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Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selectivecatalytic oxidation of cyclohexane

《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    

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Co-present Pb(II) accelerates the oxidation of organic contaminants by permanganate: Role of Pb(III)

《环境科学与工程前沿（英文）》 2022年 第16卷 第8期 doi: 10.1007/s11783-022-1530-y

摘要：

• Simultaneous removal of organic contaminants and Pb(II) was achieved by Mn(VII).

关键词： Permanganate     Pb(II) oxidation     MnO2     pH effect    

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NO oxidation over Co-La catalysts and NO

Tiejun Zhang,Jian Li,Hong He,Qianqian Song,Quanming Liang

《环境科学与工程前沿（英文）》 2017年 第11卷 第2期 doi: 10.1007/s11783-017-0906-x

摘要： The Co-La catalyst (pH= 1) exhibited maximum NO conversion of 43% at 180°C. Acid modified catalyst enhanced the resistance to SO . The formed sulfates may block the pore structure of the catalyst. The NO conversion of compact SCR was 91% at 180°C at the highest space velocity. A series of Co-La catalysts were prepared using the wet impregnation method and the synthesis of catalysts were modified by controlling pH with the addition of ammonium hydroxide or oxalic solution. All the catalysts were systematically investigated for NO oxidation and SO resistance in a fixed bed reactor and were characterized by Brunanuer–Emmett–Teller (BET) method, Fourier Transform infrared spectroscopy (FTIR), X–ray diffraction (XRD), Thermogravimetric (TG) and Ion Chromatography (IC). Among the catalysts, the one synthesized at pH= 1 exhibited the maximum NO conversion of 43% at 180°C. The activity of the catalyst was significantly suppressed by the existence of SO (300 ppm) at 220°C. Deactivation may have been associated with the generation of cobalt sulfate, and the SO adsorption quantity of the catalyst might also have effected sulfur resistance. In the case of the compact selective catalytic reduction (SCR), the activity increased from 74% to 91% at the highest gas hourly space velocity (GHSV) of 300000 h when the NO catalyst maintained the highest activity, in excess of 50% more than that of the standard SCR.

关键词： NO catalytic oxidation     pH effect     Low temperature     Sulfur dioxide     High space velocity     SCR    

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Low-temperature CO oxidation over Au-doped 13X-type zeolite catalysts: preparation and catalytic activity

Qing YE, Donghui LI, Jun ZHAO, Jiansheng ZHAO, Tianfang KANG, Shuiyuan CHENG

《环境科学与工程前沿（英文）》 2011年 第5卷 第4期   页码 497-504 doi: 10.1007/s11783-011-0256-z

摘要： Au-supported 13X-type zeolite (Au/13X) was synthesized using a common deposition–precipitation (DP) method with a solution of sodium carbonate as a precipitate agent. Further testing was conducted to test for catalytic oxidation of CO. A study was conducted on the effects of different preparation conditions (i.e., chloroauric acid concentration, solution temperature, pH of solution, and calcinations temperature) on Au/13X for CO oxidation. In respect to the catalytic activity, the relationship between different the preparation conditions and gold particles in 13X zeolite was analyzed using X-ray diffraction, TEM and XPS. The activity of Au/13X catalysts in CO oxidation was dependent on the chloroauric acid concentration. From XRD results, a higher chloroauric acid concentration induced larger gold nanoparticles, which resulted in lower catalytic activity. Results revealed that higher temperatures induced higher Au loading, homogeneous deposit, and smaller gold clusters on the support of 13X, resulting in higher CO activity. Furthermore, a pH of 5 or 6 generated greater amounts of Au loading and smaller Au particles on 13X than at a pH of 8 or 9. This may be a result of an effective exchange between and Au(OH) Cl on specific surface sites of zeolite under the pH’s 5 and 6. The sample calcined at 300°C showed the highest activity, which may be due to the sample’s calcined at 200°C inability to decompose completely to metallic gold while the sample calcined at 400°C had larger particles of gold deposited on the support. It can be concluded from this study that Au/13X prepared from a gold solution with an initial chloroauric acid solution concentration of 1.5 × 10 mol·L gold solution pH of 6, solution temperature of around 90°C, and a calcination temperature of 300°C provides optimum catalytic activity for CO oxidation.

