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Characterization and catalytic activity of soft-templated NiO-CeO

Luciano Atzori, Maria Giorgia Cutrufello, Daniela Meloni, Barbara Onida, Delia Gazzoli, Andrea Ardu, Roberto Monaci, Maria Franca Sini, Elisabetta Rombi

《化学科学与工程前沿(英文)》 2021年 第15卷 第2期   页码 251-268 doi: 10.1007/s11705-020-1951-8

摘要: Nanosized NiO, CeO and NiO-CeO mixed oxides with different Ni/Ce molar ratios were prepared by the soft template method. All the samples were characterized by different techniques as to their chemical composition, structure, morphology and texture. On the catalysts submitted to the same reduction pretreatment adopted for the activity tests the surface basic properties and specific metal surface area were also determined. NiO and CeO nanocrystals of about 4 nm in size were obtained, regardless of the Ni/Ce molar ratio. The Raman and X-ray photoelectron spectroscopy results proved the formation of defective sites at the NiO-CeO interface, where Ni species are in strong interaction with the support. The microcalorimetric and Fourier transform infrared analyses of the reduced samples highlighted that, unlike metallic nickel, CeO is able to effectively adsorb CO , forming carbonates and hydrogen carbonates. After reduction in H at 400 °C for 1 h, the catalytic performance was studied in the CO and CO co-methanation reaction. Catalytic tests were performed at atmospheric pressure and 300 °C, using CO/CO /H molar compositions of 1/1/7 or 1/1/5, and space velocities equal to 72000 or 450000 cm ∙h ∙g . Whereas CO was almost completely hydrogenated in any investigated experimental conditions, CO conversion was strongly affected by both the CO/CO /H ratio and the space velocity. The faster and definitely preferred CO hydrogenation was explained in the light of the different mechanisms of CO and CO methanation. On a selected sample, the influence of the reaction temperature and of a higher number of space velocity values, as well as the stability, were also studied. Provided that the Ni content is optimized, the NiCe system investigated was very promising, being highly active for the CO co-methanation reaction in a wide range of operating conditions and stable (up to 50 h) also when submitted to thermal stress.

关键词: soft template method     NiO-CeO2 catalysts     CO and CO2 co-methanation     synthetic natural gas production    

Catalytic combustion of methane over a highly active and stable NiO/CeO

Xiuhui Huang, Junfeng Li, Jun Wang, Zeqiu Li, Jiayin Xu

《化学科学与工程前沿(英文)》 2020年 第14卷 第4期   页码 534-545 doi: 10.1007/s11705-019-1821-4

摘要: In the last decades, many reports dealing with technology for the catalytic combustion of methane (CH ) have been published. Recently, attention has increasingly focused on the synthesis and catalytic activity of nickel oxides. In this paper, a NiO/CeO catalyst with high catalytic performance in methane combustion was synthesized via a facile impregnation method, and its catalytic activity, stability, and water-resistance during CH combustion were investigated. X-ray diffraction, low-temperature N adsorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, hydrogen temperature programmed reduction, methane temperature programmed surface reaction, Raman spectroscopy, electron paramagnetic resonance, and transmission electron microscope characterization of the catalyst were conducted to determine the origin of its high catalytic activity and stability in detail. The incorporation of NiO was found to enhance the concentration of oxygen vacancies, as well as the activity and amount of surface oxygen. As a result, the mobility of bulk oxygen in CeO was increased. The presence of CeO prevented the aggregation of NiO, enhanced reduction by NiO, and provided more oxygen species for the combustion of CH . The results of a kinetics study indicated that the reaction order was about 1.07 for CH and about 0.10 for O over the NiO/CeO catalyst.

关键词: methane combustion     NiO/CeO2 catalyst     interaction     oxygen vacancy     kinetic study    

Characterization and performance of V

Caiting LI, Qun LI, Pei LU, Huafei CUI, Guangming ZENG

《环境科学与工程前沿(英文)》 2012年 第6卷 第2期   页码 156-161 doi: 10.1007/s11783-010-0295-x

摘要: A series of CeO supported V O catalysts with various loadings were prepared with different calcination temperatures by the incipient impregnation. The catalysts were evaluated for low temperature selective catalytic reduction (SCR) of NO with ammonia (NH ). The effects of O and SO on catalytic activity were also studied. The catalysts were characterized by specific surface areas (S ) and X–ray diffraction (XRD) methods. The experimental results showed that NO conversion changed significantly with the different V O loading and calcination temperature. With the V O loading increasing from 0 to 10 wt%, NO conversion increased significantly, but decreased at higher loading. The optimum calcination temperature was 400°C. The best catalyst yielded above 80% NO conversion in the reaction temperature range of 160°C–300°C. The formation of CeVO on the surface of catalysts caused the decrease of redox ability.

