Interfacial engineering to alter the configuration of active sites in heterogeneous catalysts is a potential strategy for activity enhancement,but it remains unelucidated for metal-organic frameworks(MOFs).Here,we dem...Interfacial engineering to alter the configuration of active sites in heterogeneous catalysts is a potential strategy for activity enhancement,but it remains unelucidated for metal-organic frameworks(MOFs).Here,we demonstrate that the surface of two-dimensional Co-based MOF is modified by decorating Ag quantum dots(QDs)simply through in-situ reduction of Ag+ions.Toward oxygen evolution reaction(OER),it reveals that the catalysis is mediated by the reversible redox of Co sites between Co^(3+) and Co^(4+) states coupling with transfer of OHions.The decoration of Ag QDs decreases the redox potential of Co sites,and thus effectively decreases the overpotential of OER.The TOFs of Co sites are increased by 77 times to reach 5.4 s^(-1) at an overpotential of 0.35 V.We attribute the activity enhancement to the tuning of the coupling process between Co sites and OHions during the redox of Co sites by Ag QDs decoration based on Pourbaix analysis.展开更多
Hydroxyl release of red soil and latosol surfaces was quantitatively measured using a self-made constantpH automated titration instrument, to study the changes of hydroxyl release with different added seleniteamounts ...Hydroxyl release of red soil and latosol surfaces was quantitatively measured using a self-made constantpH automated titration instrument, to study the changes of hydroxyl release with different added seleniteamounts and pH levels, and to study the effects of electrolytes on hydroxyl release. Hydroxyl release increasedwith the selenite concentration, with a rapid increase at a low selenite concentration while slowing down ata high concentration. The pH where maximum of hydroxyl release appeared was not constant, shifting toa lower valus with increasing selenite concentration. Hydroxyl release decreased with increasing electrolyteconcentration, and the decrease was very rapid at a low electrolyte concentration but slow at a high electrolyteconcentration. For NaC1O4, NaC1 and Na2SO4, hydroxyl release was in the order of NaClO4 ＞ NaCl >Na2SO4, and the difference was very significant. But for NaCl, KCl and CaCl2, the order of hydroxyl releasewas NaCl ＞ KCl ＞ CaCl2, and the difference was smaller. The amount of hydroxyl release from Xuwenlatosol was greater than that from Jinxian red soil. Hydroxyl release existed in a wider range of pH withXuwen latosol than with Jinxian red soil, due to their difference in soil properties. However, both soils hadsimilar curves of hydroxyl release, indicating the common characteristics of variable charge soils.展开更多
A self-made constant pH automated titration instrument was used to study the kinetics of hydroxyl release during selenite reacting with variable charge soils. The rate of hydroxyl release was very rapid at the first s...A self-made constant pH automated titration instrument was used to study the kinetics of hydroxyl release during selenite reacting with variable charge soils. The rate of hydroxyl release was very rapid at the first several minutes, then graduallyslowed down, and at last did not change any more. The experimental data was well fitted by the Langmuir kinetic equation, and with increasing selenite concentration or decreasing solution pH, the reaction lasted longer, the maximum of hydroxyl release (xm) increased, and the binding constant (k) decreased. The time of hydroxyl release with Xuwen latosol was much longer than that with Jinxian red soil.展开更多
Highly sensitive methods are important for monitoring the concentration of metal ions in industrial wastewater.Here,we developed a new probe for the determination of metal ions by fluorescence quenching.The probe cons...Highly sensitive methods are important for monitoring the concentration of metal ions in industrial wastewater.Here,we developed a new probe for the determination of metal ions by fluorescence quenching.The probe consists of hydroxylated graphene quantum dots(H-GQDs),prepared from GQDs by electrochemical method followed by surface hydroxylation.It is a non-reactive indicator with high sensitivity and detection limits of 0.01μM for Cu2+,0.005μM for Al3+,0.04μM for Fe3+,and 0.02μM for Cr3+.In addition,the low biotoxicity and excellent solubility of H-GQDs make them promising for application in wastewater metal ion detection.展开更多
