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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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Ni/MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performance

Yan LI,Zhehao WEI,Yong WANG

《化学科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 133-140 doi: 10.1007/s11705-014-1422-1

摘要： A Ni/MgO catalyst was prepared via novel dielectric-barrier discharge (DBD) plasma decomposition method. The combined characterization of Brunauer-Emmett-Teller measurement, X-ray diffraction, hydrogen temperature-programmed reduction and transmission electron microscopy shows that DBD plasma treatment enhances the support-metal interaction of Ni/MgO catalyst and facilitates the formation of smaller Ni particles. Sphere-like Ni particles form on plasma treated Ni/MgO catalysts. The plasma treated Ni/MgO catalyst shows a significantly improved low temperature activity and good stability for CO reforming of methane to syngas.

关键词： CO2 reforming     methane     dielectric-barrier discharge (DBD)     plasma     Ni/MgO    

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PSS sorbents for removing trace hydrogen sulfide in methane

Limei ZHONG, Li ZHOU

《化学科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 339-342 doi: 10.1007/s11705-010-0569-7

摘要： Sorbents of the pressure swing sorption process (PSS) to remove trace amount of H S (190 ppm) contained in methane were experimentally studied. The sorbents consist of adsorbent carrier (silica gel or activated carbon) and absorbent which spreads outside the carrier granules’ pores (triethanolamine, TEA or -methyl-2-pyrrolidone, NMP). The results of breakthrough and regeneration tests show that silica gel is more suitable to be the carrier than activated carbon and TEA is more suitable to be the absorbent than NMP. The loaded absorbent could enlarge the sorption capacity of H S considerably. And the BET tests indicate that the absorbent deposits on the surface of the carrier’s pores and can reduce the mesopores’ size and block the micropores.

关键词： pressure swing sorption     H2S     methane     carrier     absorbent    

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Methane partial oxidation over NiO-MgO/Ce

Piyawat PUE-ON, Vissanu MEEYOO, Thirasak RIRKSOMBOOON

《化学科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 289-296 doi: 10.1007/s11705-013-1345-2

摘要： Methane partial oxidation (MPO) is considered as an alternative method to produce hydrogen because it is an exothermic reaction to afford a suitable H /CO ratio of 2. However, carbon deposition on a catalyst is observed as a major cause of catalyst deactivation in MPO. In order to find suitable catalysts that prevent the carbon deposition, NiO-MgO/Ce Zr O (CZO) supported catalysts were prepared via the co-impregnation (C) and sequential incipient wetness impregnation (S) methods. The amount of Ni loading was fixed at 15 wt-% whereas the amount of MgO loading was varied from 5 to 15 wt-%. The results revealed that the addition of MgO shifted the light-off temperatures to higher temperatures. This is because the Ni surface was partially covered with MgO, and the strong interaction between NiO and NiMgO over CZO support led to the difficulty in reducing NiO to active Ni and thus less catalytic activity. However, among the catalysts tested, the 15Ni5Mg/CZO (S) catalyst exhibited the best catalytic stability for MPO after 18 h on stream at 750°C. Moreover, this catalyst had a better resistance to carbon deposition due to its high metallic Ni dispersion at high temperature.

关键词： methane partial oxidation     NiO     ceria-zirconia     MgO     mixed oxide solid solution    

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A density functional theory study of methane activation on MgO supported NiM cluster: role of M on C–H

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1485-1492 doi: 10.1007/s11705-022-2169-8

摘要： Methane activation is a pivotal step in the application of natural gas converting into high-value added chemicals via methane steam/dry reforming reactions. Ni element was found to be the most widely used catalyst. In present work, methane activation on MgO supported Ni–M (M = Fe, Co, Cu, Pd, Pt) cluster was explored through detailed density functional theory calculations, compared to pure Ni cluster. CH4 adsorption on Cu promoted Ni cluster requires overcoming an energy of 0.07 eV, indicating that it is slightly endothermic and unfavored to occur, while the adsorption energies of other promoters M (M = Fe, Co, Pd and Pt) are all higher than that of pure Ni cluster. The role of M on the first C–H bond cleavage of CH4 was investigated. Doping elements of the same period in Ni cluster, such as Fe, Co and Cu, for C–H bond activation follows the trend of the decrease of metal atom radius. As a result, Ni–Fe shows the best ability for C–H bond cleavage. In addition, doping the elements of the same family, like Pd and Pt, for CH4 activation is according to the increase of metal atom radius. Consequently, C–H bond activation demands a lower energy barrier on Ni–Pt cluster. To illustrate the adsorptive dissociation behaviors of CH4 at different Ni–M clusters, the Mulliken atomic charge was analyzed. In general, the electron gain of CH4 binding at different Ni–M clusters follows the sequence of Ni–Cu (–0.02 e) < Ni (–0.04 e) < Ni–Pd (–0.08 e) < Ni–Pt (–0.09 e) < Ni–Co (–0.10 e) < Ni–Fe (–0.12 e), and the binding strength between catalysts and CH 4 raises with the CH4 electron gain increasing. This work provides insights into understanding the role of promoter metal M on thermal-catalytic activation of CH4 over Ni/MgO catalysts, and is useful to interpret the reaction at an atomic scale.