关键词: V2O5/CeO2 catalysts     NH3-SCR (selective catalytic reduction)     the incipient impregnation     low temperatures    

Al<sub>2sub>O<sub>3sub> and CeO<sub>2sub>-promoted MgO sorbents for CO<sub>2sub> capture at moderate

Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song

《化学科学与工程前沿(英文)》 2018年 第12卷 第1期   页码 83-93 doi: 10.1007/s11705-017-1691-6

摘要: A series of Al O and CeO modified MgO sorbents was prepared and studied for CO sorption at moderate temperatures. The CO sorption capacity of MgO was enhanced with the addition of either Al O or CeO . Over Al O -MgO sorbents, the best capacity of 24.6 mg-CO /g-sorbent was attained at 100 °C, which was 61% higher than that of MgO (15.3 mg-CO /g-sorbent). The highest capacity of 35.3 mg-CO /g-sorbent was obtained over the CeO -MgO sorbents at the optimal temperature of 200 °C. Combining with the characterization results, we conclude that the promotion effect on CO sorption with the addition of Al O and CeO can be attributed to the increased surface area with reduced MgO crystallite size. Moreover, the addition of CeO increased the basicity of MgO phase, resulting in more increase in the CO capacity than Al O promoter. Both the Al O -MgO and CeO -MgO sorbents exhibited better cyclic stability than MgO over the course of fifteen CO sorption-desorption cycles. Compared to Al O , CeO is more effective for promoting the CO capacity of MgO. To enhance the CO capacity of MgO sorbent, increasing the basicity is more effective than the increase in the surface area.

关键词: CO2 capture     MgO sorbents     Al2O3     CeO2     flue gas    

Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

《化学科学与工程前沿(英文)》 2022年 第16卷 第8期   页码 1211-1223 doi: 10.1007/s11705-022-2145-3

摘要: The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging. Therefore, an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process. In this study, a Co3O4–CeO2 composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation. This catalyst exhibited a higher selectivity to KA-oil, which was benefited from the synergistic effects between Co3+/Co2+ and Ce4+/Ce3+ redox pairs, than bulk CeO2 and/or Co3O4. Under the optimum reaction conditions, 89.6% selectivity to KA-oil with a cyclohexane conversion of 5.8% was achieved over Co3O4–CeO2. Its catalytic performance remained unchanged after five runs. Using the synergistic effects between the redox pairs of different transition metals, this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.

关键词: Co3O4–CeO2 composite oxides     cyclohexanone     cyclohexanol     ultrasonic-assisted co-precipitation     selective oxidation     solvent-free    

Interface engineering for enhancing electrocatalytic oxygen evolution reaction of CoS/CeO heterostructures

《化学科学与工程前沿(英文)》 2022年 第16卷 第3期   页码 376-383 doi: 10.1007/s11705-021-2062-x

摘要: To realize renewable energy conversion, it is important to develop low-cost and high-efficiency electrocatalyst for oxygen evolution reaction. In this communication, a novel bijunction CoS/CeO2 electrocatalyst grown on carbon cloth is prepared by the interface engineering. The interface engineering of CoS and CeO2 facilitates a rapid charge transfer from CeO2 to CoS. Such an electrocatalyst exhibits outstanding electrocatalytic activity with a low overpotential of 311 mV at 10 mA∙cm−2 and low Tafel slope of 76.2 mV∙dec–1, and is superior to that of CoS (372 mV) and CeO2 (530 mV) counterparts. And it has long-term durability under alkaline media.

关键词: interface engineering     CoS/CeO2     electrodeposition     electrocatalyst     oxygen evolution reaction    

Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1412-1422 doi: 10.1007/s11705-023-2312-1

摘要: In this paper, Cu-doped Bi2WO6 was synthesized via a solvothermal method and applied it in photocatalytic N2 immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi2WO6 composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi3+. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi2WO6. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH3 generation rates of Bi/Cu-Bi2WO6 reached 624 and 243 μmol·L–1·g–1·h–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi2WO6, respectively. This research provides a method for improving the photocatalytic N2 fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N2-to-NH3 conversion.

关键词: Bi2WO6     Cu doping     work function     photocatalytic N2 fixation     charge separation    

CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction

《环境科学与工程前沿(英文)》 2022年 第16卷 第5期 doi: 10.1007/s11783-022-1539-2

摘要:

• CeO2 doping significantly improved low-temperature NH3-SCR activity on FeTiOx.

