The adsorption of NO on alumina supported Pd catalysts and the effect of adding Li 2O on NO adsorption have been investigated by using TPD MS method. Experimental results certify the existence of three types of surfac...The adsorption of NO on alumina supported Pd catalysts and the effect of adding Li 2O on NO adsorption have been investigated by using TPD MS method. Experimental results certify the existence of three types of surface species. The adsorptive dissociation of NO gives a relatively inactive intermediate N 2O. Its desorption amount is larger on Al 2O 3 and Pd/Al 2O 3 Li 2O than that on Pd/Al 2O 3. The adsorption intensity of N 2O is the strongest on Pd/Al 2O 3 Li 2O. The experiments of competitive adsorption of O 2 and NO reveal that the presence of O 2 has two effects: (1) the O atom sticks to the Pd site on the surface and inhibits the adsorption of NO, as well as the decomposition of NO; (2) O 2 can react with NO to form nitrite or nitrate species which can adsorb strongly on the surface. The relative efficiency of the two effects differs with temperature, and this can be applied to explain some phenomena in the adsorption of NO, and the selective catalytic reduction of NO as well.展开更多
CaC12 can be sprayed onto sinter surface, which can improve the low temperature reduction degradation index （RDI＋3.15） of sinter. This has been recognized; however, there are various opinions on the inhibition mech...CaC12 can be sprayed onto sinter surface, which can improve the low temperature reduction degradation index （RDI＋3.15） of sinter. This has been recognized; however, there are various opinions on the inhibition mechanism of it. At the same time, the corrosion of C1 element on equipment is very serious. First-principle calculations based on density functional theory were performed to investigate the binding mechanisms of calcium species on a a-Fe2 03 （0 0 1） surface. This is crucial in demonstrating the role of the CaC12 on improving the low temperature reduction degrada tion index. It has been determined that C1 could greatly increase the adsorption of the vacuum layer for the Ca/Fe2 03 system and the relaxation produced by adsorption made bond length decrease, bond energies increase and structure compact. Those are the main reasons that inhibiting the reduction disintegration of sinter.展开更多
Carbon nitride has been extensively used as a visible-light photocatalyst,but it has the disadvantages of a low specific surface area,rapid electron-hole recombination,and relatively low light absorbance.In this study...Carbon nitride has been extensively used as a visible-light photocatalyst,but it has the disadvantages of a low specific surface area,rapid electron-hole recombination,and relatively low light absorbance.In this study,single-atom Ag was successfully anchored on ultrathin carbon nitride(UTCN)via thermal polymerization,the catalyst obtained is called AgUTCN.The Ag hardly changed the carbon nitride's layered and porous physical structure.AgUTCN exhibited efficient visible-light photocatalytic performances in the degradation of various recalcitrant pollutants,eliminations of 85% were achieved by visible-light irradiation for 1hr.Doping with Ag improved the photocatalytic performance of UTCN by narrowing the forbidden band gap from 2.49 to 2.36 e V and suppressing electron-hole pair recombination.In addition,Ag doping facilitated O_(2) adsorption on UTCN by decreasing the adsorption energy from -0.2 to -2.22 e V and favored the formation of O_(2)^(·-).Electron spin resonance and radical-quenching experiments showed that O_(2)^(·-)was the major reactive species in the degradation of Acetaminophen(paracetamol,APAP).展开更多
This work reports on applying iron oxide coated sand (IOCS) media in an experimental permeable reactive barrier to remove uranium (U) species from uranium containing water. A field study was conducted at the legacy Gu...This work reports on applying iron oxide coated sand (IOCS) media in an experimental permeable reactive barrier to remove uranium (U) species from uranium containing water. A field study was conducted at the legacy Gunnar uranium mine & mill site that was abandoned in the 1960s with limited to no decommissioning. The flooded Gunnar mine pit presently contains about 3.2 million m<sup>3</sup> of water contaminated by dissolved U (1.2 mg/L), Ra-226 (0.4 Bq/L), and minor concentrations of other contaminants (As, Se, etc.). The water is seeping over the pit rim into Lake Athabasca, posing potential environmental and health concerns. IOCS media can be used to immobilize uranium species through an adsorption process. Herein, the preparation of hydrous ferric oxide sorbents and their supported forms onto silica sands is described. Fourier transform infrared spectroscopy (FTIR) and powder X-ray diffraction (pXRD) were used for structural characterization. The adsorption properties of the IOCS sorbent media were modeled by the Langmuir adsorption isotherm, where a maximum uranium uptake capacity was estimated. Bench-scale adsorption kinetic experiments were also performed before moving to a field trial. Based on these lab results and input on field-scale parameters, a pilot permeable reactive barrier was fabricated and a field test conducted near the Gunnar pit in June 2019. This pilot test provided technical data and information needed for designing a full-scale permeable barrier that employs the IOCS media. This approach can be applied for in-situ water treatment at Gunnar and other legacy uranium sites.展开更多
