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Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of

Bei Ye, Zhuo Chen, Xinzheng Li, Jianan Liu, Qianyuan Wu, Cheng Yang, Hongying Hu, Ronghe Wang

《环境科学与工程前沿（英文）》 2019年 第13卷 第6期 doi: 10.1007/s11783-019-1170-z

摘要： GO or RGO promotes bromate formation during ozonation of bromide-containing water. CeO2/RGO significantly inhibits bromate formation compared to RGO during ozonation. CeO2/RGO shows an enhancement on DEET degradation efficiency during ozonation. Ozone (O3) is widely used in drinking water disinfection and wastewater treatment. However, when applied to bromide-containing water, ozone induces the formation of bromate, which is carcinogenic. Our previous study found that graphene oxide (GO) can enhance the degradation efficiency of micropollutants during ozonation. However, in this study, GO was found to promote bromate formation during ozonation of bromide-containing waters, with bromate yields from the O3/GO process more than twice those obtained using ozone alone. The promoted bromate formation was attributed to increased hydroxyl radical production, as confirmed by the significant reduction (almost 75%) in bromate yield after adding t-butanol (TBA). Cerium oxide (less than 5 mg/L) supported on reduced GO (xCeO2/RGO) significantly inhibited bromate formation during ozonation compared with reduced GO alone, and the optimal Ce atomic percentage (x) was determined to be 0.36%, achieving an inhibition rate of approximately 73%. Fourier transform infrared (FT-IR) spectra indicated the transformation of GO into RGO after hydrothermal treatment, and transmission electron microscope (TEM) results showed that CeO2 nanoparticles were well dispersed on the RGO surface. The X-ray photoelectron spectroscopy (XPS) spectra results demonstrated that the Ce3+/Ce4+ ratio in xCeO2/RGO was almost 3‒4 times higher than that in pure CeO2, which might be attributed to the charge transfer effect from GO to CeO2. Furthermore, Ce3+ on the xCeO2/RGO surface could quench Br⋅ and BrO⋅ to further inhibit bromate formation. Meanwhile, 0.36CeO2/RGO could also enhance the degradation efficiency of N,N-diethyl-m-toluamide (DEET) in synthetic and reclaimed water during ozonation.

关键词： Bromate     Catalytic ozonation     Graphene oxide     Cerium dioxide    

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Cuprous oxide/copper oxide interpenetrated into ordered mesoporous cellulose-based carbon aerogels for

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 918-929 doi: 10.1007/s11705-023-2305-0

摘要： The casual discharge of dyes from industrial settings has seriously polluted global water systems. Owing to the abundance of biomass resources, preparing photocatalysts for photocatalytic degradation of dyes is significant; however, it still remains challenging. In this work, a cuprous oxide/copper oxide composite was interpenetrated onto carbon nanosheets of cellulose-based flexible carbon aerogels (Cu2O/CuO@CAx) via a simple freeze-drying-calcination method. The introduction of the carbon aerogel effectively prevents the aggregation of the cuprous oxide/copper oxide composite. In addition, Cu2O/CuO@CA0.2 has a larger specific surface area, stronger charge transfer capacity, and lower recombination rate of photogenerated carriers than copper oxide. Moreover, Cu2O/CuO@CA0.2 exhibited high photocatalytic activity in decomposing methylene blue, with a degradation rate reaching up to 99.09% in 60 min. The active oxidation species in the photocatalytic degradation process were systematically investigated by electron spin resonance characterization and poisoning experiments, among which singlet oxygen played a major role. In conclusion, this work provides an effective method for preparing photocatalysts using biomass resources in combination with different metal oxides. It also promotes the development of photocatalytic degradation of dyes.

关键词： carbon aerogel     photocatalysis     dye degradation     biomass     cuprous oxide/copper oxide    

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Removal and recovery of toxic nanosized Cerium Oxide using eco-friendly Iron Oxide Nanoparticles

