To replace precious metal oxygen reduction reaction(ORR)electrocatalysts,many transition metals and N-doped car-bon composites have been proposed in the last decade resulting in their rapid development as promising no...To replace precious metal oxygen reduction reaction(ORR)electrocatalysts,many transition metals and N-doped car-bon composites have been proposed in the last decade resulting in their rapid development as promising non-precious metal catalysts.We used Ketjenblack carbon as the precursor and mixed it with a polymeric ionic liquid(PIL)of[Hvim]NO_(3) and Fe(NO_(3))_(3),which was thermally calcined at 900℃ to produce a porous FeO_(x),N co-doped carbon material denoted FeO_(x)-N/C.Because the PIL of[Hvim]NO_(3) strongly combines with and disperses Fe^(3+)ions,and NO_(3)−is thermally pyrolyzed to form the porous structure,the FeO_(x)-N/C catalyst has a high electrocatalytic activity for the ORR in both 0.1 mol L^(−1) KOH and 0.5 mol L^(−1) H_(2)SO_(4) electrolytes.It was used as the catalyst to assemble a zinc-air battery,which had a peak power density of 185 mW·cm^(−2).Its superior electrocatalytic activity,wide pH range,and easy preparation make FeO_(x)-N/C a promising electrocatalyst for fuel cells and metal-air batteries.展开更多
The carbothermic reduction of Panzhihua ilmenite with various additions of activated carbon was investigated byisothermal experiments over the temperature range of1373to1773K in the argon atmosphere.According to the r...The carbothermic reduction of Panzhihua ilmenite with various additions of activated carbon was investigated byisothermal experiments over the temperature range of1373to1773K in the argon atmosphere.According to the reaction kineticsrecorded by the infrared gas analyzer,it was found that the amount of carbon addition had little influence on the reaction rates atvarious temperatures except1473K.When the reaction temperature was above the eutectic temperature of1427K of Fe?C binarysystem,part of carbon would dissolve into Fe to form a liquid phase,which made the liquid Fe as a diffusion channel of carbon todiffuse to the reaction interface.The carbothermic reduction above1573K obeyed the shrinking-core model.The mass fraction ofTiC could be determined by the standard addition technique.展开更多
This paper documents a 7800-year proxy record from the Shenjiadian peatland on the Sanjiang Plain in Northeast China.High-resolution plant macrofossil and colorimetric humification methods were used to reconstruct the...This paper documents a 7800-year proxy record from the Shenjiadian peatland on the Sanjiang Plain in Northeast China.High-resolution plant macrofossil and colorimetric humification methods were used to reconstruct the vegetation and hydrologic history from a 193 cm-long sedimentary profile.Detrended correspondence analysis(DCA) was applied to transform the raw plant macrofossil data into latent indices of peatland water level.The vegetation community transited from an Equisetum fluviatile community to a Carex lasiocarpa community at approximately 3800 cal yr BP and was followed by a Carex-shrub community at approximately 480 cal yr BP.Based on the plant macrofossil DCA axis 1 scores and humification values,we distinguished four hydrologic periods:a wet period from 7800 cal yr BP to 4500 cal yr BP,dry periods up to 1600 cal yr BP,drier periods until 300 cal yr BP,and the driest period from 300 cal yr BP until the present.Through a comparison with other climate records,we suggest that the East Asian summer monsoon(EAM) was the main driving force for vegetation and water level changes to the Shenjiadian peatland through its impacts on precipitation.展开更多
Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons(NOMCs) by the nanocasting method.The effect of the ...Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons(NOMCs) by the nanocasting method.The effect of the precursor on the resultant NOMC is extensively investigated by nitrogen adsorption-desorption measurements,scanning electron microscopy,X-ray photoelectron spectroscopy(XPS),cyclic voltammetry and rotating ring-disk electrode measurements.Salient findings are as follows.First,the precursor has a significant influence on the specific surface area and textural properties.The NOMC materials derived from pyrrole(C-PY-900:765 m^2/) and phenanthroline(C-Phen-900:746 m^2/) exhibit higher specific surface areas than the aniline analog(C-PA-900:569 m^2/).Second,the XPS results indicate that the total nitrogen content(ca.3.1–3.3 at%) is similar for the three carbon sources,except for a slight difference in the nitrogen configuration.Furthermore,the content of the nitrogen-activated carbon atoms is found to closely depend on the precursor,which is the highest for the phenanthroline-derived carbon.Third,the electrochemical results reveal that the electrocatalytic activity follows in the order C-PA-900 C-PY-900 C-Phen-900,confirming that the nitrogen-activated carbon atoms are the active sites for the oxygen reduction reaction(ORR).In summary,the precursor has considerable influence on the composition and textural properties of the NOMC materials,of which the ORR electrocatalytic activity can be enhanced through optimization of the NOMCs.展开更多
