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Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 443-460 doi: 10.1007/s11705-021-2079-1

摘要： Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n-pentadecane and n-C6–n-C16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO2 recovered the catalyst reactivity.

关键词： Stöber method     carbon-coated Ni-Co alloy     in-situ hydrodeoxygenation     methyl palmitate     decarbonylation/decarboxylation    

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Carbon-coated lithium titanate: effect of carbon precursor addition processes on the electrochemical

Shilei Ding, Zelong Jiang, Jing Gu, Hongliang Zhang, Jiajia Cai, Dongdong Wang

《化学科学与工程前沿（英文）》 2021年 第15卷 第1期   页码 148-155 doi: 10.1007/s11705-020-2022-x

摘要： In this paper, two carbon-coated lithium titanate (LTO-C1 and LTO-C2) composites were synthesized using the ball-milling-assisted calcination method with different carbon precursor addition processes. The physical and electrochemical properties of the as-synthesized negative electrode materials were characterized to investigate the effects of two carbon-coated LTO synthesis processes on the electrochemical performance of LTO. The results show that the LTO-C2 synthesized by using Li CO and TiO as the raw materials and sucrose as the carbon source in a one-pot method has less polarization during lithium insertion and extraction, minimal charge transfer impedance value and the best electrochemical performance among all samples. At the current density of 300 mA·h·g , the LTO-C2 composite delivers a charge capacity of 126.9 mA·h·g , and the reversible capacity after 300 cycles exceeds 121.3 mA·h·g in the voltage range of 1.0–3.0 V. Furthermore, the electrochemical impedance spectra show that LTO-C2 has higher electronic conductivity and lithium diffusion coefficient, which indicates the advantages in electrode kinetics over LTO and LTO-C1. The results clarify the best electrochemical properties of the carbon-coated LTO-C2 composite prepared by the one-pot method.

关键词： lithium titanate     carbon-coated     carbon precursor     synthetic process    

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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production ofsyngas with potential-independent CO/H ratios

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO2-H2O into CO-H2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H2 ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (MxNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The MxNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H2 ratios, from 0.5:1 to 3.4:1, can be produced on MxNi-NCNT. More importantly, stable CO/H2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co1Ni-NCNT and Co2Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H2 ratio from electrochemical CO2 reduction.

关键词： electrochemical reduction of CO2     syngas     N-doped carbon nanotubes     encapsulated alloy nanoparticles     CO/H2 ratio    

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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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Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 613-623 doi: 10.1007/s11705-017-1664-9

摘要： Carbon deposition and sintering of active components such as nano particles are great challenges for Ni-based catalysts for CO methanation to generate synthetic natural gas from syngas. Facing the challenges, bimetallic catalysts with different Fe content derived from layered double hydroxide containing Ni, Fe, Mg, Al elements were prepared by co-precipitation method. Nanoparticles of Ni-Fe alloy were supported on mixed oxides of aluminium and magnesium after calcination and reduction. The catalysts were characterized by Brunner-Emmett-Teller (BET), X-ray diffraction, hydrogen temperature programmed reduction, inductively coupled plasma, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric techniques, and their catalytic activity for CO methanation was investigated. The results show that the Ni-Fe alloy catalysts exhibit better catalytic performance than monometallic catalysts except for the Ni4Fe-red catalyst. The Ni2Fe-red catalyst shows the highest CO conversion (100% at 260–350 °C), as well as the highest CH selectivity (over 95% at 280–350 °C), owing to the formation of Ni-Fe alloy. In stability test, the Ni2Fe-red catalyst exhibits great improvement in both anti-sintering and resistance to carbon formation compared with the Ni0Fe-red catalyst. The strong interaction between Ni and Fe element in alloy and surface distribution of Fe element not only inhibits the sintering of nanoparticles but restrains the formation of Ni clusters.

