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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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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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On the monolayer dispersion behavior of Co3O4 on HZSM-5 support: designing applicable

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要： Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2–) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2– species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

关键词： Co3O4/ZSM-5     NOx-SCR by NH3     monolayer dispersion threshold effect     surface acid sites     surface active O2– anions    

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Rh2O3/hexagonal CePO4 nanocatalysts for N2O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要： Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词： Rh2O3     CePO4     N2O decomposition    

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ZnFe2O4 deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2 in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 197-204 doi: 10.1007/s11705-016-1606-y

摘要： ZnFe O -BiOCl composites were prepared by both hydrothermal and direct precipitation processes and the structures and properties of the samples were characterized by various instrumental techniques. The samples were then used as catalysts for the photocatalytic reduction of CO in cyclohexanol under ultraviolet irradiation to give cyclohexanone (CH) and cyclohexyl formate (CF). The photocatalytic CO reduction activities over the hydrothermally prepared ZnFe O -BiOCl composites were higher than those over the directly-precipitated composites. This is because compared to the direct-precipitation sample, the ZnFe O nanoparticles in the hydrothermal sample were smaller and more uniformly distributed on the surface of BiOCl and so more heterojunctions were formed. Higher CF and CH yields were obtained for the pure BiOCl and BiOCl composite samples with more exposed (001) facets than for the samples with more exposed (010) facets. This is due to the higher density of oxygen atoms in the exposed (001) facets, which creates more oxygen vacancies, and thereby improves the separation efficiency of the electron-hole pairs. More importantly, irradiation of the (001) facets with ultraviolet light produces photo-generated electrons which is helpful for the reduction of CO to ·CO . The mechanism for the photocatalytic reduction of CO in cyclohexanol over ZnFe O -BiOCl composites with exposed (001) facets involves electron transfer and carbon radical formation.

关键词： reduction of CO2     cyclohexanol     ZnFe2O4 deposited BiOCl     facet     composite photocatalyst    

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CO2 methanation and co-methanation of CO and CO2 over Mn-promoted Ni/Al2O3 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    

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Al2O3 and CeO2-promoted MgO sorbents for CO2 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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铝电解用Fe-Ni-Co-Al2O3金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

《中国工程科学》 2004年 第6卷 第8期   页码 35-39

摘要：

研制了一种新型铝电解金属陶瓷惰性阳极，阳极基体由Fe-Ni-CoAl2O3构成。在石墨坩埚中，960℃温度下，电解质中的氧化铝质量分数为6.0%，摩尔比为2.6；阳极电流密度为1.0 A/cm2，阳极尺寸大小为120 mm×80 mm×，石墨阴极尺寸大小为120 mm×40 mm×20 mm，通入的直流电为100～300 A，电解时间各为10 h；实验所得的电解铝产品纯度达到98%以上，杂质主要为Fe，Ni，Co阳极的反电动势为2.45 V，比理论分解电压仅高出0.25 V证明该阳极为惰性阳极，在电解槽中进行的是Al2O3的分解反应。

关键词： 铝电解     惰性阳极     反电动势    

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ZnFe2O4/BiVO4 Z-scheme heterojunction for efficient visible-light photocatalytic

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1728-1740 doi: 10.1007/s11705-023-2322-z

摘要： A novel Z-scheme ZnFe2O4/BiVO4 heterojunction photocatalyst was successfully synthesized using a convenient solvothermal method and applied in the visible light photocatalytic degradation of ciprofloxacin, which is a typical antibiotic contaminant in wastewater. The heterostructure of as-synthesized catalysts was confirmed using X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy characterizations. Compared with the single-phase counterparts, ZnFe2O4/BiVO4 demonstrated considerably enhanced photogenerated charge separation efficiencies because of the Z-scheme transfer mechanism of electrons between the composite photocatalysts. Consequently, the 30% ZnFe2O4/BiVO4 catalyst afforded a degradation rate of up to 97% of 20 mg/L ciprofloxacin under 30 min of visible light irradiation with a total organic carbon removal rate of 50%, which is an excellent activity compared with ever reported BiVO4-based catalysts. In addition, the liquid chromatography-mass spectrometry and quantitative structure-activity relationships model analyses demonstrated that the toxicity of the intermediates was lower than that of the parent ciprofloxacin. Moreover, the as-synthesized ZnFe2O4/BiVO4 heterojunctions were quite stable and could be reused at least four times. This study thus provides a promising Z-scheme heterojunction photocatalyst for the efficient removal and detoxication of antibiotic pollutants from wastewater.