关键词: NH3-SCR     CeO2 doping     Low-temperature NOx removal     Improved redox property     In situ XAFS analysis    

CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

《化学科学与工程前沿(英文)》 2016年 第10卷 第2期   页码 273-280 doi: 10.1007/s11705-016-1563-5

摘要: A series of Mn-promoted 15 wt-% Ni/Al O catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al O catalysts for CO methanation and the co-methanation of CO and CO in a fixed-bed reactor was investigated. The catalysts were characterized by N physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and high-resolution transmission electron microscopy. The presence of Mn increased the number of CO adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al O catalysts had improved CO methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO conversion was achieved with the 1.71Mn-Ni/Al O catalyst. The co-methanation tests on the 1.71Mn-Ni/Al O catalyst indicated that adding Mn markedly enhanced the CO methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.

关键词: Mn promotion     nickel catalysts     CO2 methanation     co-methanation of CO and CO2    

Effect of different acid anions on highly efficient Ce-based catalysts for selective catalytic reductionof NO with NH<sub>3sub>

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要: Three kinds of Ce-based catalysts (CePO4, CeVO4, Ce2(SO4)3) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH3. NH3-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO4 > CeVO4 > Ce2(SO4)3, which is in agreement with their abilities of NH3 adsorption capacities. The highest NO conversion rate of CePO4 could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO43–, VO43– and SO42– on NH3-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH3 temperature programmed desorption, H2 temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce4+, large NH3 adsorption capacity, high and early H2 consumptions, and suitable microstructures for gas adsorption. Finally, CePO4 and CeVO4 catalysts also exhibited relatively strong tolerance of SO2, and the upward trend about 8% was detected due to the sulfation enhancement by SO2 for Ce2(SO4)3.

关键词: CePO4     CeVO4     Ce2(SO4)3     selective catalytic reduction     NO removal    

H<sub>2sub> 对Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub> 催化剂NO<sub>xsub> 存储和还原机理的影响研究 Article

王攀, 裔静, 孙川, 罗鹏, 雷利利

《工程(英文)》 2019年 第5卷 第3期   页码 568-575 doi: 10.1016/j.eng.2019.02.005

摘要:

本研究采用浸渍法制备了Pt-Ba-Ce/γ-Al<sub>2sub>O<sub>3sub>催化剂,利用实验评价了H<sub>2sub> 对NSR(NO<sub>xsub> storage and reduction)催化剂存储和还原机理的影响,并采用综合表征技术研究了Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub结果表明,透射电子显微镜(TEM)显示X 射线衍射(XRD)光谱中观察到的PtO<sub>xsub>CeO<sub>2sub> 和BaCO<sub>3sub> 峰很好地分散在γ-Al<sub>2sub>O<sub>3sub> 上,X 射线光电子能谱(XPS)检测到Ce3+ 和Ce4+ 之间的差异,Ce3+ 和Ce4+ 促进了活性氧在催化剂上的迁移。适当增加H<sub>2sub>量加速了硝酸盐或亚硝酸盐的分解,有利于NO<sub>xsub> 存储-还原,并促进了下一循环NSR吸附位点的再生。

关键词: Pt–Ba–Ce/γ-Al<sub>2sub>O<sub>3sub> 催化剂,物理化学性质,NO<sub>xsub>存储和还原,NO<sub>xsub> 排放,H<sub>2sub> 还原剂    

Size and shape effects of MnFeO nanoparticles as catalysts for reductive degradation of dye pollutants

《环境科学与工程前沿(英文)》 2021年 第15卷 第5期   页码 108-171 doi: 10.1007/s11783-021-1396-4

摘要: The magnetic nanoparticles that are easy to recycle have tremendous potential as a suitable catalyst for environmental toxic dye pollutant degradation. Rationally engineering shapes and tailoring the size of nanocatalysts are regarded as an effective manner for enhancing performances. Herein, we successfully synthesized three kinds of MnFe2O4 NPs with distinctive sizes and shapes as catalysts for reductive degradation of methylene blue, rhodamine 6G, rhodamine B, and methylene orange. It was found that the catalytic activities were dependent on the size and shape of the MnFe2O4 NPs and highly related to the surface-to-volume ratio and atom arrangements. Besides, all these nanocatalysts exhibit selectivity to different organic dyes, which is beneficial for their practical application in dye pollutant treatment. Furthermore, the MnFe2O4 NPs could be readily recovered by a magnet and reused more than ten times without appreciable loss of activity. The size and shape effects of MnFe2O4 nanoparticles demonstrated in this work not only accelerate further understanding the nature of nanocatalysts but also contribute to the precise design of nanoparticles catalyst for pollutant degradation.

关键词: Dye degradation     MnFe2O4 nanoparticles     Size and shape-control    

Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

《环境科学与工程前沿(英文)》 2022年 第16卷 第10期 doi: 10.1007/s11684-022-1565-0

摘要:

● Cu addition enhances CH3OH oxidation and alleviates its inhibitory effect on SCR.

