Hydrophobic magnesium hydroxide(MH) nanoparticles were prepared by a one-step synthesis method in a high-gravity environment generated by a novel impinging stream–rotating packed bed(IS-RPB) reactor. The reactant sol...Hydrophobic magnesium hydroxide(MH) nanoparticles were prepared by a one-step synthesis method in a high-gravity environment generated by a novel impinging stream–rotating packed bed(IS-RPB) reactor. The reactant solutions were simultaneously and continuously pumped into the IS-RPB reactor, and then Tween80 was added as a surface modifier. The morphology, structure, and properties of blank and hydrophobic MH were characterized. The effects of MH nanoparticles on the flame retardancy, thermal stability, and mechanical properties of PP/MH composites were also studied. We found that the obtained MH nanoparticles exhibited hexagonal lamella with a mean size of 30 nm, excellent hydrophobic properties(e.g., high water contact angle of 112°), and improved thermal stability of MH. The limiting oxygen index(LOI) further showed that increased MH loading can significantly improve flame-retardant performance, which reached 29.3% for PP/MH composites with 30 wt% hydrophobic samples. The thermal stability and mechanical properties of the PP/MH composites with hydrophobic samples were also much higher than those of PP/MH composites with blank MH. Results showed that the one-step synthesis had high potential application in the large-scale production of hydrophobic MH nanoparticles.展开更多
The epoxidation of methyl oleate(MO)was conducted in the presence of aqueous H2O2 as the oxidant and hierarchical TS-1(HTS-1)as the catalyst;the catalyst was synthesized using polyquaternium-6 as the mesopore template...The epoxidation of methyl oleate(MO)was conducted in the presence of aqueous H2O2 as the oxidant and hierarchical TS-1(HTS-1)as the catalyst;the catalyst was synthesized using polyquaternium-6 as the mesopore template.The effects of various parameters,i.e.,H2O2/C=C molar ratio,oxidant concentration,amount of the catalyst,reaction temperature,and time,were systematically studied.Furthermore,response surface methodology(RSM)was used to optimize the conditions to maximize the yield of epoxy MO and to evaluate the significance and interplay of the factors affecting the epoxy MO production.The H2O2/C=C molar ratio and catalyst amount were the determining factors for MO epoxidation,wherein the maximum yield of epoxy MO reached 94.9%over HTS-1 under the optimal conditions.展开更多
The Changling fault depression passed through three stages of evolution: a period of faulting, a period of subsidence, and an inversion period. The fault lifted the whole area and the formation was eroded during the l...The Changling fault depression passed through three stages of evolution: a period of faulting, a period of subsidence, and an inversion period. The fault lifted the whole area and the formation was eroded during the late Yingcheng formation, the late Nenjiang formation, and the late Mingshui formation. The denudation quantity of eight wells located in the study area is estimated by the interval transit time method and by the formation trend extension method using seismic and drilling data. Inversion back stripping technology with de-compaction correction was used to restore the original sedimentary thickness step by step and to recover the burial history at a single well. Two profiles were selected for the recovery and study of the tectonic evolution. The study confirmed that the primary major gas bearing structure formed due to thermal shrinkage lifting during the late Yingcheng formation. Successive development in a pattern during the late Mingshui formation led to the formation of the primary gas pool. Vertical differential uplift during the late Nenjiang formation formed the Fulongquan structure during the late Paleogene. At this same time a secondary gas pool formed. A large scale reverse developed late in the Mingshui formation that provided the impetus for formation of a secondary gas pool. It is thought that the migration and accumulation of oil and gas was controlled by lithologic character, fracture, and structure. The local uplift in the vicinity of the hydrocarbon recession is most conducive to the collection of hydrocarbon gas.展开更多
Thick GaN films were grown on the sapphire substrate by hydride vapour phase epitaxy. The properties of GaN films were found to be significantly influenced by the duration of exposing the sapphire substrate to ammonia...Thick GaN films were grown on the sapphire substrate by hydride vapour phase epitaxy. The properties of GaN films were found to be significantly influenced by the duration of exposing the sapphire substrate to ammonia prior to the GaN growth initiation. The crystalline quality of GaN films revealed by high resolution X-ray diffraction were strongly dependent on the nitridation time, which determined substrate surface topography. The different nitridation schemes strongly affected the morphology of GaN overlayers resulting in the blue shift of the main excitonic peak in photoluminescence spectra at room temperature.展开更多
