Apatite-type lanthanum silicate with special conduction mechanism via interstitial oxygen has attracted considerable interest in recent years. In this work, pure powder of La9.33 2x/3MxSi6O26 （M=Mg, Ca, Sr） is prepa...Apatite-type lanthanum silicate with special conduction mechanism via interstitial oxygen has attracted considerable interest in recent years. In this work, pure powder of La9.33 2x/3MxSi6O26 （M=Mg, Ca, Sr） is prepared by the sol-gel method with sintering at 1000℃. The powder is characterized by X-ray diffraction （XRD） and scanning electron micrograph （SEM）. The apatite can be obtained at relatively low temperature as compared to the conventional solid-state reaction method. The measurements of conductivity of a series of doped samples La9.33-2x/3MxSi6O26 （M=Ca, Mg, Sr） indicate that the type of dopant and the amount have a significant effect on the conductivity. The greatest decrease in conductivity is observed for Mg doping, following the Ca and the Sr doped apatites. The effect is ultimately attributed to the amount of oxygen interstitials, which is affected by the crystal lattice distortion arising from cation vacancies.展开更多
AB-8 resin was used as an adsorbent for the removal of trans-1,2-cyclohexandiol(CHD) from aqueous solutions.Batch experiments were carried out to investigate the effect of contact time and temperature on sorption effi...AB-8 resin was used as an adsorbent for the removal of trans-1,2-cyclohexandiol(CHD) from aqueous solutions.Batch experiments were carried out to investigate the effect of contact time and temperature on sorption efficiency.The adsorptive thermodynamic properties and kinetics of CHD from water onto AB-8 resin were studied.The Langmuir and Freundlich isotherm models were employed to discuss the adsorption behavior.Thermodynamic parameters such as G,H and S were calculated.The results indicate that the equilibrium data are perfectly represented by Langmuir isotherm model.Thermodynamic study reveals that it is an exothermic process in nature and mainly physical adsorption enhanced by chemisorption with a decrease of entropy process.The kinetics of CHD adsorption is well described by the pseudo second-order model.The adsorbed CHD can be eluted from AB-8 resin by 5% ethanol aqueous solution with 100% elution percentage.展开更多
Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ has been successfully prepared by using citrate-EDTA complexation method at relatively low calcination temperature. The structure and thermal decomposition process of ...Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ has been successfully prepared by using citrate-EDTA complexation method at relatively low calcination temperature. The structure and thermal decomposition process of the complex precursor have been investigated by means of differential scanning calorimetry-thermal gravimetric analysis （DSC/TGA）, X-ray diffraction （XRD）, and Fourier transform infrared spectroscopic （FT-IR） measurements. The precursor decomposed completely and started to form perovskite-type oxide above 420 ℃ according to the differential scanning calorimetry （DSC） and thermal gravimetric analysis （TGA） results. Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ obtained has been confirmed from the XRD pattern, and no peak of SrCO3 was found by XRD of the oxides synthesized at a relatively low temperature of 800℃. The reducibility of La0.6Sr0.4Co0.8Fe0.2O3-δ was also characterized by the temperature programmed reduction （TPR） technique. Disk shaped dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was prepared by the isostatical pressing method. The oxygen flux rate of dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was （2.8-18）× 10^-8 mol/（cm^2.s） in the temperature range of 800-1000 ℃.展开更多
In this work, the thermodynamic parameters for the adsorption of water vapor on untreated silica gel and silica gel treated with hygroscopic salts and silane coupling agent were determined by lnverse Gas Chromatograp...In this work, the thermodynamic parameters for the adsorption of water vapor on untreated silica gel and silica gel treated with hygroscopic salts and silane coupling agent were determined by lnverse Gas Chromatography （IGC） in the infinite dilution region. The desorption activation energies of the water vapor on virgin and modified silica gels were estimated by using the Temperature Programmed Desorption （TPD） technique. The interactions between the water and the virgin and modified silica gels were discussed. Results showed that the thermodynamic parameters and desorption activation energy of water vapour on the silica gels increase with decreasing pore size and increasing the surface hydrophilic properties. The desorption activation energy of virgin and modified silica gels was found to increase with increasing the thermodynamic parameters. The larger the adsorption parameters and the desorption activation energy were, the interactions between water and virgin and modified silica gels were.展开更多