关键词： CH4 dissociation     Ni–M     C–H bond activation     charge transfer    

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New nanostructured sorbents for desulfurization of natural gas

Lifeng WANG, Ralph T. YANG

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 8-19 doi: 10.1007/s11705-014-1411-4

摘要： Desulfurization of natural gas is achieved commercially by absorption with liquid amine solutions. Adsorption technology could potentially replace the solvent extraction process, particularly for the emerging shale gas wells with production rates that are generally lower than that from the large conventional reservoirs, if a superior adsorbent (sorbent) is developed. In this review, we focus our discussion on three types of sorbents: metal-oxide based sorbents, Cu/Ag-based and other commercial sorbents, and amine-grafted silicas. The advantages and disadvantages of each type are analyzed. Possible approaches for future developments to further improve these sorbents are suggested, particularly for the most promising amine-grafted silicas.

关键词： desulfurization     natural gas desulfurization     hydrogen sulfide sorbent     amine-silica sorbent    

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Development of solid base catalyst X/Y/MgO/-AlO for optimization of preparation of biodiesel from L.seed

WANG Rui, YANG Song, YIN Shitao, SONG Baoan, BHADURY Pinaki S., XUE Wei, TAO Shuwei, JIA Zhaohui, LIU Da, GAO Liang

《化学科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 468-472 doi: 10.1007/s11705-008-0074-4

摘要： The preparation and regeneration conditions of the identified catalyst X/Y/MgO/-AlO with high catalytic activity were studied and optimized. The biodiesel was prepared by transesterification of seed oil produced in Guizhou with methanol at its reflux temoerature in the presence of X/Y/MgO/-AlO The pilot plant tests were carried out in a 100 L reaction vessel. Both average yield and fatty acid methyl esters (FAME) content reached more than 96.50% under the optimum reaction conditions of the pilot plant tests designed with an oil/methanol molar ratio of 1 : 10, catalyst concentration of 1.00%, and reaction time of 3 h at reflux temperature. In addition, analysis shows that the quality of biodiesel meets the standard EN 14214.

关键词： temperature     presence     addition     catalytic activity     catalyst X/Y/MgO/-AlO    

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Efficient MgO-doped CaO sorbent pellets for high temperature CO

Zhihong Xu, Tao Jiang, Hao Zhang, Yujun Zhao, Xinbin Ma, Shengping Wang

《化学科学与工程前沿（英文）》 2021年 第15卷 第3期   页码 698-708 doi: 10.1007/s11705-020-1981-2

摘要： Novel MgO-doped CaO sorbent pellets were prepared by gel-casting and wet impregnation. The effect of Na and MgO on the structure and CO adsorption performance of CaO sorbent pellets was elucidated. MgO-doped CaO sorbent pellets with the diameter range of 0.5 1.5 mm exhibited an excellent capacity for CO adsorption and adsorption rate due to the homogeneous dispersion of MgO in the sorbent pellets and its effects on the physical structure of sorbents. The results show that MgO can effectively inhibit the sintering of CaO and retain the adsorption capacity of sorbents during multiple adsorption-desorption cycles. The presence of mesopores and macropores resulted in appreciable change of volume from CaO (16.7 cm ∙mol ) to CaCO (36.9 cm ∙mol ) over repeated operation cycles. Ca2Mg1 sorbent pellets exhibited favorable CO capture capacity (9.49 mmol∙g ), average adsorption rate (0.32 mmol∙g ∙min ) and conversion rate of CaO (74.83%) after 30 cycles.

关键词： MgO doping     CaO sorbent pellets     gel-casting technique     CO2 capture    

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experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-based CO2 capture sorbents

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1460-1475 doi: 10.1007/s11705-022-2159-x