A modified Miedema model, using interrelationship among the basic properties of elements Ti and H, is employed to calculate the standard enthalpy of formation of titanium hydride TiHx (1≤x≤2). Based on Debye theor...A modified Miedema model, using interrelationship among the basic properties of elements Ti and H, is employed to calculate the standard enthalpy of formation of titanium hydride TiHx (1≤x≤2). Based on Debye theories of solid thermal capacity, the vibrational entropy, as well as electronic entropy, is acquired by quantum mechanics and statistic thermodynamics methods, and a new approach is presented to calculate the standard entropy of formation of TiH2. The values of standard enthalpy of formation of TiHx decrease linearly with increase of x. The calculated results of standard enthalpy, entropy, and free energy of formation of TiH2 at 298.16 K are -142.39 kJ/mol, -143.0 J/(mol·K) and -99.75 kJ/mol, respectively, which is consistent with the previously-reported data obtained by either experimental or theoretical calculation methods. The results show that the thermodynamic model for titanium hydride is reasonable.展开更多
Hydrocarbon contamination may affect the soil microbial community, in terms of both diversity and function. A laboratory experiment was set-up, with a semi-arid control soil and the same soil but artificially contamin...Hydrocarbon contamination may affect the soil microbial community, in terms of both diversity and function. A laboratory experiment was set-up, with a semi-arid control soil and the same soil but artificially contaminated with diesel oil, to follow changes in the dominant species of the microbial community in the hydrocarbon-polluted soil via proteomics. Analysis of the proteins extracted from enriched cultures growing in Luria-Bertani (LB) media showed a change in the microbial community. The majority of the proteins were related to gIycolysis pathways, structural or protein synthesis. The results showed a relative increase in the complexity of the soil microbial community with hydrocarbon contamination, especially after 15 days of incubation. Species such as Ralstonia solanacearum, Synechococcus elongatus and different Clostridium sp. were adapted to contamination, not appearing in the control soil, although Bacillus sp. dominated the growing in LB in any of the treatments. We conclude that the identification of microbial species in soil extracts by culture-dependent proteomics is able to partially explain the changes in the diversity of the soil microbial community in hydrocarbon polluted semi-arid soils, but this information is much more limited than that provided by molecular methods.展开更多
Introducing purifiers into hydrogen network can enhance the recovery and reuse of hydrogen in refineries, further reducing the consumption of fresh hydrogen. Based on previous graphical methods, this work proposes a s...Introducing purifiers into hydrogen network can enhance the recovery and reuse of hydrogen in refineries, further reducing the consumption of fresh hydrogen. Based on previous graphical methods, this work proposes a simple and unified graphical method for integration of hydrogen networks with purification processes. Scenarios with different hydrogen concentrations of purified product can be analyzed by the unified procedure. As a result, the maximum hydrogen saved by purification reuse can he identified and the corresponding purification process can be optimized, The proposed method is easy and non-iterative, and it is valid to purification processes with any feed concentration. A conventional hydrogen network is analyzed to test the effectiveness of the proposed method.展开更多
Based on the dynamic simulation of the 3 D structure the sedimentary modeling, the unit entity model has been adopted to transfer the heterogeneous complex passage system into limited simple homogeneous entity, and th...Based on the dynamic simulation of the 3 D structure the sedimentary modeling, the unit entity model has been adopted to transfer the heterogeneous complex passage system into limited simple homogeneous entity, and then the traditional dynamic simulation has been used to calculate the phase and the drive forces of the hydrocarbon , and the artificial neural network(ANN) technology has been applied to resolve such problems as the direction, velocity and quantity of the hydrocarbon migration among the unit entities. Through simulating of petroleum migration and accumulation in Zhu Ⅲ depression, the complex mechanism of hydrocarbon migration and accumulation has been opened out.展开更多
