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In situ regulating intimately connected heterostructure by decomposition of solid solution oxides toward high-efficient water oxidation
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作者 Shao-Fei Zhang Xiao-Lu Yin +7 位作者 Jin Wang Jian-Li Kang Tian-Tian Li Jin-Feng Sun Yong-Qiang Meng Jian-Jiang Wang Dian-Long Wang Kai-Qiang Qin 《Rare Metals》 SCIE EI CAS CSCD 2024年第4期1557-1569,共13页
Heterogeneous interfaces produced by interdomain interactions on a nanoscale performs a crucial role in boosting the properties of an electrocatalyst toward oxygen evolution reaction(OER)process.Herein,a series of dua... Heterogeneous interfaces produced by interdomain interactions on a nanoscale performs a crucial role in boosting the properties of an electrocatalyst toward oxygen evolution reaction(OER)process.Herein,a series of dual-phase electrodes with intimately connected heterointerfaces are prepared by in situ decomposing solid solution oxide of Ni_(x)Co_(y)Fe_(100-x-y)O,which grew on Ni foam massively via an ultrafast combustion approach.Particularly,with high-reaction kinetics caused by the reduction treatment at 450℃,the less electronegative Fe and Co are more oxyphilic than Ni,which facilitated their co-exsolution and formation of CoFe_2O_4/NiO oxide with enriched oxygen vacancies.Benefiting from the nanoporous framework,heterojunction structure,and oxygen defects,the self-supporting electrodes present rapid charge/mass transmission and provide abundant active sites for OER.The optimized sample(R-SNCF4.5)shows low overpotentials of 226 and 324 mV at 10 and100 mA·cm^(-2),a small Tafel slope(46.7 mV·dec^(-1)),and excellent stability.The assembled R-SNCF4.5//Pt/C/NF electrolyzer demonstrates continuous electrolysis over 50 h at a current density of 10 mA·cm^(-2),under 1.51 V.Density functional theory(DFT)calculations verify that the strong electronic modulation plays a critical part in the CoFe_2O_4/NiO hybrid by lowering the energy barriers for the ratedetermining steps,and Fe sites are the most active OER sites. 展开更多
关键词 Rapid combustion Decomposition of solid solution oxide Dual-phase heterostructure Oxygen evolution reaction Theoretical calculation
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INVESTIGATION OF SURFACE MORPHOLOGY, STRUCTURE AND ELECTROCATALYTIC PROPERTIES FOR O_2 EVOLUTION OF TITANIUM BASED IrO_2+Ta_2O_5 COATINGS 被引量:3
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作者 J.M Hu J.X. Wu +2 位作者 H.M Meng YR. Zhu D.B. Sun and D.J. Yang(Beijing Corrosion and Protection Center, Open Laboratory of Corrosion, Erosion and Surface Technology,University of Science and Technology Beijing, Beijing 100083, China) 《Acta Metallurgica Sinica(English Letters)》 SCIE EI CAS CSCD 2000年第3期849-856,共8页
Titanium based IrO2 +Ta2O5 oxide anodes with different compositions and pyrolysis temperatures were prepared by termodecompoisition method. By using X-ray diffraction (XRD), the structure and texture coefficient of th... Titanium based IrO2 +Ta2O5 oxide anodes with different compositions and pyrolysis temperatures were prepared by termodecompoisition method. By using X-ray diffraction (XRD), the structure and texture coefficient of the coatings, TC(hkl), of IrO2 rutile crystal have been tested. It showed that, the crystallization processes of IrO2 and Ta2O5 in xIrO2 +(100-x) Ta2 O5 (x is in mol%) films affected and confined each other.In the mixed system, IrO2 rutile phase existed as a solid solution with Ta, and attained the maximum solubility when x=70mol%, i.e. for the coating of 70% IrO2 +Ta2O5.For the coatings of low iridium content or at low preparing tem pemture, (110) and (101) pwtered orientations were dominant. However, preferred growth of IrO2 weakened with increasing either iridium content or temperature. Three typical surface morphologies were observed by using scanning electron tnicroscopy(SEM). The crystallite size of the mixed oxide coatings were finest for the the film of 70%IrO2 +30%Ta2O5,and decreased with the pyrolysis tempemture. As the results of the finest crystallite segregating on sudece and the maxitnum solid solubility of Ir and Ta component in deposits, the coatings with the composition of 70%IrO2 +Ta2O5 prepared at 450℃ presented the mdrimutn electrocatalgtic activitg for O2 evolution in 0. 5M H2SO4 solution.UP to 550℃, Ti base suffered to oxidation resulting in decreasing anode conductivity,therefore, coatings performed a low activity. 展开更多