The carbonization process of a sucrose‐RuCl3/SBA‐15composite towards a Ru‐containing ordered mesoporous carbon(Ru‐OMC)catalyst was studied by in situ temperature‐programmed infrared spectroscopy to identify the s...The carbonization process of a sucrose‐RuCl3/SBA‐15composite towards a Ru‐containing ordered mesoporous carbon(Ru‐OMC)catalyst was studied by in situ temperature‐programmed infrared spectroscopy to identify the stabilization role of organic carbon precursors during the formation of highly dispersed Ru nanoparticles.The results show that the formation of metal carbonyl species results in the formation of homogeneously distributed Ru nanoparticles,and the rigid silica support and carbon matrix around the Ru(CO)x complex can significantly avoid the sintering and agglomeration of Ru metal particles during elevated temperature thermal treatment.These results ultimately demonstrate that sucrose plays important roles in the formation of homogeneously distributed Ru nanoparticles in a porous carbon matrix.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
The exploration of highly active and durable cathodic oxygen reduction reaction(ORR)catalysts with economical production cost is still the bottleneck to realize the large‐scale commercialization of fuel cells and me...The exploration of highly active and durable cathodic oxygen reduction reaction(ORR)catalysts with economical production cost is still the bottleneck to realize the large‐scale commercialization of fuel cells and metal‐air batteries.Given that carbon support is crucial to the electrocatalysts,and Pt is the best‐known ORR catalyst so far,in this work,we employed a simple impregnation method for synthesizing a kind of defective activated carbon(D‐AC)supported low Pt content electrocatalysts for the ORR.The reduction conditions of the Pt‐containing precursor were firstly optimized,and the influence of the Pt loading amount on the ORR was investigated as well.The results show that the obtained D‐AC@5.0%Pt sample(contains5wt%Pt)has surpassed the commercial Pt/C with20wt%Pt for the ORR in an alkaline solution.In the meantime,it is more stable than the commercial Pt/C.The outstanding ORR performance of the D‐AC@5.0%Pt confirms that both the unique defects in the D‐AC and the introduced Pt particles are indispensable to the ORR.Particularly,m the ORR activity of the synthesized catalysts is superior to most of the reported counterparts,but with much easier preparation methods and lower production cost,making them more advantageous in practical fuel cell applications.展开更多
Crucible lead smelting, a traditional technology unique to China, refers to the production of lead by reducing lead sulfide with iron metal in crucibles. In recent years, a number of crucible lead production sites of ...Crucible lead smelting, a traditional technology unique to China, refers to the production of lead by reducing lead sulfide with iron metal in crucibles. In recent years, a number of crucible lead production sites of the Liao-Jin-Yuan periods(tenth–fourteenth centuries CE) have been found in northern China, providing opportunities for the study of the technology. This paper provides a comprehensive overview of this technology based on the historical and archaeological evidence, with particular emphasis on the crucibles used. Firstly, it reviews the historical records on crucible lead smelting, and introduces, in detail, the technology used in Gansu during the Qing period(1644–1911) as well as indigenous methods used in the twentieth century;secondly, it summarizes the discoveries of crucible lead smelting sites in recent years, and reconstructs the manufacturing of crucibles and the iron reduction method by analysis of the crucible and slag;finally, it expounds the technical characteristics of crucible lead smelting, and explores the origin and development of the technology.展开更多
In our previous work,we calculated transport properties of pure gaseous polyatomic carbon tetrafluoride(CF4) and five equimolar binary gas mixtures of CF4 with noble gases through inversion technique.The present work ...In our previous work,we calculated transport properties of pure gaseous polyatomic carbon tetrafluoride(CF4) and five equimolar binary gas mixtures of CF4 with noble gases through inversion technique.The present work is a continuation of our studies on determining the transport properties of binary gas mixtures CF4 with some gases including three diatomic molecules CO,N2,and O2,a linear polyatomic CO2,and two non-linear polyatomic molecules SF6 and CH4.The Chapman-Enskog and Vesovic-Wakeham methods as well as inversion procedure are used to determine the viscosities,diffusivities,and thermal conductivities,which deviates from the literature values within 1%,4%,and 5%,respectively.展开更多
Nitrogen-doped carbon materials exhibiting high oxygen reduction reaction activity were prepared via the pyrolysis of a poly-p-phenylenediamine/carbon black composite. The as-synthesized cata- lyst showed excellent ca...Nitrogen-doped carbon materials exhibiting high oxygen reduction reaction activity were prepared via the pyrolysis of a poly-p-phenylenediamine/carbon black composite. The as-synthesized cata- lyst showed excellent catalytic activity in alkaline solution, and outperformed commercial Pt/C in KOH solution (0.1 mol/L), as demonstrated by the higher current density and the more positive half-wave potential. Scanning electron microscopy and N2 adsorption-desorption analyses indicated that a composite structure, in which the N-rich surface of the poly-p-phenylenediamine had an in- creased active center concentration and the high external surface area of the carbon black was conducive to the mass transport, is highly beneficial in terms of promoting the oxygen reduction reaction. However, the activity of this catalyst underwent an obvious decrease following exposure to air for 30 d. X-ray photoelectron spectroscopy showed that the oxygen content in the catalyst was increased by prolonged air exposure. O ls spectrum showed increases in the C:O and C-O compo- nents, suggesting that atmospheric oxygen reacted with the catalyst. This oxidation leaded to the deactivation of active center, thus the catalytic activity decreased. Based on these results, the stabil- ity in air of nitrogen-doped carbon materials must be taken into consideration when assessing ap- plications as alternatives to platinum-based materials.展开更多
Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization met...Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.展开更多
The adsorption kinetics of platinum(IV) chloride complex ions on the activated carbon Norit GF40 was investigated. Experiments were carried out at different initial concentrations of Pt(IV) chloride complex ions, ...The adsorption kinetics of platinum(IV) chloride complex ions on the activated carbon Norit GF40 was investigated. Experiments were carried out at different initial concentrations of Pt(IV) chloride complex ions, temperature, rate of mixing and pH. It was found that the value of activation energy of the studied process is equal to 19.7 kJ/mol. From the ICP MS analysis it was confirmed that platinum ions (Pt(IV) and Pt(II)) are removed from the solution due to the adsorption and are further reduced to the metallic state. Such mechanism was confirmed by XPS analysis which showed that on the carbon surface three forms of platinum species, i.e. Pt(0), Pt(II) and Pt(IV), exist. The presence of platinum in the solution at different oxidation states was also confirmed spectrophotometrically by identification of their characteristic absorption bands. The metallic form of Pt present on the surface of activated carbon was observed in the form of small spherical islands with the diameter not exceeding 500 nm. Those islands consist of smaller, flake-shape particles with a thickness of about 35 nm.展开更多
Activated carbons (ACs) with different surface properties were prepared from different raw materials. N2 adsorption, pH value, Boehm titration, Temperature-programmed reduction (TPR) and FTIR were employed to char...Activated carbons (ACs) with different surface properties were prepared from different raw materials. N2 adsorption, pH value, Boehm titration, Temperature-programmed reduction (TPR) and FTIR were employed to characterize the pore structure and surface chemical properties of the ACs. The results show that AC from bituminous coal (AC-B) has more meso-pores, higher pH value, more carboxylic groups and basic site than ACs from coconut shell and hawthorn(AC-C, AC-H). Oxygen in the mixture gas has great effect on S02 catalytic oxidation/oxidation ability of AC-B. In the absence of oxygen, the adsorbed SO2 on AC-B is 0.16 mmollg and the conversion ratio of adsorbed S02 to S03 is 22.07~; while in the presence of oxygen, the adsorbed amount of S02 is 0.42 retool/g, and all of the adsorbed S02 was totally converted to SO3. This feature of AC-B is consistent with its higher pH value, basic site and the reaction ability with H2 from TPR. The conversion ratios of S02 absorbed on both AC-C and AC-H were 100%, respectively.展开更多
Based on element geochemical studies of the main Permian exploitable coal measure strata in Western Guizhou, the element geochemical distribution characteristics of the main exploitable coal measures were revealed in ...Based on element geochemical studies of the main Permian exploitable coal measure strata in Western Guizhou, the element geochemical distribution characteristics of the main exploitable coal measures were revealed in the regions of Dafang, Qianxi, Weining, Hezhang, Zhijin, etc., of Guizhou Province, and the results show that their element contents are mainly affected by terrestrial material supply. Coal measures formed in the delta plain environment where sufficient terrestrial materials are supplied contain relatively abundant trace elements and rare-earth elements, whereas those formed in the tidal-fiat environment influenced greatly by seawater have relatively low contents of trace elements and rare-earth elements, mainly con- trolled by the geological fact that basalts the parent rocks from source regions contain high trace elements and rare-earth elements. In addition, coal measures affected by later hydrothermal activities and fault tectonics contain a large amount of harmful elements. According to the rules of distribution of elements in coal measures, a new idea was put forward to classify coal-forming environments by using the geochemical composition characteristics, which is of great significance in dissolving the problem of whether coal measures were fbrmed either in delta environments or in tidal-flat environments in Western Gui- zhou. At the same time, the rules of distribution of elements in the main exploitable coal measures in Western Guizhou were fully understood, which is of direct significance in utilizing coal resources on the basis of classification of coals, as well as in developing the coal chemical industry.展开更多
Reduction roasting-acid leaching process was utilized to process high-iron-content manganese oxide ore using black charcoal as reductant. The results indicate that, compared with the traditional reductant of anthracit...Reduction roasting-acid leaching process was utilized to process high-iron-content manganese oxide ore using black charcoal as reductant. The results indicate that, compared with the traditional reductant of anthracite, higher manganese extraction efficiency is achieved at lower roasting temperature and shorter residence time. The effects of roasting parameters on the leaching efficiency of Mn and Fe were studied, and the optimal parameters are determined as follows: roasting temperature is 650 °C, residence time is 40 min, and black charcoal dosage is 10%(mass fraction). Under these conditions, the leaching efficiency of Mn reaches 82.37% while that of Fe is controlled below 7%. XRD results show that a majority of MnO2 and Fe2O3 in the raw ore are reduced to MnO and Fe3O4, respectively.展开更多