Thin calcium phosphate catings on titanium alloy substrates were prepared by Ar^+ ion beam assisted deposition(IBAD) from hydroxyl-poly-calcium sodium phosphate(HPPA) target.The coatings were analyzed by XRD,FTIR,XPS,...Thin calcium phosphate catings on titanium alloy substrates were prepared by Ar^+ ion beam assisted deposition(IBAD) from hydroxyl-poly-calcium sodium phosphate(HPPA) target.The coatings were analyzed by XRD,FTIR,XPS,These analyses revealed that the as-deposited films were amorphous or no apparent crystallinity.No distinct absorption band of the hydroxyl group was observed in FTIR spectra of the coatings but new absorption bands were presented for CO3^-2,The calcium to phosphorous ratio of these catings in different IBAD conditions varied from 0.46 to 3.36.展开更多
The solvent extraction of La 3+ from hydrochloric acid solutions was investigated using bis (2, 4, 4-trimethylpentyl) monothiophosphinic acid (Cyanex 302, HL) as an extractant. The effect of equilibrium of aqueous ac...The solvent extraction of La 3+ from hydrochloric acid solutions was investigated using bis (2, 4, 4-trimethylpentyl) monothiophosphinic acid (Cyanex 302, HL) as an extractant. The effect of equilibrium of aqueous acidity on extraction of La 3+ using Cyanex 302 in different diluents was discussed. The effects of extractant concentration and chloride ion on the extraction reaction were also studied. Stoichiometry of the extraction reactions and the nature of metal complexes formed were determined using slope analysis technique and IR measurement.展开更多
An alkaline precipitation method was introduced to produce hydrous cerium oxides.The prepared powder was characterized by Brunauer-Emmett-Teller（BET） nitrogen adsorption-desorption,X-ray diffraction（XRD）,Fourier t...An alkaline precipitation method was introduced to produce hydrous cerium oxides.The prepared powder was characterized by Brunauer-Emmett-Teller（BET） nitrogen adsorption-desorption,X-ray diffraction（XRD）,Fourier transform infrared（FTIR） spectrometry,and thermal gravimetry（TG） approaches.The adsorbent has a chemical formula of CeO2·nH2O（n 2） and a cubic fluorite-type structure after high temperature treatment.Adsorption capacity of different temperature treated hydrous cerium oxides does not directly correlate with BET specific surface area.Phosphate adsorption isotherms follow the Langmuir equation below the treatment temperature of 800°C.Phosphate adsorption causes no change on the structure of a hydrous cerium oxides,and no signs of CePO4 precipitates are found.The ion-exchanging structure of hydrous cerium oxide plays a fundamental role in phosphate adsorption.The structure is highly temperature resistant and forms adsorption sites which adsorb both water and some anions.Complete loss of adsorption ability cannot be achieved unless the treatment temperature is higher than 1200°C.Mechanism study shows that the adsorption of phosphates is mainly an anion-exchange process.展开更多
Dependence of yields of OH (hydroxyl) radicals on the mass and specific energy of heavy ions and elapsed time after irradiation was investigated,to understand chemical reactions of aqueous solutions.The yields of irra...Dependence of yields of OH (hydroxyl) radicals on the mass and specific energy of heavy ions and elapsed time after irradiation was investigated,to understand chemical reactions of aqueous solutions.The yields of irradiation products of phenol,super-linearly increased with the incident energy of He,C,and Ne ions ranging from 2 to 18 MeV/u.The yields of the OH radicals were estimated by analyzing the yields of the irradiation products of phenol. The yields of the OH radicals increased with the specific energy for each ion,but decreased both with the mass of each ion at the same specific energy and elapsed time after irradiation.展开更多
The photodegradation of bisphenol A （BPA） in aqueous solution containing metal ions and ascorbic acid （AsA） was investigated. After strong irradiation, the aqueous solution containing AsA and Cu^2＋ could produce ...The photodegradation of bisphenol A （BPA） in aqueous solution containing metal ions and ascorbic acid （AsA） was investigated. After strong irradiation, the aqueous solution containing AsA and Cu^2＋ could produce hydroxyl radicals that induced the photodegradation of BPA. The photodegradation efficiency of BPA in the solution containing 70 μmol·L^1 Cu^2＋ and 15 mg·L^1 AsA reached 59% at pH 6.0 after 4 hours irradiation with high pressure mercury lamp. The photodegradation efficiency of BPA reached 10% after 4 hours irradiation with daylight lamp in the presence of 70 μmol·L^1 Cu^2＋ and 15 mg·L^1 ascorbic acid. BPA was not degraded in the aqueous solution only containing AsA or Cu^2＋. The BPA photodegradation in aqueous solution containing AsA and Fe^3＋ was weaker than in aqueous solution that containing AsA and Cu^2＋ at the same concentration. This work showed a new route of the BPA photodegradation in aqueous environment.展开更多
