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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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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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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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Impact of Ni particle size on CO activation and CO formation during reforming process: A density functional

《能源前沿（英文）》 2024年 第18卷 第4期   页码 525-534 doi: 10.1007/s11708-024-0952-6

摘要： In recent years, the dry reforming of methane (DRM) reaction has gained widespread attention due to its effective utilization of two major greenhouse gases. Supported Ni-based catalysts for DRM exhibit a strong dependence on particle size, however, the reaction mechanisms involved remain unclear. In this work, the effect of metal particle size on CO2 activation and CO formation was explored in the DRM reaction using the density functional theory. Nix/MgO (x = 13, 25, 37) was constructed to investigate the CO2 activation and the formation of CO during the DRM reaction. It is found that CO2 is more inclined to undergo chemisorption on Nix/MgO before activation. With the variation in particle size, the main activation pathway of CO2 on the catalyst changes. On the smallest Ni13/MgO, CO2 tends to directly dissociate, while on the larger Ni25/MgO and Ni37/MgO, the hydrogenation dissociation of CO2 is more kinetically favorable. Compared to Ni13/MgO and Ni37/MgO, the oxidation of surface C atoms and the oxidation of CH occur more readily on Ni25/MgO. This indicates that C atoms are less likely to form on Ni25 particle and are more easily to be oxidized. To some extent, the results suggest that Ni25/MgO exhibits superior resistance to carbon formation.

关键词： particle size     Ni/MgO catalyst     CO2 activation     CO formation    

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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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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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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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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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The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 397-407 doi: 10.1007/s11705-021-2076-4

摘要： The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of biomass. Herein, a series of Ni-doped PtSn catalysts were prepared, characterized and studied in the hydrogenation of acetic acid. The Ni dopant has a strong interaction with Pt, which promotes the hydrogen adsorption, providing an activated hydrogen-rich environment for the hydrogenation. Meanwhile, the presence of Ni also improves the Pt dispersion, giving more accessible active sites for hydrogen activation. The cooperation of Pt and Ni significantly promotes the catalytic activity of the hydrogenation of acetic acid to ethanol. As a result, the catalyst with 0.1% Ni exhibits the best reaction activity, and its space time yield is twice as that of the PtSn/SiO2 catalyst. It provides a meaningful instruction on the catalyst design for the carboxylic acid hydrogenation.

关键词： acetic acid     ethanol     hydrogenation     Pt     Ni     cooperation effect    

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Single-Ni-atoms on nitrogenated humic acid based porous carbon for CO electroreduction

《化学科学与工程前沿（英文）》 2024年 第18卷 第5期 doi: 10.1007/s11705-024-2411-7

摘要： We proposed a facile synthesis of single-Ni-atom catalysts on low-cost porous carbon using a calcination method at the temperatures of 850–1000 °C, which were used for CO2 electrochemical reduction to CO. The porous carbon was prepared by carbonizing cheap and abundant humic acid. The structural characterizations of the as-synthesized catalysts and their electrocatalytic performances were analyzed. The results showed that the single-Ni-atom catalyst activated at 950 °C showed an optimum catalytic performance, and it reached a CO Faradaic efficiency of 91.9% with a CO partial current density of 6.9 mA·cm−2 at −0.9 V vs. reversible hydrogen electrode (RHE). Additionally, the CO Faradaic efficiency and current density of the optimum catalyst changed slightly after 8 h of continuous operation, suggesting that it possessed an excellent stability. The structure-activity relations indicate that the variation in the CO2 electrochemical reduction performance for the as-synthesized catalysts is ascribed to the combined effects of the increase in the content of pyrrolic N, the evaporation of Ni and N, the decrease in pore volume, and the change in graphitization degree.