The solubility data of diosgenin in mixed systems of ethanol ＋ 1-propanol （1 ： 1）, ethanol ＋ 1-butanol （1 ： 1）, ethanol ＋ isobutyl alcohol （1 ： 1）, methanol ＋ isobutyl alcohol （1 ： 1）, methanol ＋ isob...The solubility data of diosgenin in mixed systems of ethanol ＋ 1-propanol （1 ： 1）, ethanol ＋ 1-butanol （1 ： 1）, ethanol ＋ isobutyl alcohol （1 ： 1）, methanol ＋ isobutyl alcohol （1 ： 1）, methanol ＋ isobutyl alcohol （1 ： 4）, ethanol ＋ 1-pentanol （1 ： 1） and carbon tetrachloride were measured over the temperature range from 289.15 K to 334.15 K by a laser monitoring observation technique at atmospheric pressure, with all mixtures mixed by volume ratio. The Apelblat equation, the ideal solution model, and the 2h equation are used to correlate the solubility data. The results show that the three models agree well with the experimental data, providing essential support for industrial design and further theoretical study.展开更多
[ Objectives] The paper was to study effects of different microbial agents on occurrence of tobacco bacterial wilt. [ Methods I Antagonistic strains against Ralstonia solanacearum were screened from in situ soil, and ...[ Objectives] The paper was to study effects of different microbial agents on occurrence of tobacco bacterial wilt. [ Methods I Antagonistic strains against Ralstonia solanacearum were screened from in situ soil, and prepared into four different combinations. The number of soil microorganisms and incidence of bacterial wilt of four combinations were observed. [ Results] The incidence rate of bacterial wilt treated by microbial agent OR-1 was significantly lower than that in control, and the control efficacy against bacterial wilt reached 67%. [ Conclusions] Application of microbial agent OR-1 could effectively reduce the incidence rate and disease index of bacterial wilt, thus improving the quality of tobacco.展开更多
A fibrous strong base anion exchanger （QAPPS） was prepared for the first time via chloromethylation and quaternary amination reaction of polyphenylene sulfide fiber （PPS）, and its physical-chemical structure and a...A fibrous strong base anion exchanger （QAPPS） was prepared for the first time via chloromethylation and quaternary amination reaction of polyphenylene sulfide fiber （PPS）, and its physical-chemical structure and adsorption behavior for Cr（VI） were characterized by FT- IR, Energy Dispersive Spectrometry, TG-DTG, elemental analysis and batch adsorptive technique, respectively. The novel fibrous adsorbent could effectively adsorb Cr（VI） over the pH range 1-12, the maximum adsorption capacity was 166.39 mg/g at pH 3.5, and the adsorption behavior could be described well by Langmuir isotherm equation model. The adsorption kinetics was studied using pseudo first-order and pseudo second-order models, and the 4/2 and equilibrium adsorption time were 5 and 20 min respectively when initial Cr（VI） concentration was 100 mg/L. The saturated fibers could be regenerated rapidly by a mixed solution of 0.5 mol/L NaOH and 0.5 mol/L NaCl, and the adsorption capacity was well maintained after six adsorption-desorption cycles.展开更多
A series of novel chelating fibers containing sulfur, nitrogen, oxygen heteroatoms were prepared via the functionalization of chloromethylated polyphenylene sulfide （CMPPS）. The structures, micromorpholo- gy and phy...A series of novel chelating fibers containing sulfur, nitrogen, oxygen heteroatoms were prepared via the functionalization of chloromethylated polyphenylene sulfide （CMPPS）. The structures, micromorpholo- gy and physicochemical properties of these fibrous adsorptive materials were characterized by FT-IR, elementary analysis, TG and SEM-EDS. The results show that chelating fibers had high functional group contents （3.94 mmol/g for thiourea, 3.85 mmol/g for mercapto, 5.00 mmol/g for methylamine and 6.07 mmol/g for ethylenediamine, respectively）. Owing to the unique matrix of polyphenylene sulfide fiber, these fibrous adsorbents possess excellent thermostability. This synthetic method proved a simple and efficient way for the preparation of chelating fibers.展开更多