The oxidative dehydrogenation of isobutane to isobutene was examined for the use in the preparation of FSM-16 and related compounds doped by chromium with expectations that a yield of isobutene of greater than 8% coul...The oxidative dehydrogenation of isobutane to isobutene was examined for the use in the preparation of FSM-16 and related compounds doped by chromium with expectations that a yield of isobutene of greater than 8% could be achieved. The activity depended on the molding procedure of the catalyst and the doping method of the chromium species. In the present study, 8.8% and 8.3% of the yield of isobutene were obtained at 0.75 h and 6 h on-stream for the catalyst (Cr-loading; 6.2 wt.%) molded using wet treatment hut not pressurization treatment, in which the chromium species were directly added into the aqueous solution containing raw FSM-16 (hydrated sodium silicate powder) at an initial stage of the catalyst preparation. The structure information was based on XRD (X-ray diffraction), the specific surface area was determined using a conventional BET (Brunauer-Emmett-Teller) nitrogen adsorption and the loading of chromium was estimated using ICP (inductively coupled plasma). All those parameters combined with the molding method indicated that the catalytic activity was more influenced by the loading of chromium into bulk but not on surface of the catalyst rather than by the hexagonal structure of FSM-16 and the surface area.展开更多
The objective of this work is using the online measurement method to study the process of precipitation of nickel hydroxide in a single-feed semi-batch stirred reactor with an internal diameter ofD = 240mm. The effect...The objective of this work is using the online measurement method to study the process of precipitation of nickel hydroxide in a single-feed semi-batch stirred reactor with an internal diameter ofD = 240mm. The effects of impeller speed, impeller type, impeller diameter and feed location on the mean particle size d43 and particle size distribution (PSD) were investigated, d43 and PSD were measured online using a Malvern Insitec Liquid Pro- cess Sizer every 20 s. It was found that d43 varied between 13 kwh and 26 lain under different operating conditions, and it decreased with increasing impeller diameter. When feeding at the off-bottom distance of D/2 under lower impeller speeds, d43 was significantly smaller than that at D/3. PSDs were slightly influenced by operating conditions.展开更多
The linear and nonlinear optical properties of a hydrogenic donor in a disc-like parabolic quantum dot in the presence of an external magnetic field are studied. The calculations were performed within the effective ma...The linear and nonlinear optical properties of a hydrogenic donor in a disc-like parabolic quantum dot in the presence of an external magnetic field are studied. The calculations were performed within the effective mass approximation, using the matrix diagonalization method and the compact density-matrix approach. The linear and nonlinear optical absorption coefficients between the ground (L =0) and the first excited state (L = 1) have been examined based on the computed energies and wave functions. We find that the linear, nonlinear third-order, and total optical absorption coefficients are strongly affected by the confinement strength of QDs, the external magnetic field, and the incident optical intensity.展开更多
Exfoliated graphite oxide was prepared by an improved Hummers method and was then reduced to graphene with hydrazine in the presence of ammonium hydroxide.N2adsorption–desorption measurement showed that graphene so o...Exfoliated graphite oxide was prepared by an improved Hummers method and was then reduced to graphene with hydrazine in the presence of ammonium hydroxide.N2adsorption–desorption measurement showed that graphene so obtained had a specific surface area as high as 818 m2/g.Galvanostatic charge/discharge curves demonstrated that the as-prepared graphene exhibited a specific capacitance of 186.9 F/g at a current density of 0.1 A/g and that about 96%of the specific capacitance was retained after 2000 cycles at a current density of 5 A/g.展开更多
Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion e...Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion efficiency.Herein we report a strategy of boosting H_(2)production at low voltages by replacing OER with a bioelectrochemical cascade reaction at a triphase bioanode.In the presence of oxygen,oxidase enzymes can convert biomass into valuable products,and concurrently generate H_(2)O_(2) that can be further electrooxidized at the bioanode.Benefiting from the efficient oxidase kinetics at an oxygen-rich triphase bioanode and the more favorable thermodynamics of H_(2)O_(2)oxidation than that of OER,the cell voltage and energy consumption are reduced by~0.70 V and~36%,respectively,relative to regular water electrolysis.This leads to an efficient H_(2)production at the cathode and valuable product generation at the bioanode.Integration of a bioelectrochemical cascade into the water splitting process provides an energy-efficient and promising pathway for achieving a renewable fuel.展开更多
The adsorption and dissociation of CH3OH on TiO2 (110) were studied using density functional theory methods. Our results suggest that CH3OH molecules can adsorb up to 3/4 ML (1 ML=5.2× 10^14 molecules/cm2) co...The adsorption and dissociation of CH3OH on TiO2 (110) were studied using density functional theory methods. Our results suggest that CH3OH molecules can adsorb up to 3/4 ML (1 ML=5.2× 10^14 molecules/cm2) coverage at five-coordinated titanium (Tisc) sites to form the first layer. In the second layer, the CH3OH is adsorbed at bridge-bonded oxygen, and from the third layer, the CH3OH molecules form a hydrogen-bonded network with each other. The theoretical results show that dissociation of multilayer adsorbed methanol to aldehyde occurs through a stepwise pathway, with easy O-H bond dissociation and rate-determining C-H bond dissociation. The dissociation barriers for 8 or 12 CH3OH molecules on TiO2 are higher than that for low coverage by 0.15-0.21 eV; this suggests that the dissociation of multilayer adsorbed CH3OH is harder.展开更多
Different from the conventional synthesis methods and substrates, we designed a brand new method for synthesizing amides with platinum nanowires as catalysts and tert-butylhydroperoxide(TBHP) as the oxidant. Influence...Different from the conventional synthesis methods and substrates, we designed a brand new method for synthesizing amides with platinum nanowires as catalysts and tert-butylhydroperoxide(TBHP) as the oxidant. Influence of factors, such as the catalyst, solvents, and the reaction temperature, were studied to determine the optimal reaction conditions. In addition, we explored the substrate generality and observed excellent yields.展开更多
In this article, we present a facile, direct, synthetic approach of preparing monodisperse [Au2s(SePh)ls]- nanoclusters in high yield. In this synthetic approach, two-phase Brust-Schiffrin method is used. Both PhSeH...In this article, we present a facile, direct, synthetic approach of preparing monodisperse [Au2s(SePh)ls]- nanoclusters in high yield. In this synthetic approach, two-phase Brust-Schiffrin method is used. Both PhSeH and NaBH4 should be added drop-wise to the solution of Au (III) at the same time. The formula and molecular purity of [Au25(SePh)ls] TOA+ clusters are characterized by MALDI-TOF mass spectrometry, NMR and TGA analysis. Furthermore, some critical parameters to obtain pure [Au25(SePh)18]-TOA+ are identified, including the NaBH4-to-Au ratio, the selenolate-to-Au ratio and the temperature. The facile, direct, high yield synthetic method can be widely applied in the theoretical research of Au clusters protected by selenol.展开更多
基金Supported by the National Natural Science Foundation of China(21376229)the Science and Technology of Shanxi Province(2015031019-5)the Natural Science Foundation for Young Scientists of Shanxi Province(2015021033)
文摘Hydrophobic magnesium hydroxide(MH) nanoparticles were prepared by a one-step synthesis method in a high-gravity environment generated by a novel impinging stream–rotating packed bed(IS-RPB) reactor. The reactant solutions were simultaneously and continuously pumped into the IS-RPB reactor, and then Tween80 was added as a surface modifier. The morphology, structure, and properties of blank and hydrophobic MH were characterized. The effects of MH nanoparticles on the flame retardancy, thermal stability, and mechanical properties of PP/MH composites were also studied. We found that the obtained MH nanoparticles exhibited hexagonal lamella with a mean size of 30 nm, excellent hydrophobic properties(e.g., high water contact angle of 112°), and improved thermal stability of MH. The limiting oxygen index(LOI) further showed that increased MH loading can significantly improve flame-retardant performance, which reached 29.3% for PP/MH composites with 30 wt% hydrophobic samples. The thermal stability and mechanical properties of the PP/MH composites with hydrophobic samples were also much higher than those of PP/MH composites with blank MH. Results showed that the one-step synthesis had high potential application in the large-scale production of hydrophobic MH nanoparticles.