Since the application in fuel cell,the electrochemical adsorption of hydroxyl has received considerable attention in recent years.While most research mainly focus on the room temperature,in this paper,the electrochemi...Since the application in fuel cell,the electrochemical adsorption of hydroxyl has received considerable attention in recent years.While most research mainly focus on the room temperature,in this paper,the electrochemical adsorption of hydroxyl in alkaline solution at high temperature was investigated.An unusual oxidation peak was observed at-0.27 V,suggesting new behavior of hydroxyl adsorption occurred.As is known two kinds of cation hydrated clusters exist in alkaline solution,(H_(2)O)_(x-1)M^(+)-H_(2)O-O_(ad)H and(H_(2)O)_xM^(+)-O_(ad)H.For K^(+)and Cs^(+),the cluster shows unstable structure due to the weak interaction between hydrated cation and OH^(-)especially at high temperature.However,For Li^(+),Na^(+)the cluster structure would be stable,as the interaction force between the hydrated cation and OH^(-)is so strong.It was revealed that the unusual oxidation peak has some relationship with the(H_(2)O)_(x-1)M^(+)-H_(2)O-O_(ad)H cluster(K^(+)and Cs^(+))absorbed at Pt electrode surface.When the temperature was raised,(H_(2)O)_(x-1)M^(+)-H_(2)O-and-O_(ad)H was disconnected,then the O_(ad)H absorbed at Pt surface got oxidated.Based on the SEM observation,it was showed the unusual electrochemical oxidation reaction would generate platinum oxides,blocking the reactive sites at Pt electrode surface,thus reducing the electrochemical reactivity of Pt electrode.Accordingly,parameters of alkaline concentration and temperature were systematically studied,it was found that increase temperature or alkaline concentration was in favor of the unusual oxidation reaction.This study provides more understanding of hydroxyl adsorption behavior at Pt electrode surface for the high temperature water solution environment.展开更多
本文以实验结果为基础,根据 ALE GaAs 生长过程中的自限特性和 Langmiur 单层吸附模型,计算了在 TMGa 暴露周期各化学物种的气相分压和表面复盖度随温度、TMGa 注入量和反应系统压力的变化关系。讨论了生长参数的改变对生长速率和 C 掺...本文以实验结果为基础,根据 ALE GaAs 生长过程中的自限特性和 Langmiur 单层吸附模型,计算了在 TMGa 暴露周期各化学物种的气相分压和表面复盖度随温度、TMGa 注入量和反应系统压力的变化关系。讨论了生长参数的改变对生长速率和 C 掺杂的影响。计算结果表明,温度对各物种在 GaAs 表面复盖度的影响十分显著,随着温度的上升,主要含 Ga 吸附物从(CH_3)_2Ca,CH_3Ga 转变为 GaH 和 Ga 原子。另外,在 GaAs 表面含 C 物种的复盖度随温度和反应系统压力的降低及TMGa 注入压力的上升而增加。ALE GaAs 生长较合适的反应温度和系统压力分别为700～800K 和几十～几百个托。展开更多
文摘The adsorption of NO on alumina supported Pd catalysts and the effect of adding Li 2O on NO adsorption have been investigated by using TPD MS method. Experimental results certify the existence of three types of surface species. The adsorptive dissociation of NO gives a relatively inactive intermediate N 2O. Its desorption amount is larger on Al 2O 3 and Pd/Al 2O 3 Li 2O than that on Pd/Al 2O 3. The adsorption intensity of N 2O is the strongest on Pd/Al 2O 3 Li 2O. The experiments of competitive adsorption of O 2 and NO reveal that the presence of O 2 has two effects: (1) the O atom sticks to the Pd site on the surface and inhibits the adsorption of NO, as well as the decomposition of NO; (2) O 2 can react with NO to form nitrite or nitrate species which can adsorb strongly on the surface. The relative efficiency of the two effects differs with temperature, and this can be applied to explain some phenomena in the adsorption of NO, and the selective catalytic reduction of NO as well.
基金Item Sponsored by National Natural Science Foundation of China(51174074)Open Fund Project of National Key Laboratory in University of Science and Technology Beijing of China(KF13-02)
文摘CaC12 can be sprayed onto sinter surface, which can improve the low temperature reduction degradation index （RDI＋3.15） of sinter. This has been recognized; however, there are various opinions on the inhibition mechanism of it. At the same time, the corrosion of C1 element on equipment is very serious. First-principle calculations based on density functional theory were performed to investigate the binding mechanisms of calcium species on a a-Fe2 03 （0 0 1） surface. This is crucial in demonstrating the role of the CaC12 on improving the low temperature reduction degrada tion index. It has been determined that C1 could greatly increase the adsorption of the vacuum layer for the Ca/Fe2 03 system and the relaxation produced by adsorption made bond length decrease, bond energies increase and structure compact. Those are the main reasons that inhibiting the reduction disintegration of sinter.
