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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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Frontier science and challenges on offshore carbon storage

《环境科学与工程前沿（英文）》 2023年第17卷第7期 doi: 10.1007/s11783-023-1680-6

摘要：

● The main direct seal up carbon options and challenges are reviewed.

关键词： Offshore carbon storage Direct CO₂ injection CO₂-CH₄ replacement CO₂-EOR CCS hubs CO₂ transport

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Effect of carbon deposition over carbonaceous catalysts on CH

Yongfa ZHANG, Meng ZHANG, Guojie ZHANG, Huirong ZHANG

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 481-485 doi: 10.1007/s11705-010-0523-8

摘要： An investigation was made using a continuous fixed bed reactor to understand the influence of carbon deposition obtained under different conditions on CH -CO reforming. Thermogravimetry (TG) and X-ray diffraction (XRD) were employed to study the characteristics of carbon deposition. It was found that the carbonaceous catalyst is an efficient catalyst in methane decomposition and CH -CO reforming. The trend of methane decomposition at lower temperatures is similar to that at higher temperatures. The methane conversion is high during the initial of stage of the reaction, and then decays to a relatively fixed value after about 30 min. With temperature increase, the methane decomposition rate increases quickly. The reaction temperature has significant influence on methane decomposition, whereas the carbon deposition does not affect methane decomposition significantly. Different types of carbon deposition were formed at different methane decomposition reaction temperatures. The carbon deposition Type I generated at 900°C has a minor effect on CH -CO reforming and it easily reacts with carbon dioxide, but the carbon deposition Type II generated at 1000°C and 1100°C clearly inhibits CH -CO reforming and it is difficult to react with carbon dioxide. The results of XRD showed that some graphite structures were found in carbon deposition Type II.

关键词： carbon deposition carbonaceous catalyst CH₄-CO₂ reforming

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Design and analysis of dual fuel methanol-power poly-generation

Minghua WANG , Zheng LI , Weidou NI ,

《能源前沿（英文）》 2009年第3卷第3期页码 341-347 doi: 10.1007/s11708-009-0023-z

摘要： A dual fuel head poly-generation flowsheet was designed based on coal gas and coke oven gas. To help clearly understand the system performance, a 1.2×10−3.2×10kg methanol and 274―496MW power poly-generation system was simulated by using the commercially available software ASPEN Plus and GT Pro. The technology scheme, the operating parameters, and the efficiency of the system were also analyzed and evaluated, which will be used for building industrial devices.

关键词： dual fuel methanol-power poly-generation CO₂ and CH₄ reforming splitting ratio

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Review on cryogenic technologies for CO removal from natural gas

Yujing BI, Yonglin JU

《能源前沿（英文）》 2022年第16卷第5期页码 793-811 doi: 10.1007/s11708-022-0821-0

摘要： CO₂ in natural gas (NG) is prone to condense directly from gas to solid or solidify from liquid to solid at low temperatures due to its high triple point and boiling temperature, which can cause a block of equipment. Meanwhile, CO₂ will also affect the calorific value of NG. Based on the above reasons, CO₂ must be removed during the NG liquefaction process. Compared with conventional methods, cryogenic technologies for CO₂ removal from NG have attracted wide attention due to their non-polluting and low-cost advantages. Its integration with NG liquefaction can make rational use of the cold energy and realize the purification of NG and the production of by-product liquid CO₂. In this paper, the phase behavior of the CH₄-CO₂ binary mixture is summarized, which provides a basis for the process design of cryogenic CO₂ removal from NG. Then, the detailed techniques of design and optimization for cryogenic CO₂ removal in recent years are summarized, including the gas-liquid phase change technique and the gas-solid phase change technique. Finally, several improvements for further development of the cryogenic CO₂ removal process are proposed. The removal process in combination with the phase change and the traditional techniques with renewable energy will be the broad prospect for future development.

关键词： cryogenic CO₂ removal purification of natural gas (NG) biogas upgrading CH₄-CO₂ binary system

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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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Effect of TiO

Navid Azizi, Mojgan Isanejad, Toraj Mohammadi, Reza M. Behbahani

《化学科学与工程前沿（英文）》 2019年第13卷第3期页码 517-530 doi: 10.1007/s11705-018-1781-0

摘要： Membranes have attracted much attention as economical methods for industrial chemical processes. The effects of the titanium dioxide nanoparticle load on the morphology and CO /CH separation performance of poly (ether-block-amide) (PEBAX-1657) mixed matrix membranes (MMMs) were investigated from pressures of 3–12 bar and temperatures of 30°C–60°C. The PEBAX membranes were characterized by scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, thermal gravimetric analysis, atomic force microscopy and tensile strength analysis. The incorporation of TiO nanoparticles into the polymeric MMMs improved the CO /CH gas separation performance (both the permeability and selectivity) of the membranes. The CO permeability and ideal CO /CH selectivity values of the nanocomposite membrane loaded with 8 wt-% TiO were 172.32 Barrer and 24.79, respectively whereas those of the neat membrane were 129.87 Barrer and 21.39, respectively.

关键词： mixed matrix membrane TiO₂ nanoparticles PEBAX-1657 CO₂/CH₄ separation

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ZnFe2sub>O4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2sub> 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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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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CH4sub> and N2sub>O emissions from double-rice cropping system as affected by Chinese milk

Heshui XU,Dengyun LI,Bo ZHU,Kai ZHANG,Yadong YANG,Chen WANG,Ying JIANG,Zhaohai ZENG

《农业科学与工程前沿（英文）》 2017年第4卷第1期页码 59-68 doi: 10.15302/J-FASE-2017137

摘要： Chinese milk vetch (CMV) and rice straw (RS) were incorporated into soil to substitute for synthetic N fertilizers and to maintain soil fertility. However, little is known about the integrated impacts of CMV and RS incorporation on CH and N O emissions in double-rice cropping systems in southern China. A field experiment was conducted to estimate the integrated impacts of CMV and RS incorporation in the early- and late-rice seasons on CH and N O emissions. All treatments received uniform N inputs, 6%–37% of which was replaced by CMV and RS crop residue. CMV and/or RS incorporation produced equivalent or slightly more grain yield, while reducing N O emissions by 3%–43%. However, both CMV and RS incorporation increased CH emissions. Annual CH emissions ranged from 321 to 614 kg·hm from CMV and RS amendment treatments, which were 1.5–2.9 times higher than that from synthetic N. Compared with single synthetic N fertilizer, incorporation of CMV and/or RS increased GWP and yield-scaled GWP by 45%–164% and 45%–153%, respectively. Our results demonstrate CMV and RS amendments replacing N fertilizer, maintained stable yield, mitigated N O emission, but enhanced CH emission. Further study is needed on crop residue management in double-cropping rice systems.

关键词： Chinese milk vetch CH₄ double-rice cropping system grain yield N₂O rice straw

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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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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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CO2sub> methanation and co-methanation of CO and CO2sub> over Mn-promoted Ni/Al2sub>O3sub> 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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On the monolayer dispersion behavior of Co3sub>O4sub> 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 NO_x 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 NO_x-SCR by NH₃ monolayer dispersion threshold effect surface acid sites surface active O₂^– anions

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Rh2sub>O3sub>/hexagonal CePO4sub> nanocatalysts for N2sub>O 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