基金supported by the Evonik Industries AGthe Program for New Century Excellent Talents in University(NCET-04-0270)~~
文摘The epoxidation of methyl oleate(MO)was conducted in the presence of aqueous H2O2 as the oxidant and hierarchical TS-1(HTS-1)as the catalyst;the catalyst was synthesized using polyquaternium-6 as the mesopore template.The effects of various parameters,i.e.,H2O2/C=C molar ratio,oxidant concentration,amount of the catalyst,reaction temperature,and time,were systematically studied.Furthermore,response surface methodology(RSM)was used to optimize the conditions to maximize the yield of epoxy MO and to evaluate the significance and interplay of the factors affecting the epoxy MO production.The H2O2/C=C molar ratio and catalyst amount were the determining factors for MO epoxidation,wherein the maximum yield of epoxy MO reached 94.9%over HTS-1 under the optimal conditions.
基金the Marine Prospective Project of China Petrochemical Corporation (No.G0800-06-ZS324) for the financial support
文摘The Changling fault depression passed through three stages of evolution: a period of faulting, a period of subsidence, and an inversion period. The fault lifted the whole area and the formation was eroded during the late Yingcheng formation, the late Nenjiang formation, and the late Mingshui formation. The denudation quantity of eight wells located in the study area is estimated by the interval transit time method and by the formation trend extension method using seismic and drilling data. Inversion back stripping technology with de-compaction correction was used to restore the original sedimentary thickness step by step and to recover the burial history at a single well. Two profiles were selected for the recovery and study of the tectonic evolution. The study confirmed that the primary major gas bearing structure formed due to thermal shrinkage lifting during the late Yingcheng formation. Successive development in a pattern during the late Mingshui formation led to the formation of the primary gas pool. Vertical differential uplift during the late Nenjiang formation formed the Fulongquan structure during the late Paleogene. At this same time a secondary gas pool formed. A large scale reverse developed late in the Mingshui formation that provided the impetus for formation of a secondary gas pool. It is thought that the migration and accumulation of oil and gas was controlled by lithologic character, fracture, and structure. The local uplift in the vicinity of the hydrocarbon recession is most conducive to the collection of hydrocarbon gas.
基金National"863"Project of China (2001AA311100 and 2002AA305304) Sino French Cooperation Project:CNRS/ASC Chine 2003 Project(14915)
文摘Thick GaN films were grown on the sapphire substrate by hydride vapour phase epitaxy. The properties of GaN films were found to be significantly influenced by the duration of exposing the sapphire substrate to ammonia prior to the GaN growth initiation. The crystalline quality of GaN films revealed by high resolution X-ray diffraction were strongly dependent on the nitridation time, which determined substrate surface topography. The different nitridation schemes strongly affected the morphology of GaN overlayers resulting in the blue shift of the main excitonic peak in photoluminescence spectra at room temperature.
文摘A modified Miedema model, using interrelationship among the basic properties of elements Ti and H, is employed to calculate the standard enthalpy of formation of titanium hydride TiHx (1≤x≤2). Based on Debye theories of solid thermal capacity, the vibrational entropy, as well as electronic entropy, is acquired by quantum mechanics and statistic thermodynamics methods, and a new approach is presented to calculate the standard entropy of formation of TiH2. The values of standard enthalpy of formation of TiHx decrease linearly with increase of x. The calculated results of standard enthalpy, entropy, and free energy of formation of TiH2 at 298.16 K are -142.39 kJ/mol, -143.0 J/(mol·K) and -99.75 kJ/mol, respectively, which is consistent with the previously-reported data obtained by either experimental or theoretical calculation methods. The results show that the thermodynamic model for titanium hydride is reasonable.
基金Supported by the JAE-Program for Ph.D. Students of Spanish Research Council
文摘Hydrocarbon contamination may affect the soil microbial community, in terms of both diversity and function. A laboratory experiment was set-up, with a semi-arid control soil and the same soil but artificially contaminated with diesel oil, to follow changes in the dominant species of the microbial community in the hydrocarbon-polluted soil via proteomics. Analysis of the proteins extracted from enriched cultures growing in Luria-Bertani (LB) media showed a change in the microbial community. The majority of the proteins were related to gIycolysis pathways, structural or protein synthesis. The results showed a relative increase in the complexity of the soil microbial community with hydrocarbon contamination, especially after 15 days of incubation. Species such as Ralstonia solanacearum, Synechococcus elongatus and different Clostridium sp. were adapted to contamination, not appearing in the control soil, although Bacillus sp. dominated the growing in LB in any of the treatments. We conclude that the identification of microbial species in soil extracts by culture-dependent proteomics is able to partially explain the changes in the diversity of the soil microbial community in hydrocarbon polluted semi-arid soils, but this information is much more limited than that provided by molecular methods.