Two-dimensional carbon nitride(2 D-C_(3) N_(4))nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.T...Two-dimensional carbon nitride(2 D-C_(3) N_(4))nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.To tackle this issue,herein,a hierarchical Nb_(2) O_(5)/2 D-C_(3) N_(4) heterostructure is precisely constructed and the built-in electric field between Nb_(2)O_(5) and 2 D-C_(3) N_(4) can provide the driving force to separate/transfer the charge carriers efficiently.Moreover,the strongly Lewis acidic Nb_(2)O_(5) can adsorb TEOA molecules on its surface at locally high concentrations to facilitate the oxidation reaction kinetics under irradiation,resulting in efficient photogene rated electrons-holes separation and exceptional photocatalytic hydrogen evolution.As expected,the champion Nb_(2)O_(5)/2 D-C_(3)N_(4) heterostructure achieves an exceptional H2 evolution rate of 31.6 mmol g^(-1) h^(-1),which is 213.6 times and 4.3 times higher than that of pristine Nb_(2)O_(5) and2 D-C_(3)N_(4),respectively.Moreover,the champion heterostructure possesses a high apparent quantum efficiency(AQE)of 45.08%atλ=405 nm and superior cycling stability.Furthermore,a possible photocatalytic mechanism of the energy band alignment at the hetero-interface is proposed based on the systematical characterizations accompanied by density functional theory(DFT)calculations.This work paves the way for the precise construction of a high-quality heterostructured photocatalyst with efficient charge separation to boost hydrogen production.展开更多
Heterojunction structure has been extensively employed for the design of novel catalysts.In the present study,density functional theory was utilized to investigate the electronic structure and hydrogen evolution perfo...Heterojunction structure has been extensively employed for the design of novel catalysts.In the present study,density functional theory was utilized to investigate the electronic structure and hydrogen evolution performance of Ti_(3)C_(2)O_(2)MXene quantum dots/graphene(QDs/G)heterostructure.Results show that a slight distortion can be observed in graphene after hybriding with QDs,due to which the electronic structure of QDs have been changed.Associated with such QDs-graphene interaction,the catalytic activity of Ti_(3)C_(2)O_(2)QDs has been optimized,leading to excellent HER catalytic performance.展开更多
Water electrolysis is to split water into hydrogen and oxygen using electricity as the driving force.To obtain low-cost hydrogen in a large scale,it is critical to develop electrocatalysts based on earth abundant elem...Water electrolysis is to split water into hydrogen and oxygen using electricity as the driving force.To obtain low-cost hydrogen in a large scale,it is critical to develop electrocatalysts based on earth abundant elements with a high efficiency.This computational work started with Cobalt on CoTh_(2)C)_(6)surface as the active site,CoTa_(2)O_(6)/Graphene heterojunctions have been explored as potential oxygen evolution reaction(OER)catalysts through density functional theory(DFT).We demonstrated that the electron transfer(_(6))from CoTa_(2)C)_(6)to graphene substrate can be utilized to boost the reactivity of Co-site,leading to an OER overpotential as low as 0.30 V when N-doped graphene is employed.Our findings offer novel design of heterojunctions as high performance OER catalysts.展开更多
The large-scale production of ammonia mainly depends on the Haber-Bosch process,which will lead to the problems of high energy consumption and carbon dioxide emission.Electrochemical nitrogen fixation is considered to...The large-scale production of ammonia mainly depends on the Haber-Bosch process,which will lead to the problems of high energy consumption and carbon dioxide emission.Electrochemical nitrogen fixation is considered to be an environmental friendly and sustainable process,but its efficiency largely depends on the activity and stability of the catalyst.Therefore,it is imperative to develop high-efficient electrocatalysts in the field of nitrogen reduction reaction(NRR).In this paper,we developed a BiVO_(4)/TiO_(2) nanotube(BiVO_(4)/TNT)heterojunction composite with rich oxygen vacancies as an electrocatalytic NRR catalyst.The heterojunction interface and oxygen vacancy of BiVO_(4)/TNT can be the active site of N2 dynamic activation and proton transition.The synergistic effect of TiO_(2) and BiVO_(4) shortens the proton transport path and reduces the over potential of chemical reaction.BiVO_(4)/TNT has high ammonia yield of 8.54µg·h^(−1)·cm^(−2) and high Faraday efficiency of 7.70%in−0.8 V vs.RHE in 0.1 M Na_(2)SO_(4) solution.展开更多