关键词： 13X-type zeolite     CO oxidation     gold solution     pH     calcination temperature    

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Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1139-1148 doi: 10.1007/s11705-021-2111-5

摘要： The solubility of Pd(NO3)2 in water is moderate whereas it is completely soluble in diluted HNO3 solution. Pd/MIL-101(Cr) and Pd/MIL-101-NH2(Cr) were synthesized by aqueous solution of Pd(NO3)2 and Pd(NO3)2 solution in dilute HNO3 and used for CO oxidation reaction. The catalysts synthesized with Pd(NO3)2 solution in dilute HNO3 showed lower activity. The aqueous solution of Pd(NO3)2 was used for synthesis of mono-metal Ni, Pd and bimetallic PdNi nanoparticles with various molar ratios supported on MOF. Pd70Ni30/MIL-101(Cr) catalyst showed higher activity than monometallic counterparts and Pd+ Ni physical mixture due to the strong synergistic effect of PdNi nanoparticles, high distribution of PdNi nanoparticles, and lower dissociation and desorption barriers. Comparison of the catalysts synthesized by MIL-101(Cr) and MIL-101-NH2(Cr) as the supports of metals showed that Pd/MIL-101-NH2(Cr) outperforms Pd/MIL-101-(Cr) because of the higher electron density of Pd resulting from the electron donor ability of the NH2 functional group. However, the same activities were observed for Pd70Ni30/MIL-101(Cr) and Pd70Ni30/MIL-101-NH2(Cr), which is due to a less uniform distribution of Pd nanoparticles in Pd70Ni30/MIL-101-NH2(Cr) originated from amorphization of MIL-101-NH2(Cr) structure during the reduction process. In contrast, Pd70Ni30/MIL-101(Cr) revealed the stable structure and activity during reduction and CO oxidation for a long time.

关键词： CO oxidation     heterogeneous catalysis     metal-organic framework     NH2 functional group     PdNi    

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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)    

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“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 207-212 doi: 10.1007/s11705-009-0240-3

摘要： With the rapid expansion of the global motor vehicle population, the transportation sector has taken up a growing proportion among all the carbon dioxide emission-related sectors. To contribute to solutions of the carbon dioxide-oriented problem in transportation, this paper proposes the “ALL FREE” concept that applies partial oxidation process instead of the conventional complete oxidation to vehicle engines. In such an engine, the fuels are partially oxidized into corresponding chemical products, which, as a result, enable the process to be theoretically free of CO, while the heat output of the partial oxidation could drive the vehicle. On the other hand, the resulting products are of great value, which could decrease or even counteract the cost of fuels in transportation. In this paper, the thermodynamic and kinetic data (e.g., the heat output and heat release rate) of five selected partial oxidation reactions were calculated at length to demonstrate and exemplify the theoretical feasibility of the “ALL FREE” concept. It turned out that the partial oxidation of -butane to maleic anhydride has the most potential to meet the basic requirements of this concept. To sum up, this design concept is of significant application potential for the reduction of CO emissions in the transportation industry, although there remain many technical challenges.

关键词： oxidation process     CO     complete oxidation     ALL FREE     -butane    

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Catalytic oxidation of CO over Pt/Fe

Zihao Li, Yang Geng, Lei Ma, Xiaoyin Chen, Junhua Li, Huazhen Chang, Johannes W. Schwank

