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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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Catalytic performance of Co-Mo-Ce-K/γ-Al

Yuqiong ZHAO, Yongfa ZHANG

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 457-460 doi: 10.1007/s11705-010-0524-7

摘要： The catalytic performance of Co-Mo-Ce-K/γ-Al O catalyst for the shift reaction of CO in coke oven gas is investigated using X-ray diffraction (XRD) and temperature-programmed reduction (TPR). The results indicate that Ce and K have a synergistic effect on promoting the catalytic activity, and the Co-Mo-Ce-K/γ-Al O catalyst with 3.0 wt-% CeO and 6.0 wt-% K O exhibits the highest activity. CeO favors Co dispersion and mainly produces an electronic effect. TPR characterization results indicate that the addition of CeO -K O in the Co-Mo-Ce-K/γ-Al O catalyst decreases the reduction temperature of active components, and part of octahedrally coordinated Mo transforms into tetrahedrally coordinated Mo , which has a close relationship with the catalytic activity.

关键词： coke oven gas     water gas shift reaction     sulfur-tolerant catalyst     cerium dioxide    

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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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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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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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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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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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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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Investigation of carbon dioxide photoreduction process in a laboratory-scale photoreactor by computational

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1149-1163 doi: 10.1007/s11705-021-2096-0

摘要： The production of solar fuels via the photoreduction of carbon dioxide to methane by titanium oxide is a promising process to control greenhouse gas emissions and provide alternative renewable fuels. Although several reaction mechanisms have been proposed, the detailed steps are still ambiguous, and the limiting factors are not well defined. To improve our understanding of the mechanisms of carbon dioxide photoreduction, a multiphysics model was developed using COMSOL. The novelty of this work is the computational fluid dynamic model combined with the novel carbon dioxide photoreduction intrinsic reaction kinetic model, which was built based on three-steps, namely gas adsorption, surface reactions and desorption, while the ultraviolet light intensity distribution was simulated by the Gaussian distribution model and Beer-Lambert model. The carbon dioxide photoreduction process conducted in a laboratory-scale reactor under different carbon dioxide and water moisture partial pressures was then modeled based on the intrinsic kinetic model. It was found that the simulation results for methane, carbon monoxide and hydrogen yield match the experiments in the concentration range of 10−4 mol·m–3 at the low carbon dioxide and water moisture partial pressure. Finally, the factors of adsorption site concentration, adsorption equilibrium constant, ultraviolet light intensity and temperature were evaluated.

关键词： carbon dioxide photoreduction     computational fluid dynamic simulation     kinetic model     Langmuir adsorption    

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Scale up of reactors for carbon dioxide reduction

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 116-122 doi: 10.1007/s11705-022-2178-7

摘要： In recent times there has been a great deal of interest in the conversion of carbon dioxide into more useful chemical compounds. On the other hand, the translation of these developments in electrochemical reduction of carbon dioxide from the laboratory bench to practical scale remains an underexplored topic. Here we examine some of the major challenges, demonstrating some promising strategies towards such scale-up, including increased electrode area and stacking of electrode pairs in different configurations. We observed that increasing the electrode area from 1 to 10 cm2 led to only a 4% drop in current density, with similarly small penalties realised when stacking sub-cells together.

关键词： CO2 reduction     electrochemical cell     electrosynthesis     upscaling    

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Renewable synthetic fuel: turning carbon dioxide back into fuel

《能源前沿（英文）》 2022年 第16卷 第2期   页码 145-149 doi: 10.1007/s11708-022-0828-6

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Synthesis of ordered cerium-doped cubic mesoporous silica using long-chain ionic liquid as template

YUE Hongxia, ZHAO Hongmei, LIU Longjiang, WANG Siping, Ruan Qiong, WANG Tongwen

《化学科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 135-139 doi: 10.1007/s11705-008-0031-2

摘要： The long-chain ionic liquid 1-hexadecyl-3-methylimidazolium chloride (CmimCl) was used as a template to prepare cerium-doped MCM-48 materials in basic medium by a hydrothermal synthesis procedure. The effect of the amount of Ce salt and CmimCl/Si on the synthesis were discussed in detail. This mesoporous material exhibits a pore architecture which is cubic 3 gyroid and possesses a large surface area and a narrow pore distribution. Cerium in calcined porous framework exists in the form of well-dispersed tetrahedral coordination. The CmimCl shows a high tendency toward self-aggregation that allows the formation of the cerium-doped gyroid mesostructure by using the appropriate amount of Ce salt.

关键词： mesoporous     CmimCl/Si     tendency     mesostructure     synthesis procedure    

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Removal of lead from aqueous solution by hydroxyapatite/manganese dioxide composite

Lijing DONG,Zhiliang ZHU,Yanling QIU,Jianfu ZHAO

《环境科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 28-36 doi: 10.1007/s11783-014-0722-5

摘要： A novel composite adsorbent, hydroxyapatite/manganese dioxide (HAp/MnO ), has been developed for the purpose of removing lead ions from aqueous solutions. The combination of HAp with MnO is meant to increase its adsorption capacity. Various factors that may affect the adsorption efficiency, including solution pH, coexistent substances such as humic acid and competing cations (Ca , Mg ), initial solute concentration, and the duration of the reaction, have been investigated. Using this composite adsorbent, solution pH and coexistent calcium or magnesium cations were found to have no significant influence on the removal of lead ions under the experimental conditions. The adsorption equilibrium was described well by the Langmuir isotherm model, and the calculated maximum adsorption capacity was 769 mg·g . The sorption processes obeyed the pseudo-second-order kinetics model. The experimental results indicate that HAp/MnO composite may be an effective adsorbent for the removal of lead ions from aqueous solutions.

