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Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1311-1319 doi: 10.1007/s11705-022-2281-9

摘要： A reconstructed Cu–ZnO catalyst with improved stability was fabricated by organic acid treatment method for the liquid-phase hydrogenation of dimethyl succinate to 1,4-butanediol. According to the characterization results of the fresh Cu–ZnO and reconstructed Cu–ZnO, three different forms of ZnO were suggested to be presented on the catalysts: ZnO having strong interaction with Cu species, ZnO that weakly interacted with Cu species and isolated ZnO. The first form of ZnO was believed to be beneficial to the formation of efficient active site Cu+, while the latter two forms of ZnO took the main responsibility for the deactivation of Cu–ZnO catalysts in the liquid-phase hydrogenation of diesters. The reconstruction of the Cu–ZnO catalyst by the organic acid treatment method resulted in a new Cu–ZnO catalyst with more Cu+ and less ZnO species that leads to deactivation. Furthermore, the deactivation mechanism of Cu–ZnO catalysts in liquid-phase diester hydrogenation in continuous flow system was proposed: the deposition of the polyesters on the catalysts via transesterification catalyzed by weakly interacted ZnO and isolated ZnO leads to the deactivation. These results provided meaningful instructions for designing highly efficient Cu–Zn catalysts for similar ester hydrogenation systems.

关键词： liquid phase     hydrogenation     Cu–ZnO     deactivation mechanism     1     4-butanediol     diester    

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Deactivation and regeneration of TS-1/SiO

Hainan SHI, Yaquan WANG, Guoqiang WU, Wenping FENG, Yi Lin, Teng ZHANG, Xing JIN, Shuhai WANG, Xiaoxue WU, Pengxu YAO

《化学科学与工程前沿（英文）》 2013年 第7卷 第2期   页码 202-209 doi: 10.1007/s11705-013-1328-3

摘要： TS-1/SiO catalyst for the epoxidation of propylene with hydrogen peroxide in a fixed-bed reactor has been investigated. The catalyst activity decreases gradually with the online reaction time, but the selectivity of propylene epoxide is kept at about 93%. The fresh, deactivated and regenerated catalysts were characterized with X-ray diffraction, Fourier transform infrared spectroscopy, ultra-violet-visible diffuse reflectance, Brunner-Emmett-Teller method and thermogravimetric analysis, and the deactivated catalyst was regenerated with H O /methanol solution. Compared with the fresh catalyst, both the framework structure and the content of titanium in the framework of the deactivated and regenerated TS-1/SiO catalysts were not changed. The major reason of the catalyst deactivation was the blockage of the channels of the catalyst by bulky organic by-products, which covered the active centers of titanium in TS-1. The deposited materials on the deactivated TS-1/SiO catalyst could be removed by treatment with hydrogen peroxide/methanol solution or pure methanol; the higher the treatment temperature and the higher the concentration of H O in methanol, the higher the extent of the regeneration. The regeneration treatment did not influence the product selectivity in the propylene epoxidation.

关键词： TS-1/SiO2     epoxidation of propylene     fixed-bed reactor     deactivation     regeneration    

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Catalysis and deactivation of montmorillonite K10 in the aryl O -glycosylation of glycosyl trichloroacetoimidates

Xiaoliu LI, Xinhao YAN, Zhiwei LI, Hua CHEN, Pingzhu ZHANG,

《化学科学与工程前沿（英文）》 2010年 第4卷 第3期   页码 342-347 doi: 10.1007/s11705-009-0279-1

摘要： The catalysis of montmorillonite K10 (MK10) for aryl -glycosylation of glycosyl trichloroacetimidates was investigated. It was found that the catalyst MK10 is deactivated gradually in the recycle glycosylation. The fresh and the deactivated catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Thermogravimetric analysis (TGA), and N adsorption-desorption. The results show that the eliminated trichloroacetamide molecule deposits on the MK10, which blocks and poisons the active sites, resulting in the deactivation of the catalyst. The regeneration of the deactivated MK10 by calcination was studied preliminarily.