《环境科学与工程前沿（英文）》 2020年 第14卷 第4期 doi: 10.1007/s11783-020-1244-y

摘要： Abstract • Strong metal-support interaction exists on Pt/Fe3O4 catalysts. • Pt metal particles facilitate the formation of oxygen vacancies on Fe3O4. • Fe3O4 supports enhance the strength of CO adsorption on Pt metal particles. The self-inhibition behavior due to CO poisoning on Pt metal particles strongly impairs the performance of CO oxidation. It is an effective method to use reducible metal oxides for supporting Pt metal particles to avoid self-inhibition and to improve catalytic performance. In this work, we used in situ reductions of chloroplatinic acid on commercial Fe3O4 powder to prepare heterogeneous-structured Pt/Fe3O4 catalysts in the solution of ethylene glycol. The heterogeneous Pt/Fe3O4 catalysts achieved a better catalytic performance of CO oxidation compared with the Fe3O4 powder. The temperatures of 50% and 90% CO conversion were achieved above 260°C and 290°C at Pt/Fe3O4, respectively. However, they are accomplished on Fe3O4 at temperatures higher than 310°C. XRD, XPS, and H2-TPR results confirmed that the metallic Pt atoms have a strong synergistic interaction with the Fe3O4 supports. TGA results and transient DRIFTS results proved that the Pt metal particles facilitate the release of lattice oxygen and the formation of oxygen vacancies on Fe3O4. The combined results of O2-TPD and DRIFTS indicated that the activation step of oxygen molecules at surface oxygen vacancies could potentially be the rate-determining step of the catalytic CO oxidation at Pt/Fe3O4 catalysts. The reaction pathway involves a Pt-assisted Mars-van Krevelen (MvK) mechanism.

关键词： Strong metal-support interaction (SMSI)     Surface oxygen vacancy     Lattice oxygen     Magnetite     Platinum metals    

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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 Ce0.7−xZrxCu0.3O2 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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Mass Transfer-Promoted Fe2+/Fe3+ Circulation Steered by 3D Flow-Through Co-Catalyst System Toward SustainableAdvanced Oxidation Processes

Weiyang Lv,Hao Li,Jinhui Wang,Lixin Wang,Zenglong Wu,Yuge Wang,Wenkai Song,Wenkai Cheng,Yuyuan Yao,

《工程（英文）》 doi: 10.1016/j.eng.2023.06.010

摘要： Realizing fast and continuous generation of reactive oxygen species (ROSs) via iron-based advanced oxidation processes (AOPs) is significant in the environmental and biological fields. However, current AOPs assisted by co-catalysts still suffer from the poor mass/electron transfer and non-durable promotion effect, giving rise to the sluggish Fe2+/Fe3+ cycle and low dynamic concentration of Fe2+ for ROS production. Herein, we present a three-dimensional (3D) macroscale co-catalyst functionalized with MoS2 to achieve ultra-efficient Fe2+ regeneration (equilibrium Fe2+ ratio of 82.4%) and remarkable stability (more than 20 cycles) via a circulating flow-through process. Unlike the conventional batch-type reactor, experiments and computational fluid dynamics simulations demonstrate that the optimal utilization of the 3D active area under the flow-through mode, initiated by the convection-enhanced mass/charge transfer for Fe2+ reduction and then strengthened by MoS2-induced flow rotation for sufficient reactant mixing, is crucial for oxidant activation and subsequent ROS generation. Strikingly, the flow-through co-catalytic system with superwetting capabilities can even tackle the intricate oily wastewater stabilized by different surfactants without the loss of pollutant degradation efficiency. Our findings highlight an innovative co-catalyst system design to expand the applicability of AOPs based technology, especially in large-scale complex wastewater treatment.

关键词： Advanced oxidation processes     3D co-catalyst     Flow-through mode     Enhanced mass transfer     Complex wastewater treatment    

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Excellent performance of Cu-Mn/Ti-sepiolite catalysts for low-temperature CO oxidation