关键词： methanation     layered double hydroxide     bimetal Ni-Fe alloy     sintering     carbon deposition    

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3D Network nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly active

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 417-424 doi: 10.1007/s11705-018-1711-1

摘要：

A highly active bi-functional electrocatalyst towards both hydrogen and oxygen evolution reactions is critical for the water splitting. Herein, a self-supported electrode composed of 3D network nanostructured NiCoP nanosheets grown on N-doped carbon coated Ni foam (NiCoP/NF@NC) has been synthesized by a hydrothermal route and a subsequent phosphorization process. As a bifunctional electrocatalyst, the NiCoP/NF@NC electrode needs overpotentials of 31.8 mV for hydrogen evolution reaction and 308.2 mV for oxygen evolution reaction to achieve the current density of 10 mA·cm−2 in 1 mol·L−1 KOH electrolyte. This is much better than the corresponding monometal catalysts of CoP/NF@NC and NiP/NF@NC owing to the synergistic effect. NiCoP/NF@NC also exhibits low Tafel slope, and excellent long-term stability, which are comparable to the commercial noble catalysts of Pt/C and RuO2.

关键词： bimetallic phosphides     N-doped carbon     self-support     hydrogen evolution     oxygen evolution    

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Phosphorus-doped Ni–Co sulfides connected by carbon nanotubes for flexible hybrid supercapacitor

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 491-503 doi: 10.1007/s11705-022-2257-9

摘要： As promising electrode materials for supercapacitors, nickel-cobalt bimetallic sulfides render the advantages of abundant redox reactions and inherently high conductivity. However, in general, unsatisfactory performance of low specific capacity, low rate capability, and fast capacity loss exist in Ni–Co sulfide electrodes. Herein, we rationally regulate phosphorus-doped nickel–cobalt sulfides (P-NCS) to enhance the electrochemical performance by gas–solid phosphorization. Moreover, carbon nanotubes (CNTs) as conductive additives are added to improve the cycle stability and conductivity and form the composite P-NCS/C/CNT. According to density functional theory, more electrons near the Fermi surface of P-NCS are demonstrated notionally than those of simple CoNi2S4. Electrochemical results manifest that P-NCS/C/CNT exhibits superior electrochemical performance, e.g., high specific capacity (932.0 C∙g‒1 at 1 A∙g‒1), remarkable rate capability (capacity retention ratio of 69.1% at 20 A∙g‒1), and lower charge transfer resistance. More importantly, the flexible hybrid asymmetric supercapacitor is assembled using P-NCS/C/CNT and activated carbon, which renders an energy density of 34.875 W·h∙kg‒1 at a power density of 375 W∙kg‒1. These results show that as-prepared P-NCS/C/CNT demonstrates incredible possibility as a battery-type electrode for high-performance supercapacitors.

关键词： cobalt nickel sulfide     phosphorus-doping     hybrid supercapacitor     carbon nanotube     density functional theory    

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Synergistic utilization of coal and other energy – Key to low carbon economy

Weidou NI, Zhen CHEN

《能源前沿（英文）》 2011年 第5卷 第1期   页码 1-19 doi: 10.1007/s11708-010-0136-4

摘要： In China, coal is a dominant component of energy mix, and it is expected to remain as such over the next 30 to 40 years. Coal is expected to be used even more in power generation. The direct combustion of coal already has been causing severe pollution and ecological degradation, and it is quite difficult to address the need to reduce greenhouse gas (GHG) given the direct combustion of coal. Therefore, the polygeneration system based on coal gasification, which is one of the major examples of synergistic utilization of coal, is proposed. It is a comprehensive solution to meet the energy challenges China is facing. Furthermore, the synergy of fossil fuels (especially coal) with renewable energy, the synergy of different kinds of energy for energy storage, the synergy of centralized and distributed supply of different kinds of energy, and the synergy of different kinds of energy in smart energy grid (power, gas, heat, and water) are the keys to making China a low-carbon economy. Carbon dioxide (CO ) mitigation in China should begin from the coal-chemical industry given their accumulated relevant experiences. The mitigation process should gradually be transformed into the “IGCC+ polygeneration+ CCUS”. The objectives of this paper are to describe the synergistic utilization of coal, and to analyze the synergy of coal with other energy resources, and to propose the scientific and technological problems to achieve these synergies.