Acrylonitrile-methyl methacrylate (AN-MMA) copolymer/silica nanocomposites were synthesized by in-situ emulsion polymerization initiated by 2,2'-azobis(2-amidinopropane) dihydrochloride absorbed onto colloidal si...Acrylonitrile-methyl methacrylate (AN-MMA) copolymer/silica nanocomposites were synthesized by in-situ emulsion polymerization initiated by 2,2'-azobis(2-amidinopropane) dihydrochloride absorbed onto colloidal silica particles, and the mesoporous carbon materials were prepared through carbonization of the obtained AN-MMA copolymer/silica nanocomposites, followed by HF etching. Thermogravimetric analysis of AN-MMAcopolymer/silica nanocomposltes snoweO mat me caroon ylelCl or copolymer was slgnuy oecreaseo as Silica parucle incorporated. N2 adsorption-desorption, scan electron microscopy (SEM) and transmission electron microscopy (TEM) were used to characterize the structure and morphology of the mesoporous carbon materials. Both SEM and展开更多
Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on...Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on catalytic performance of activated cokes of NO reduction with NH3 was investigated in a fixed-bed quartz micro reactor at 150 ℃. The results indicate that the selective catalytic reduction(SCR) activity of activated cokes with the increase of its surface acidic sites and oxygen content,obviously, a correlation between catalytic activity and surface acidic sites content by titration has higher linearity than catalytic activity and surface oxygen content by XPS. While basic sites content by acid-base titration have not correlation with SCR activity. It has been proposed that surface basic sites content measured by titration may not be on adjacent of acidic surface oxides and then cannot form of NO2-like species, thus the reaction of reduction of NO with NH3 have been retarded.展开更多
The aim of this study is to express the receptor-binding domain of Bacillus anthracis protective antigen in E.coli . Signal sequence of the outer membrane protein A (OmpA) of E.coli was attached to the 5′ end of the ...The aim of this study is to express the receptor-binding domain of Bacillus anthracis protective antigen in E.coli . Signal sequence of the outer membrane protein A (OmpA) of E.coli was attached to the 5′ end of the gene encoding protective antigen receptor-binding domain (the 4 th domain of PA, PAD4). The plasmid carrying the fusion gene was then transformed into E.coli and induced to express recombinant PAD4 by IPTG. The recombinant protein was purified by chromatography and then identified by N-terminal sequencing and Western blot. The recombinant protein, about 10% of the total bacterial protein in volume, was secreted to the periplasmic space of the cell. After a purification procedure including ion-exchange chromatography and gel filtration, about 10 mg of homogenous recombinant PAD4 was obtained from 1 L culture. Data from N-terminal sequencing suggested that the amino acid sequence of recombinant PAD4 was identical with its natural counterpart. And the result of Western blot showed the recombinant protein could bind with anti-PA serum from rabbit. High level secreted expression of PAD4 was obtained in E.coli . The results reported here are parts of a continuing research to evaluate PAD4 as a potential drug for anthrax therapy or a candidate of new vaccine.展开更多
Optimal charcoal concentrations were examined for tuff formation of SBIs (single-basidiospore isolates) obtained from Rhizoctonia solani AG-1 IC, AG-2-2 IV and AG-2-3, and SPIs (single-protoplast isolates) from AG...Optimal charcoal concentrations were examined for tuff formation of SBIs (single-basidiospore isolates) obtained from Rhizoctonia solani AG-1 IC, AG-2-2 IV and AG-2-3, and SPIs (single-protoplast isolates) from AG-1 IA by using PDCA with different charcoal concentrations. The best charcoal concentration for SBIs from AG-1 IC was 0.5%, from AG-2-3 was 1%, and from AG-2-2 IV was 2%. The optimal concentration was 0% for SPIs from AG-1 IA. The optimal charcoal concentrations used for tuff formation between SBIs and between SPIs are quite varied, depending on the different AGs. The results of AFLP haplotypes suggest that tuff isolates formed between SBIs/SPIs are heterokaryon.展开更多
文摘To replace precious metal oxygen reduction reaction(ORR)electrocatalysts,many transition metals and N-doped car-bon composites have been proposed in the last decade resulting in their rapid development as promising non-precious metal catalysts.We used Ketjenblack carbon as the precursor and mixed it with a polymeric ionic liquid(PIL)of[Hvim]NO_(3) and Fe(NO_(3))_(3),which was thermally calcined at 900℃ to produce a porous FeO_(x),N co-doped carbon material denoted FeO_(x)-N/C.Because the PIL of[Hvim]NO_(3) strongly combines with and disperses Fe^(3+)ions,and NO_(3)−is thermally pyrolyzed to form the porous structure,the FeO_(x)-N/C catalyst has a high electrocatalytic activity for the ORR in both 0.1 mol L^(−1) KOH and 0.5 mol L^(−1) H_(2)SO_(4) electrolytes.It was used as the catalyst to assemble a zinc-air battery,which had a peak power density of 185 mW·cm^(−2).Its superior electrocatalytic activity,wide pH range,and easy preparation make FeO_(x)-N/C a promising electrocatalyst for fuel cells and metal-air batteries.