Kanha Gupta, Nitin Khandelwal, Gopala Krishna Darbha

《环境科学与工程前沿（英文）》 2020年 第14卷 第1期 doi: 10.1007/s11783-019-1194-4

摘要： Eco-friendly IONPs were synthesized through solvothermal method. IONPs show very high removal efficiency for CeO2 NPs i.e. 688 mg/g. Removal was >90% in all synthetic and real water samples. >80% recovery of CeO2 NPs through sonication confirms reusability of IONPs. Increasing applications of metal oxide nanoparticles and their release in the natural environment is a serious concern due to their toxic nature. Therefore, it is essential to have eco-friendly solutions for the remediation of toxic metal oxides in an aqueous environment. In the present study, eco-friendly Iron Oxide Nanoparticles (IONPs) are synthesized using solvothermal technique and successfully characterized using scanning and transmission electron microscopy (SEM and TEM respectively) and powder X-Ray diffraction (PXRD). These IONPs were further utilized for the remediation of toxic metal oxide nanoparticle, i.e., CeO2. Sorption experiments were also performed in complex aqueous solutions and real water samples to check its applicability in the natural environment. Reusability study was performed to show cost-effectiveness. Results show that these 200 nm-sized spherical IONPs, as revealed by SEM and TEM analysis, were magnetite (Fe3O4) and contained short-range crystallinity as confirmed from XRD spectra. Sorption experiments show that the composite follows the pseudo-second-order kinetic model. Further R2>0.99 for Langmuir sorption isotherm suggests chemisorption as probable removal mechanism with monolayer sorption of CeO2 NPs on IONP. More than 80% recovery of adsorbed CeO2 NPs through ultrasonication and magnetic separation of reaction precipitate confirms reusability of IONPs. Obtained removal % of CeO2 in various synthetic and real water samples was>90% signifying that IONPs are candidate adsorbent for the removal and recovery of toxic metal oxide nanoparticles from contaminated environmental water samples.

关键词： Adsorption     toxic metal oxide remediation     eco-friendly IONP     Iron oxide     CeO2 removal    

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Plasma-electrochemical synthesis of europium doped cerium oxide nanoparticles

Liangliang Lin, Xintong Ma, Sirui Li, Marly Wouters, Volker Hessel

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 501-510 doi: 10.1007/s11705-019-1810-7

摘要： In the present study, a plasma-electrochemical method was demonstrated for the synthesis of europium doped ceria nanoparticles. Ce(NO ) ·6H O and Eu(NO ) ·5H O were used as the starting materials and being dissolved in the distilled water as the electrolyte solution. The plasma-liquid interaction process was investigated by an optical emission spectroscopy, and the obtained products were characterized by complementary analytical methods. Results showed that crystalline cubic CeO :Eu nanoparticles were successfully obtained, with a particle size in the range from 30 to 60 nm. The crystal structure didn’t change during the calcination at a temperature from 400°C to 1000°C, with the average crystallite size being estimated to be 52 nm at 1000°C. Eu ions were shown to be effectively and uniformly doped into the CeO lattices. As a result, the obtained nanophosphors emit apparent red color under the UV irradiation, which can be easily observed by naked eye. The photoluminescence spectrum further proves the downshift behavior of the obtained products, where characteristic D → F transitions of Eu ions had been detected. Due to the simple, flexible and environmental friendly process, this plasma-electrochemical method should have great potential for the synthesis of a series of nanophosphors, especially for bio-application purpose.

关键词： plasma-electrochemical method     europium doped ceria     rare earth nanoparticles     photoluminescence    

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Halide-free carbonylation of methanol with H-MOR supported CuCeO

Chaoli Tong, Jiachang Zuo, Danlu Wen, Weikun Chen, Linmin Ye, Youzhu Yuan

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1075-1087 doi: 10.1007/s11705-020-2019-5

摘要： Heterogeneous halide-free carbonylation of methanol to acetates, including methyl acetate (MA) and acetic acid, using non-precious metal catalysts has been a topic of interest for decades. The key issue is that the water produced by methanol dehydration inhibits the formation of acetyl species and reduces the MA selectivity. Here, we report that CuCeO /H-mordenite (H-MOR) catalyst can nearly eliminate the inhibiting effect of water on carbonylation by a water-gas shift reaction (WGSR) on-site, and can thus achieve 96.5% methanol conversion with 87.4% MA selectivity for the halide-free carbonylation of methanol. The results of powder X-ray diffraction, transmission electron microscopy, and scanning electron microscopy show that the Cu and Ce species are highly dispersed on H-MOR even when the CuCeO contents are as high as 29 wt-%. Fourier transform infrared spectroscopy and CO chemisorption analysis reveal that a small portion of Cu species can migrate into the channel of H-MOR when CuCeO /H-MOR is calcined at 500 °C and these Cu species are converted into Cu sites upon reduction. The Cu sites facilitate the WGSR and are also active sites for methanol carbonylation. The introduction of Ce benefits the inhibition of coke deposits and thus enhances the catalyst stability.