关键词： synergy     clean and efficient utilization of coal     coal-based polygenration     CO2 mitigation     energy storage    

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Performance of activated carbon coated graphite bipolar electrodes on capacitive deionization method

Hossein D. Atoufi, Hasti Hasheminejad, David J. Lampert

《环境科学与工程前沿（英文）》 2020年 第14卷 第6期 doi: 10.1007/s11783-020-1278-1

摘要： Abstract • Graphite bipolar electrodes act as an appropriate bed for the CDI process. • Activated carbon Coating improves the application of the electrodes. • CDI is an environmentally friendly method to apply for brackish water. • Initial concentration is the most important parameter in the CDI method. • CDI process in a batch-mode setup needs more development. This research investigates a capacitive deionization method for salinity reduction in a batch reactor as a new approach for desalination. Reductions of cost and energy compared with conventional desalination methods are the significant advantages of this approach. In this research, experiments were performed with a pair of graphite bipolar electrodes that were coated with a one-gram activated carbon solution. After completing preliminary tests, the impacts of four parameters on electrical conductivity reduction, including (1) the initial concentration of feed solution, (2) the duration of the tests, (3) the applied voltage, and (4) the pH of the solution, were examined. The results show that the maximum efficiency of electrical conductivity reduction in this laboratory-scale reactor is about 55%. Furthermore, the effects of the initial concentration of feed solution are more significant than the other parameters. Thus, using the capacitive deionization method for water desalination with low and moderate salt concentrations (i.e., brackish water) is proposed as an affordable method. Compared with conventional desalination methods, capacitive deionization is not only more efficient but also potentially more environmentally friendly.

关键词： Capacitive deionization (CDI)     Desalination     Electrical conductivity (EC)     Graphite bipolar electrode     Activated carbon coated (ACC)    

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Ni/MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performancefor carbon dioxide reforming of methane

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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高酸性腐蚀气田用BG2250-125镍基合金油管开发

沈琛,张忠铧,张春霞

《中国工程科学》 2010年 第12卷 第10期   页码 35-38

摘要：

综述了高酸性腐蚀气田用BG2250镍基合金油井管国产化开发进展情况。通过与国外同类产品的实物质量分析以及成分、电弧炉冶炼、电渣重溶、锻造、热挤压、冷轧、特殊扣设计与加工、腐蚀评价等工艺技术的研究，宝钢开发的BG2250-125等镍基合金油管的产品质量达到了国际同类产品的先进水平，并已在普光气田成功下井使用，为我国高酸性气田的开发提供了重要的物资保障。

关键词： 镍基合金     油管     酸性井     产品性能    

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CO2 methanation and co-methanation of CO and CO2 over Mn-promoted Ni/Al2

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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environmental temperature and relative humidity on photocatalytic oxidation of toluene on activated carbonfibers coated TiO

GUO Ting, BAI Zhipeng, WU Can, ZHU Tan

《环境科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 224-229 doi: 10.1007/s11783-008-0039-3

摘要： TiO supported on active carbon fiber (TiO/ACF), an absorbable photocatalyst, is a new kind of material applied in air purification. In this paper, the influence of environmental temperature (T) and relative humidity (RH) on the gas-solid adsorption of toluene and the photocatalytic oxidation (PCO) efficiency of adsorbed toluene on TiO/ACF were studied, and then, the purification capability of TiO/ACF was estimated. PCO results showed that although the PCO efficiency increased under high RH and T levels, the amount of adsorption of toluene decreased. Moreover, quantitative analysis results of intermediates indicated that more environmental risk emerged when PCO of toluene was carried out at higher environmental T and RH levels because more toxic intermediates would be accumulated on the TiO/ACF. So, it is significant to control the environmental T and RH conditions in the application of the PCO technique. T = 25°C and RH = 30% is the optimal condition for purifying toluene in our experimental system.