关键词： ZnFe2O4/BiVO4     Z-scheme heterojunction     photocatalytic degradation     ciprofloxacin    

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固体氧化物电解池共电解H2O/CO2研究进展

范慧,宋世栋,韩敏芳

《中国工程科学》 2013年 第15卷 第2期   页码 107-112

摘要： 本文介绍了固体氧化物电解池的结构特点及其用于H2O/CO2的共电解制备H2和CO的工作原理，综述了固体氧化物电解池的组成形式，以及单片电解池和电解池堆用于H2O/CO2共电解反应的国内外研究进展，并阐述了提高固体氧化物电解池共电解效率所亟需解决的问题

关键词： 固体氧化物电解池     H2O/CO2共电解     合成气     电解效率     水电解    

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Pd/Fe3O4 supported on bio-waste derived cellulosic-carbon as a nanocatalyst for C–C coupling and electrocatalytic

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1514-1525 doi: 10.1007/s11705-022-2158-y

摘要： The current work describes the synthesis of a new bio-waste derived cellulosic-carbon supported-palladium nanoparticles enriched magnetic nanocatalyst (Pd/Fe3O4@C) using a simple multi-step process under aerobic conditions. Under mild reaction conditions, the Pd/Fe3O4@C magnetic nanocatalyst demonstrated excellent catalytic activity in the Hiyama cross-coupling reaction for a variety of substrates. Also, the Pd/Fe3O4@C magnetic nanocatalyst exhibited excellent catalytic activity up to five recycles without significant catalytic activity loss in the Hiyama cross-coupling reaction. Also, we explored the use of Pd/Fe3O4@C magnetic nanocatalyst as an electrocatalyst for hydrogen evolution reaction. Interestingly, the Pd/Fe3O4@C magnetic nanocatalyst exhibited better electrochemical activity compared to bare carbon and magnetite (Fe3O4 nanoparticles) with an overpotential of 293 mV at a current density of 10 mA·cm–2.

关键词： bio-waste     cellulosic-carbon     Pd/Fe3O4     Hiyama cross-coupling     hydrogen evolution reaction     recyclability    

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Preparation and property characterization of PAA/Fe3O4 nanocomposite

WEI Shanshan, ZHANG Yi, XU Jiarui

《化学科学与工程前沿（英文）》 2007年 第1卷 第3期   页码 233-237 doi: 10.1007/s11705-007-0042-4

摘要： PAA/FeO nanocomposites were prepared by mixing nano-FeOvent. The materials were characterized by transmission electron microscope (TEM), Fourier transform infrared spectroscope (FTIR), thermogravimetry analysis (TGA), dynamic ultra-micro hardness tester (DUMHT) and superconducting quantum interference device (SQUID) magnetometer. Results showed that PAA coordinated with nano-FeO to form a cross-linking structure. The presence of nano-FeO enhanced the thermal stability of the nanocomposite. The elasticity and hardness of the nanocomposite increased, and the indentation depth reduced with the increase of FeO content in the composites. The nanocomposites showed superparamagnetic properties at 300 K.

关键词： magnetometer     superparamagnetic     ultra-micro     thermogravimetry     transmission    

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Greenhouse gas emissions during co-composting of cattle feedlot manure with construction and demolition

Xiying Hao, Francis J. Larney

《环境科学与工程前沿（英文）》 2017年 第11卷 第3期 doi: 10.1007/s11783-017-0955-1

摘要： Manure management strategies should reflect current animal feeding practices and encourage recycling of organic waste to help protect our environment. This research investigated greenhouse gas (GHG) emissions during cattle manure stockpiling or composting with and without construction and demolition (C&D) waste. Manure was collected from cattle fed a typical finishing diet (CK manure) and from cattle on diets which included 30% dried distillers grains with solubles (DG manure). The CK and DG manures were co-composted with (4:1) C&D waste (treatments: CK_CD DG_CD), composted alone (treatments: CK and DG) in 13 m bins or stockpiled without C&D waste (treatments: CK_ST and DG_ST) for 99 days. Manure type (CK vs. DG manure) had no effect on GHG emissions over the 99 day manure composting or stockpiling. Composting with C&D waste produced similar CO emissions, about double that from manure stockpiling (7.0 kgC·m ). In contrast, CH emissions were reduced by the inclusion of C&D waste (64 gC·m with C&D vs. 244 gC·m without C&D) while the manure stockpile emitted the greatest amount of CH (464 gC·m ). Additionally, only 0.48% of C was emitted in CH form with C&D waste, compared to 1.68% when composting without C&D waste and 7.00% when cattle manure was stockpiled. The N O emissions (12.4 to 18.0 gN·m ) were similar across all treatments. The lower CH emissions with C&D waste are beneficial in reducing overall GHG emissions from manure composting, while reducing the amount of material entering landfills.