关键词： methanol carbonylation     halide-free     methyl acetate     H-mordenite     copper and cerium oxide    

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Reduction of CeO

Elena Yu. KONYSHEVA

《化学科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 249-261 doi: 10.1007/s11705-013-1333-6

摘要： Reduction behavior of pure and doped CeO , the multi-phase La Sr CoO ? CeO , La Sr MnO ? CeO , and La Ni Fe O ? CeO composites, was studied under hydrogen containing atmosphere to address issues related to the improvement of electrochemical and catalytic performance of electrodes in fuel cells. The enhanced reduction of cerium oxide was observed initially at 800°C in all composites in spite of the presence of highly reducible transition metal cations that could lead to the increase in surface concentration of oxygen vacancies and generation of the electron enriched surface. Due to continuous reduction of cerium oxide in La Sr CoO ? CeO and La Sr MnO ? CeO (up to 10 h) composites the redox activity of the Ce /Ce pair could be suppressed and additional measures are required for reversible spontaneous regeneration of Ce . After 3 h exposure to H -Ar at 800°C the reduction of cerium oxides and perovskite phases in La Ni Fe O ? CeO composites was diminished. The extent of cerium oxide involvement in the reduction process varies with time, and depends on its initial deviation from oxygen stoichiometry (that results in the larger lattice parameter and the longer pathway for O transport through the fluorite lattice), chemical origin of transition metal cations in the perovskite, and phase diversity in multi-phase composites.

关键词： reduction of cerium oxide     composites     perovskites     catalyst under hydrogen containing atmosphere    

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Efficient base-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over copper-dopedmanganese oxide nanorods with

Feng Cheng, Dongwen Guo, Jinhua Lai, Meihui Long, Wenguang Zhao, Xianxiang Liu, Dulin Yin

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 960-968 doi: 10.1007/s11705-020-1999-5

摘要： 2,5-Furandicarboxylic acid (FDCA) is an important and renewable building block and can serve as an alternative to terephthalic acid in the production of bio-based degradable plastic. In this study, Cu-doped MnO  nanorods were prepared by a facile hydrothermal redox method and employed as catalysts for the selective oxidation of 5-hydroxymethylfurfural (HMF) to FDCA using -butyl hydroperoxide (TBHP) as an oxidant. The catalysts were characterized using X-ray diffraction analysis, Fourier transform infrared spectroscopy, thermogravimetric analysis, and transmission electron microscopy. The effects of oxidants, solvents, and reaction conditions on the oxidation of HMF were investigated, and a reaction mechanism was proposed. Experimental results demonstrated that 99.4% conversion of HMF and 96.3% selectivity of FDCA were obtained under suitable conditions, and -butanol was the most suitable solvent when TBHP was used as an oxidant. More importantly, the Cu-doped MnO catalyst can maintain durable catalytic activity after being recycled for more than ten times.

关键词： 5-hydroxymethylfurfural     25-furandicarboxylic acid     selective oxidation     Cu-doped MnO2     biomass transformation    

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Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

《环境科学与工程前沿（英文）》 2008年 第2卷 第3期   页码 354-357 doi: 10.1007/s11783-008-0059-z

摘要： In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/AlO catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/AlO catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto AlO support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru–Ce/AlO on catalytic activity.

关键词： Ru–Ce/AlO     dimethyl phthalate     mineralization     comparison experiment     catalytic ozonation    

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Copper and zinc interaction on water clearance and tissue metal distribution in the freshwater mussel

Tianxiang XIA, Xuehua LIU

《环境科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 236-242 doi: 10.1007/s11783-010-0218-8

摘要： Copper and zinc interaction on clearance from water and distribution in different tissues was investigated for the freshwater mussel, , under laboratory conditions. Clearance rate of Cu or Zn from water was highly dependent on exposure concentration. Interaction effect was most evident at 300 μg·L Cu exposure and depressed the Zn clearance rate significantly ( <0.05). However, the presence of 100 μg·L and 300 μg·L Zn hardly affected the Cu clearance rate. The 300 μg·L Cu presence enhanced Cu accumulation in each tissue most significantly ( <0.01), but caused Zn content to decrease in the gills by 62% ( <0.05), viscera by 49% ( <0.05) and foot by 31% ( <0.05), and increase in the mantle by 97% ( <0.05) and the muscles by 243% ( <0.05) for different Zn exposure treatments. The response of metal accumulation in various tissues of the test mussels indicated that Zn transferred from the gills, viscera and foot to the mantle and muscles might be one of the important characteristics of the Zn regulatory mechanism by leading to a narrow range of Zn concentration in the different tissues.