关键词： lead     composite materials     manganese dioxide     hydroxyapatite     adsorption    

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The carbon dioxide removal potential of Liquid Air Energy Storage: A high-level technical and economic

Andrew LOCKLEY, Ted von HIPPEL

《工程管理前沿（英文）》 2021年 第8卷 第3期   页码 456-464 doi: 10.1007/s42524-020-0102-8

摘要： Liquid Air Energy Storage (LAES) is at pilot scale. Air cooling and liquefaction stores energy; reheating revaporises the air at pressure, powering a turbine or engine (Ameel et al., 2013). Liquefaction requires water & CO removal, preventing ice fouling. This paper proposes subsequent geological storage of this CO – offering a novel Carbon Dioxide Removal (CDR) by-product, for the energy storage industry. It additionally assesses the scale constraint and economic opportunity offered by implementing this CDR approach. Similarly, established Compressed Air Energy Storage (CAES) uses air compression and subsequent expansion. CAES could also add CO scrubbing and subsequent storage, at extra cost. CAES stores fewer joules per kilogram of air than LAES – potentially scrubbing more CO per joule stored. Operational LAES/CAES technologies cannot offer full-scale CDR this century (Stocker et al., 2014), yet they could offer around 4% of projected CO disposals for LAES and<25% for current-technology CAES. LAES CDR could reach trillion-dollar scale this century (20 billion USD/year, to first order). A larger, less certain commercial CDR opportunity exists for modified conventional CAES, due to additional equipment requirements. CDR may be commercially critical for LAES/CAES usage growth, and the necessary infrastructure may influence plant scaling and placement. A suggested design for low-pressure CAES theoretically offers global-scale CDR potential within a century (ignoring siting constraints) – but this must be costed against competing CDR and energy storage technologies.

关键词： carbon dioxide removal     Liquid Air Energy Storage     Compressed Air Energy Storage     geoengineering    

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Tripotassium citrate monohydrate derived carbon nanosheets as a competent assistant to manganese dioxide

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 420-432 doi: 10.1007/s11705-021-2065-7

摘要： Production cost, capacitance, and electrode materials safety are the key factors to be concerned about for supercapacitors. In this work, a type of carbon nanosheets was produced through the carbonization of tripotassium citrate monohydrate and nitric acidification. Subsequently, a well-designed manganese dioxide/carbon nanosheets composite was synthesized through hydrothermal treating. The carbon nanosheets served as the substrate for growing the manganese dioxide, regulating its distribution, and preventing it from inhomogeneous dimensions and severe agglomeration. Many manganese dioxide nanosheets grew vertically on the numerous functional groups generated on the surface of the carbon nanosheets during acidification. The synergistic combination of carbon nanosheets and manganese dioxide tailors the electrochemical performance of the composite, which benefits from the excellent conductivity and stability of carbon nanosheets. The carbon nanosheets derived from tripotassium citrate monohydrate are conducive to the remarkable performance of manganese dioxide/carbon nanosheets electrode. Finally, an asymmetric supercapacitor with active carbon as the cathode and manganese dioxide/carbon nanosheets as the anode was assembled, achieving an outstanding energy density of 54.68 Wh·kg–1 and remarkable power density of 6399.2 W·kg–1 superior to conventional lead-acid batteries. After 10000 charge-discharge cycles, the device retained 75.3% of the initial capacitance, showing good cycle stability. Two assembled asymmetric supercapacitors in series charged for 3 min could power a yellow light emitting diode with an operating voltage of 2 V for 2 min. This study may provide valuable insights for applying carbon materials and manganese dioxide in the energy storage field.

关键词： carbon nanosheets     manganese dioxide     asymmetric supercapacitors     energy density     power density    

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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

Catalytic performance of Co-Mo-Ce-K/γ-Al

Yuqiong ZHAO, Yongfa ZHANG

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

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

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

期刊论文

Reduction of CeO

Elena Yu. KONYSHEVA

期刊论文

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

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

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

Investigation of carbon dioxide photoreduction process in a laboratory-scale photoreactor by computational

期刊论文

Scale up of reactors for carbon dioxide reduction

期刊论文

Renewable synthetic fuel: turning carbon dioxide back into fuel

期刊论文

Synthesis of ordered cerium-doped cubic mesoporous silica using long-chain ionic liquid as template

YUE Hongxia, ZHAO Hongmei, LIU Longjiang, WANG Siping, Ruan Qiong, WANG Tongwen

期刊论文

Removal of lead from aqueous solution by hydroxyapatite/manganese dioxide composite

Lijing DONG,Zhiliang ZHU,Yanling QIU,Jianfu ZHAO

期刊论文

The carbon dioxide removal potential of Liquid Air Energy Storage: A high-level technical and economic

Andrew LOCKLEY, Ted von HIPPEL

期刊论文

Tripotassium citrate monohydrate derived carbon nanosheets as a competent assistant to manganese dioxide

期刊论文