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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    

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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    

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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    

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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    

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用于CO甲烷化的Ni/CeO<sub>2sub>催化剂还原过程重构行为调控研究 Article

曹昕宇, 浦天成, Bar Mosevitzky Lis, Israel E. Wachs, 彭冲, 朱明辉, 胡永康

《工程（英文）》 2022年 第14卷 第7期   页码 94-99 doi: 10.1016/j.eng.2021.08.023

摘要：

还原预处理是活化负载型金属催化剂的重要步骤，但很少受到关注。本研究发现负载型镍催化剂的重构过程对预处理条件非常敏感。与使用氢气的传统活化方式相比，用合成气活化催化剂可以产生具有多晶结构的负载型镍纳米颗粒，其中包含丰富的晶界。独特的活化方式使得催化剂上CO吸附得到增强，提高了CO甲烷化率。通过操纵活化条件来调整催化剂结构的策略也可以被用于指导其他负载型金属催化剂的理性设计。

关键词： 镍-氧化铈催化剂     催化剂活化     结晶性     甲烷化     原位谱学    

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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    

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The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1423-1429 doi: 10.1007/s11705-023-2315-y

摘要： Similar to Sn, Pb located at the same group (IVA) in the periodic table of elements, can also catalyze propane dehydrogenation to propene, while a fast deactivation can be observed. To enhance the stability, the traditional carrier Al2O3 with a small amount, was introduced into Pb/SiO2 catalyst in this study. It has been proved that Al2O3 can inhibit the reduction of PbO, and weaken the agglomeration and loss of Pb species due to its enhanced interaction with Pb species. As a result, 3Al15Pb/SiO2 catalyst exhibits a much higher stability up to more than 150 h. In addition, a simple schematic diagram of the change of surface species on the catalyst surface after Al2O3 addition was also proposed.

关键词： Pb/SiO2     Al2O3     propane dehydrogenation     propene     stability    

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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    

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Piezocatalytic performance of FeO−BiMoO catalyst for dye degradation

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 716-725 doi: 10.1007/s11705-022-2265-9

摘要： A Fe2O3−Bi2MoO6 heterojunction was synthesized via a hydrothermal method. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray, powder X-ray diffraction, Fourier transform infrared spectroscopy and ultra-violet−visible near-infrared spectrometry were performed to measure the structures, morphologies and optical properties of the as-prepared samples. The various factors that affected the piezocatalytic property of composite catalyst were studied. The highest rhodamine B degradation rate of 96.6% was attained on the 3% Fe2O3−Bi2MoO6 composite catalyst under 60 min of ultrasonic vibration. The good piezocatalytic activity was ascribed to the formation of a hierarchical flower-shaped microsphere structure and the heterostructure between Fe2O3 and Bi2MoO6, which effectively separated the ultrasound-induced electron–hole pairs and suppressed their recombination. Furthermore, a potential piezoelectric catalytic dye degradation mechanism of the Fe2O3−Bi2MoO6 catalyst was proposed based on the band potential and quenching effect of radical scavengers. The results demonstrated the potential of using Fe2O3−Bi2MoO6 nanocomposites in piezocatalytic applications.

关键词： piezocatalysis     Fe2O3−Bi2MoO6     dye decomposition     ultrasonic vibration    

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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    

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Simultaneous removal of NO and chlorobenzene on VO/TiO granular catalyst: Kinetic study and performance

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1363-5

摘要：

• A V2O5/TiO2 granular catalyst for simultaneous removal of NO and chlorobenzene.

关键词： NOx     Chlorobenzene     Simultaneous removal     Kinetic study     Performance prediction     V2O5/TiO2     Graphical abstract    

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Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 476-480 doi: 10.1007/s11705-010-0512-y