关键词： application     gas-solid adsorption     technique     TiO/ACF     experimental    

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A coal-fired power plant integrated with biomass co-firing and CO capture for zero carbon emission

《能源前沿（英文）》 2022年 第16卷 第2期   页码 307-320 doi: 10.1007/s11708-021-0790-8

摘要： A promising scheme for coal-fired power plants in which biomass co-firing and carbon dioxide capture technologies are adopted and the low-temperature waste heat from the CO2 capture process is recycled to heat the condensed water to achieve zero carbon emission is proposed in this paper. Based on a 660 MW supercritical coal-fired power plant, the thermal performance, emission performance, and economic performance of the proposed scheme are evaluated. In addition, a sensitivity analysis is conducted to show the effects of several key parameters on the performance of the proposed system. The results show that when the biomass mass mixing ratio is 15.40% and the CO2 capture rate is 90%, the CO2 emission of the coal-fired power plant can reach zero, indicating that the technical route proposed in this paper can indeed achieve zero carbon emission in coal-fired power plants. The net thermal efficiency decreases by 10.31%, due to the huge energy consumption of the CO2 capture unit. Besides, the cost of electricity (COE) and the cost of CO2 avoided (COA) of the proposed system are 80.37 $/MWh and 41.63 $/tCO2, respectively. The sensitivity analysis demonstrates that with the energy consumption of the reboiler decreasing from 3.22 GJ/tCO2 to 2.40 GJ/ tCO2, the efficiency penalty is reduced to 8.67%. This paper may provide reference for promoting the early realization of carbon neutrality in the power generation industry.

关键词： coal-fired power plant     biomass co-firing     CO2 capture     zero carbon emission     performance evaluation    

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Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulatedNi–Sn intermetallic compounds with methanol as hydrogen donor

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 139-155 doi: 10.1007/s11705-022-2217-4

摘要： Porous carbon-encapsulated Ni and Ni–Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen donor. During the catalyst preparation, Sn doping reduces the size of carbon spheres, and the formation of Ni–Sn intermetallic compounds restrain the graphitization, contributing to larger pore volume and pore diameter. Consequently, a more facile mass transfer occurs in carbon-encapsulated Ni–Sn intermetallic compound catalysts than in carbon-encapsulated Ni catalysts. During the in-situ hydrothermal deoxygenation, the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to hexadecanol. At high reaction temperature, hexadecanol undergoes dehydrogenation–decarbonylation, generating n-pentadecane. Also, the C–C bond hydrolysis and methanation are suppressed on Ni–Sn intermetallic compounds, favorable for increasing the carbon yield and reducing the H2 consumption. The n-pentadecane and n-hexadecane yields reached 88.1% and 92.8% on carbon-encapsulated Ni3Sn2 intermetallic compound at 330 °C. After washing and H2 reduction, the carbon-encapsulated Ni3Sn2 intermetallic compound remains stable during three recycling cycles. This is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词： extended Stöber method     carbon encapsulated Ni–Sn intermetallic compounds     confinement     in-situ hydrothermal deoxygenation     hydrogenation     decarbonylation    

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标题 作者 时间 类型 操作

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation

期刊论文

Carbon-coated lithium titanate: effect of carbon precursor addition processes on the electrochemical

Shilei Ding, Zelong Jiang, Jing Gu, Hongliang Zhang, Jiajia Cai, Dongdong Wang

期刊论文

Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production ofsyngas with potential-independent CO/H ratios

期刊论文

Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

期刊论文

Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

期刊论文

3D Network nanostructured NiCoP nanosheets supported on N-doped carbon coated Ni foam as a highly active

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

期刊论文

Phosphorus-doped Ni–Co sulfides connected by carbon nanotubes for flexible hybrid supercapacitor

期刊论文

Synergistic utilization of coal and other energy – Key to low carbon economy

Weidou NI, Zhen CHEN

期刊论文

Performance of activated carbon coated graphite bipolar electrodes on capacitive deionization method

Hossein D. Atoufi, Hasti Hasheminejad, David J. Lampert

期刊论文

Ni/MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performancefor carbon dioxide reforming of methane

Yan LI,Zhehao WEI,Yong WANG

期刊论文

高酸性腐蚀气田用BG2250-125镍基合金油管开发

沈琛,张忠铧,张春霞

期刊论文

CO2 methanation and co-methanation of CO and CO2 over Mn-promoted Ni/Al2

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文

environmental temperature and relative humidity on photocatalytic oxidation of toluene on activated carbonfibers coated TiO

GUO Ting, BAI Zhipeng, WU Can, ZHU Tan

期刊论文

A coal-fired power plant integrated with biomass co-firing and CO capture for zero carbon emission

期刊论文

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulatedNi–Sn intermetallic compounds with methanol as hydrogen donor

期刊论文