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An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

《化学科学与工程前沿（英文）》 2022年第16卷第6期页码 950-962 doi: 10.1007/s11705-022-2162-2

摘要： A series of Cu–Ce–Zr catalysts with different Ce contents are applied to the hydrogenation of CO₂ to CO/CH₃OH products. The Cu–Ce–Zr catalyst with 2 wt% Ce loading shows higher CO selectivity (S_CO = 0.0%–87.8%) from 200–300 °C, while the Cu–Ce–Zr catalyst with 8 wt% Ce loading presents higher CO₂ conversion (

X C O 2

= 5.4%–15.6%) and CH₃OH selectivity (

S C H 3 O H

= 97.8%–40.6%). The number of hydroxyl groups and solid solution nature play a significant role in changing the reaction pathway. The solid solution enhances the CO₂ adsorption ability. At the CO₂ adsorption step, a larger number of hydroxyl groups over the Cu–Ce–Zr catalyst with 8 wt% Ce loading leads to the production of H-containing adsorption species. At the CO₂ hydrogenation step, a larger number of hydroxyl groups assists in encouraging the further hydrogenation of intermediate species to CH₃OH and improving the hydrogenation rate. Hence, the Cu–Ce–Zr catalyst with 8 wt% Ce loading favors CH₃OH selectivity and CO₂ activation, while CO is preferred on the Cu–Ce–Zr catalyst with 2 wt% Ce loading, a smaller number of hydroxyl groups and a solid solution nature. Additionally, high-pressure in situ diffuse reflectance infrared Fourier transform spectroscopy shows that CO is produced from formate decomposition and that both monodentate formate and bidentate formate are active intermediate species of CO₂ hydrogenation to CH₃OH.

关键词： CO₂ hydrogenation Cu–Ce–Zr hydroxyls CO/CH₃OH selectivity

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PM-support interfacial effect and oxygen mobility in Pt, Pd or Rh-loaded (Ce,Zr,La)O catalysts

《环境科学与工程前沿（英文）》 2021年第15卷第4期 doi: 10.1007/s11783-020-1369-z

摘要：

• Pt/CZL exhibits the optimum catalytic performance for HC and NO_x elimination.

关键词： Precious metal-loaded (Ce Zr La)O₂ catalysts Oxygen mobility Catalytic performance

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Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide oxidation

《化学科学与工程前沿（英文）》 2021年第15卷第6期页码 1524-1536 doi: 10.1007/s11705-021-2106-2

摘要： The effects of Zr doping on the existence of Cu and the catalytic performance of Ce_0.7−_xZr_xCu_0.3O₂ for CO oxidation were investigated. The characterization results showed that all samples have a cubic structure, and a small amount of Zr doping facilitates Cu²⁺ ions entering the CeO₂ lattice, but excessive Zr doping leads to the formation of surface CuO crystals again. Thus, the number of oxygen vacancies caused by the Cu²⁺ entering the lattice (e.g., Cu²⁺–□–Ce⁴⁺; □: oxygen vacancy), and the amount of reducible copper species caused by CuO crystals, varies with the Zr doping. Catalytic CO oxidation tests indicated that the oxygen vacancy and the reducible copper species were the adsorption and activation sites of O₂ and CO, respectively, and the cooperative effects between them accounted for the high CO oxidation activity. Thus, the samples x = 0.1 and 0.3, which possessed the most oxygen vacancy or reducible copper species, showed the best activity for CO oxidation, with full CO conversion obtained at 110 °C. The catalyst is also stable and has good resistance to water during the reaction.

关键词： Ce–Zr–Cu–O CO oxidation reducible copper species oxygen vacancy cooperative effect

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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-CeZr₂O_x catalyst NO_x Methanol Simultaneous removal

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Microwave-assisted catalytic oxidation of gaseous toluene with a Cu-Mn-Ce/cordierite honeycomb catalyst

Longli Bo, Shaoyuan Sun

《化学科学与工程前沿（英文）》 2019年第13卷第2期页码 385-392 doi: 10.1007/s11705-018-1738-3

摘要： A novel Cu-Mn-Ce/cordierite honeycomb catalyst was prepared by an incipient wetness method and the catalyst was characterized. The active ingredients were present as various spinel species of Cu, Mn and Ce oxides with different valences and they were unevenly dispersed over the surface of the catalyst. The catalytic oxidation of gaseous toluene was primarily investigated using a fixed bed reactor under microwave heating in the continuous flow mode. Under the optimal conditions of 6.7 wt-% loading of the active component, a bed temperature of 200°C, a flow rate of 0.12 m ·h and an initial concentration of toluene of 1000 mg·m , the removal and mineralization efficiencies of toluene were 98% and 70%, respectively. Thus the use of the microwave effectively improved the oxidation of toluene and this is attributed to dipole polarization and hotspot effects. After four consecutive cycles (a total of 1980 min), the Cu-Mn-Ce/cordierite catalyst still exhibited excellent catalytic activity and structural stability, and the toluene removal was higher than 90%. This work demonstrates the possibility of treating volatile organic compounds in exhaust gases by microwave-assisted catalytic oxidation.