摘要： A co-precipitation method was employed to prepare Ni/Al O -ZrO , Co/Al O -ZrO and Ni-Co/Al O -ZrO catalysts. Their properties were characterized by N adsorption (BET), thermogravimetric analysis TGA , temperature-programmed reduction (TPR), temperature-programmed desorption (CO -TPD), and temperature-programmed surface reaction (CH -TPSR and CO -TPSR). Ni-Co/Al O -ZrO bimetallic catalyst has good performance in the reduction of active components Ni, Co and CO adsorption. Compared with mono-metallic catalyst, bimetallic catalyst could provide more active sites and CO adsorption sites (C+ CO = 2CO) for the methane-reforming reaction, and a more appropriate force formed between active components and composite support (SMSI) for the catalytic reaction. According to the CH -CO -TPSR, there were 80.9% and 81.5% higher CH and CO conversion over Ni-Co/Al O -ZrO catalyst, and its better resistance to carbon deposition, less than 0.5% of coke after 4 h reaction, was found by TGA. The high activity and excellent anti-coking of the Ni-Co/Al O -ZrO catalyst were closely related to the synergy between Ni and Co active metal, the strong metal-support interaction and the use of composite support.

关键词： Ni-Co bimetallic catalyst     composite support     CH4 reforming with CO2    

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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    

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NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1973-1985 doi: 10.1007/s11705-023-2364-2

摘要： Ammonia is crucial in industry and agriculture, but its production is hindered by environmental concerns and energy-intensive processes. Hence, developing an efficient and environmentally friendly catalyst is imperative. In this study, we employed a straightforward and efficient impregnation technique to create various Cu-doped catalysts. Notably, the optimized 10Fe-8Cu/TiO2 catalyst exhibited exceptional catalytic performance in converting NO to NH3, achieving an NO conversion rate exceeding 80% and an NH3 selectivity exceeding 98% at atmospheric pressure and 350 °C. We employed in situ diffuse reflectance Fourier transform infrared spectroscopy and conducted density functional theory calculations to investigate the intermediates and subsequent adsorption. Our findings unequivocally demonstrate that Cu doping enhances the rate-limiting hydrogenation step and lowers the energy barrier for NH3 desorption, thereby resulting in improved NO conversion and enhanced selectivity toward ammonia. This study presents a pioneering approach toward energy-efficient ammonia synthesis and recycling of nitrogen sources.

关键词： NO hydrogenation     synthetic ammonia     10Fe-xCu/TiO2     high selectivity    

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New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

《能源前沿（英文）》 2021年 第15卷 第2期   页码 421-430 doi: 10.1007/s11708-021-0727-2

摘要： In recent years, Fe-N-C catalyst is particularly attractive due to its high oxygen reduction reaction (ORR) activity and low cost for proton exchange membrane fuel cells (PEMFCs). However, the durability problems still pose challenge to the application of Fe-N-C catalyst. Although considerable work has been done to investigate the degradation mechanisms of Fe-N-C catalyst, most of them are simply focused on the active-site decay, the carbon oxidation, and the demetalation problems. In fact, the 2e pathway in the ORR process of Fe-N-C catalyst would result in the formation of H O , which is proved to be a key degradation source. In this paper, a new insight into the effect of potential on degradation of Fe-N-C catalyst was provided by quantifying the H O intermediate. In this case, stability tests were conducted by the potential-static method in O saturated 0.1 mol/L HClO . During the tests, H O was quantified by rotating ring disk electrode (RRDE). The results show that compared with the loading voltage of 0.4 V, 0.8 V, and 1.0 V, the catalysts being kept at 0.6 V exhibit a highest H O yield. It is found that it is the combined effect of electrochemical oxidation and chemical oxidation (by aggressive radicals like H O /radicals) that triggered the highest H O release rate, with the latter as the major cause.

关键词： proton exchange membrane fuel cells (PEMFCs)     oxygen reduction reaction (ORR)     Fe-N-C catalyst     potential     H2O2     degradation    

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标题 作者 时间 类型 操作

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 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

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

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

用于CO甲烷化的Ni/CeO<sub>2sub>催化剂还原过程重构行为调控研究

曹昕宇, 浦天成, Bar Mosevitzky Lis, Israel E. Wachs, 彭冲, 朱明辉, 胡永康

期刊论文

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

期刊论文

The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

期刊论文

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

期刊论文

Piezocatalytic performance of FeO−BiMoO catalyst for dye degradation

期刊论文

Characterization and performance of V

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

期刊论文

Simultaneous removal of NO and chlorobenzene on VO/TiO granular catalyst: Kinetic study and performance

期刊论文

Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong 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

NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

期刊论文

New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

期刊论文