基于密度泛函理论,采用Materials Studio 7.0软件进行了锡石{100}、{110}、{101}解理面的电子结构及表面能的第一性原理计算,并以此为基础进一步研究了氢氧根离子在锡石{100}表面上吸附的羟基化影响。计算结果表明:与{101}面相比,{100}...基于密度泛函理论,采用Materials Studio 7.0软件进行了锡石{100}、{110}、{101}解理面的电子结构及表面能的第一性原理计算,并以此为基础进一步研究了氢氧根离子在锡石{100}表面上吸附的羟基化影响。计算结果表明:与{101}面相比,{100}面和{110}面具有更低的表面能,是锡石最常见的解理面;氢氧根离子主要通过带负电的氧原子与表面上五配位的锡原子发生键合形成吸附,这种具有悬挂键的锡原子是锡石表面的活性位点。理论模拟计算能为新型锡石捕收剂的开发提供指导。展开更多
基金gratefully acknowledge the financial support from the National Natural Science Foundation of China(51802265,22002119)the Fundamental Research Funds for the Central Universities of China+2 种基金the Initiative Postdocs Supporting Program(BX20190281)the General Program,Science and Technology Program of Taicang,China(TC2020JC01)the National Natural Science Foundation of Jiangsu,China(BK20200261)。
文摘Interfacial engineering to alter the configuration of active sites in heterogeneous catalysts is a potential strategy for activity enhancement,but it remains unelucidated for metal-organic frameworks(MOFs).Here,we demonstrate that the surface of two-dimensional Co-based MOF is modified by decorating Ag quantum dots(QDs)simply through in-situ reduction of Ag+ions.Toward oxygen evolution reaction(OER),it reveals that the catalysis is mediated by the reversible redox of Co sites between Co^(3+) and Co^(4+) states coupling with transfer of OHions.The decoration of Ag QDs decreases the redox potential of Co sites,and thus effectively decreases the overpotential of OER.The TOFs of Co sites are increased by 77 times to reach 5.4 s^(-1) at an overpotential of 0.35 V.We attribute the activity enhancement to the tuning of the coupling process between Co sites and OHions during the redox of Co sites by Ag QDs decoration based on Pourbaix analysis.
基金Project supported by the National Natural Science Foundation of China(Nos.49971046 and 49831005).
文摘Hydroxyl release of red soil and latosol surfaces was quantitatively measured using a self-made constantpH automated titration instrument, to study the changes of hydroxyl release with different added seleniteamounts and pH levels, and to study the effects of electrolytes on hydroxyl release. Hydroxyl release increasedwith the selenite concentration, with a rapid increase at a low selenite concentration while slowing down ata high concentration. The pH where maximum of hydroxyl release appeared was not constant, shifting toa lower valus with increasing selenite concentration. Hydroxyl release decreased with increasing electrolyteconcentration, and the decrease was very rapid at a low electrolyte concentration but slow at a high electrolyteconcentration. For NaC1O4, NaC1 and Na2SO4, hydroxyl release was in the order of NaClO4 ＞ NaCl >Na2SO4, and the difference was very significant. But for NaCl, KCl and CaCl2, the order of hydroxyl releasewas NaCl ＞ KCl ＞ CaCl2, and the difference was smaller. The amount of hydroxyl release from Xuwenlatosol was greater than that from Jinxian red soil. Hydroxyl release existed in a wider range of pH withXuwen latosol than with Jinxian red soil, due to their difference in soil properties. However, both soils hadsimilar curves of hydroxyl release, indicating the common characteristics of variable charge soils.
基金Project supported by the National Natural Science Foundation of China (Nos. 49971046 and 49831005).
文摘A self-made constant pH automated titration instrument was used to study the kinetics of hydroxyl release during selenite reacting with variable charge soils. The rate of hydroxyl release was very rapid at the first several minutes, then graduallyslowed down, and at last did not change any more. The experimental data was well fitted by the Langmuir kinetic equation, and with increasing selenite concentration or decreasing solution pH, the reaction lasted longer, the maximum of hydroxyl release (xm) increased, and the binding constant (k) decreased. The time of hydroxyl release with Xuwen latosol was much longer than that with Jinxian red soil.
基金financially supported by the National Natural Science Foundation of China (No. 21674011)Beijing Municipal Natural Science Foundation (No. 2172040)
文摘Highly sensitive methods are important for monitoring the concentration of metal ions in industrial wastewater.Here,we developed a new probe for the determination of metal ions by fluorescence quenching.The probe consists of hydroxylated graphene quantum dots(H-GQDs),prepared from GQDs by electrochemical method followed by surface hydroxylation.It is a non-reactive indicator with high sensitivity and detection limits of 0.01μM for Cu2+,0.005μM for Al3+,0.04μM for Fe3+,and 0.02μM for Cr3+.In addition,the low biotoxicity and excellent solubility of H-GQDs make them promising for application in wastewater metal ion detection.