基金Supported by the National Basic Research Program of China(2012CB720500)the National Natural Science Foundation of China(21276204)
文摘Introducing purifiers into hydrogen network can enhance the recovery and reuse of hydrogen in refineries, further reducing the consumption of fresh hydrogen. Based on previous graphical methods, this work proposes a simple and unified graphical method for integration of hydrogen networks with purification processes. Scenarios with different hydrogen concentrations of purified product can be analyzed by the unified procedure. As a result, the maximum hydrogen saved by purification reuse can he identified and the corresponding purification process can be optimized, The proposed method is easy and non-iterative, and it is valid to purification processes with any feed concentration. A conventional hydrogen network is analyzed to test the effectiveness of the proposed method.
文摘Based on the dynamic simulation of the 3 D structure the sedimentary modeling, the unit entity model has been adopted to transfer the heterogeneous complex passage system into limited simple homogeneous entity, and then the traditional dynamic simulation has been used to calculate the phase and the drive forces of the hydrocarbon , and the artificial neural network(ANN) technology has been applied to resolve such problems as the direction, velocity and quantity of the hydrocarbon migration among the unit entities. Through simulating of petroleum migration and accumulation in Zhu Ⅲ depression, the complex mechanism of hydrocarbon migration and accumulation has been opened out.
文摘The oxidative dehydrogenation of isobutane to isobutene was examined for the use in the preparation of FSM-16 and related compounds doped by chromium with expectations that a yield of isobutene of greater than 8% could be achieved. The activity depended on the molding procedure of the catalyst and the doping method of the chromium species. In the present study, 8.8% and 8.3% of the yield of isobutene were obtained at 0.75 h and 6 h on-stream for the catalyst (Cr-loading; 6.2 wt.%) molded using wet treatment hut not pressurization treatment, in which the chromium species were directly added into the aqueous solution containing raw FSM-16 (hydrated sodium silicate powder) at an initial stage of the catalyst preparation. The structure information was based on XRD (X-ray diffraction), the specific surface area was determined using a conventional BET (Brunauer-Emmett-Teller) nitrogen adsorption and the loading of chromium was estimated using ICP (inductively coupled plasma). All those parameters combined with the molding method indicated that the catalytic activity was more influenced by the loading of chromium into bulk but not on surface of the catalyst rather than by the hexagonal structure of FSM-16 and the surface area.
基金the State Key Development Program for Basic Research of China(2013CB632601)the National High Technology Research and Development Program of China(2011AA060704)+1 种基金the National Natural Science Foundation of China(21476236,91434126)the National Science Fund for Distinguished Young Scholars(21025627)
文摘The objective of this work is using the online measurement method to study the process of precipitation of nickel hydroxide in a single-feed semi-batch stirred reactor with an internal diameter ofD = 240mm. The effects of impeller speed, impeller type, impeller diameter and feed location on the mean particle size d43 and particle size distribution (PSD) were investigated, d43 and PSD were measured online using a Malvern Insitec Liquid Pro- cess Sizer every 20 s. It was found that d43 varied between 13 kwh and 26 lain under different operating conditions, and it decreased with increasing impeller diameter. When feeding at the off-bottom distance of D/2 under lower impeller speeds, d43 was significantly smaller than that at D/3. PSDs were slightly influenced by operating conditions.
基金supported by National Natural Science Foundation of China under Grant No.10775035
文摘The linear and nonlinear optical properties of a hydrogenic donor in a disc-like parabolic quantum dot in the presence of an external magnetic field are studied. The calculations were performed within the effective mass approximation, using the matrix diagonalization method and the compact density-matrix approach. The linear and nonlinear optical absorption coefficients between the ground (L =0) and the first excited state (L = 1) have been examined based on the computed energies and wave functions. We find that the linear, nonlinear third-order, and total optical absorption coefficients are strongly affected by the confinement strength of QDs, the external magnetic field, and the incident optical intensity.
