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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

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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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Synthesis of cobalt vanadium nanomaterials for efficient electrocatalysis of oxygen evolution

Meifeng Hao, Mingshu Xiao, Lihong Qian, Yuqing Miao

《化学科学与工程前沿（英文）》 2018年第12卷第3期页码 409-416 doi: 10.1007/s11705-017-1689-0

摘要：

A low-cost and high-activity catalyst for oxygen evolution reaction (OER) is the key to the water splitting technology for hydrogen generation. Here we report the use of three solvents, DMF, ethanol and glycol, in the solvothermal synthesis of three nano-catalysts, Co₃(VO₄)₂-I, Co₃(VO₄)₂-II, and Co₃(VO₄)₂-III, respectively. Transmission electron microscope shows Co₃(VO₄)₂-I, II, and III exist as ultrafine nanosheets, ultrathin nanofilms, and ultrafine nanosheet-comprised microspheres, respectively. These Co₃(VO₄)₂ catalysts exhibit OER electrocatalysis, among which the Co₃(VO₄)₂-II shows the lowest onset overpotential of 310 mV and only requires a small overpotential of 330 mV to drive current density of 10 mA/cm². Due to their high surface free energy, the ultrathin nanofilms of Co₃(VO₄)₂-II exhibits a good immobilization effect with the high electrocatalytic activity for OER.

关键词： Co₃(VO₄)₂ oxygen evolution reaction electrocatalyst water splitting

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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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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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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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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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Al2sub>O3sub> and CeO2sub>-promoted MgO sorbents for CO2sub> 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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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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acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH3sub>

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要： Three kinds of Ce-based catalysts (CePO₄, CeVO₄, Ce₂(SO₄)₃) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH₃. NH₃-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO₄ > CeVO₄ > Ce₂(SO₄)₃, which is in agreement with their abilities of NH₃ adsorption capacities. The highest NO conversion rate of CePO₄ could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO₄^3–, VO₄^3– and SO₄^2– on NH₃-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH₃ temperature programmed desorption, H₂ temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce⁴⁺, large NH₃ adsorption capacity, high and early H₂ consumptions, and suitable microstructures for gas adsorption. Finally, CePO₄ and CeVO₄ catalysts also exhibited relatively strong tolerance of SO₂, and the upward trend about 8% was detected due to the sulfation enhancement by SO₂ for Ce₂(SO₄)₃.

关键词： CePO₄ CeVO₄ Ce₂(SO₄)₃ selective catalytic reduction NO removal

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以净零排放为目标的封存驱动型CO2sub>提高采收率方法 Article

刘月亮, 芮振华

《工程（英文）》 2022年第18卷第11期页码 79-87 doi: 10.1016/j.eng.2022.02.010

摘要：可通过驱油过程将CO2sub>封存在油藏地质体中，因此，CO2sub>驱油与封存被视为降低CO2sub>排放的重要手段之一。本研究提出了一种新型的CO2sub>提高采收率（EOR）方法，即封存驱动型CO2sub>提高采收率，其主要目标是通过在油藏中封存尽可能多的CO2sub>来实现CO结果表明，DME可提高CO2sub>在原油中的溶解度，有利于CO2sub>的溶解封存；可抑制因CO2sub>的抽提作用造成的原油轻质组分“逃逸&rdquo封存驱动型CO2sub> EOR方法在提高波及效率方面优于传统的CO2sub> EOR，尤其是在采油后期更为明显；同时，封存驱动型CO2sub> EOR比传统的此外，通过封存驱动型CO2sub> EOR封存的CO2sub>量远超采出原油燃烧产生的碳排放总量。

关键词： CO2sub> EOR CO2sub>净排放量二甲醚封存驱动型CO2sub> EOR CO2sub>封存

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催化氧化净化黄磷尾气中的磷和硫

宁平,Hans-JörgBart,王学谦,马丽萍,陈梁

《中国工程科学》 2005年第7卷第6期页码 27-35

摘要：研究了用普通活性炭和自制催化剂KU2催化氧化净化黄磷尾气的方法；讨论了固定床系统中常压下、温度20～140℃，催化剂上磷和硫化氢的吸附特征。KU2和活性炭都能通过催化氧化过程有效脱除黄磷尾气中的P4sub>，PH3sub>和H2sub>S杂质，随着反应温度和氧含量增加可显著提高净化效果，在最优条件下，经催化氧化净化后的总磷含量＜5mg/m³，硫化氢＜5mg/m³，失效后的催化剂易于再生，催化剂经多次再生后催化性能恢复良好；提出了活性炭固定床稳定流动吸附过程的数学模型

关键词：催化剂催化氧化 H2sub>S P4sub> PH3sub> 固定床

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固体氧化物电解池共电解H2sub>O/CO2sub>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 H2sub>O/CO2sub>共电解合成气电解效率水电解

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A CO and CO

Guoxing Chen, Marc Widenmeyer, Binjie Tang, Louise Kaeswurm, Ling Wang, Armin Feldhoff, Anke Weidenkaff

《化学科学与工程前沿（英文）》 2020年第14卷第3期页码 405-414 doi: 10.1007/s11705-019-1886-0

摘要： A series of novel dense mixed conducting ceramic membranes based on K NiF -type (La Ca ) (Ni Cu )O was successfully prepared through a sol-gel route. Their chemical compatibility, oxygen permeability, CO and CO tolerance, and long-term CO resistance regarding phase composition and crystal structure at different atmospheres were studied. The results show that higher Ca contents in the material lead to the formation of CaCO . A constant oxygen permeation flux of about 0.63 mL·min ·cm at 1173 K through a 0.65 mm thick membrane was measured for (La Ca ) (Ni Cu )O , using either helium or pure CO as sweep gas. Steady oxygen fluxes with no sign of deterioration of this membrane were observed with increasing CO concentration. The membrane showed excellent chemical stability towards CO for more than 1360 h and phase stability in presence of CO for 4 h at high temperature. In addition, this membrane did not deteriorate in a high-energy CO plasma. The present work demonstrates that this (La Ca ) (Ni Cu )O membrane is a promising chemically robust candidate for oxygen separation applications.

关键词： K₂NiF₄ structure oxygen permeation membrane CO₂ and CO resistances CO₂ plasma resistance long-term robustness

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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