关键词： microwave catalytic oxidation toluene Cu-Mn-Ce/cordierite mineralization

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Promoting effect of Zr on the catalytic combustion of methane over Pd/γ-Al

Hongbo NA,Tianle ZHU,Zhiming LIU,Yifei SUN

《环境科学与工程前沿（英文）》 2014年第8卷第5期页码 659-665 doi: 10.1007/s11783-013-0613-1

摘要： The effect of Zr on the catalytic performance of Pd/γ-Al O for the methane combustion was investigated. The results show that the addition of Zr can improve the activity and stability of Pd/γ-Al O catalyst, which, based on the catalyst characterization (N adsorption, XRD, CO-Chemisorption, XPS, CH -TPR and O -TPO), is ascribed to the interaction between Pd and Zr. The active phase of methane combustion over supported palladium catalyst is the Pd /Pd mixture. Zr addition inhibits Pd aggregation and enhances the redox properties of active phase Pd / Pd . H reduction could effectively reduce the oxidation degree of Pd species and regenerate the active sites (Pd / Pd ).

关键词： Pd-Zr/Al₂O₃ methane catalytic combustion catalyst regeneration

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Promotion of transition metal oxides on the NH

Weiman Li, Haidi Liu, Yunfa Chen

《环境科学与工程前沿（英文）》 2017年第11卷第2期 doi: 10.1007/s11783-017-0914-x

摘要： Manganese and chromium oxides promote the NH -SCR activity of Zr-Ce mixed oxide. Cr-Zr-Ce mixed oxide exhibited>80% NO conversion at a wide temperature window. More acid sites and higher reducibility may responsible for the high SCR ability. Chromium oxide and manganese oxide promoted ZrO -CeO catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NO with NH . A series of characterization including X-ray diffraction (XRD), high-resolution transmission electron microscope (HR-TEM), Brunauer–Emmett–Teller (BET) surface area analysis, H temperature-programmed reduction (H -TPR), and X-ray photoelectron spectroscopy (XPS) were used to evaluate the influence of the physicochemical properties on NH -SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO -CeO binary oxide for the low temperature NH -SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO and H O. Cr-Zr-Ce mixed oxide exhibited>80% NO conversion at a wide temperature window of 100°C–300°C. DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence of Cr . The present mixed oxide can be a candidate for the low temperature abatement of NO .

关键词： NH₃-selective catalytic reduction NO_x Low temperature Cr-Zr-Ce

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Zr₆₆Al₉Cu₁₆Ni₉块体非晶合金制备工艺研究

阮许平,阮宏伟

《中国工程科学》 2004年第6卷第5期页码 76-78

摘要：

运用真空电弧炉熔炼合金制备试样，采用三种不同的方法对金属熔体进行处理，试样的X射线衍射晶化相分析结果表明，B₂O₃和Na₂SiO₃的混合物与所选组分的熔体发生了反应，不适合作Zr基合金的包裹物；组分为CaF₂(45%)，AlF₃(50%)，CaO(5%)以及微量的TiO₂的氟盐，由于该净化剂与所选的组分发生了反应，不适合Zr基合金的净化；设备的高真空度、原材料成分的高纯度是促进合金形成非晶态的重要因素。

关键词：块体非晶合金制备工艺玻璃熔盐真空度

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Preparation of Cu/ZnO/Al

Hui FAN, Huayan ZHENG, Zhong LI

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 445-451 doi: 10.1007/s11705-010-0521-x

摘要： Cu/ZnO/Al O catalysts with Cu/Zn/Al ratios of 6/3/1 were precipitated and aged by conventional and microwave heating methods and tested in the slurry phase reactor for methanol synthesis. The effect of technological condition of precipitation and aging process under microwave irradiation on the catalytic performance was investigated to optimize the preparing condition of Cu/ZnO/Al O catalyst. The results showed that the microwave irradiation during precipitation process could improve the activity of the catalyst, but had little effect on the stability. While the microwave irradiation during aging process has a great benefit to both the activity and stability of the catalyst, the catalyst aged at 80°C for 1 h under microwave irradiation possessed higher methanol space time yield (STY) and more stable catalytic activity. The activity and stability of the catalyst was further enhanced when microwave irradiation was used in both precipitation and aging processes; the optimized condition for the catalyst precursor preparation was precipitation at 60°C and aging at 80°C under microwave irradiation.