关键词： Livestock manure     greenhouse gas flux     straw bale compost bin     N2O     CH4     CO2    

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NiCo2O4@quinone-rich N–C core–shell nanowires as composite electrode for electric double layer capacitor

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 373-386 doi: 10.1007/s11705-022-2223-6

摘要： The bind-free carbon cloth-supported electrodes hold the promises for high-performance electrochemical capacitors with high specific capacitance and good cyclic stability. Considering the close connection between their performance and the amount of carbon material loaded on the electrodes, in this work, NiCo2O4 nanowires were firstly grown on the substrate of active carbon cloth to provide the necessary surface area in the longitudinal direction. Then, the quinone-rich nitrogen-doped carbon shell structure was formed around NiCo2O4 nanowires, and the obtained composite was used as electrode for electric double layer capacitor. The results showed that the composite electrode displayed an area-specific capacitance of 1794 mF∙cm–2 at the current density of 1 mA∙cm–2. The assembled symmetric electric double layer capacitor achieved a high energy density of 6.55 mW∙h∙cm–3 at a power density of 180 mW∙cm–3. The assembled symmetric capacitor exhibited a capacitance retention of 88.96% after 10000 charge/discharge cycles at the current density of 20 mA∙cm–2. These results indicated the potentials in the preparation of the carbon electrode materials with high energy density and good cycling stability.

关键词： carbon cloth     NiCo2O4 nanowires     core−shell structure     quinone-rich     electric double layer capacitor    

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Enhanced 4-chlorophenol biodegradation by integrating FeO nanoparticles into an anaerobic reactor: Long-term

《环境科学与工程前沿（英文）》 2022年 第16卷 第8期 doi: 10.1007/s11783-022-1519-6

摘要：

• 4-chlorophenol biodegradation could be enhanced in Fe2O3 coupled anaerobic system.

关键词： Dechlorination     Fe2O3 nanoparticles     Electron transfer     Microbial community    

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标题 作者 时间 类型 操作

Complete oxidation of methane on CoO-SnO catalysts

Xingfu TANG , Jiming HAO , Junhua LI ,

期刊论文

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

期刊论文

On the monolayer dispersion behavior of Co3O4 on HZSM-5 support: designing applicable

期刊论文

Rh2O3/hexagonal CePO4 nanocatalysts for N2O decomposition

Huan Liu, Zhen Ma

期刊论文

ZnFe2O4 deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2 in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

期刊论文

CO2 methanation and co-methanation of CO and CO2 over Mn-promoted Ni/Al2O3 catalysts

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文

Al2O3 and CeO2-promoted MgO sorbents for CO2 capture at moderate

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

期刊论文

铝电解用Fe-Ni-Co-Al2O3金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

期刊论文

ZnFe2O4/BiVO4 Z-scheme heterojunction for efficient visible-light photocatalytic

期刊论文

固体氧化物电解池共电解H2O/CO2研究进展

范慧,宋世栋,韩敏芳

期刊论文

Pd/Fe3O4 supported on bio-waste derived cellulosic-carbon as a nanocatalyst for C–C coupling and electrocatalytic

期刊论文

Preparation and property characterization of PAA/Fe3O4 nanocomposite

WEI Shanshan, ZHANG Yi, XU Jiarui

期刊论文

Greenhouse gas emissions during co-composting of cattle feedlot manure with construction and demolition

Xiying Hao, Francis J. Larney

期刊论文

NiCo2O4@quinone-rich N–C core–shell nanowires as composite electrode for electric double layer capacitor

期刊论文

Enhanced 4-chlorophenol biodegradation by integrating FeO nanoparticles into an anaerobic reactor: Long-term

期刊论文