摘要： Carbon nanotubes-based materials have been identified as promising sorbents for efficient CO2 capture in fluidized beds, suffering from insufficient contact with CO2 for the high-level CO2 capture capacity. This study focuses on promoting the fluidizability of hard-to-fluidize pure and synthesized silica-coated amine-functionalized carbon nanotubes. The novel synthesized sorbent presents a superior sorption capacity of about 25 times higher than pure carbon nanotubes during 5 consecutive adsorption/regeneration cycles. The low-cost fluidizable-SiO2 nanoparticles are used as assistant material to improve the fluidity of carbon nanotubes-based sorbents. Results reveal that a minimum amount of 7.5 and 5 wt% SiO2 nanoparticles are required to achieve an agglomerate particulate fluidization behavior for pure and synthesized carbon nanotubes, respectively. Pure carbon nanotubes + 7.5 wt% SiO2 and synthesized carbon nanotubes + 5 wt% SiO2 indicates an agglomerate particulate fluidization characteristic, including the high-level bed expansion ratio, low minimum fluidization velocity (1.5 and 1.6 cm·s–1), high Richardson−Zakin index (5.2 and 5.3 > 5), and low Π value (83.2 and 84.8 < 100, respectively). Chemical modification of carbon nanotubes causes not only enhanced CO 2 uptake capacity but also decreases the required amount of silica additive to reach a homogeneous fluidization behavior for synthesized carbon nanotubes sorbent.

关键词： CO2 capture     CNT-based sorbents     fluidization     SiO2 nanoparticles     fluidized bed reactors    

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A review on research and development of iron-based sorbents for removal of hydrogen sulfide from hot

Jianglong YU, Liping CHANG, Fan LI, Kechang XIE

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 529-535 doi: 10.1007/s11705-010-0519-4

摘要： In poly-generation and integrated gasification-combined cycle (IGCC) systems for clean energy conversion, it is essential to remove impurities such as sulfur species from hot coal gases prior to entering the subsequent units. This paper provides a comprehensive review on previous studies on high temperature removal of hydrogen sulfide from high temperature coal gases using iron-based sorbents. A two-step desulphurization process for hot coal gas cleanup is highlighted, which is integrated with direct production of elemental sulfur during regeneration of iron-based sorbents in the primary desulphurization step. Different kinetic modeling approaches for sulfidation and regeneration were compared. Limited research on activated carbon supported sorbents was also briefly summarized.

关键词： hot coal gas cleanup     iron-based sorbents     sulfidation     regeneration     sulphur recovery    

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Operando modeling and measurements: Powerful tools for revealing the mechanism of alkali carbonate-based sorbents

《能源前沿（英文）》 2023年 第17卷 第3期   页码 380-389 doi: 10.1007/s11708-023-0872-x

摘要： Alkali carbonate-based sorbents (ACSs), including Na2CO3- and K2CO3-based sorbents, are promising for CO2 capture. However, the complex sorbent components and operation conditions lead to the versatile kinetics of CO2 sorption on these sorbents. This paper proposed that operando modeling and measurements are powerful tools to understand the mechanism of sorbents in real operating conditions, facilitating the sorbent development, reactor design, and operation parameter optimization. It reviewed the theoretical simulation achievements during the development of ACSs. It elucidated the findings obtained by utilizing density functional theory (DFT) calculations, ab initio molecular dynamics (AIMD) simulations, and classical molecular dynamics (CMD) simulations as well. The hygroscopicity of sorbent and the humidity of gas flow are crucial to shifting the carbonation reaction from the gas−solid mode to the gas−liquid mode, boosting the kinetics. Moreover, it briefly introduced a machine learning (ML) approach as a promising method to aid sorbent design. Furthermore, it demonstrated a conceptual compact operando measurement system in order to understand the behavior of ACSs in the real operation process. The proposed measurement system includes a micro fluidized-bed (MFB) reactor for kinetic analysis, a multi-camera sub-system for 3D particle movement tracking, and a combined Raman and IR sub-system for solid/gas components and temperature monitoring. It is believed that this system is useful to evaluate the real-time sorbent performance, validating the theoretical prediction and promoting the industrial scale-up of ACSs for CO2 capture.

关键词： CO2 capture     carbonation     theoretical modeling     operando techniques     reaction visualization    

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Effects of MgO promoter on properties of Ni/Al2O3 catalysts for partial oxidation of methane to syngas

QIU Yejun, CHEN Jixiang, ZHANG Jiyan

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 167-171 doi: 10.1007/s11705-007-0031-7

摘要： The effects of MgO promoter on the physico-chemical properties and catalytic performance of Ni/AlO catalysts for the partial oxidation of methane to syngas were studied by means of BET, XRD, H-TPR, TEM and performance evaluation. It was found that the MgO promoter benefited from the uniformity of nickel species in the catalysts, inhibited the formation of NiAlO spinel and improved the interaction between nickel species and support. These results were related to the formation of NiO MgO solid solution and MgAlO spinel. Moreover, for the catalysts with a proper amount of MgO promoter, the nickel dispersiveness was enhanced, therefore making their catalytic performance in methane partial oxidation improved. However, the excessive MgO promoter exerted a negative effect on the catalytic performance. Meanwhile, the basicity of MgO promoted the reversed water gas shift reaction, which led to an increase in CO selectivity and a decrease in H2 selectivity. The suitable content of MgO promoter in Ni/AlO catalyst was ?7 wt-%.