Confined metal clusters as sub-nanometer reactors for electrocatalytic N_(2) reduction reaction(eNRR)have received increasing attention due to the unique metal-metal interaction and higher activity than singleatom cat...Confined metal clusters as sub-nanometer reactors for electrocatalytic N_(2) reduction reaction(eNRR)have received increasing attention due to the unique metal-metal interaction and higher activity than singleatom catalysts.Herein,the inspiration of the superior capacitance and unique microenvironment with regular surface cavities of the porous boron nitride(p-BN)nanosheets,we systematically studied the catalytic activity for NRR of transition-metal single-clusters in the triplet form(V_(3),Fe_(3),Mo_(3) and W_(3))confined in the surface cavities of the p-BN sheets by spin-polarized density functional theory(DFT)calculations.After a two-step screening strategy,Mo_(3)@p-BN was found to have high catalytic activity and selectivity with a rather low limiting potential(-0.34 V)for the NRR.The anchored Mo_(3) singlecluster can be stably embedded on the surface cavities of the substrate preventing the diffusion of the active Mo atoms.More importantly,the Mo atoms in the Mo_(3) single-cluster would act as“cache”to accelerate electron transfer between active metal centers and nitrogen-containing intermediates via the intimate Mo-Mo interactions.The cooperation of Mo atoms can also provide a large number of occupied and unoccupied d orbitals to make the"donation-backdonation"mechanism more effective.This work not only provides a quite promising electrocatalyst for NRR,but also brings new insights into the rational design of triple-atom NRR catalysts.展开更多
基金Supported by the Natural Science Foundation of Guangdong PrOvince （06025657） and Guangdong Provincial Green Chemicals.
文摘Apatite-type lanthanum silicate with special conduction mechanism via interstitial oxygen has attracted considerable interest in recent years. In this work, pure powder of La9.33 2x/3MxSi6O26 （M=Mg, Ca, Sr） is prepared by the sol-gel method with sintering at 1000℃. The powder is characterized by X-ray diffraction （XRD） and scanning electron micrograph （SEM）. The apatite can be obtained at relatively low temperature as compared to the conventional solid-state reaction method. The measurements of conductivity of a series of doped samples La9.33-2x/3MxSi6O26 （M=Ca, Mg, Sr） indicate that the type of dopant and the amount have a significant effect on the conductivity. The greatest decrease in conductivity is observed for Mg doping, following the Ca and the Sr doped apatites. The effect is ultimately attributed to the amount of oxygen interstitials, which is affected by the crystal lattice distortion arising from cation vacancies.
文摘AB-8 resin was used as an adsorbent for the removal of trans-1,2-cyclohexandiol(CHD) from aqueous solutions.Batch experiments were carried out to investigate the effect of contact time and temperature on sorption efficiency.The adsorptive thermodynamic properties and kinetics of CHD from water onto AB-8 resin were studied.The Langmuir and Freundlich isotherm models were employed to discuss the adsorption behavior.Thermodynamic parameters such as G,H and S were calculated.The results indicate that the equilibrium data are perfectly represented by Langmuir isotherm model.Thermodynamic study reveals that it is an exothermic process in nature and mainly physical adsorption enhanced by chemisorption with a decrease of entropy process.The kinetics of CHD adsorption is well described by the pseudo second-order model.The adsorbed CHD can be eluted from AB-8 resin by 5% ethanol aqueous solution with 100% elution percentage.
基金Sponsored by SRF for ROCS, key lab of enhanced heat transfer and energy conservation (MOE)Guangdong provincial natural science foundation (04020126).