基金Project(FRF-TP-15-009A3) supported by the Fundamental Research Funds for the Central Universities,ChinaProject(U1460201) supported by the National Natural Science Foundation of China
文摘The carbothermic reduction of Panzhihua ilmenite with various additions of activated carbon was investigated byisothermal experiments over the temperature range of1373to1773K in the argon atmosphere.According to the reaction kineticsrecorded by the infrared gas analyzer,it was found that the amount of carbon addition had little influence on the reaction rates atvarious temperatures except1473K.When the reaction temperature was above the eutectic temperature of1427K of Fe?C binarysystem,part of carbon would dissolve into Fe to form a liquid phase,which made the liquid Fe as a diffusion channel of carbon todiffuse to the reaction interface.The carbothermic reduction above1573K obeyed the shrinking-core model.The mass fraction ofTiC could be determined by the standard addition technique.
基金Under the auspices of Chinese Academy of Sciences/State Administration of Foreign Experts Affairs(CAS/SAFEA)International Partnership Program for Creative Research Teams(No.KZZD-EW-TZ-07)National Basic Research Program of China(No.2012CB956100)National Natural Science Foundation of China(No.41271209,41401099)
文摘This paper documents a 7800-year proxy record from the Shenjiadian peatland on the Sanjiang Plain in Northeast China.High-resolution plant macrofossil and colorimetric humification methods were used to reconstruct the vegetation and hydrologic history from a 193 cm-long sedimentary profile.Detrended correspondence analysis(DCA) was applied to transform the raw plant macrofossil data into latent indices of peatland water level.The vegetation community transited from an Equisetum fluviatile community to a Carex lasiocarpa community at approximately 3800 cal yr BP and was followed by a Carex-shrub community at approximately 480 cal yr BP.Based on the plant macrofossil DCA axis 1 scores and humification values,we distinguished four hydrologic periods:a wet period from 7800 cal yr BP to 4500 cal yr BP,dry periods up to 1600 cal yr BP,drier periods until 300 cal yr BP,and the driest period from 300 cal yr BP until the present.Through a comparison with other climate records,we suggest that the East Asian summer monsoon(EAM) was the main driving force for vegetation and water level changes to the Shenjiadian peatland through its impacts on precipitation.
基金supported by the National Natural Science Foundation of China(21476087,21576101)the Innovation Project of Guangdong Department of Education(2014KTSCX016)+1 种基金the Science&Technology Research Project of Guangdong Province(2013B010405005,2014A010105041)the Fundamental Research Funds for the Central Universities~~
文摘Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons(NOMCs) by the nanocasting method.The effect of the precursor on the resultant NOMC is extensively investigated by nitrogen adsorption-desorption measurements,scanning electron microscopy,X-ray photoelectron spectroscopy(XPS),cyclic voltammetry and rotating ring-disk electrode measurements.Salient findings are as follows.First,the precursor has a significant influence on the specific surface area and textural properties.The NOMC materials derived from pyrrole(C-PY-900:765 m^2/) and phenanthroline(C-Phen-900:746 m^2/) exhibit higher specific surface areas than the aniline analog(C-PA-900:569 m^2/).Second,the XPS results indicate that the total nitrogen content(ca.3.1–3.3 at%) is similar for the three carbon sources,except for a slight difference in the nitrogen configuration.Furthermore,the content of the nitrogen-activated carbon atoms is found to closely depend on the precursor,which is the highest for the phenanthroline-derived carbon.Third,the electrochemical results reveal that the electrocatalytic activity follows in the order C-PA-900 C-PY-900 C-Phen-900,confirming that the nitrogen-activated carbon atoms are the active sites for the oxygen reduction reaction(ORR).In summary,the precursor has considerable influence on the composition and textural properties of the NOMC materials,of which the ORR electrocatalytic activity can be enhanced through optimization of the NOMCs.
