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Stability of Ni/SiO

Bettina Stolze,Juliane Titus,Stephan A. Schunk,Andrian Milanov,Ekkehard Schwab,Roger Gläser

《化学科学与工程前沿（英文）》 2016年第10卷第2期页码 281-293 doi: 10.1007/s11705-016-1568-0

摘要： Ni/SiO -ZrO catalysts with Ni loadings of 1 to 13 wt-% were prepared, characterized by elemental analysis, X-ray diffraction, N sorption, temperature programmed oxidation, temperature programmed reduction, and tested for their activity and stability in the dry reforming of methane with carbon dioxide at 850 °C, gas hourly space velocity of 6000 and 1800 h and atmospheric pressure. The SiO -ZrO support as obtained through a simple and efficient sol-gel synthesis is highly porous ( = 90 m ·g , = 4.4 nm) with a homogeneously distributed Si-content of 3 wt-%. No loss of Si or formation of monoclinic ZrO , even after steaming at 850 °C for 160 h, was detectable. The catalyst with 5 wt-% Ni loading in its fully reduced state is stable over 15?h on-stream in the dry reforming reaction. If the catalyst was not fully reduced, a reduction during the early stages of dry reforming is accompanied by the deposition of up to 44 mg·g carbon as shown by experiments in a magnetic suspension balance. Rapid coking occurs for increased residence times and times-on-stream starting at 50 h. The Ni loading of 5 wt-% on SiO -ZrO was shown to provide an optimal balance between activity and coking tendency.

关键词： Ni/SiO₂-ZrO₂ synthesis gas dry reforming coking steaming

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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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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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The kinetic study of light alkene syntheses by CO 2 hydrogenation over Fe-Ni catalysts

Yaling ZHAO, Li WANG, Xiwei HAO, Jiazhou WU,

《化学科学与工程前沿（英文）》 2010年第4卷第2期页码 153-162 doi: 10.1007/s11705-009-0241-2

摘要： A kinetics model of CO hydrogenation over iron-nickel catalysts was developed based on the detailed mechanism of alkenes re-adsorption and secondary reaction. The corresponding kinetical experiments are conducted in a continuous fixed bed reactor. The effect of reaction conditions on catalyst performance was analyzed according to the results of orthogonal experiments. The results of the experiments show that more methane in products can be obtained with iron-nickel catalysts, the trend of which is consistent with the thermodynamic analysis. However, the content of alkenes in products is equivalent with that of alkanes. This shows that the reaction is controlled by kinetics. In all, the results of the experiments also substantiate that the model can give a good representation of the reaction mechanism of CO hydrogenation over iron-nickel catalysts. The parameters of this model give a better explanation for the question why the iron-nickel catalysts have a higher selectivity toward alkenes compared with other iron-based catalysts.

关键词： representation corresponding orthogonal thermodynamic consistent

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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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Corrosion behavior of Fe–Cr–Ni based alloys exposed to molten MgCl₂–KCl–NaCl salt with over-added

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1608-1619 doi: 10.1007/s11705-023-2349-1

摘要： MgCl₂–NaCl–KCl salts mixture shows great potential as a high-temperature (> 700 °C) thermal energy storage material in next-generation concentrated solar power plants. Adding Mg into molten MgCl₂–NaCl–KCl salt as a corrosion inhibitor is one of the most effective and cost-effective methods to mitigate the molten salt corrosion of commercial Fe–Cr–Ni alloys. However, it is found in this work that both stainless steel 310 and Incoloy 800H samples were severely corroded after 500 h immersion test at 700 °C when the alloy samples directly contacted with the over-added Mg in the liquid form. The corrosion attack is different from the classical impurity-driven corrosion in molten chloride salts found in previous work. Microscopic analysis indicates that Ni preferentially leaches out of alloy matrix due to the tendency to form MgNi₂/Mg₂Ni compounds. The Ni-depletion leads to the formation of a porous corrosion layer on both alloys, with the thickness around 204 µm (stainless steel 310) and 1300 µm (Incoloy 800H), respectively. These results suggest that direct contact of liquid Mg with Ni-containing alloys should be avoided during using Mg as a corrosion inhibitor for MgCl₂–NaCl–KCl or other chlorides for high temperature heat storage and transfer.

关键词： concentrated solar power (CSP) Mg corrosion inhibitor Mg–Ni intermetallic salt purification thermal energy storage (TES)

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and bacteriophage MS2 disinfection by UV, ozone and the combined UV and ozone processes

Jingyun FANG,Huiling LIU,Chii SHANG,Minzhen ZENG,Mengling NI,Wei LIU

《环境科学与工程前沿（英文）》 2014年第8卷第4期页码 547-552 doi: 10.1007/s11783-013-0620-2

摘要： The combination of low-dose ozone with ultraviolet (UV) irradiation should be an option to give benefit to disinfection and reduce drawbacks of UV and ozone disinfection. However, less is known about the disinfection performance of UV and ozone (UV/ozone) coexposure and sequential UV-followed-by-ozone (UV-ozone) and ozone-followed-by-UV (ozone-UV) exposures. In this study, inactivation of and bacteriophage MS2 by UV, ozone, UV/ozone coexposure, and sequential UV-ozone and ozone-UV exposures was investigated and compared. Synergistic effects of 0.5–0.9 log kill on inactivation, including increases in the rate and efficiency, were observed after the UV/ozone coexposure at ozone concentrations as low as 0.05 mg·L in ultrapure water. The coexposure with 0.02-mg·L ozone did not enhance the inactivation but repressed photoreactivation. Little enhancement on inactivation was found after the sequential UV-ozone or ozone-UV exposures. The synergistic effect on MS2 inactivation was less significant after the UV/ozone coexposure, and more significant after the sequential ozone-UV and UV-ozone exposures, which was 0.2 log kill for the former and 0.8 log kill for the latter two processes, at ozone dose of 0.1 mg·L and UV dose of 8.55 mJ·cm in ultrapure water. The synergistic effects on disinfection were also observed in tap water. These results show that the combination of UV and low-dose ozone is a promising technology for securing microbiological quality of water.