关键词： excessive     selectivity     decrease     dispersiveness     physico-chemical    

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Sponge-based materials for oil spill cleanups: A review

Edward Mohamed Hadji, Bo Fu, Ayob Abebe, Hafiz Muhammad Bilal, Jingtao Wang

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 749-762 doi: 10.1007/s11705-019-1890-4

摘要： Elimination of leaked oil from aquatic environs has recently gained importance owing to the disasters associated with leakages into marine environments. The need for an environmentally friendly and viable line of action concerning the environs has brought forward numerous affordable, non-toxic, and decomposable materials; further, diverse biomasses for fabricating nano- to micro-scale materials, membranes, and sponges/aerogels have also been incorporated for the elimination and retrieval of oils from water. Moreover, selectivity, sorption capacity, and reusability of these materials after the retrieval of oils are also desired from the viewpoint of sustainability. This review encompasses the recent progress in the field of elimination and retrieval of oil spills using various sponge-based materials.

关键词： membranes     sponges     reusability     sorbents     selectivity     sorption capacity    

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Encapsulation of 2-amino-2-methyl-1-propanol with tetraethyl orthosilicate for CO2 capture

Sidra Rama, Yan Zhang, Fideline Tchuenbou-Magaia, Yulong Ding, Yongliang Li

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 672-683 doi: 10.1007/s11705-019-1856-6

摘要： Carbon capture is widely recognised as an essential strategy to meet global goals for climate protection. Although various CO capture technologies including absorption, adsorption and membrane exist, they are not yet mature for post-combustion power plants mainly due to high energy penalty. Hence researchers are concentrating on developing non-aqueous solvents like ionic liquids, CO -binding organic liquids, nanoparticle hybrid materials and microencapsulated sorbents to minimize the energy consumption for carbon capture. This research aims to develop a novel and efficient approach by encapsulating sorbents to capture CO in a cold environment. The conventional emulsion technique was selected for the microcapsule formulation by using 2-amino-2-methyl-1-propanol (AMP) as the core sorbent and silicon dioxide as the shell. This paper reports the findings on the formulated microcapsules including key formulation parameters, microstructure, size distribution and thermal cycling stability. Furthermore, the effects of microcapsule quality and absorption temperature on the CO loading capacity of the microcapsules were investigated using a self-developed pressure decay method. The preliminary results have shown that the AMP microcapsules are promising to replace conventional sorbents.

关键词： carbon capture     microencapsulated sorbents     emulsion technique     low temperature adsorption and absorption    

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标题 作者 时间 类型 操作

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

Ni/MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performance

Yan LI,Zhehao WEI,Yong WANG

期刊论文

PSS sorbents for removing trace hydrogen sulfide in methane

Limei ZHONG, Li ZHOU

期刊论文

Methane partial oxidation over NiO-MgO/Ce

Piyawat PUE-ON, Vissanu MEEYOO, Thirasak RIRKSOMBOOON

期刊论文

A density functional theory study of methane activation on MgO supported NiM cluster: role of M on C–H

期刊论文

New nanostructured sorbents for desulfurization of natural gas

Lifeng WANG, Ralph T. YANG

期刊论文

Development of solid base catalyst X/Y/MgO/-AlO for optimization of preparation of biodiesel from L.seed

WANG Rui, YANG Song, YIN Shitao, SONG Baoan, BHADURY Pinaki S., XUE Wei, TAO Shuwei, JIA Zhaohui, LIU Da, GAO Liang

期刊论文

Efficient MgO-doped CaO sorbent pellets for high temperature CO

Zhihong Xu, Tao Jiang, Hao Zhang, Yujun Zhao, Xinbin Ma, Shengping Wang

期刊论文

experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-based CO2 capture sorbents

期刊论文

A review on research and development of iron-based sorbents for removal of hydrogen sulfide from hot

Jianglong YU, Liping CHANG, Fan LI, Kechang XIE

期刊论文

Operando modeling and measurements: Powerful tools for revealing the mechanism of alkali carbonate-based sorbents

期刊论文

Effects of MgO promoter on properties of Ni/Al2O3 catalysts for partial oxidation of methane to syngas

QIU Yejun, CHEN Jixiang, ZHANG Jiyan

期刊论文

Sponge-based materials for oil spill cleanups: A review

Edward Mohamed Hadji, Bo Fu, Ayob Abebe, Hafiz Muhammad Bilal, Jingtao Wang

期刊论文

Encapsulation of 2-amino-2-methyl-1-propanol with tetraethyl orthosilicate for CO2 capture

Sidra Rama, Yan Zhang, Fideline Tchuenbou-Magaia, Yulong Ding, Yongliang Li

期刊论文