关键词： interaction     mussel     copper     zinc     clearance     distribution    

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Identification and assessment of environmental burdens of Chinese copper production from a life cycle

Xiaolong SONG,Jianxin YANG,Bin LU,Bo LI,Guangyuan ZENG

《环境科学与工程前沿（英文）》 2014年 第8卷 第4期   页码 580-588 doi: 10.1007/s11783-013-0599-8

摘要： The environmental burdens of Chinese copper production have been identified and quantified in the context of typical technologies, materials supplies and environmental emissions by a life cycle approach. Primary and secondary copper production using copper ores and scraps, respectively, were analyzed in detail. The flash and bath smelting approaches and the recycling of copper scraps were selected as representative copper production processes. A quantitative analysis was also conducted to assess the influence of material transport distance in copper production. Life cycle assessment (LCA) results showed that resources depletion and human health contribute significantly to environmental burdens in Chinese copper production. In addition, the secondary copper production has dramatically lower environmental burdens than the primary production. There is no obvious distinction in overall environmental burdens in primary copper production by flash or bath smelting approach. However, resources depletion is lower and the damage to human health is higher for flash smelting approach. Ecosystem quality damage is slight for both approaches. Environmental burdens from the mining stage contribute most in all life cycle stages in primary copper production. In secondary copper production, the electrolytic refining stage dominates. Based on the life cycle assessment results, some suggestions for improving environmental performance were proposed to meet the sustainable development of Chinese copper industry.

关键词： copper production     environmental burden     life cycle assessment     refined copper    

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迎接铜工业挑战——低成本处理硫化铜精矿途径的思考

朱祖泽

《中国工程科学》 2000年 第2卷 第2期   页码 87-90

摘要：

对过去10年来铜冶炼的技术进步和铜价格的变化作出的简要回顾指出，未来铜市场的竞争是取决于冶炼技术的生产成本的竞争。坚持自我研究开发和引进相结合才能保证我国铜工业健康稳定发展，并能应付国际竞争。评述了现在强氧化-PS转炉吹炼-火法精炼-电解流程的不足；分析了火湿法联合流程的可能性及依据；新的火湿法联合流程将有更强的竞争优势。

关键词： 未来铜工业     硫化铜精矿     低成本处理    

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Reductive amination of -hexanol to -hexylamine over Ni–Ce/-AlO catalysts

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 82-92 doi: 10.1007/s11705-022-2181-z

摘要： The amination of alkyl alcohols is one of the most promising paths in synthesis of aliphatic amines. Herein, cerium doped nickel-based catalysts were synthesized and tested in a gas-phase amination of n-hexanol to n-hexylamine. It was found that the activity of the Ni/γ-Al2O3 catalyst is significantly improved by doping an appropriate amount of cerium. The presence of cerium effectively inhibits the agglomeration of nickel particle, resulting in better Ni dispersion. As Ni particle size plays critical role on the catalytic activity, higher turnover frequency of n-hexanol amination was achieved. Cerium doping also improves the reduction ability of nickel and enhances the interactions between Ni and the catalyst support. More weak acid sites were also found in those cerium doped catalysts, which promote another key step—ammonia dissociative adsorption in this reaction system. The overall synergy of Ni nanoparticles and acid sites of this Ni–Ce/γ-Al2O3 catalyst boosts its superior catalytic performance in the amination of n-hexanol.

关键词： amination     alcohol     cerium     nickel     acidity     interaction    

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Variability of waste copper slag concrete and its effect on the seismic safety of reinforced concrete

《结构与土木工程前沿（英文）》 2022年 第16卷 第1期   页码 117-130 doi: 10.1007/s11709-021-0788-7

摘要： Proven research output on the behavior of structures made of waste copper slag concrete can improve its utilization in the construction industry and thereby help to develop a sustainable built environment. Although numerous studies on waste copper slag concrete can be found in the published literature, no research has focused on the structural application of this type of concrete. In particular, the variability in the strength properties of waste copper slag concrete, which is required for various structural applications, such as limit state design formulation, reliability-based structural analysis, etc., has so far not attracted the attention of researchers. This paper quantifies the uncertainty associated with the compressive-, flexural- and split tensile strength of hardened concrete with different dosages of waste copper slag as fine aggregate. Best-fit probability distribution models are proposed based on statistical analyses of strength data generated from laboratory experiments. In addition, the paper presents a reliability-based seismic risk assessment of a typical waste copper slag incorporated reinforced concrete framed building, considering the proposed distribution model. The results show that waste copper slag can be safely used for seismic resistant structures as it results in an identical probability of failure and dispersion in the drift demand when compared with a conventional concrete building made of natural sand.