文摘Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ has been successfully prepared by using citrate-EDTA complexation method at relatively low calcination temperature. The structure and thermal decomposition process of the complex precursor have been investigated by means of differential scanning calorimetry-thermal gravimetric analysis （DSC/TGA）, X-ray diffraction （XRD）, and Fourier transform infrared spectroscopic （FT-IR） measurements. The precursor decomposed completely and started to form perovskite-type oxide above 420 ℃ according to the differential scanning calorimetry （DSC） and thermal gravimetric analysis （TGA） results. Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ obtained has been confirmed from the XRD pattern, and no peak of SrCO3 was found by XRD of the oxides synthesized at a relatively low temperature of 800℃. The reducibility of La0.6Sr0.4Co0.8Fe0.2O3-δ was also characterized by the temperature programmed reduction （TPR） technique. Disk shaped dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was prepared by the isostatical pressing method. The oxygen flux rate of dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was （2.8-18）× 10^-8 mol/（cm^2.s） in the temperature range of 800-1000 ℃.
文摘In this work, the thermodynamic parameters for the adsorption of water vapor on untreated silica gel and silica gel treated with hygroscopic salts and silane coupling agent were determined by lnverse Gas Chromatography （IGC） in the infinite dilution region. The desorption activation energies of the water vapor on virgin and modified silica gels were estimated by using the Temperature Programmed Desorption （TPD） technique. The interactions between the water and the virgin and modified silica gels were discussed. Results showed that the thermodynamic parameters and desorption activation energy of water vapour on the silica gels increase with decreasing pore size and increasing the surface hydrophilic properties. The desorption activation energy of virgin and modified silica gels was found to increase with increasing the thermodynamic parameters. The larger the adsorption parameters and the desorption activation energy were, the interactions between water and virgin and modified silica gels were.
基金Supported by Science and Technology Breakthrough Major Project in Henan Province(112101210200)
文摘The solubility data of diosgenin in mixed systems of ethanol ＋ 1-propanol （1 ： 1）, ethanol ＋ 1-butanol （1 ： 1）, ethanol ＋ isobutyl alcohol （1 ： 1）, methanol ＋ isobutyl alcohol （1 ： 1）, methanol ＋ isobutyl alcohol （1 ： 4）, ethanol ＋ 1-pentanol （1 ： 1） and carbon tetrachloride were measured over the temperature range from 289.15 K to 334.15 K by a laser monitoring observation technique at atmospheric pressure, with all mixtures mixed by volume ratio. The Apelblat equation, the ideal solution model, and the 2h equation are used to correlate the solubility data. The results show that the three models agree well with the experimental data, providing essential support for industrial design and further theoretical study.
基金Supported by Science and Technology Project of Nanping Branch of Fujian Tobacco Company(NYK2012-14-3)
文摘[ Objectives] The paper was to study effects of different microbial agents on occurrence of tobacco bacterial wilt. [ Methods I Antagonistic strains against Ralstonia solanacearum were screened from in situ soil, and prepared into four different combinations. The number of soil microorganisms and incidence of bacterial wilt of four combinations were observed. [ Results] The incidence rate of bacterial wilt treated by microbial agent OR-1 was significantly lower than that in control, and the control efficacy against bacterial wilt reached 67%. [ Conclusions] Application of microbial agent OR-1 could effectively reduce the incidence rate and disease index of bacterial wilt, thus improving the quality of tobacco.
基金support of the National Natural Science Foundation of China (No. 20574063,21004055)
文摘A fibrous strong base anion exchanger （QAPPS） was prepared for the first time via chloromethylation and quaternary amination reaction of polyphenylene sulfide fiber （PPS）, and its physical-chemical structure and adsorption behavior for Cr（VI） were characterized by FT- IR, Energy Dispersive Spectrometry, TG-DTG, elemental analysis and batch adsorptive technique, respectively. The novel fibrous adsorbent could effectively adsorb Cr（VI） over the pH range 1-12, the maximum adsorption capacity was 166.39 mg/g at pH 3.5, and the adsorption behavior could be described well by Langmuir isotherm equation model. The adsorption kinetics was studied using pseudo first-order and pseudo second-order models, and the 4/2 and equilibrium adsorption time were 5 and 20 min respectively when initial Cr（VI） concentration was 100 mg/L. The saturated fibers could be regenerated rapidly by a mixed solution of 0.5 mol/L NaOH and 0.5 mol/L NaCl, and the adsorption capacity was well maintained after six adsorption-desorption cycles.