关键词 titanium based coating anode iridium oxide tantalum oxide solid solution crystallite orientation electrocatalytic activity
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Enhancement of Fenton oxidation for removing organic matter from hypersaline solution by accelerating ferric system with hydroxylamine hydrochloride and benzoquinone 被引量:11
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作者 Siwei Peng Weijun Zhang +3 位作者 Jie He Xiaofang Yang Dongsheng Wang Guisheng Zeng 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2016年第3期16-23,共8页
Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone(BQ) and hydroxylamine hydrochloride(HA) as Fenton enha... Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone(BQ) and hydroxylamine hydrochloride(HA) as Fenton enhancers for the removal of glycerin from saline water under ambient temperature by accelerating the ferric system.It was found that organics removal was not obviously affected by chloride ions of low concentration(less than 0.1 mol/L),while the mineralization rate was strongly inhibited in the presence of a large amount of chloride ions.In addition,ferric hydrolysis-precipitation was significantly alleviated in the presence of HA and BQ,and HA was more effective in reducing ferric ions into ferrous ions than HA,while the H_2O_2 decomposition rate was higher in the BQ-Fenton system.Electron spin resonance analysis revealed that OH production was reduced in high salinity conditions,while it was enhanced after the addition of HA and BQ(especially HA).This study provided a possible solution to control and alleviate the inhibitory effect of chloride ions on the Fenton process for organics removal. 展开更多
关键词 Saline solution Fenton oxidation Hydroxyl radicals Benzoquinone Hydroxylamine hydrochloride
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Activity Calculation by Application of Sub-Regular Solution Model in Binary Oxide Systems 被引量:1
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作者 HOU Yan-qing XIE Gang +2 位作者 TAO Dong-ping LI Rong-xing YU Xiao-hua 《Journal of Iron and Steel Research International》 SCIE CAS CSCD 2012年第7期33-38,共6页
To confirm sub-regular solution model valid for predicting the activity of component in binary oxide systems, seven systems in the whole concentration and twelve systems presenting saturation concentration have been s... To confirm sub-regular solution model valid for predicting the activity of component in binary oxide systems, seven systems in the whole concentration and twelve systems presenting saturation concentration have been studied. The total average relative errors of component 1 and 2 are 3.2 % and 4.1% respectively by application of the sub-regular solution model into the systems within the whole concentration. However, the total average relative errors are 16 % and 1088 % in the systems presenting saturation concentration. The results show that sub-regular solu- tion model is not good for predicting the systems presenting saturation concentration, especially for the systems con- taining acidic or neutral oxide. The reason may be that the influence of the two types of oxide on the configuration is greater in binary oxide systems. These oxides can be present in the form of complex anion partly, Si-O, Al-O, Ti-O and so on, for example (SiO4)4-. That is contrary to sub-regular solution model which is supposed that the oxide systems consist of cation and O2-. But compared with regular solution model and quasi-regular solution model, sub- regular solution model is closer to the characteristics of actual solution and the calculated results are superior. 展开更多
关键词 sub-regular solution models binary oxide system activity
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Electrochemical quartz crystal microbalance study on Au-supported Pt adlayers for electrocatalytic oxidation of methanol in alkaline solution