关键词： photoelectron spectroscopy     adsorption-desorption     glycosylation     deactivated     diffraction    

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Chemical deactivation of V

Xiaodong WU, Wenchao YU, Zhichun SI, Duan WENG

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 420-427 doi: 10.1007/s11783-013-0489-0

摘要： V O -WO /TiO catalyst was poisoned by impregnation with NH Cl, KOH and KCl solution, respectively. The catalysts were characterized by X-ray diffraction (XRD), inductively coupled plasma (ICP), N physisorption, Raman, UV-vis, NH adsorption, temperature-programmed reduction of hydrogen (H -TPR), temperature-programmed oxidation of ammonia (NH -TPO) and selective catalytic reduction of NO with ammonia (NH -SCR). The deactivation effects of poisoning agents follow the sequence of KCl>KOH>>NH Cl. The addition of ammonia chloride enlarges the pore size of the titania support, and promotes the formation of highly dispersed V=O vanadyl which improves the oxidation of ammonia and the high-temperature SCR activity. K ions are suggested to interact with vanadium and tungsten species chemically, resulting in a poor redox property of catalyst. More importantly, potassium can reduce the Br?nsted acidity of catalysts and decrease the stability of Br?nsted acid sites significantly. The more severe deactivation of the KCl-treated catalyst can be mainly ascribed to the higher amount of potassium resided on catalyst.

关键词： V2O5-WO3/TiO2     potassium chloride     poisoning     reducibility     acid sites    

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Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

《化学科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 38-46 doi: 10.1007/s11705-011-1167-z

摘要： An effective method for the regeneration of thermally deactivated commercial monolith SCR catalysts was investigated. Two types of regenerated solutions, namely NH Cl (1 mol/L) and dilute H SO (0.5 mol/L), were employed to treat the used catalyst. The effects of temperature and the regeneration process on the structural and textural properties of the catalysts were determined by X-ray diffraction, scanning electron microscopy, N adsorption/desorption, elemental analysis and Fourier transform infrared spectroscopy. The results suggest that the anatase phase of the used catalyst is maintained after exposure to high temperatures. Some of the catalytic activity was restored after regeneration. The catalyst regenerated by aqueous NH Cl had a higher activity than that of the catalyst treated by dilute H SO . The main reason is that the NH generated from the decomposition of NH Cl at high temperatures can be adsorbed onto the catalyst which promotes the reaction. The aggregated V O were partially re-dispersed during the regeneration process, and the intrinsic oxidation of ammonia with high concentrations of O is a factor that suppresses the catalytic activity.

关键词： V2O5-WO3/TiO2 catalysts     thermal deactivation     regeneration     NH4Cl     dilute H2SO4 solution    

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Influence evaluation of loading conditions during pressurized thermal shock transients based on thermal-hydraulics

Jinya KATSUYAMA, Shumpei UNO, Tadashi WATANABE, Yinsheng LI

《机械工程前沿（英文）》 2018年 第13卷 第4期   页码 563-570 doi: 10.1007/s11465-018-0487-9

摘要：

The thermal hydraulic (TH) behavior of coo-lant water is a key factor in the structural integrity assessments on reactor pressure vessels (RPVs) of pressurized water reactors (PWRs) under pressurized thermal shock (PTS) events, because the TH behavior may affect the loading conditions in the assessment. From the viewpoint of TH behavior, configuration of plant equipment and their dimensions, and operator action time considerably influence various parameters, such as the temperature and flow rate of coolant water and inner pressure. In this study, to investigate the influence of the operator action time on TH behavior during a PTS event, we developed an analysis model for a typical Japanese PWR plant, including the RPV and the main components of both primary and secondary systems, and performed TH analyses by using a system analysis code called RELAP5. We applied two different operator action times based on the Japanese and the United States (US) rules: Operators may act after 10 min (Japanese rules) and 30 min (the US rules) after the occurrence of PTS events. Based on the results of TH analysis with different operator action times, we also performed structural analyses for evaluating thermal-stress distributions in the RPV during PTS events as loading conditions in the structural integrity assessment. From the analysis results, it was clarified that differences in operator action times significantly affect TH behavior and loading conditions, as the Japanese rule may lead to lower stresses than that under the US rule because an earlier operator action caused lower pressure in the RPV.