关键词： microwave irradiation precipitation temperature aging temperature methanol synthesis Cu/ZnO/Al₂O₃ catalyst

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H₂ 对Pt-Ba-Ce /γ-Al₂O₃ 催化剂NO_x 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-Al₂O₃催化剂，利用实验评价了H₂ 对NSR（NO_x 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-Al₂O_{3_x、CeO₂ 和BaCO₃ 峰很好地分散在γ-Al₂O₃ 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。}

关键词： Pt–Ba–Ce/γ-Al₂O₃ 催化剂，物理化学性质，NO_x存储和还原，NO_x 排放

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Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

《环境科学与工程前沿（英文）》 2016年第10卷第6期 doi: 10.1007/s11783-016-0872-8

摘要： ? The Cu–Ni/γ-Al O catalyst was prepared to study HCN hydrolysis ? On catalyst calcined at 400°C, the HCN removal efficiency reaches a maximum. ? HCN removal is the highest at 480 min at a H O/HCN volume ratio of 150 ? The presence of CO facilitates HCN hydrolysis and increases NH production. ? O increases the HCN removal and NO production but decreases NH production GRAPHIC ABSTRACT To decompose efficiently hydrogen cyanide (HCN) in exhaust gas, g-Al O -supported bimetallic-based Cu–Ni catalyst was prepared by incipient-wetness impregnation method. The effects of the calcination temperature, H O/HCN volume ratio, reaction temperature, and the presence of CO or O on the HCN removal efficiency on the Cu–Ni/g-Al O catalyst were investigated. To examine further the efficiency of HCN hydrolysis, degradation products were analyzed. The results indicate that the HCN removal efficiency increases and then decreases with increasing calcination temperature and H O/HCN volume ratio. On catalyst calcined at 400°C, the efficiency reaches a maximum close to 99% at 480 min at a H O/HCN volume ratio of 150. The HCN removal efficiency increases with increasing reaction temperature within the range of 100°C–500°C and reaches a maximum at 500°C. This trend may be attributed to the endothermicity of HCN hydrolysis; increasing the temperature favors HCN hydrolysis. However, the removal efficiencies increases very few at 500°C compared with that at 400°C. To conserve energy in industrial operations, 400°C is deemed as the optimal reaction temperature. The presence of CO facilitates HCN hydrolysis andincreases NH production. O substantially increases the HCN removal efficiency and NO production but decreases NH production.

关键词： Hydrogen cyanide Cu–Ni/g-Al₂O₃ Catalytic hydrolysis

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Preparation of ceria-zirconia solid solution with enhanced oxygen storage capacity and redox performance

Lijing MENG, Licheng LIU, Xuehong ZI, Hongxing DAI, Hong HE, Zhen ZHAO, Xinping WANG,

《环境科学与工程前沿（英文）》 2010年第4卷第2期页码 164-171 doi: 10.1007/s11783-010-0019-2

摘要： A new method called ultrasonic-assisted membrane reaction (UAMR) was reported for the fabrication of ceria-zirconia solid solution. A series of ceria-zirconia solid solutions with different Ce/Zr molar ratios were prepared by the UAMR method and characterized by X-ray diffraction (XRD), N adsorption, hydrogen temperature-programmed reduction (H-TPR), scanning electron microscope (SEM), and transmission electron microscopy (TEM) techniques. The UAMR method proved to be superior, especially when the Ce/Zr molar ratio was lower than 1, in fabricating ceria-zirconia solid solutions with large BET surface area, high oxygen storage capacity (OSC), and low reduction temperature.

关键词： membrane reaction ceria-zirconia Ce/Zr molar ratio solid solution hydrogen temperature-programmed reduction (H2-TPR)

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FeNi/Al-Ce-O催化剂上的乙烷干重整——组成诱导的金属-载体强相互作用 Article

张涛, 刘志成, 叶迎春, 王毓, 杨贺勤, 高焕新, 杨为民

《工程（英文）》 2022年第18卷第11期页码 173-185 doi: 10.1016/j.eng.2021.11.027

摘要：氧化铈中Al的引入增强了金属与载体之间的相互作用，显著影响了Al-Ce-O载体表面FeNi活性组分的分散度，从而提升了FeNi/Al-Ce-O催化剂的乙烷干重整反应性能。其中，Al含量为50%的FeNi/Ce-Al_0.5催化剂在873 K下具有最好的乙烷干重整反应性能。结合原位傅里叶变换红外光谱（FTIR）分析观察到，Al的引入不仅增加了表面Ce³⁺和氧空位的含量，同时也促进了表面活性组分的分散，提升了负载FeNi催化剂的乙烷干重整性能。

