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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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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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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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Photocatalytic reduction of carbon dioxide by titanium oxide-based semiconductors to produce fuels

Xi CHEN, Fangming JIN

《能源前沿（英文）》 2019年 第13卷 第2期   页码 207-220 doi: 10.1007/s11708-019-0628-9

摘要： To tackle the crisis of global warming, it is imperative to control and mitigate the atmospheric carbon dioxide level. Photocatalytic reduction of carbon dioxide into solar fuels furnishes a gratifying solution to utilize and reduce carbon dioxide emission and simultaneously generate renewable energy to sustain the societies. So far, titanium oxide-based semiconductors have been the most prevalently adopted catalysts in carbon dioxide photoreduction. This mini-review provides a general summary of the recent progresses in titanium oxide-catalyzed photocatalytic reduction of carbon dioxide. It first illustrates the use of structural engineering as a strategy to adjust and improve the catalytic performances. Then, it describes the introduction of one/two exogenous elements to modify the photocatalytic activity and/or selectivity. Lastly, it discusses multi-component hybrid titanium oxide composites.

关键词： photocatalysis     carbon dioxide reduction     semiconductors     titanium oxide     renewable fuels    

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Nitrous oxide formation and emission in selective non-catalytic reduction process

YANG Weijuan, ZHOU Junhu, ZHOU Zhijun, CEN Kefa

《能源前沿（英文）》 2007年 第1卷 第2期   页码 228-232 doi: 10.1007/s11708-007-0031-9

摘要： Pulverized coal-fired boilers are not nitrous oxide sources because of high temperature combustion. But selective non-catalytic reduction may produce NO by NO reduction reactions. Chemical kinetics calculation and experimental research were used to find out the mechanism between NO and N-agent species, N-agent/NO nitrogen stoichiometric ratio (NSR), reaction temperature, reaction time, etc. The results show that NO emission decreases with increasing reaction temperature and NSR decreases when reaction time is enough. NO concentration first increases then decreases as SNCR reactions keep on occuring. Ammonia SNCR tests indicated that NO emission was 0 7 μmol/mol. About 8.7% of NO was transformed to NO, and NO emission was 27.8 μmol/mol at urea-SNCR test. Urea-SNCR is likely to bring NO emission problem.
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Electrocatalytic reduction of NO to NH in ionic liquids by P-doped TiO nanotubes

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 726-734 doi: 10.1007/s11705-022-2274-8

摘要： Designing advanced and cost-effective electrocatalytic system for nitric oxide (NO) reduction reaction (NORR) is vital for sustainable NH3 production and NO removal, yet it is a challenging task. Herein, it is shown that phosphorus (P)-doped titania (TiO2) nanotubes can be adopted as highly efficient catalyst for NORR. The catalyst demonstrates impressive performance in ionic liquid (IL)-based electrolyte with a remarkable high Faradaic efficiency of 89% and NH3 yield rate of 425 μg·h−1·mgcat.−1, being close to the best-reported results. Noteworthy, the obtained performance metrics are significantly larger than those for N2 reduction reaction. It also shows good durability with negligible activity decay even after 10 cycles. Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites, thereby enhancing the NO adsorption and facilitating the desorption of *NH3. Moreover, the utilization of IL further suppresses the competitive hydrogen evolution reaction. This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH3 at a high efficiency and rate.

关键词： nitric oxide reduction reaction     electrcatalysis     ammonia production     phosphorus-doped titania    

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Biotoxicity evaluation of zinc oxide nanoparticles on bacterial performance of activated sludge at COD, nitrogen, and phosphorus reduction

《环境科学与工程前沿（英文）》 2022年 第16卷 第2期 doi: 10.1007/s11783-021-1453-z

摘要：

• ZnO-NP disrupted metabolic/catabolic balance of bacteria by affecting DHA activity.

关键词： Granular sludge     Biotoxicity     Reactive oxygen species     Extracellular polymeric substances    

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Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

《环境科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 186-193 doi: 10.1007/s11783-009-0016-5

摘要： The reaction mechanisms of selective catalytic reduction (SCR) of nitric oxide (NO) by methane (CH ) over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models. Catalysts derived from different supports would lead to different reaction pathways, and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities. Higher ratios of Br?nsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation. Strong Br?nsted acid sites would not necessarily lead to better catalytic performance, however, since the active surface NO species and the corresponding reaction routes were determined by the overall acidity strength of the support. The reaction routes where NO moiety was engaged as an important intermediate involved moderate oxidation of methane, the rate of which could determine the overall activity. The reaction involving NO moiety was likely to be determined by the step of reduction of NO. Therefore, to enhance the SCR activity of solid superacid catalysts, reactions between appropriate couples of active NO species and activated hydrocarbon intermediates should be realized by modification of the support acidity.