关键词： structural integrity     reactor pressure vessel     pressurized thermal shock     thermal hydraulic analysis     pressurized water reactor     weld residual stress    

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Kinetic model for hydroisomerization reaction of C-aromatics

XU Ouguan, SU Hongye, JIN Xiaoming, CHU Jian

《化学科学与工程前沿（英文）》 2008年 第2卷 第1期   页码 10-16 doi: 10.1007/s11705-008-0015-2

摘要： Based on the reported reaction networks, a novel six-component hydroisomerization reaction network with a new lumped species including C-naphthenes and C-paraffins is proposed and a kinetic model for a commercial unit is also developed. An empirical catalyst deactivation function is incorporated into the model accounting for the loss in activity because of coke formation on the catalyst surface during the long-term operation. The Runge-Kutta method is used to solve the ordinary differential equations of the model. The reaction kinetic parameters are benchmarked with several sets of balanced plant data and estimated by the differential variable metric optimization method (BFGS). The kinetic model is validated by an industrial unit with sets of plant data under different operating conditions and simulation results show a good agreement between the model predictions and the plant observations.

关键词： ordinary differential     Runge-Kutta     catalyst deactivation     C-paraffins     optimization    

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Assessment indices for uniform and non-uniform thermal environments

ZHANG Yufeng, SUN Shufeng, ZHAO Rongyi

《能源前沿（英文）》 2008年 第2卷 第2期   页码 129-133 doi: 10.1007/s11708-008-0029-y

摘要： Different assessment indices for thermal environments were compared and selected for proper assessment of indoor thermal environments. 30 subjects reported their overall thermal sensation, thermal comfort, and thermal acceptability in uniform and non-uniform conditions. The results show that these three assessment indices provide equivalent evaluations in uniform environments. However, overall thermal sensation differs from the other two indices and cannot be used as a proper index for the evaluation of non-uniform environments. The relationship between the percentage and the mean vote for each index is established.

关键词： thermal sensation     proper assessment     relationship     equivalent     thermal acceptability    

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Liquid metal thermal hydraulics R&D at European scale: achievements and prospects

《能源前沿（英文）》 2021年 第15卷 第4期   页码 842-853 doi: 10.1007/s11708-021-0743-2

摘要： A significant role for a future nuclear carbon-free energy production is attributed to fast reactors, mostly employing a liquid metal as a coolant. This paper summarizes the efforts that have been undertaken in collaborative projects sponsored by the European Commission in the past 20 years in the fields of liquid-metal heat transfer modeling, fuel assembly and core thermal hydraulics, pool and system thermal hydraulics, and establishment of best practice guidelines and verification, validation, and uncertainty quantification (UQ). The achievements in these fields will be presented along with the prospects on topics which will be studied collaboratively in Europe in the years to come. These prospects include further development of heat transfer models for applied computational fluid dynamics (CFD), further analysis of the consequences of fuel assembly blockages on coolant flow and temperature, analysis of the thermal hydraulic effects in deformed fuel assemblies, extended validation of three-dimensional pool thermal hydraulic CFD models, and further development and validation of multi-scale system thermal hydraulic methods.

关键词： liquid metal     thermal hydraulics     Europe    

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Coupling evaluation for material removal and thermal control on precision milling machine tools

《机械工程前沿（英文）》 2022年 第17卷 第1期   页码 12-12 doi: 10.1007/s11465-021-0668-9

摘要： Machine tools are one of the most representative machining systems in manufacturing. The energy consumption of machine tools has been a research hotspot and frontier for green low-carbon manufacturing. However, previous research merely regarded the material removal (MR) energy as useful energy consumption and ignored the useful energy consumed by thermal control (TC) for maintaining internal thermal stability and machining accuracy. In pursuit of energy-efficient, high-precision machining, more attention should be paid to the energy consumption of TC and the coupling relationship between MR and TC. Hence, the cutting energy efficiency model considering the coupling relationship is established based on the law of conservation of energy. An index of energy consumption ratio of TC is proposed to characterize its effect on total energy usage. Furthermore, the heat characteristics are analyzed, which can be adopted to represent machining accuracy. Experimental study indicates that TC is the main energy-consuming process of the precision milling machine tool, which overwhelms the energy consumption of MR. The forced cooling mode of TC results in a 7% reduction in cutting energy efficiency. Regression analysis shows that heat dissipation positively contributes 54.1% to machining accuracy, whereas heat generation negatively contributes 45.9%. This paper reveals the coupling effect of MR and TC on energy efficiency and machining accuracy. It can provide a foundation for energy-efficient, high-precision machining of machine tools.