基金supported by the Natural Science Foundation of Zhejiang Province(LY17B030010)~~
文摘The carbonization process of a sucrose‐RuCl3/SBA‐15composite towards a Ru‐containing ordered mesoporous carbon(Ru‐OMC)catalyst was studied by in situ temperature‐programmed infrared spectroscopy to identify the stabilization role of organic carbon precursors during the formation of highly dispersed Ru nanoparticles.The results show that the formation of metal carbonyl species results in the formation of homogeneously distributed Ru nanoparticles,and the rigid silica support and carbon matrix around the Ru(CO)x complex can significantly avoid the sintering and agglomeration of Ru metal particles during elevated temperature thermal treatment.These results ultimately demonstrate that sucrose plays important roles in the formation of homogeneously distributed Ru nanoparticles in a porous carbon matrix.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
基金financially supported by the Australian Research Council (ARC)
文摘The exploration of highly active and durable cathodic oxygen reduction reaction(ORR)catalysts with economical production cost is still the bottleneck to realize the large‐scale commercialization of fuel cells and metal‐air batteries.Given that carbon support is crucial to the electrocatalysts,and Pt is the best‐known ORR catalyst so far,in this work,we employed a simple impregnation method for synthesizing a kind of defective activated carbon(D‐AC)supported low Pt content electrocatalysts for the ORR.The reduction conditions of the Pt‐containing precursor were firstly optimized,and the influence of the Pt loading amount on the ORR was investigated as well.The results show that the obtained D‐AC@5.0%Pt sample(contains5wt%Pt)has surpassed the commercial Pt/C with20wt%Pt for the ORR in an alkaline solution.In the meantime,it is more stable than the commercial Pt/C.The outstanding ORR performance of the D‐AC@5.0%Pt confirms that both the unique defects in the D‐AC and the introduced Pt particles are indispensable to the ORR.Particularly,m the ORR activity of the synthesized catalysts is superior to most of the reported counterparts,but with much easier preparation methods and lower production cost,making them more advantageous in practical fuel cell applications.
基金This paper is sponsored by“Preliminary Research on Ancient Chinese Crucible Smelting Technology”(Approval No.:51404242)“Research on Ancient Iron Reducing Silver and Lead Smelting Technology”(Approval No.:51704023)of the Youth Science Foundation of the National Natural Science Foundation of Chinathe Major Breakthrough project“Research on Ancient Chinese Crucible Smelting Technology”(Approval No.:Y621011003)of the Institute for the History of Natural Sciences,Chinese Academy of Sciences.
文摘Crucible lead smelting, a traditional technology unique to China, refers to the production of lead by reducing lead sulfide with iron metal in crucibles. In recent years, a number of crucible lead production sites of the Liao-Jin-Yuan periods(tenth–fourteenth centuries CE) have been found in northern China, providing opportunities for the study of the technology. This paper provides a comprehensive overview of this technology based on the historical and archaeological evidence, with particular emphasis on the crucibles used. Firstly, it reviews the historical records on crucible lead smelting, and introduces, in detail, the technology used in Gansu during the Qing period(1644–1911) as well as indigenous methods used in the twentieth century;secondly, it summarizes the discoveries of crucible lead smelting sites in recent years, and reconstructs the manufacturing of crucibles and the iron reduction method by analysis of the crucible and slag;finally, it expounds the technical characteristics of crucible lead smelting, and explores the origin and development of the technology.
文摘In our previous work,we calculated transport properties of pure gaseous polyatomic carbon tetrafluoride(CF4) and five equimolar binary gas mixtures of CF4 with noble gases through inversion technique.The present work is a continuation of our studies on determining the transport properties of binary gas mixtures CF4 with some gases including three diatomic molecules CO,N2,and O2,a linear polyatomic CO2,and two non-linear polyatomic molecules SF6 and CH4.The Chapman-Enskog and Vesovic-Wakeham methods as well as inversion procedure are used to determine the viscosities,diffusivities,and thermal conductivities,which deviates from the literature values within 1%,4%,and 5%,respectively.
