogen evolution reaction with low overpotentials of 380 and 107 mV, respectively. When the electrochemical properties are further evaluated, the electrocatalyst as an air cathode for Zn-air batteries exhibits a high cycling stability for63 h as well as a maximum power density of 308 mW cm^(-2), which is better than those for most Zn-air batteries reported to date. In addition, a power density of 152 mW cm^(-2) is provided by the solid-state Zn-air batteries, and the cycling stability is outstanding for 24 h. The remarkable electrocatalytic properties are attributed to the synergistic effect of the 3 D porous carbon nanofibers network and abundant inserted CoNxC active sites, which enable the fast transmission of ions and mass and simultaneously provide a large contact area for the electrode/electrolyte.