关键词： selective catalytic reduction (SCR)     nitric oxide (NO)     methane     support acidity     Br?nsted acid sites     NOy species    

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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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Tuning the catalytic selectivity in electrochemical CO

Jiafang XIE,Yuxi HUANG,Hanqing YU

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 861-866 doi: 10.1007/s11783-014-0742-1

摘要： Electrochemical conversion of CO to hydrocarbons can relieve both environmental and energy stresses. However, electrocatalysts for this reaction usually suffer from a poor product selectivity and a large overpotential. Here we report that tunable catalytic selectivity for hydrocarbon formation could be achieved on Cu nanomaterials with different morphologies. By tuning the electrochemical parameters, either Cu oxide nanowires or nanoneedles were fabricated and then electrochemically reduced to the corresponding Cu nanomaterials. The Cu nanowires preferred the formation of C H , while the Cu nanoneedles favored the production of more CH , rather than C H . Our work provides a facile synthetic strategy for preparing Cu-based nanomaterials to achieve selective CO reduction.

关键词： electrochemical CO2 reduction     Cu oxide     nanostructure     selectivity     hydrocarbon formation    

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多目标自适应优化模型预测控制——降低氧化锌回转窑的碳排放 Article

Ke Wei, Keke Huang, Chunhua Yang, Weihua Gui

《工程（英文）》 2023年 第27卷 第8期   页码 96-105 doi: 10.1016/j.eng.2023.01.017

摘要：

The zinc oxide rotary kiln, as an essential piece of equipment in the zinc smelting industrial process, is presenting new challenges in process control. China's strategy of achieving a carbon peak and carbon neutrality is putting new demands on the industry, including green production and the use of fewer resources; thus, traditional stability control is no longer suitable for multi-objective control tasks. Although researchers have revealed the principle of the rotary kiln and set up computational fluid dynamics (CFD) simulation models to study its dynamics, these models cannot be directly applied to process control due to their high computational complexity. To address these issues, this paper proposes a multi-objective adaptive optimization model predictive control (MAO-MPC) method based on sparse identification. More specifically, with a large amount of data collected from a CFD model, a sparse regression problem is first formulated and solved to obtain a reduction model. Then, a two-layered control framework including real-time optimization (RTO) and model predictive control (MPC) is designed. In the RTO layer, an optimization problem with the goal of achieving optimal operation performance and the lowest possible resource consumption is set up. By solving the optimization problem in real time, a suitable setting value is sent to the MPC layer to ensure that the zinc oxide rotary kiln always functions in an optimal state. Our experiments show the strength and reliability of the proposed method, which reduces the usage of coal while maintaining high profits. 

关键词： Zinc oxide rotary kiln     Model reduction     Sparse identification     Real-time optimization     Model predictive control     Process control    

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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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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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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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标题 作者 时间 类型 操作

Reduction of CeO

Elena Yu. KONYSHEVA

期刊论文

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

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

Photocatalytic reduction of carbon dioxide by titanium oxide-based semiconductors to produce fuels

Xi CHEN, Fangming JIN

期刊论文

Nitrous oxide formation and emission in selective non-catalytic reduction process

YANG Weijuan, ZHOU Junhu, ZHOU Zhijun, CEN Kefa

期刊论文

Electrocatalytic reduction of NO to NH in ionic liquids by P-doped TiO nanotubes

期刊论文

Biotoxicity evaluation of zinc oxide nanoparticles on bacterial performance of activated sludge at COD, nitrogen, and phosphorus reduction

期刊论文

Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

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

Tuning the catalytic selectivity in electrochemical CO

Jiafang XIE,Yuxi HUANG,Hanqing YU

期刊论文

多目标自适应优化模型预测控制——降低氧化锌回转窑的碳排放

Ke Wei, Keke Huang, Chunhua Yang, Weihua Gui

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

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

期刊论文

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

期刊论文