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Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed

《化学科学与工程前沿（英文）》 2022年第16卷第12期页码 1782-1792 doi: 10.1007/s11705-022-2220-9

摘要： Ultra-dispersed Ni nanoparticles (7.5 nm) on nitrogen-doped carbon nanoneedles (Ni@NCNs) were prepared by simple pyrolysis of Ni-based metal–organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding anilines. Two different crystallization methods (stirring and static) were compared and the optimal pyrolysis temperature was explored. Ni@NCNs were systematically characterized by wide analytical techniques. In the hydrogenation of p-chloronitrobenzene, Ni@NCNs-600 (pyrolyzed at 600 °C) exhibited extraordinarily high performance with 77.9 h^–1 catalytic productivity and > 99% p-chloroaniline selectivity at full p-chloronitrobenzene conversion under mild conditions (90 °C, 1.5 MPa H₂), showing obvious superiority compared with reported Ni-based catalysts. Notably, the reaction smoothly proceeded at room temperature with full conversion and > 99% selectivity. Moreover, Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups (halogen, nitrile, keto, carboxylic, etc.), and could be easily recycled by magnetic separation and reused for 5 times without deactivation. The adsorption tests showed that the preferential adsorption of –NO₂ on the catalyst can restrain the dehalogenation of p-chloronitrobenzene, thus achieving high p-chloroaniline selectivity. While the high activity can be attributed to high Ni dispersion, special morphology, and rich pore structure of the catalyst.

关键词： halogenated nitrobenzenes room-temperature hydrogenation Ni nanoparticles nitrogen-doped carbon nanoneedles metal–organic-framework

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Liquid metal material genome: Initiation of a new research track towards discovery of advanced energy materials

Lei WANG, Jing LIU

《能源前沿（英文）》 2013年第7卷第3期页码 317-332 doi: 10.1007/s11708-013-0271-9

摘要： As the basis of modern industry, the roles materials play are becoming increasingly vital in this day and age. With many superior physical properties over conventional fluids, the low melting point liquid metal material, especially room-temperature liquid metal, is recently found to be uniquely useful in a wide variety of emerging areas from energy, electronics to medical sciences. However, with the coming enormous utilization of such materials, serious issues also arise which urgently need to be addressed. A biggest concern to impede the large scale application of room-temperature liquid metal technologies is that there is currently a strong shortage of the materials and species available to meet the tough requirements such as cost, melting point, electrical and thermal conductivity, etc. Inspired by the Material Genome Initiative as issued in 2011 by the United States of America, a more specific and focused project initiative was proposed in this paper—the liquid metal material genome aimed to discover advanced new functional alloys with low melting point so as to fulfill various increasing needs. The basic schemes and road map for this new research program, which is expected to have a worldwide significance, were outlined. The theoretical strategies and experimental methods in the research and development of liquid metal material genome were introduced. Particularly, the calculation of phase diagram (CALPHAD) approach as a highly effective way for material design was discussed. Further, the first-principles (FP) calculation was suggested to combine with the statistical thermodynamics to calculate the thermodynamic functions so as to enrich the CALPHAD database of liquid metals. When the experimental data are too scarce to perform a regular treatment, the combination of FP calculation, cluster variation method (CVM) or molecular dynamics (MD), and CALPHAD, referred to as the mixed FP-CVM-CALPHAD method can be a promising way to solve the problem. Except for the theoretical strategies, several parallel processing experimental methods were also analyzed, which can help improve the efficiency of finding new liquid metal materials and reducing the cost. The liquid metal material genome proposal as initiated in this paper will accelerate the process of finding and utilization of new functional materials.

关键词： liquid metal material genome energy material material discovery advanced material room-temperature liquid alloy thermodynamics phase diagram

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A nano-scale alignment method for imprint lithography

WANG Li, LU Bing-heng, DING Yu-cheng, QIU Zhi-hui, LIU Hong-zhong

《机械工程前沿（英文）》 2006年第1卷第2期页码 157-161 doi: 10.1007/s11465-006-0014-2

摘要： A novel nano-scale alignment technique based on moiré signal for room-temperature imprint lithography in the submicron realm is proposed. The moiré signals generated by two pairs of quadruple gratings on mold and wafer are optically projected onto two photo-detector arrays, then the detected moiré signals are used to estimate the alignment errors in the x and y directions. The experiment results indicate that complex differential moiré signal is sensitive to relative displacement of the mold and wafer, and the alignment accuracy obtained in the x and γ directions and in θ are 20 nm , 25 nm and 1 μrad (3σ), respectively. They can meet the requirements of alignment accuracy for submicron imprint lithography.