基金supported by the National Natural Science Foundation of China(21476104)the Natural Science Foundation for Distinguished Young Scholars of Jiangsu Province(BK20150009)+4 种基金the Natural Science Foundation for Young Scholars of Jiangsu Province(BK20150396)the Soft Science Research Program of Jiangsu Province(BR2015009)the Nanotechnology Program of Suzhou(ZXG2013029)the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions,Qing Lan Project of Jiangsu Provincethe Fundamental Research Funds for the Central Universities,China
文摘Nitrogen-doped carbon materials exhibiting high oxygen reduction reaction activity were prepared via the pyrolysis of a poly-p-phenylenediamine/carbon black composite. The as-synthesized cata- lyst showed excellent catalytic activity in alkaline solution, and outperformed commercial Pt/C in KOH solution (0.1 mol/L), as demonstrated by the higher current density and the more positive half-wave potential. Scanning electron microscopy and N2 adsorption-desorption analyses indicated that a composite structure, in which the N-rich surface of the poly-p-phenylenediamine had an in- creased active center concentration and the high external surface area of the carbon black was conducive to the mass transport, is highly beneficial in terms of promoting the oxygen reduction reaction. However, the activity of this catalyst underwent an obvious decrease following exposure to air for 30 d. X-ray photoelectron spectroscopy showed that the oxygen content in the catalyst was increased by prolonged air exposure. O ls spectrum showed increases in the C:O and C-O compo- nents, suggesting that atmospheric oxygen reacted with the catalyst. This oxidation leaded to the deactivation of active center, thus the catalytic activity decreased. Based on these results, the stabil- ity in air of nitrogen-doped carbon materials must be taken into consideration when assessing ap- plications as alternatives to platinum-based materials.
文摘Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.
基金supported by the European Grant No. POIG.01.01.02.-00-015/09-00
文摘The adsorption kinetics of platinum(IV) chloride complex ions on the activated carbon Norit GF40 was investigated. Experiments were carried out at different initial concentrations of Pt(IV) chloride complex ions, temperature, rate of mixing and pH. It was found that the value of activation energy of the studied process is equal to 19.7 kJ/mol. From the ICP MS analysis it was confirmed that platinum ions (Pt(IV) and Pt(II)) are removed from the solution due to the adsorption and are further reduced to the metallic state. Such mechanism was confirmed by XPS analysis which showed that on the carbon surface three forms of platinum species, i.e. Pt(0), Pt(II) and Pt(IV), exist. The presence of platinum in the solution at different oxidation states was also confirmed spectrophotometrically by identification of their characteristic absorption bands. The metallic form of Pt present on the surface of activated carbon was observed in the form of small spherical islands with the diameter not exceeding 500 nm. Those islands consist of smaller, flake-shape particles with a thickness of about 35 nm.
基金support from the National Natural Science Foundation of China (No.50204011)
文摘Activated carbons (ACs) with different surface properties were prepared from different raw materials. N2 adsorption, pH value, Boehm titration, Temperature-programmed reduction (TPR) and FTIR were employed to characterize the pore structure and surface chemical properties of the ACs. The results show that AC from bituminous coal (AC-B) has more meso-pores, higher pH value, more carboxylic groups and basic site than ACs from coconut shell and hawthorn(AC-C, AC-H). Oxygen in the mixture gas has great effect on S02 catalytic oxidation/oxidation ability of AC-B. In the absence of oxygen, the adsorbed SO2 on AC-B is 0.16 mmollg and the conversion ratio of adsorbed S02 to S03 is 22.07~; while in the presence of oxygen, the adsorbed amount of S02 is 0.42 retool/g, and all of the adsorbed S02 was totally converted to SO3. This feature of AC-B is consistent with its higher pH value, basic site and the reaction ability with H2 from TPR. The conversion ratios of S02 absorbed on both AC-C and AC-H were 100%, respectively.
文摘Based on element geochemical studies of the main Permian exploitable coal measure strata in Western Guizhou, the element geochemical distribution characteristics of the main exploitable coal measures were revealed in the regions of Dafang, Qianxi, Weining, Hezhang, Zhijin, etc., of Guizhou Province, and the results show that their element contents are mainly affected by terrestrial material supply. Coal measures formed in the delta plain environment where sufficient terrestrial materials are supplied contain relatively abundant trace elements and rare-earth elements, whereas those formed in the tidal-fiat environment influenced greatly by seawater have relatively low contents of trace elements and rare-earth elements, mainly con- trolled by the geological fact that basalts the parent rocks from source regions contain high trace elements and rare-earth elements. In addition, coal measures affected by later hydrothermal activities and fault tectonics contain a large amount of harmful elements. According to the rules of distribution of elements in coal measures, a new idea was put forward to classify coal-forming environments by using the geochemical composition characteristics, which is of great significance in dissolving the problem of whether coal measures were fbrmed either in delta environments or in tidal-flat environments in Western Gui- zhou. At the same time, the rules of distribution of elements in the main exploitable coal measures in Western Guizhou were fully understood, which is of direct significance in utilizing coal resources on the basis of classification of coals, as well as in developing the coal chemical industry.