基金support by the National Natural Science Foundation of China(No.20574063)Doctoral Foundation of Ministry of Education of China(No. 20104101110005)
文摘A series of novel chelating fibers containing sulfur, nitrogen, oxygen heteroatoms were prepared via the functionalization of chloromethylated polyphenylene sulfide （CMPPS）. The structures, micromorpholo- gy and physicochemical properties of these fibrous adsorptive materials were characterized by FT-IR, elementary analysis, TG and SEM-EDS. The results show that chelating fibers had high functional group contents （3.94 mmol/g for thiourea, 3.85 mmol/g for mercapto, 5.00 mmol/g for methylamine and 6.07 mmol/g for ethylenediamine, respectively）. Owing to the unique matrix of polyphenylene sulfide fiber, these fibrous adsorbents possess excellent thermostability. This synthetic method proved a simple and efficient way for the preparation of chelating fibers.
基金Finacial support from the Natural Science Foundation of Jiangsu Province(BK20170549,BK20180887)the National Natural Science Foundation of China(21706103,62004084)+3 种基金Guangdong Innovation Research Team for Higher Education(2017KCXTD030)the High-level Talents Project of Dongguan University of Technology(KCYKYQD2017017)the Young Talent Cultivation Plan of Jiangsu UniversityJiangsu Provincial Program for High-Level Innovative and Entrepreneurial Talents Introduction。
文摘Two-dimensional carbon nitride(2 D-C_(3) N_(4))nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.To tackle this issue,herein,a hierarchical Nb_(2) O_(5)/2 D-C_(3) N_(4) heterostructure is precisely constructed and the built-in electric field between Nb_(2)O_(5) and 2 D-C_(3) N_(4) can provide the driving force to separate/transfer the charge carriers efficiently.Moreover,the strongly Lewis acidic Nb_(2)O_(5) can adsorb TEOA molecules on its surface at locally high concentrations to facilitate the oxidation reaction kinetics under irradiation,resulting in efficient photogene rated electrons-holes separation and exceptional photocatalytic hydrogen evolution.As expected,the champion Nb_(2)O_(5)/2 D-C_(3)N_(4) heterostructure achieves an exceptional H2 evolution rate of 31.6 mmol g^(-1) h^(-1),which is 213.6 times and 4.3 times higher than that of pristine Nb_(2)O_(5) and2 D-C_(3)N_(4),respectively.Moreover,the champion heterostructure possesses a high apparent quantum efficiency(AQE)of 45.08%atλ=405 nm and superior cycling stability.Furthermore,a possible photocatalytic mechanism of the energy band alignment at the hetero-interface is proposed based on the systematical characterizations accompanied by density functional theory(DFT)calculations.This work paves the way for the precise construction of a high-quality heterostructured photocatalyst with efficient charge separation to boost hydrogen production.
基金The authors would like to acknowledge funding from the National Natural Science Foundation of China(Grant No.11832007)China Postdoctoral Science Foundation(Grant No.2018M631082)+2 种基金Application and Foundation Research Projects of Sichuan Province(Grant Nos.2018JY0062 and 2019YJ0668)Guangdong Innovation Research Team for Higher Education(Grant No.2017KCXTD030)High-level Talents Project of Dongguan University of Technology(Grant No.KCYKYQD2017017).
文摘Heterojunction structure has been extensively employed for the design of novel catalysts.In the present study,density functional theory was utilized to investigate the electronic structure and hydrogen evolution performance of Ti_(3)C_(2)O_(2)MXene quantum dots/graphene(QDs/G)heterostructure.Results show that a slight distortion can be observed in graphene after hybriding with QDs,due to which the electronic structure of QDs have been changed.Associated with such QDs-graphene interaction,the catalytic activity of Ti_(3)C_(2)O_(2)QDs has been optimized,leading to excellent HER catalytic performance.