基金supported by the Shenzhen Science,Technology and Innovation Commission(No.JCYJ20200109142829123)the National Natural Science Foundation of China(No.52022049)。
文摘Carbon nitride has been extensively used as a visible-light photocatalyst,but it has the disadvantages of a low specific surface area,rapid electron-hole recombination,and relatively low light absorbance.In this study,single-atom Ag was successfully anchored on ultrathin carbon nitride(UTCN)via thermal polymerization,the catalyst obtained is called AgUTCN.The Ag hardly changed the carbon nitride's layered and porous physical structure.AgUTCN exhibited efficient visible-light photocatalytic performances in the degradation of various recalcitrant pollutants,eliminations of 85% were achieved by visible-light irradiation for 1hr.Doping with Ag improved the photocatalytic performance of UTCN by narrowing the forbidden band gap from 2.49 to 2.36 e V and suppressing electron-hole pair recombination.In addition,Ag doping facilitated O_(2) adsorption on UTCN by decreasing the adsorption energy from -0.2 to -2.22 e V and favored the formation of O_(2)^(·-).Electron spin resonance and radical-quenching experiments showed that O_(2)^(·-)was the major reactive species in the degradation of Acetaminophen(paracetamol,APAP).
文摘This work reports on applying iron oxide coated sand (IOCS) media in an experimental permeable reactive barrier to remove uranium (U) species from uranium containing water. A field study was conducted at the legacy Gunnar uranium mine & mill site that was abandoned in the 1960s with limited to no decommissioning. The flooded Gunnar mine pit presently contains about 3.2 million m<sup>3</sup> of water contaminated by dissolved U (1.2 mg/L), Ra-226 (0.4 Bq/L), and minor concentrations of other contaminants (As, Se, etc.). The water is seeping over the pit rim into Lake Athabasca, posing potential environmental and health concerns. IOCS media can be used to immobilize uranium species through an adsorption process. Herein, the preparation of hydrous ferric oxide sorbents and their supported forms onto silica sands is described. Fourier transform infrared spectroscopy (FTIR) and powder X-ray diffraction (pXRD) were used for structural characterization. The adsorption properties of the IOCS sorbent media were modeled by the Langmuir adsorption isotherm, where a maximum uranium uptake capacity was estimated. Bench-scale adsorption kinetic experiments were also performed before moving to a field trial. Based on these lab results and input on field-scale parameters, a pilot permeable reactive barrier was fabricated and a field test conducted near the Gunnar pit in June 2019. This pilot test provided technical data and information needed for designing a full-scale permeable barrier that employs the IOCS media. This approach can be applied for in-situ water treatment at Gunnar and other legacy uranium sites.
基金the National Key Research and Development Program of China(2020YFC1909703)S&T Program of Hebei Province(21284402Z)+1 种基金Fangchenggang Key Research and Development(AB20014008)Lvliang Key Research and Development Program(2020GXZDYF7)。
文摘Since the application in fuel cell,the electrochemical adsorption of hydroxyl has received considerable attention in recent years.While most research mainly focus on the room temperature,in this paper,the electrochemical adsorption of hydroxyl in alkaline solution at high temperature was investigated.An unusual oxidation peak was observed at-0.27 V,suggesting new behavior of hydroxyl adsorption occurred.As is known two kinds of cation hydrated clusters exist in alkaline solution,(H_(2)O)_(x-1)M^(+)-H_(2)O-O_(ad)H and(H_(2)O)_xM^(+)-O_(ad)H.For K^(+)and Cs^(+),the cluster shows unstable structure due to the weak interaction between hydrated cation and OH^(-)especially at high temperature.However,For Li^(+),Na^(+)the cluster structure would be stable,as the interaction force between the hydrated cation and OH^(-)is so strong.It was revealed that the unusual oxidation peak has some relationship with the(H_(2)O)_(x-1)M^(+)-H_(2)O-O_(ad)H cluster(K^(+)and Cs^(+))absorbed at Pt electrode surface.When the temperature was raised,(H_(2)O)_(x-1)M^(+)-H_(2)O-and-O_(ad)H was disconnected,then the O_(ad)H absorbed at Pt surface got oxidated.Based on the SEM observation,it was showed the unusual electrochemical oxidation reaction would generate platinum oxides,blocking the reactive sites at Pt electrode surface,thus reducing the electrochemical reactivity of Pt electrode.Accordingly,parameters of alkaline concentration and temperature were systematically studied,it was found that increase temperature or alkaline concentration was in favor of the unusual oxidation reaction.This study provides more understanding of hydroxyl adsorption behavior at Pt electrode surface for the high temperature water solution environment.
文摘本文以实验结果为基础,根据 ALE GaAs 生长过程中的自限特性和 Langmiur 单层吸附模型,计算了在 TMGa 暴露周期各化学物种的气相分压和表面复盖度随温度、TMGa 注入量和反应系统压力的变化关系。讨论了生长参数的改变对生长速率和 C 掺杂的影响。计算结果表明,温度对各物种在 GaAs 表面复盖度的影响十分显著,随着温度的上升,主要含 Ga 吸附物从(CH_3)_2Ca,CH_3Ga 转变为 GaH 和 Ga 原子。另外,在 GaAs 表面含 C 物种的复盖度随温度和反应系统压力的降低及TMGa 注入压力的上升而增加。ALE GaAs 生长较合适的反应温度和系统压力分别为700～800K 和几十～几百个托。