关键词： machine tools     cutting energy efficiency     thermal stability     machining accuracy     coupling evaluation    

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An autonomous system for thermal convection of viscoelastic fluids in a porous layer using a thermal

Qi WEI, Xiaohui ZHANG

《能源前沿（英文）》 2010年 第4卷 第4期   页码 507-516 doi: 10.1007/s11708-010-0017-x

摘要： Thermal convection of viscoelastic fluids saturating a horizontal porous layer heated from below is analyzed using a thermal nonequilibrium model to take account of the interphase heat transfer between the fluid and the solid. The viscoelastic character of the flow is considered by a modified Darcy’s law. An autonomous system with five differential equations is deduced by applying the truncated Galerkin expansion to the momentum and heat transfer equations. The effects of interphase heat transfer on the thermal convection of viscoelastic fluids in a porous medium are analyzed and discussed. The results show that the weak interphase heat transfer tends to stabilize the steady convection.

关键词： thermal convection     porous media     viscoelastic fluid     thermal nonequilibrium model    

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ANN-exhaustive-listing method for optimization of multiple building shapes and envelope properties with maximum thermal

Yaolin LIN, Wei YANG

《能源前沿（英文）》 2021年 第15卷 第2期   页码 550-563 doi: 10.1007/s11708-019-0607-1

摘要： With increasing awareness of sustainability, demands on optimized design of building shapes with a view to maximize its thermal performance have become stronger. Current research focuses more on building envelopes than shapes, and thermal comfort of building occupants has not been considered in maximizing thermal performance in building shape optimization. This paper attempts to develop an innovative ANN (artificial neural network)-exhaustive-listing method to optimize the building shapes and envelope physical properties in achieving maximum thermal performance as measured by both thermal load and comfort hour. After verified, the developed method is applied to four different building shapes in five different climate zones in China. It is found that the building shape needs to be treated separately to achieve sufficient accuracy of prediction of thermal performance and that the ANN is an accurate technique to develop models of discomfort hour with errors of less than 1.5%. It is also found that the optimal solutions favor the smallest window-to-external surface area with triple-layer low-E windows and insulation thickness of greater than 90 mm. The merit of the developed method is that it can rapidly reach the optimal solutions for most types of building shapes with more than two objective functions and large number of design variables.

关键词： ANN (artificial neural network)     exhaustive-listing     building shape     optimization     thermal load     thermal comfort    

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Flow and thermal modeling of liquid metal in expanded microchannel heat sink

《能源前沿（英文）》   页码 796-810 doi: 10.1007/s11708-023-0877-5

摘要： Liquid metal-based microchannel heat sinks (MCHSs) suffer from the low heat capacity of coolant, resulting in an excessive temperature rise of coolant and heat sink when dealing with high-power heat dissipation. In this paper, it was found that expanded space at the top of fins could distribute the heat inside microchannels, reducing the temperature rise of coolant and heat sink. The orthogonal experiments revealed that expanding the top space of channels yielded similar temperature reductions to changing the channel width. The flow and thermal modeling of expanded microchannel heat sink (E-MCHS) were analyzed by both using the 3-dimensional (3D) numerical simulation and the 1-dimensional (1D) thermal resistance model. The fin efficiency of E-MCHS was derived to improve the accuracy of the 1D thermal resistance model. The heat conduction of liquid metal in Z direction and the heat convection between the top surface of fins and the liquid metal could reduce the total thermal resistance (Rt). The above process was effective for microchannels with low channel aspect ratio, low mean velocity (Um) or long heat sink length. The maximum thermal resistance reduction in the example of this paper reached 36.0%. The expanded space endowed the heat sink with lower pressure, which might further reduce the pumping power (P). This rule was feasible both when fins were truncated (h2 < 0, h2 is the height of expanded channel for E-MCHS) and when over plate was raised (h2 > 0).

关键词： liquid metal cooling     heat sink     expanded microchannel     flow and thermal modeling    

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Encapsulation of polyethylene glycol in cellulose-based porous capsules for latent heat storage and light-to-thermal