关键词：乙烷干重整金属-载体强相互作用二氧化碳氧化铈氧空位反应机理

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Modeling of Ce(IV) transport through a dispersion flat combined liquid membrane with carrier P507

Liang PEI,Liming WANG,Zhanying MA

《环境科学与工程前沿（英文）》 2014年第8卷第4期页码 503-509 doi: 10.1007/s11783-013-0540-1

摘要： A mathematical model for the transport of Ce(IV) from hydrochloric acid solutions through dispersion flat combined liquid membrane (DFCLM) with contain 2-ethyl hexyl phosphonic acid-mono-2-ethyl hexyl ester (P507) as the carrier, dissolved in kerosene as the membrane solution have been studied. This process of facilitated transport, based on membrane technology, is a variation on the conventional technique of solvent extraction and may be described mathematically using Fick’s second law. The equations for transport velocity are derived considering the diffusion of P507 and its metallic complexes through the liquid membrane. In this work, the system is considered to be in a transient state, and chemical reaction between Ce(IV) and the carrier to take place only at the solvent–aqueous interfaces. Model concentration profiles are obtained for the Ce(IV), from which extraction velocities are predicted. The experimental and simulated Ce(IV) extractions showed similar tendencies for a high Ce(IV) concentration and acidity case.The model results indicate that high initial Ce(IV) concentrations and acidity both have detrimental effects on Ce(IV) extraction and stripping. The diffusion coefficient of Ce(IV) in the membrane and the thickness of diffusion layer between feed phase and membrane phase are obtained and the values are 6.31 × 10 m ·s and 31.2 μm, respectively. The results are in good agreement with experimental results.

关键词： Dispersion flat combined liquid membrane (DFCLM) dispersion phase feed phase 2-ethyl hexyl phosphonic acid-mono-2-ethyl hexyl ester Ce (IV)

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Research progress of defect-engineered UiO-66(Zr) MOFs for photocatalytic hydrogen production

《能源前沿（英文）》 2021年第15卷第3期页码 656-666 doi: 10.1007/s11708-021-0765-9

摘要： In recent years, defect-engineered Zr-based UiO-66 metal-organic frameworks (UiO-66(Zr) metal-organic frameworks (MOFs)) have shown huge advantages in catalytic, functional materials, adsorption, and other fields due to their large surface areas, well-ordered porous structures, and flexible tailorability. It is extremely challenging to introduce defect sites in the synthesis of MOFs to regulate the physicochemical properties of materials such as (energy band structure, pore structure, etc.) to obtain an excellent performance. This paper reviews the recent research results of synthesis methods, characterization technologies, and application fields of defect-engineered UiO-66(Zr) MOFs materials in order to provide new insights to synthesize high-performance UiO-66(Zr) MOFs materials and promote the development of UiO-66(Zr) in various fields.

关键词： defect engineering metal-organic frameworks UiO-66 photocatalysis

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标题作者时间类型操作

An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

期刊论文

PM-support interfacial effect and oxygen mobility in Pt, Pd or Rh-loaded (Ce,Zr,La)O catalysts

期刊论文

Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide oxidation

期刊论文

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

期刊论文

Microwave-assisted catalytic oxidation of gaseous toluene with a Cu-Mn-Ce/cordierite honeycomb catalyst

Longli Bo, Shaoyuan Sun

期刊论文

Promoting effect of Zr on the catalytic combustion of methane over Pd/γ-Al

Hongbo NA,Tianle ZHU,Zhiming LIU,Yifei SUN

期刊论文

Promotion of transition metal oxides on the NH

Weiman Li, Haidi Liu, Yunfa Chen

期刊论文

Zr₆₆Al₉Cu₁₆Ni₉块体非晶合金制备工艺研究

阮许平,阮宏伟

期刊论文

Preparation of Cu/ZnO/Al

Hui FAN, Huayan ZHENG, Zhong LI

期刊论文

H₂ 对Pt-Ba-Ce /γ-Al₂O₃ 催化剂NO_x 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

Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

期刊论文

Preparation of ceria-zirconia solid solution with enhanced oxygen storage capacity and redox performance

Lijing MENG, Licheng LIU, Xuehong ZI, Hongxing DAI, Hong HE, Zhen ZHAO, Xinping WANG,

期刊论文

FeNi/Al-Ce-O催化剂上的乙烷干重整——组成诱导的金属-载体强相互作用

张涛, 刘志成, 叶迎春, 王毓, 杨贺勤, 高焕新, 杨为民

期刊论文

Modeling of Ce(IV) transport through a dispersion flat combined liquid membrane with carrier P507

Liang PEI,Liming WANG,Zhanying MA

期刊论文

Research progress of defect-engineered UiO-66(Zr) MOFs for photocatalytic hydrogen production

期刊论文

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