关键词： CO2 electroreduction     single-Ni-atom catalysts     humic acid based porous carbon    

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Pt-Ni nanourchins as electrocatalysts for oxygen reduction reaction

Qiaowan CHANG, Yuan XU, Shangqian ZHU, Fei XIAO, Minhua SHAO

《能源前沿（英文）》 2017年 第11卷 第3期   页码 254-259 doi: 10.1007/s11708-017-0493-3

摘要： Pt-Ni bimetallic alloys with various nanostructures have shown excellent activity toward oxygen reduction reaction (ORR). The ORR activity is highly dependent on the structure of the catalyst. In this paper, Pt-Ni nanourchins were synthesized with an average size of 50 nm consisting of 10–20 nanorods and nanooctahedra by adjusting the synthesis condition. The formation of Pt-Ni nanourchins is mainly dependent on the adding order of solvents (benzyl ether, oleylamine and oleic acid). Pt-Ni nanourchins present a reasonable high ORR activity (0.81 A/mg at 0.9 V).

关键词： Pt-Ni alloys     nanourchins     oxygen reduction reaction     shape control     fuel cells    

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Breaking the Ni loading-reducibility-dispersion dependence achieved by solid-state co-grinding

《化学科学与工程前沿（英文）》 2024年 第18卷 第12期 doi: 10.1007/s11705-024-2499-9

摘要： The loading-dispersion-reducibility dependence has always been one of the most critical issues in the development of high-performance supported metal catalysts. Herein, up to 40 wt % NiO over ordered mesoporous alumina (OMA) was prepared by co-grinding the hybrid of template-containing OMA and Ni(NO3)2·6H2O. Characterization results confirmed that the OMA mesostructure was still preserved even after loading NiO at a content as high as 40 wt %. More importantly, the reduction extent, dispersion, and average particle size of the Ni/OMA catalysts were maintained at ≥ 91.0%, ~13.5%, and ~4.0–5.0 nm, respectively, when the NiO loading was increased from 20 to 40 wt %. The catalysts were evaluated for the CO methanation as a model reaction, and the similarly high turnover frequency of 24.0 h–1 was achieved at 300 °C for all of the Ni/OMA catalysts. For the catalyst with the highest NiO loading of 40 wt % (40Ni/OMA), the low-temperature activity at 300 °C indexed by the space-time yield of methane (over 325.8 molCH4⋅kgcat−1⋅h−1) was achieved, while the catalyst was operated without an observable deactivation for a time on stream of 120 h under severe reaction conditions of 600 °C and a very high gas hourly space velocity of 240000 mL·g–1·h–1. With these significant results, this work paves the way for a rational and controllable design of supported Ni catalysts by breaking the loading-dispersion-reducibility dependence and stabilizing Ni nanoparticles under harsh reaction conditions.

关键词： Ni-supported catalyst     solid-state grinding     metal-support interactions     high Ni loading     high dispersion     CO methanation    

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Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

《环境科学与工程前沿（英文）》 2016年 第10卷 第6期 doi: 10.1007/s11783-016-0872-8

摘要： ? The Cu–Ni/γ-Al O catalyst was prepared to study HCN hydrolysis ? On catalyst calcined at 400°C, the HCN removal efficiency reaches a maximum. ? HCN removal is the highest at 480 min at a H O/HCN volume ratio of 150 ? The presence of CO facilitates HCN hydrolysis and increases NH production. ? O increases the HCN removal and NO production but decreases NH production GRAPHIC ABSTRACT To decompose efficiently hydrogen cyanide (HCN) in exhaust gas, g-Al O -supported bimetallic-based Cu–Ni catalyst was prepared by incipient-wetness impregnation method. The effects of the calcination temperature, H O/HCN volume ratio, reaction temperature, and the presence of CO or O on the HCN removal efficiency on the Cu–Ni/g-Al O catalyst were investigated. To examine further the efficiency of HCN hydrolysis, degradation products were analyzed. The results indicate that the HCN removal efficiency increases and then decreases with increasing calcination temperature and H O/HCN volume ratio. On catalyst calcined at 400°C, the efficiency reaches a maximum close to 99% at 480 min at a H O/HCN volume ratio of 150. The HCN removal efficiency increases with increasing reaction temperature within the range of 100°C–500°C and reaches a maximum at 500°C. This trend may be attributed to the endothermicity of HCN hydrolysis; increasing the temperature favors HCN hydrolysis. However, the removal efficiencies increases very few at 500°C compared with that at 400°C. To conserve energy in industrial operations, 400°C is deemed as the optimal reaction temperature. The presence of CO facilitates HCN hydrolysis andincreases NH production. O substantially increases the HCN removal efficiency and NO production but decreases NH production.