关键词： waste copper slag     quantification of variability     goodness-of-fit test     seismic risk assessment     PSDM    

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Microwave enhanced stabilization of copper in artificially contaminated soil

Hua ZHANG, Zhiliang ZHU, Noboru YOSHIKAWA

《环境科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 205-211 doi: 10.1007/s11783-010-0290-2

摘要： Microwave processing was used to stabilize copper ions in soil samples. Its effects on the stabilization efficiency were studied as a function of additive, microwave power, process time, and reaction atmosphere. The stabilization efficiency of the microwave process was evaluated based on the results of the toxicity characteristic leaching procedure (TCLP) test. The results showed that the optimal experimental condition contained a 700 W microwave power, 20 min process time and 3 iron wires as the additive, and that the highest stabilization efficiency level was more than 70%. In addition, the different reaction atmospheres showed no apparent effect on the stabilization efficiency of copper in the artificially contaminated soil. According to the result of the Tessier sequential extraction, the partial species of copper in the contaminated soil was deduced to transform from unstable species to stable states after the microwave process.

关键词： microwave     copper     stabilization    

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Pressure drop analysis on the positive half-cell of a cerium redox flow battery using computational fluid

Fernando F. Rivera, Berenice Miranda-Alcántara, Germán Orozco, Carlos Ponce de León, Luis F. Arenas

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 399-409 doi: 10.1007/s11705-020-1934-9

摘要： Description of electrolyte fluid dynamics in the electrode compartments by mathematical models can be a powerful tool in the development of redox flow batteries (RFBs) and other electrochemical reactors. In order to determine their predictive capability, turbulent Reynolds-averaged Navier-Stokes (RANS) and free flow plus porous media (Brinkman) models were applied to compute local fluid velocities taking place in a rectangular channel electrochemical flow cell used as the positive half-cell of a cerium-based RFB for laboratory studies. Two different platinized titanium electrodes were considered, a plate plus a turbulence promoter and an expanded metal mesh. Calculated pressure drop was validated against experimental data obtained with typical cerium electrolytes. It was found that the pressure drop values were better described by the RANS approach, whereas the validity of Brinkman equations was strongly dependent on porosity and permeability values of the porous media.

关键词： CFD simulation     porous media     porous electrode     pressure drop     redox flow battery    

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标题 作者 时间 类型 操作

Inhibition of bromate formation by reduced graphene oxide supported cerium dioxide during ozonation of

Bei Ye, Zhuo Chen, Xinzheng Li, Jianan Liu, Qianyuan Wu, Cheng Yang, Hongying Hu, Ronghe Wang

期刊论文

Cuprous oxide/copper oxide interpenetrated into ordered mesoporous cellulose-based carbon aerogels for

期刊论文

Removal and recovery of toxic nanosized Cerium Oxide using eco-friendly Iron Oxide Nanoparticles

Kanha Gupta, Nitin Khandelwal, Gopala Krishna Darbha

期刊论文

Plasma-electrochemical synthesis of europium doped cerium oxide nanoparticles

Liangliang Lin, Xintong Ma, Sirui Li, Marly Wouters, Volker Hessel

期刊论文

Halide-free carbonylation of methanol with H-MOR supported CuCeO

Chaoli Tong, Jiachang Zuo, Danlu Wen, Weikun Chen, Linmin Ye, Youzhu Yuan

期刊论文

Reduction of CeO

Elena Yu. KONYSHEVA

期刊论文

Efficient base-free oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over copper-dopedmanganese oxide nanorods with

Feng Cheng, Dongwen Guo, Jinhua Lai, Meihui Long, Wenguang Zhao, Xianxiang Liu, Dulin Yin

期刊论文

Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

期刊论文

Copper and zinc interaction on water clearance and tissue metal distribution in the freshwater mussel

Tianxiang XIA, Xuehua LIU

期刊论文

Identification and assessment of environmental burdens of Chinese copper production from a life cycle

Xiaolong SONG,Jianxin YANG,Bin LU,Bo LI,Guangyuan ZENG

期刊论文

迎接铜工业挑战——低成本处理硫化铜精矿途径的思考

朱祖泽

期刊论文

Reductive amination of -hexanol to -hexylamine over Ni–Ce/-AlO catalysts

期刊论文

Variability of waste copper slag concrete and its effect on the seismic safety of reinforced concrete

期刊论文

Microwave enhanced stabilization of copper in artificially contaminated soil

Hua ZHANG, Zhiliang ZHU, Noboru YOSHIKAWA

期刊论文

Pressure drop analysis on the positive half-cell of a cerium redox flow battery using computational fluid

Fernando F. Rivera, Berenice Miranda-Alcántara, Germán Orozco, Carlos Ponce de León, Luis F. Arenas

期刊论文