Yong Song,Lisha Liu,Zhidan Fu,Qing Ye,Shuiyuan Cheng,Tianfang Kang,Hongxing Dai

《环境科学与工程前沿（英文）》 2017年 第11卷 第2期 doi: 10.1007/s11783-017-0908-8

摘要： Sepiolite is clay mineral with a 2:1 layered structure. Ti-pillars have an impact on physicochemical property of the sample. 30Mn5Cu/Ti-Sep shows excellent catalytic activity for the oxidation of CO. The interaction, reducibility, and oxygen mobility govern the activity. The Ti-modified sepiolite (Ti-Sep)-supported Mn-Cu mixed oxide ( Mn5Cu/Ti-Sep) catalysts were synthesized using the co-precipitation method. The materials were characterized by the X-ray diffraction scanning electron microscope, N adsorption-desorption, H -TPR, O -TPD, and XPS techniques, and their catalytic activities for CO oxidation were evaluated. It was found that the catalytic activities of Mn5Cu/Ti-Sep were higher than those of 5Cu/Ti-Sep and 30Mn/Ti-Sep, and the Mn/Cu molar ratio had a distinct influence on catalytic activity of the sample. Among the Mn5Cu/Ti-Sep samples, the 30Mn5Cu/Ti-Sep catalyst showed the best activity (which also outperformed the 30Mn5Cu/Sep catalyst), giving the highest reaction rate of 0.875 × 10 mmol·g ·s and the lowest and of 56°C and 86°C, respectively. Moreover, the 30Mn5Cu/Ti-Sep possessed the best low-temperature reducibility, the lowest O desorption temperature, and the highest surface Mn /Mn atomic ratio. It is concluded that factors, such as the strong interaction between the copper or manganese oxides and the Ti-Sep support, good low-temperature reducibility, and good mobility of chemisorbed oxygen species, were responsible for the excellent catalytic activity of 30Mn5Cu/Ti-Sep.

关键词： Ti-modified sepiolite     Supported Mn-Cu mixed oxide     Low-temperature reducibility     Strong metal-support interaction     CO oxidation    

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Effects of preparation methods on the activity of CuO/CeO

Huanhuan Shang, Xiaoman Zhang, Jing Xu, Yifan Han

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 603-612 doi: 10.1007/s11705-017-1661-z

摘要： CO oxidation has been investigated on three CuO/CeO catalysts prepared by impregnation, co-precipitation and mechanical mixing. The origin of active sites was explored by the multiple techniques. The catalyst prepared by impregnation has more highly dispersed CuO and stronger interactions between CuO and CeO to promote the reduction of CuO to Cu species at the Cu-Ce interface, leading to its highest catalytic activity. For the catalyst prepared by co-precipitation, solid solution structures observed in Raman spectra suppress the formation of the Cu-Ce interface, where the adsorbed CO will react with active lattice oxygen to form CO , and thus it displays a lower catalytic performance. No Cu-Ce interface exists in the catalyst prepared by the mechanical mixing method due to the separate phases of CuO and CeO , resulting in its lowest activity among the three catalysts.

关键词： CuO/CeO2     CO oxidation     interfaces     structure-performance relationship     active sites    

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Microbial responses to combined oxidation and catalysis treatment of 1,4-dioxane and co-contaminants

Yu Miao, Nicholas W. Johnson, Kimberly Heck, Sujin Guo, Camilah D. Powell, Thien Phan, Phillip B. Gedalanga, David T. Adamson, Charles J. Newell, Michael S. Wong, Shaily Mahendra

《环境科学与工程前沿（英文）》 2018年 第12卷 第5期 doi: 10.1007/s11783-018-1071-6

摘要：

Groundwater microbial community was altered after catalysis and chemical oxidation.

The coupled treatment train removed 90% 1,4-dioxane regardless of co-contaminants.

Dynamics of microbial populations varied along with different treatment stages.

Many microbial taxa exhibited resilience against oxidative and catalytic treatments.

Metagenomic analysis will be valuable for long-term management of polluted sites.

关键词： Coupled treatments     Chlorinated solvents     Diethylene ether     Biological diversity     Microbial populations     Biomarkers    

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使用傅里叶变换红外成像进行高通量筛选 Article

Erdem Sasmaz, Kathleen Mingle, Jochen Lauterbach

《工程（英文）》 2015年 第1卷 第2期   页码 234-242 doi: 10.15302/J-ENG-2015040

摘要：

组合库的有效平行筛选是高通量(HT) 多相催化工作流中最具挑战性的难题之一。目前，已有包括各种光学、质谱分析以及气相色谱技术在内的大量方法用于高通量催化剂研究。在这些技术中，快速扫描傅里叶变换红外(FTIR) 成像是最快、最通用的筛选技术。本文介绍了16 通道高通量反应器的新设计，并给出了其准确性和重复性试验结果。该系统的性能，通过在不同的还原剂–还原剂摩尔比、表面活性剂类型、金属和表面活性剂浓度、合成温度和升温速率下合成的商用Pd/Al2O3和氧化钴纳米粒子的一氧化碳氧化反应进行评估。