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作者 HUANG Zhao JIA Xue’En +5 位作者 XIE QingJi TAN YueMing HUANG SuQing HUANG JinHua MENG Yue YAO ShouZhuo 《Science China Chemistry》 SCIE EI CAS 2010年第11期2349-2356,共8页
Underpotential deposition(UPD) of Cu on an Au electrode followed by redox replacement reaction(RRR) of CuUPD with a Pt source(H2PtCl6 or K2PtCl4) yielded Au-supported Pt adlayers(for short,Pt(CuUPD-Pt4+)n/Au for H2PtC... Underpotential deposition(UPD) of Cu on an Au electrode followed by redox replacement reaction(RRR) of CuUPD with a Pt source(H2PtCl6 or K2PtCl4) yielded Au-supported Pt adlayers(for short,Pt(CuUPD-Pt4+)n/Au for H2PtCl6,or Pt(CuUPD-Pt2+)n/Au for K2PtCl4,where n denotes the number of UPD-redox replacement cycles).The electrochemical quartz crystal microbalance(EQCM) technique was used for the first time to quantitatively study the fabricated electrodes and estimate their mass-normalized specific electrocatalytic activity(SECA) for methanol oxidation in alkaline solution.In comparison with Pt(CuUPD-Pt2+)n/Au,Pt(CuUPD-Pt4+)n/Au exhibited a higher electrocatalytic activity,and the maximum SECA was obtained to be as high as 35.7 mA ?g?1 at Pt(CuUPD-Pt4+)3/Au.The layer-by-layer architecture of Pt atoms on Au is briefly discussed based on the EQCM-revealed redox replacement efficiency,and the calculated distribution percentages of bare Au sites agree with the experimental results deduced from the charge under the AuOx-reduction peaks.The EQCM is highly recommended as an efficient technique to quantitatively examine various electrode-supported catalyst adlayers,and the highly efficient catalyst adlayers of noble metals are promising in electrocatalysis relevant to biological,energy and environmental sciences and technologies. 展开更多
关键词 underpotential deposition of Cu redox replacement using H2PtCl6 or K2PtCl4 Au-supported Pt adlayers EQCM electrocatalyzed oxidation of methanol in alkaline solution
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Rare earth metal doped CeO_2-based catalytic materials for diesel soot oxidation at lower temperatures 被引量:24
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作者 A.Rangaswamy Putla Sudarsanam Benjaram M.Reddy 《Journal of Rare Earths》 SCIE EI CAS CSCD 2015年第11期1162-1169,共8页
In this work, the influence of trivalent rare-earth dopants(Sm and La) on the structure-activity properties of CeO2 was thoroughly studied for diesel soot oxidation. For this, an optimized 40% of Sm and La was incor... In this work, the influence of trivalent rare-earth dopants(Sm and La) on the structure-activity properties of CeO2 was thoroughly studied for diesel soot oxidation. For this, an optimized 40% of Sm and La was incorporated into the CeO2 using a facile coprecipitation method from ultra-high dilute aqueous solutions. A systematic physicochemical characterization was carried out using X-ray diffraction(XRD), transmission electron microscopy(TEM), Brumauer-Emmett-teller method(BET) surface area, X-ray photoelectron spectroscopy(XPS), Raman, and H2-temperature programmed reduction(TPR) techniques. The soot oxidation efficiency of the catalysts was investigated using a thermogravimetric method. The XRD results suggested the formation of nanocrystalline single phase CeO2-Sm2O3 and CeO2-La2O3 solid solutions. The Sm- and La-doped CeO2 materials exhibited smaller crystallite size and higher BET surface area compared with the pure CeO2. Owing to the difference in the oxidation states of the dopants(Sm3+ and La3+) and the Ce4+, a number of oxygen vacancies were generated in CeO2-Sm2O3 and CeO2-La2O3 samples. The H2-TPR studies evidenced the improved reducible nature of the CeO2-Sm2O3 and CeO2-La2O3 samples compared with the CeO2. It was found that the addition of Sm and La to the CeO2 outstandingly enhanced its catalytic efficiency for the oxidation of diesel soot. The observed 50% soot conversion temperatures for the CeO2-Sm2O3, CeO2-La2O3 and CeO2 were ~790, 843 and 864 K(loose contact), respectively, and similar activity order was also found under the tight contact condition. The high soot oxidation efficacy of the CeO2-Sm2O3 sample was attributed to numerous catalytically favourable properties, like smaller crystallite size, larger surface area, abundant oxygen vacancies, and superior reducible nature. 展开更多