基金Contract grant sponsor:Key Laboratory of Radiation Physics and Technology of Education Ministry (No.2000-03)
文摘Thin calcium phosphate catings on titanium alloy substrates were prepared by Ar^+ ion beam assisted deposition(IBAD) from hydroxyl-poly-calcium sodium phosphate(HPPA) target.The coatings were analyzed by XRD,FTIR,XPS,These analyses revealed that the as-deposited films were amorphous or no apparent crystallinity.No distinct absorption band of the hydroxyl group was observed in FTIR spectra of the coatings but new absorption bands were presented for CO3^-2,The calcium to phosphorous ratio of these catings in different IBAD conditions varied from 0.46 to 3.36.
文摘The solvent extraction of La 3+ from hydrochloric acid solutions was investigated using bis (2, 4, 4-trimethylpentyl) monothiophosphinic acid (Cyanex 302, HL) as an extractant. The effect of equilibrium of aqueous acidity on extraction of La 3+ using Cyanex 302 in different diluents was discussed. The effects of extractant concentration and chloride ion on the extraction reaction were also studied. Stoichiometry of the extraction reactions and the nature of metal complexes formed were determined using slope analysis technique and IR measurement.
基金support from the National Natural Science Foundation of China (No.20876157)
文摘An alkaline precipitation method was introduced to produce hydrous cerium oxides.The prepared powder was characterized by Brunauer-Emmett-Teller（BET） nitrogen adsorption-desorption,X-ray diffraction（XRD）,Fourier transform infrared（FTIR） spectrometry,and thermal gravimetry（TG） approaches.The adsorbent has a chemical formula of CeO2·nH2O（n 2） and a cubic fluorite-type structure after high temperature treatment.Adsorption capacity of different temperature treated hydrous cerium oxides does not directly correlate with BET specific surface area.Phosphate adsorption isotherms follow the Langmuir equation below the treatment temperature of 800°C.Phosphate adsorption causes no change on the structure of a hydrous cerium oxides,and no signs of CePO4 precipitates are found.The ion-exchanging structure of hydrous cerium oxide plays a fundamental role in phosphate adsorption.The structure is highly temperature resistant and forms adsorption sites which adsorb both water and some anions.Complete loss of adsorption ability cannot be achieved unless the treatment temperature is higher than 1200°C.Mechanism study shows that the adsorption of phosphates is mainly an anion-exchange process.
文摘Dependence of yields of OH (hydroxyl) radicals on the mass and specific energy of heavy ions and elapsed time after irradiation was investigated,to understand chemical reactions of aqueous solutions.The yields of irradiation products of phenol,super-linearly increased with the incident energy of He,C,and Ne ions ranging from 2 to 18 MeV/u.The yields of the OH radicals were estimated by analyzing the yields of the irradiation products of phenol. The yields of the OH radicals increased with the specific energy for each ion,but decreased both with the mass of each ion at the same specific energy and elapsed time after irradiation.
基金Supported by the National Natural Science Foundation of China (20177017, 20477031)
文摘The photodegradation of bisphenol A （BPA） in aqueous solution containing metal ions and ascorbic acid （AsA） was investigated. After strong irradiation, the aqueous solution containing AsA and Cu^2＋ could produce hydroxyl radicals that induced the photodegradation of BPA. The photodegradation efficiency of BPA in the solution containing 70 μmol·L^1 Cu^2＋ and 15 mg·L^1 AsA reached 59% at pH 6.0 after 4 hours irradiation with high pressure mercury lamp. The photodegradation efficiency of BPA reached 10% after 4 hours irradiation with daylight lamp in the presence of 70 μmol·L^1 Cu^2＋ and 15 mg·L^1 ascorbic acid. BPA was not degraded in the aqueous solution only containing AsA or Cu^2＋. The BPA photodegradation in aqueous solution containing AsA and Fe^3＋ was weaker than in aqueous solution that containing AsA and Cu^2＋ at the same concentration. This work showed a new route of the BPA photodegradation in aqueous environment.
文摘基于密度泛函理论,采用Materials Studio 7.0软件进行了锡石{100}、{110}、{101}解理面的电子结构及表面能的第一性原理计算,并以此为基础进一步研究了氢氧根离子在锡石{100}表面上吸附的羟基化影响。计算结果表明:与{101}面相比,{100}面和{110}面具有更低的表面能,是锡石最常见的解理面;氢氧根离子主要通过带负电的氧原子与表面上五配位的锡原子发生键合形成吸附,这种具有悬挂键的锡原子是锡石表面的活性位点。理论模拟计算能为新型锡石捕收剂的开发提供指导。