基金Project(2013JSJJ028)supported by the Teachers’Research Fund of Central South University,ChinaProject supported by Co-Innovation Center for Clean and Efficient Utilization of Strategic Mineral Resources,China
文摘Reduction roasting-acid leaching process was utilized to process high-iron-content manganese oxide ore using black charcoal as reductant. The results indicate that, compared with the traditional reductant of anthracite, higher manganese extraction efficiency is achieved at lower roasting temperature and shorter residence time. The effects of roasting parameters on the leaching efficiency of Mn and Fe were studied, and the optimal parameters are determined as follows: roasting temperature is 650 °C, residence time is 40 min, and black charcoal dosage is 10%(mass fraction). Under these conditions, the leaching efficiency of Mn reaches 82.37% while that of Fe is controlled below 7%. XRD results show that a majority of MnO2 and Fe2O3 in the raw ore are reduced to MnO and Fe3O4, respectively.
基金Supported by the Program for New Century Excellent Talents in University (NCET-07-0738)
文摘Acrylonitrile-methyl methacrylate (AN-MMA) copolymer/silica nanocomposites were synthesized by in-situ emulsion polymerization initiated by 2,2'-azobis(2-amidinopropane) dihydrochloride absorbed onto colloidal silica particles, and the mesoporous carbon materials were prepared through carbonization of the obtained AN-MMA copolymer/silica nanocomposites, followed by HF etching. Thermogravimetric analysis of AN-MMAcopolymer/silica nanocomposltes snoweO mat me caroon ylelCl or copolymer was slgnuy oecreaseo as Silica parucle incorporated. N2 adsorption-desorption, scan electron microscopy (SEM) and transmission electron microscopy (TEM) were used to characterize the structure and morphology of the mesoporous carbon materials. Both SEM and
基金the High Technology Research and Development Program of China(No.2011AA060803)the Beijing Key Laboratory Annual Program(No.Z121103009212039)
文摘Surface chemical properties of typical commercial coal-based activated cokes were characterized by Xray photoelectron spectroscopy(XPS) and acid-base titration, and then the influence of surface chemical properties on catalytic performance of activated cokes of NO reduction with NH3 was investigated in a fixed-bed quartz micro reactor at 150 ℃. The results indicate that the selective catalytic reduction(SCR) activity of activated cokes with the increase of its surface acidic sites and oxygen content,obviously, a correlation between catalytic activity and surface acidic sites content by titration has higher linearity than catalytic activity and surface oxygen content by XPS. While basic sites content by acid-base titration have not correlation with SCR activity. It has been proposed that surface basic sites content measured by titration may not be on adjacent of acidic surface oxides and then cannot form of NO2-like species, thus the reaction of reduction of NO with NH3 have been retarded.
文摘The aim of this study is to express the receptor-binding domain of Bacillus anthracis protective antigen in E.coli . Signal sequence of the outer membrane protein A (OmpA) of E.coli was attached to the 5′ end of the gene encoding protective antigen receptor-binding domain (the 4 th domain of PA, PAD4). The plasmid carrying the fusion gene was then transformed into E.coli and induced to express recombinant PAD4 by IPTG. The recombinant protein was purified by chromatography and then identified by N-terminal sequencing and Western blot. The recombinant protein, about 10% of the total bacterial protein in volume, was secreted to the periplasmic space of the cell. After a purification procedure including ion-exchange chromatography and gel filtration, about 10 mg of homogenous recombinant PAD4 was obtained from 1 L culture. Data from N-terminal sequencing suggested that the amino acid sequence of recombinant PAD4 was identical with its natural counterpart. And the result of Western blot showed the recombinant protein could bind with anti-PA serum from rabbit. High level secreted expression of PAD4 was obtained in E.coli . The results reported here are parts of a continuing research to evaluate PAD4 as a potential drug for anthrax therapy or a candidate of new vaccine.
文摘Optimal charcoal concentrations were examined for tuff formation of SBIs (single-basidiospore isolates) obtained from Rhizoctonia solani AG-1 IC, AG-2-2 IV and AG-2-3, and SPIs (single-protoplast isolates) from AG-1 IA by using PDCA with different charcoal concentrations. The best charcoal concentration for SBIs from AG-1 IC was 0.5%, from AG-2-3 was 1%, and from AG-2-2 IV was 2%. The optimal concentration was 0% for SPIs from AG-1 IA. The optimal charcoal concentrations used for tuff formation between SBIs and between SPIs are quite varied, depending on the different AGs. The results of AFLP haplotypes suggest that tuff isolates formed between SBIs/SPIs are heterokaryon.