关键词： 高通量     傅里叶变换红外成像     筛选     氧化钴     一氧化碳氧化    

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Phenolic compounds removal by wet air oxidation based processes

Linbi Zhou, Hongbin Cao, Claude Descorme, Yongbing Xie

《环境科学与工程前沿（英文）》 2018年 第12卷 第1期 doi: 10.1007/s11783-017-0970-2

摘要： Wet air oxidation (WAO) and catalytic wet air oxidation (CWAO) are efficient processes to degrade organic pollutants in water. In this paper, we especially reviewed the WAO and CWAO processes for phenolic compounds degradation. It provides a comprehensive introduction to the CWAO processes that could be beneficial to the scientists entering this field of research. The influence of different reaction parameters, such as temperature, oxygen pressure, pH, stirring speed are analyzed in detail; Homogenous catalysts and heterogeneous catalysts including carbon materials, transitional metal oxides and noble metals are extensively discussed, among which Cu based catalysts and Ru catalysts were shown to be the most active. Three different kinds of the reactor implemented for the CWAO (autoclave, packed bed and membrane reactors) are illustrated and compared. To enhance the degradation efficiency and reduce the cost of the CWAO process, biological degradation can be combined to develop an integrated technology.

关键词： Wet air oxidation     Catalytic wet air oxidation     Phenolic compounds     Heterogeneous catalysts     Mechanism    

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标题 作者 时间 类型 操作

Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selectivecatalytic oxidation of cyclohexane

期刊论文

Co-present Pb(II) accelerates the oxidation of organic contaminants by permanganate: Role of Pb(III)

期刊论文

NO oxidation over Co-La catalysts and NO

Tiejun Zhang,Jian Li,Hong He,Qianqian Song,Quanming Liang

期刊论文

Low-temperature CO oxidation over Au-doped 13X-type zeolite catalysts: preparation and catalytic activity

Qing YE, Donghui LI, Jun ZHAO, Jiansheng ZHAO, Tianfang KANG, Shuiyuan CHENG

期刊论文

Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

期刊论文

Complete oxidation of methane on CoO-SnO catalysts

Xingfu TANG , Jiming HAO , Junhua LI ,

期刊论文

“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

期刊论文

Catalytic oxidation of CO over Pt/Fe

Zihao Li, Yang Geng, Lei Ma, Xiaoyin Chen, Junhua Li, Huazhen Chang, Johannes W. Schwank

期刊论文

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

期刊论文

Mass Transfer-Promoted Fe2+/Fe3+ Circulation Steered by 3D Flow-Through Co-Catalyst System Toward SustainableAdvanced Oxidation Processes

Weiyang Lv,Hao Li,Jinhui Wang,Lixin Wang,Zenglong Wu,Yuge Wang,Wenkai Song,Wenkai Cheng,Yuyuan Yao,

期刊论文

Excellent performance of Cu-Mn/Ti-sepiolite catalysts for low-temperature CO oxidation

Yong Song,Lisha Liu,Zhidan Fu,Qing Ye,Shuiyuan Cheng,Tianfang Kang,Hongxing Dai

期刊论文

Effects of preparation methods on the activity of CuO/CeO

Huanhuan Shang, Xiaoman Zhang, Jing Xu, Yifan Han

期刊论文

Microbial responses to combined oxidation and catalysis treatment of 1,4-dioxane and co-contaminants

Yu Miao, Nicholas W. Johnson, Kimberly Heck, Sujin Guo, Camilah D. Powell, Thien Phan, Phillip B. Gedalanga, David T. Adamson, Charles J. Newell, Michael S. Wong, Shaily Mahendra

期刊论文

使用傅里叶变换红外成像进行高通量筛选

Erdem Sasmaz, Kathleen Mingle, Jochen Lauterbach

期刊论文

Phenolic compounds removal by wet air oxidation based processes

Linbi Zhou, Hongbin Cao, Claude Descorme, Yongbing Xie

期刊论文