《化学科学与工程前沿（英文）》 2023年 第17卷 第8期   页码 1038-1050 doi: 10.1007/s11705-022-2279-3

摘要： Phase change materials are potential candidates for the application of latent heat storage. Herein, we fabricated porous capsules as shape-stable materials from cellulose-based polyelectrolyte complex, which were first prepared using cellulose 6-(N-pyridinium)hexanoyl ester as the cationic polyelectrolyte and carboxymethyl cellulose as the anionic polyelectrolyte to encapsulate polyethylene glycol by the vacuum impregnation method. Furthermore, the multi-walled carbon nanotube or graphene oxide, which were separately composited into the polyelectrolytes complex capsules to enhance thermal conductivity and light-to-thermal conversion efficiency. These capsules owned a typical core–shell structure, with an extremely high polyethylene glycol loading up to 34.33 g∙g‒1. After loading of polyethylene glycol, the resulted cellulose-based composite phase change materials exhibited high thermal energy storage ability with the latent heat up to 142.2 J∙g‒1, which was 98.5% of pure polyethylene glycol. Further results showed that the composite phase change materials demonstrated good form-stable property and thermal stability. Moreover, studies involving light-to-thermal conversion determined that composite phase change materials exhibited outstanding light-to-thermal conversion performance. Considering their exceptional comprehensive features, innovative composite phase change materials generated from cellulose presented a highly interesting choice for thermal management and renewable thermal energy storage.

关键词： cellulose     polyelectrolytes     phase change materials     thermal energy storage     light-to-thermal conversion    

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Non-thermal plasma enhances performances of biochar in wastewater treatment and energy storage applications

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 475-483 doi: 10.1007/s11705-021-2070-x

摘要： Surface functionalization or modification to introduce more oxygen-containing functional groups to biochar is an effective strategy for tuning the physicochemical properties and promoting follow-up applications. In this study, non-thermal plasma was applied for biochar surface carving before being used in contaminant removal and energy storage applications. The results showed that even a low dose of plasma exposure could introduce a high number density of oxygen-functional groups and enhance the hydrophilicity and metal affinity of the pristine biochar. The plasma-treated biochar enabled a faster metal-adsorption rate and a 40% higher maximum adsorption capacity of heavy metal ion Pb2+. Moreover, to add more functionality to biochar surface, biochar with and without plasma pre-treatment was activated by KOH at a temperature of 800 °C. Using the same amount of KOH, the plasma treatment resulted in an activated carbon product with the larger BET surface area and pore volume. The performance of the treated activated carbon as a supercapacitor electrode was also substantially improved by>30%. This study may provide guidelines for enhancing the surface functionality and application performances of biochar using non-thermal-based techniques.

关键词： non-thermal plasma     surface functionalization     biochar modification     wastewater treatment     supercapacitor    

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标题 作者 时间 类型 操作

Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation

期刊论文

Deactivation and regeneration of TS-1/SiO

Hainan SHI, Yaquan WANG, Guoqiang WU, Wenping FENG, Yi Lin, Teng ZHANG, Xing JIN, Shuhai WANG, Xiaoxue WU, Pengxu YAO

期刊论文

Catalysis and deactivation of montmorillonite K10 in the aryl O -glycosylation of glycosyl trichloroacetoimidates

Xiaoliu LI, Xinhao YAN, Zhiwei LI, Hua CHEN, Pingzhu ZHANG,

期刊论文

Chemical deactivation of V

Xiaodong WU, Wenchao YU, Zhichun SI, Duan WENG

期刊论文

Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

期刊论文

Influence evaluation of loading conditions during pressurized thermal shock transients based on thermal-hydraulics

Jinya KATSUYAMA, Shumpei UNO, Tadashi WATANABE, Yinsheng LI

期刊论文

Kinetic model for hydroisomerization reaction of C-aromatics

XU Ouguan, SU Hongye, JIN Xiaoming, CHU Jian

期刊论文

Assessment indices for uniform and non-uniform thermal environments

ZHANG Yufeng, SUN Shufeng, ZHAO Rongyi

期刊论文

Liquid metal thermal hydraulics R&D at European scale: achievements and prospects

期刊论文

Coupling evaluation for material removal and thermal control on precision milling machine tools

期刊论文

An autonomous system for thermal convection of viscoelastic fluids in a porous layer using a thermal

Qi WEI, Xiaohui ZHANG

期刊论文

ANN-exhaustive-listing method for optimization of multiple building shapes and envelope properties with maximum thermal

Yaolin LIN, Wei YANG

期刊论文

Flow and thermal modeling of liquid metal in expanded microchannel heat sink

期刊论文

Encapsulation of polyethylene glycol in cellulose-based porous capsules for latent heat storage and light-to-thermal

期刊论文

Non-thermal plasma enhances performances of biochar in wastewater treatment and energy storage applications

期刊论文