基金supported by the National Natural Science Foundation of China(Grant Nos.51072047,21271067)the Program for Innovative Research Team in University(Grant No.IRT-1237)
文摘Exfoliated graphite oxide was prepared by an improved Hummers method and was then reduced to graphene with hydrazine in the presence of ammonium hydroxide.N2adsorption–desorption measurement showed that graphene so obtained had a specific surface area as high as 818 m2/g.Galvanostatic charge/discharge curves demonstrated that the as-prepared graphene exhibited a specific capacitance of 186.9 F/g at a current density of 0.1 A/g and that about 96%of the specific capacitance was retained after 2000 cycles at a current density of 5 A/g.
基金supported by the National Key R&D Program of China(2019YFA0709200)the National Natural Science Foundation of China(21988102,51772198 and 21975171)。
文摘Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion efficiency.Herein we report a strategy of boosting H_(2)production at low voltages by replacing OER with a bioelectrochemical cascade reaction at a triphase bioanode.In the presence of oxygen,oxidase enzymes can convert biomass into valuable products,and concurrently generate H_(2)O_(2) that can be further electrooxidized at the bioanode.Benefiting from the efficient oxidase kinetics at an oxygen-rich triphase bioanode and the more favorable thermodynamics of H_(2)O_(2)oxidation than that of OER,the cell voltage and energy consumption are reduced by~0.70 V and~36%,respectively,relative to regular water electrolysis.This leads to an efficient H_(2)production at the cathode and valuable product generation at the bioanode.Integration of a bioelectrochemical cascade into the water splitting process provides an energy-efficient and promising pathway for achieving a renewable fuel.
基金financially supported by National Natural Science Foundation of China(21173212)the Key Research Program of the Chinese Academy of Sciences
文摘The adsorption and dissociation of CH3OH on TiO2 (110) were studied using density functional theory methods. Our results suggest that CH3OH molecules can adsorb up to 3/4 ML (1 ML=5.2× 10^14 molecules/cm2) coverage at five-coordinated titanium (Tisc) sites to form the first layer. In the second layer, the CH3OH is adsorbed at bridge-bonded oxygen, and from the third layer, the CH3OH molecules form a hydrogen-bonded network with each other. The theoretical results show that dissociation of multilayer adsorbed methanol to aldehyde occurs through a stepwise pathway, with easy O-H bond dissociation and rate-determining C-H bond dissociation. The dissociation barriers for 8 or 12 CH3OH molecules on TiO2 are higher than that for low coverage by 0.15-0.21 eV; this suggests that the dissociation of multilayer adsorbed CH3OH is harder.
基金supported by the National Natural Science Foundation of China (21373006, 51402203)the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Different from the conventional synthesis methods and substrates, we designed a brand new method for synthesizing amides with platinum nanowires as catalysts and tert-butylhydroperoxide(TBHP) as the oxidant. Influence of factors, such as the catalyst, solvents, and the reaction temperature, were studied to determine the optimal reaction conditions. In addition, we explored the substrate generality and observed excellent yields.
基金the financial support by the National Natural Science Foundation of China (20871112, 21072001, 21372006)Changjiang Scholars Program+1 种基金the Scientific Research Foundation for Returning Overseas Chinese Scholars, State Education Ministry, Ministry of Human Resources and Social Security, Anhui Province International Scientific and Technological Cooperation Project211 Project of Anhui University
文摘In this article, we present a facile, direct, synthetic approach of preparing monodisperse [Au2s(SePh)ls]- nanoclusters in high yield. In this synthetic approach, two-phase Brust-Schiffrin method is used. Both PhSeH and NaBH4 should be added drop-wise to the solution of Au (III) at the same time. The formula and molecular purity of [Au25(SePh)ls] TOA+ clusters are characterized by MALDI-TOF mass spectrometry, NMR and TGA analysis. Furthermore, some critical parameters to obtain pure [Au25(SePh)18]-TOA+ are identified, including the NaBH4-to-Au ratio, the selenolate-to-Au ratio and the temperature. The facile, direct, high yield synthetic method can be widely applied in the theoretical research of Au clusters protected by selenol.