关键词 rare earths cerium oxide solid solutions oxygen vacancies soot oxidation
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Waste heat recovery and denitrification of flue gases from gas-fired boilers 被引量:2
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作者 ZHAO Yan ZHU Xiao Lei +1 位作者 MENG Ji An LI Zhi Xin 《Science China(Technological Sciences)》 SCIE EI CAS CSCD 2016年第12期1874-1881,共8页
A waste heat recovery and denitrification system was developed for improving energy conservation and emissions control especially for control of PM2.5 particles and haze. The system uses enhanced heat and mass transfe... A waste heat recovery and denitrification system was developed for improving energy conservation and emissions control especially for control of PM2.5 particles and haze. The system uses enhanced heat and mass transfer techniques in a packed heat exchange tower with self-rotation and zero-pressure spraying, low temperature NO oxidation by ozone, and neutralization with an alkali solution. Operating data in a test project gave NOx in the exhaust flue gas of less than 30 mg/Nm3 with an ozone addition rate of 8 kg/h and spray water p H of 7.5–8, an average heat recovery of 3 MW, and an average heat supply of 7.2 MW. 展开更多
关键词 flue gas waste heat recovery denitrification ozone oxidation of NO neutralization with alkali solution heat pump
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First principles materials design of novel functional oxides
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作者 Valentino R.Cooper Brian K.Voas +2 位作者 Craig A.Bridges James R.Morris Scott P.Beckman 《Journal of Advanced Dielectrics》 CAS 2016年第2期61-69,共9页
We review our efforts to develop and implement robust computational approaches for exploring phase stability to facilitate the prediction-to-synthesis process of novel functional oxides.These efforts focus on a synerg... We review our efforts to develop and implement robust computational approaches for exploring phase stability to facilitate the prediction-to-synthesis process of novel functional oxides.These efforts focus on a synergy between(i)electronic structure calculations for properties predictions,(ii)phenomenological/empirical methods for examining phase stability as related to both phase segregation and temperature-dependent transitions and(iii)experimental validation through synthesis and characterization.We illustrate this philosophy by examining an inaugural study that seeks to discover novel functional oxides with high piezoelectric responses.Our results show progress towards developing a framework through which solid solutions can be studied to predict materials with enhanced properties that can be synthesized and remain active under device relevant conditions. 展开更多
关键词 First principles materials design and discovery oxide solid solutions.
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A novel oxidation-based wet etching method for AlGaN/GaN heterostructures
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作者 蔡金宝 王金延 +5 位作者 刘洋 徐哲 王茂俊 于民 解冰 吴文刚 《Journal of Semiconductors》 EI CAS CSCD 2013年第8期201-204,共4页
A novel wet etching method for AlGaN/GaN heterojunction structures is proposed using thermal oxidation f ollowed by wet etching in KOH solution.It is found that an AlGaN/GaN heterostructure after high temperature oxid... A novel wet etching method for AlGaN/GaN heterojunction structures is proposed using thermal oxidation f ollowed by wet etching in KOH solution.It is found that an AlGaN/GaN heterostructure after high temperature oxidation above 700℃could be etched off in a homothermal(70℃) KOH solution while the KOH solution had no etching effects on the region of the AlGaN/GaN heterostructure protected by a SiO_2 layer during the oxidation process.A groove structure with 150 nm step depth on an AlGaN/GaN heterostructure was formed after 8 h thermal oxidation at 900℃followed by 30 min treatment in 70℃KOH solution.As the oxidation time increases,the etching depth approaches saturation and the roughness of the etched surface becomes much better.The physical mechanism of this phenomenon is also discussed. 展开更多
关键词 AlGaN/GaN wet etching thermal oxidation KOH solution
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