关键词： bacteria inactivation photoreactivation water disinfection UV ozone

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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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Preparation of Ni/SiO catalyst in ionic liquids for hydrogenation

FAN Qingming, LIU Yingxin, ZHENG Yifan, YAN Wei

《化学科学与工程前沿（英文）》 2008年第2卷第1期页码 63-68 doi: 10.1007/s11705-008-0013-4

摘要： A series of silica supported nickel catalysts were prepared from nickel nitrate and tetraethyl orthosilicate by the sol-gel method with the imidazolium type ionic liquids as solvents. The catalysts were characterized by means of X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). Their catalytic performances for the selective hydrogenation of cinnamaldehyde to hydrocinnamaldehyde were investigated. The results show that the Ni/SiO catalyst prepared with 1-(2-hydroxyethyl)-3-methyl-imidazole tetrafluoroborate ionic liquid as solvent exhibits the highest catalytic activity for the reaction. Under the optimal conditions of catalyst dosage (based on the mass of cinnamaldehyde used) 10%, reaction pressure 2 MPa, temperature 373 K and reaction time 2 h, the conversion of cinnamaldehyde and the selectivity to hydrocinnamaldehyde can reach 97.6% and 98.8%, respectively.

关键词： dispersive conversion catalytic 2-hydroxyethyl catalytic activity

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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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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

《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 (M_xNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The M_xNi-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 M_xNi-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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Roles of various Ni species on TiO

Xiaoping CHEN, Jihai XIONG, Jinming SHI, Song XIA, Shuanglin GUI, Wenfeng SHANGGUAN

《能源前沿（英文）》 2019年第13卷第4期页码 684-690 doi: 10.1007/s11708-018-0585-8

摘要： Low-cost nickels can be used as cocatalyst to improve the performance of photocatalysts, which may be promising materials applied in the field of photocatalytic water splitting. In this study, different nickel species Ni, Ni(OH) , NiO, NiO , and NiS are used to modified titanium dioxide (P25) to investigate their roles on the photocatalytic hydrogen evolution activities. UV-visible, X-ray diffraction (XRD), Brunner-Emmet-Teller (BET) measurements, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) analysis etc. are employed to characterize the physical and chemical properties of catalysts. The results indicate that all the nickel species can improve the photocatalytic hydrogen production activity of P25. The P25 modified with NiO and NiS has more superior photocatalytic hydrogen evolution activities than those modified with other nickel species. The reason for this is that NiO and NiS can form p-n junctions with P25 respectively. In addition, NiO can be selectively deposited on the active sites of P25 via the photodeposition method and NiS is beneficial for H reacting with photo-excited electrons.

关键词： nickel species TiO₂ photocatalytic hydrogen evolution

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Efficient degradation of orange II by ZnMn

Qingzhuo Ni, Hao Cheng, Jianfeng Ma, Yong Kong, Sridhar Komarneni

《化学科学与工程前沿（英文）》 2020年第14卷第6期页码 956-966 doi: 10.1007/s11705-019-1907-z

摘要： A ZnMn O catalyst has been synthesized via a sucrose-aided combustion method and characterized by various analytical techniques. It is composed of numerous nanoparticles (15–110 nm) assembled into a porous structure with a specific surface area (SSA) of 19.1 m ·g . Its catalytic activity has been investigated for the degradation of orange II dye using three different systems, i.e., the photocatalysis system with visible light, the chemocatalysis system with bisulfite, and the photo-chemical catalysis system with both visible light and bisulfite. The last system exhibits the maximum degradation efficiency of 90%, much higher than the photocatalysis system (15%) and the chemocatalysis system (67%). The recycling experiments indicate that the ZnMn O catalyst has high stability and reusability and is thus a green and eximious catalyst. Furthermore, the potential degradation mechanisms applicable to the three systems are discussed with relevant theoretical analysis and scavenging experiments for radicals. The active species such as Mn(III), O , h , e , SO and HO are proposed to be responsible for the excellent degradation results in the photo-chemical catalysis system with the ZnMn O catalyst.

关键词： ZnMn₂O₄ photo-chemical catalysis bisulfite dye degradation

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铝电解用Fe-Ni-Co-Al₂O₃金属陶瓷惰性阳极

邱竹贤,石忠宁,徐君莉

《中国工程科学》 2004年第6卷第8期页码 35-39

摘要：

研制了一种新型铝电解金属陶瓷惰性阳极，阳极基体由Fe-Ni-CoAl₂O₃构成。在石墨坩埚中，960℃温度下，电解质中的氧化铝质量分数为6.0%，摩尔比为2.6；阳极电流密度为1.0 A/cm²，阳极尺寸大小为120 mm×80 mm×mm，石墨阴极尺寸大小为120 mm×40 mm×20 mm，通入的直流电为100～300 A，电解时间各为10 h；实验所得的电解铝产品纯度达到98%以上，杂质主要为Fe，Ni阳极的反电动势为2.45 V，比理论分解电压仅高出0.25 V证明该阳极为惰性阳极，在电解槽中进行的是Al₂O₃的分解反应。

关键词：铝电解惰性阳极反电动势