基金support through the Australia Research Council Industrial Transformation Training Centres scheme(Grant No.IC180100005)The authors acknowledge the financial support by Guangdong Innovation Research Team for Higher Education(Grant No.2017KCXTD030)+1 种基金High-level Talents Project of Dongguan University of Technology(Grant No.KCYKYQD2017017)Engineering Research Center of None-food Biomass Efficient Pyrolysis and Utilization Technology of Guangdong Higher Education Institutes(Grant No.2016GCZX009).
文摘Water electrolysis is to split water into hydrogen and oxygen using electricity as the driving force.To obtain low-cost hydrogen in a large scale,it is critical to develop electrocatalysts based on earth abundant elements with a high efficiency.This computational work started with Cobalt on CoTh_(2)C)_(6)surface as the active site,CoTa_(2)O_(6)/Graphene heterojunctions have been explored as potential oxygen evolution reaction(OER)catalysts through density functional theory(DFT).We demonstrated that the electron transfer(_(6))from CoTa_(2)C)_(6)to graphene substrate can be utilized to boost the reactivity of Co-site,leading to an OER overpotential as low as 0.30 V when N-doped graphene is employed.Our findings offer novel design of heterojunctions as high performance OER catalysts.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.51802126 and 52072152)the Jiangsu University Jinshan Professor Fund and Jiangsu Specially-Appointed Professor Fund,Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials+1 种基金The authors also acknowledged the financial support by Guangdong Innovation Research Team for Higher Education(No.2017KCXTD030)High-level Talents Project of Dongguan University of Technology(No.KCYKYQD2017017).
文摘The large-scale production of ammonia mainly depends on the Haber-Bosch process,which will lead to the problems of high energy consumption and carbon dioxide emission.Electrochemical nitrogen fixation is considered to be an environmental friendly and sustainable process,but its efficiency largely depends on the activity and stability of the catalyst.Therefore,it is imperative to develop high-efficient electrocatalysts in the field of nitrogen reduction reaction(NRR).In this paper,we developed a BiVO_(4)/TiO_(2) nanotube(BiVO_(4)/TNT)heterojunction composite with rich oxygen vacancies as an electrocatalytic NRR catalyst.The heterojunction interface and oxygen vacancy of BiVO_(4)/TNT can be the active site of N2 dynamic activation and proton transition.The synergistic effect of TiO_(2) and BiVO_(4) shortens the proton transport path and reduces the over potential of chemical reaction.BiVO_(4)/TNT has high ammonia yield of 8.54µg·h^(−1)·cm^(−2) and high Faraday efficiency of 7.70%in−0.8 V vs.RHE in 0.1 M Na_(2)SO_(4) solution.
基金financially supported by the National Natural Science Foundation of China(Nos.21771182,21501177 and 21673240)the Guangdong Innovation Research Team for Higher Education(No.2017KCXTD030)+1 种基金the High-level Talents Project of Dongguan University of Technology(No.KCYKYQD2017017)the Open Project Program of the State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences(No.20200006)。
文摘Confined metal clusters as sub-nanometer reactors for electrocatalytic N_(2) reduction reaction(eNRR)have received increasing attention due to the unique metal-metal interaction and higher activity than singleatom catalysts.Herein,the inspiration of the superior capacitance and unique microenvironment with regular surface cavities of the porous boron nitride(p-BN)nanosheets,we systematically studied the catalytic activity for NRR of transition-metal single-clusters in the triplet form(V_(3),Fe_(3),Mo_(3) and W_(3))confined in the surface cavities of the p-BN sheets by spin-polarized density functional theory(DFT)calculations.After a two-step screening strategy,Mo_(3)@p-BN was found to have high catalytic activity and selectivity with a rather low limiting potential(-0.34 V)for the NRR.The anchored Mo_(3) singlecluster can be stably embedded on the surface cavities of the substrate preventing the diffusion of the active Mo atoms.More importantly,the Mo atoms in the Mo_(3) single-cluster would act as“cache”to accelerate electron transfer between active metal centers and nitrogen-containing intermediates via the intimate Mo-Mo interactions.The cooperation of Mo atoms can also provide a large number of occupied and unoccupied d orbitals to make the"donation-backdonation"mechanism more effective.This work not only provides a quite promising electrocatalyst for NRR,but also brings new insights into the rational design of triple-atom NRR catalysts.