关键词: Copper modification     Sb-CeZr2Ox catalyst     NOx     Methanol     Simultaneous removal    

Complete oxidation of methane on CoO-SnO catalysts

Xingfu TANG , Jiming HAO , Junhua LI ,

《环境科学与工程前沿(英文)》 2009年 第3卷 第3期   页码 265-270 doi: 10.1007/s11783-009-0019-2

摘要: CoO-SnO hybrid oxides were prepared by the coprecipitation method and were used to oxidate methane (CH) in presence of oxygen. The CoO-SnO with a molar ratio of Co/(Co+Sn) at 0.75 exhibited the highest catalytic activity among all the CoO-SnO hybrid oxides. Experimental results showed that the catalysts were considerably stable in the CH combustion reaction, and were verified by X-ray photoelectron spectra (XPS). It was found that CoO was the active species, and SnO acted as a support or a promoting component in the CoO-SnO hybrid oxides. The surface area was not a major factor that affected catalytic activity. The hydrogen temperature-programmed reduction (H-TPR) results demonstrated that the interaction between cobalt and tin oxides accelerated the mobility of oxygen species of CoO-SnO, leading to higher catalytic activity.

关键词: Co3O4-SnO2     complete oxidation     methane (CH4)    

Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

《环境科学与工程前沿(英文)》 2013年 第7卷 第3期   页码 365-381 doi: 10.1007/s11783-013-0520-5

摘要: In this work, xylene removal from waste gas streams was investigated via catalytic oxidation over Pd/carbon-zeolite and Pd/carbon-CeO nanocatalysts. Activated carbon was obtained from pine cone chemically activated using ZnCl and modified by H PO . Natural zeolite of clinoptilolite was modified by acid treatment with HCl, while nano-ceria was synthesized via redox method. Mixed supports of carbon-zeolite and carbon-ceria were prepared and palladium was dispersed over them via impregnation method. The prepared samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Brunauer-Emmett-Teller surface area (BET), Fourier transform infrared spectroscopy (FTIR) and thermogravimetric (TG) techniques. Characterization of nanocatalysts revealed a good morphology with an average particle size in a nano range, and confirmed the formation of nano-ceria with an average crystallite size below 60 nm. BET analysis indicated a considerable surface area for catalysts (~1000 m ·g ). FTIR patterns demonstrated that the surface groups of synthesized catalysts are in good agreement with the patterns of materials applied in catalyst synthesis. The performance of catalysts was assessed in a low-pressure catalytic oxidation pilot in the temperature range of 100°C–250°C. According to the reaction data, the synthesized catalysts have been shown to be so advantageous in the removal of volatile organic compounds (VOCs), representing high catalytic performance of 98% for the abatement of xylene at 250°C. Furthermore, a reaction network is proposed for catalytic oxidation of xylene over nanocatalysts.

关键词: Pd/carbon-CeO2     Pd/carbon-zeolite     pine cone     ZnCl2     catalytic oxidation     xylene    

标题 作者 时间 类型 操作

Characterization and catalytic activity of soft-templated NiO-CeO

Luciano Atzori, Maria Giorgia Cutrufello, Daniela Meloni, Barbara Onida, Delia Gazzoli, Andrea Ardu, Roberto Monaci, Maria Franca Sini, Elisabetta Rombi

期刊论文

Catalytic combustion of methane over a highly active and stable NiO/CeO

Xiuhui Huang, Junfeng Li, Jun Wang, Zeqiu Li, Jiayin Xu

期刊论文

Characterization and performance of V

Caiting LI, Qun LI, Pei LU, Huafei CUI, Guangming ZENG

期刊论文

Al<sub>2sub>O<sub>3sub> and CeO<sub>2sub>-promoted MgO sorbents for CO<sub>2sub> capture at moderate

Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song

期刊论文

Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

期刊论文

Interface engineering for enhancing electrocatalytic oxygen evolution reaction of CoS/CeO heterostructures

期刊论文

Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

期刊论文

CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction

期刊论文

CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文

Effect of different acid anions on highly efficient Ce-based catalysts for selective catalytic reductionof NO with NH<sub>3sub>

期刊论文

H<sub>2sub> 对Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub> 催化剂NO<sub>xsub> 存储和还原机理的影响研究

王攀, 裔静, 孙川, 罗鹏, 雷利利

期刊论文

Size and shape effects of MnFeO nanoparticles as catalysts for reductive degradation of dye pollutants

期刊论文

Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

期刊论文

Complete oxidation of methane on CoO-SnO catalysts

Xingfu TANG , Jiming HAO , Junhua LI ,

期刊论文

Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

期刊论文