关键词： Hydrogen cyanide     Cu–Ni/g-Al2O3     Catalytic hydrolysis    

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Emergy evaluation of polygeneration systems

WANG Lingmei, LI Zheng, NI Weidou

《能源前沿（英文）》 2007年 第1卷 第2期   页码 223-227 doi: 10.1007/s00000-007-0030-x

摘要： To expand the application range of the emergy evaluation method, an emergy evaluation index, which can reflect the particular feature of polygeneration systems, has been elaborated on the basis of energy and emergy conservation, guided by the fundamental principle of emergy analysis. With this index, the cost structure, emission effect and energy saved were all considered on the same level of importance. To exemplify, some power polygeneration systems (methanol-power generation, hydrogen-power generation) are considered using coal as the basic fuel. The results showed that emergy evaluation indices are practical for comprehensively evaluating polygeneration systems and their sustainability, which is influenced by such factors as the joining mode of polygeneration and the technologies used. The sustainability of polygeneration systems, which work on an appropriate ratio of fuel-to-electric power basis, is higher than that of singular production systems.

关键词： fuel-to-electric     sustainability     importance     polygeneration     practical    

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Removal of Ni(II) ions from wastewater by micellar enhanced ultrafiltration using mixed surfactants

Amar D. Vibhandik, Kumudini V. Marathe

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 79-86 doi: 10.1007/s11705-014-1407-0

摘要： Ni(II) ions were removed from aqueous waste using micellar enhanced ultrafiltration (MEUF) with a mixture of surfactants. The surfactant mixture was the nonionic surfactant Tween 80 (TW80) mixed with the anionic surfactant sodium dodecyl sulfate (SDS) in different molar ratios ranging from 0.1–1.5. The operational variables of the MEUF process such as pH, applied pressure, surfactant to metal ion ratio and nonionic to ionic surfactant molar ratio (α) were evaluated. Rejection of Ni and TW80 was 99% and 98% respectively whereas that for SDS was 65%. The flux and all resistances (fouling resistance, resistance due to concentration polarization) were measured and calculated for entire range of α respectively. A calculated flux was found to be declined with time, which was mainly attributed to concentration polarization rather than resistance from membrane fouling.

关键词： MEUF     Ni (II) ions     membrane resistance     concentration polarization     mixed surfactants    

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标题 作者 时间 类型 操作

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

Yan LI,Zhehao WEI,Yong WANG

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

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

Impact of Ni particle size on CO activation and CO formation during reforming process: A density functional

期刊论文

Methane partial oxidation over NiO-MgO/Ce

Piyawat PUE-ON, Vissanu MEEYOO, Thirasak RIRKSOMBOOON

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

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

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

The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

期刊论文

Single-Ni-atoms on nitrogenated humic acid based porous carbon for CO electroreduction

期刊论文

Pt-Ni nanourchins as electrocatalysts for oxygen reduction reaction

Qiaowan CHANG, Yuan XU, Shangqian ZHU, Fei XIAO, Minhua SHAO

期刊论文

Breaking the Ni loading-reducibility-dispersion dependence achieved by solid-state co-grinding

期刊论文

Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

期刊论文

Emergy evaluation of polygeneration systems

WANG Lingmei, LI Zheng, NI Weidou

期刊论文

Removal of Ni(II) ions from wastewater by micellar enhanced ultrafiltration using mixed surfactants

Amar D. Vibhandik, Kumudini V. Marathe

期刊论文