关键词： submicron alignment accuracy nano-scale alignment quadruple room-temperature

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Perspective on gallium-based room temperature liquid metal batteries

《能源前沿（英文）》 2022年第16卷第1期页码 23-48 doi: 10.1007/s11708-022-0815-y

摘要： Recent years have witnessed a rapid development of deformable devices and epidermal electronics that are in urgent request for flexible batteries. The intrinsically soft and ductile conductive electrode materials can offer pivotal hints in extending the lifespan of devices under frequent deformation. Featuring inherent liquidity, metallicity, and biocompatibility, Ga-based room-temperature liquid metals (GBRTLMs) are potential candidates to fulfill the requirement of soft batteries. Herein, to illustrate the glamour of liquid components, high-temperature liquid metal batteries (HTLMBs) are briefly summarized from the aspects of principle, application, advantages, and drawbacks. Then, Ga-based liquid metals as main working electrodes in primary and secondary batteries are reviewed in terms of battery configurations, working mechanisms, and functions. Next, Ga-based liquid metals as auxiliary working electrodes in lithium and nonlithium batteries are also discussed, which work as functional self-healing additives to alleviate the degradation and enhance the durability and capacity of the battery system. After that, Ga-based liquid metals as interconnecting electrodes in multi-scenarios including photovoltaics solar cells, generators, and supercapacitors (SCs) are interpreted, respectively. The summary and perspective of Ga-based liquid metals as diverse battery materials are also focused on. Finally, it was suggested that tremendous endeavors are yet to be made in exploring the innovative battery chemistry, inherent reaction mechanism, and multifunctional integration of Ga-based liquid metal battery systems in the coming future.

关键词： liquid metals soft electrodes flexible batteries deformable energy supply devices epidermal electronics

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Genomic and metabolomic analysis of with enhanced poly--glutamic acid production through atmospheric and roomtemperature plasma mutagenesis

《化学科学与工程前沿（英文）》 2022年第16卷第12期页码 1751-1760 doi: 10.1007/s11705-022-2211-x

摘要： Poly-γ-glutamic acid is an extracellular polymeric substance with various applications owing to its valuable properties of biodegradability, flocculating activity, water solubility, and nontoxicity. However, the ability of natural strains to produce poly-γ-glutamic acid is low. Atmospheric and room temperature plasma was applied in this study to conduct mutation breeding of Bacillus licheniformis CGMCC 2876, and a mutant strain M32 with an 11% increase in poly-γ-glutamic acid was obtained. Genome resequencing analysis identified 7 nonsynonymous mutations of ppsC encoding lipopeptide synthetase associated with poly-γ-glutamic acid metabolic pathways. From molecular docking, more binding sites and higher binding energy were speculated between the mutated plipastatin synthase subunit C and glutamate, which might contribute to the higher poly-γ-glutamic acid production. Moreover, the metabolic mechanism analysis revealed that the upregulated amino acids of M32 provided substrates for glutamate and promoted the conversion between L- and D-glutamate acids. In addition, the glycolytic pathway is enhanced, leading to a better capacity for using glucose. The maximum poly-γ-glutamic acid yield of 14.08 g·L^–1 was finally reached with 30 g·L^–1 glutamate.

关键词： ARTP mutagenesis Bacillus licheniformis poly-γ-glutamic acid metabolomics

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Room temperature liquid metal: its melting point, dominating mechanism and applications

Junheng FU, Chenglin ZHANG, Tianying LIU, Jing LIU

《能源前沿（英文）》 2020年第14卷第1期页码 81-104 doi: 10.1007/s11708-019-0653-8

摘要： The room temperature liquid metal (LM) is recently emerging as a new class of versatile materials with fascinating characteristics mostly originated from its simultaneous metallic and liquid natures. The melting point is a typical parameter to describe the peculiarity of LM, and a pivotal factor to consider concerning its practical applications such as phase change materials (PCMs) and advanced thermal management. Therefore, the theoretical exploration into the melting point of LM is an essential issue, which can be of special value for the design of new LM materials with desired properties. So far, some available strategies such as molecular dynamics (MD) simulation and classical thermodynamic theory have been applied to perform correlative analysis. This paper is primarily dedicated to performing a comprehensive overview regarding typical theoretical strategies on analyzing the melting points. It, then, presents evaluations on several factors like components, pressure, size and supercooling that may be critical for melting processes of liquid metal. After that, it discusses applications associated with the characteristic of low melting points of LM. It is expected that a great many fundamental and practical works are to be conducted in the coming future.

关键词： melting point liquid metal crystal thermodynamics molecular dynamics

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含铬废水常温合成铬铁矿的结晶行为及稳定性 Article

吕晋芳, 全英聪, 童雄, 彭勇军, 郑永兴

《工程（英文）》 2022年第9卷第2期页码 67-76 doi: 10.1016/j.eng.2020.12.018

摘要：

铁氧体法不仅能净化含重金属废水，而且能从废水中回收有价金属。因此，铁氧体法被认为是一种处理含铬废水最具潜力的技术。然而，由于高的合成温度，该技术尚未在工业上得到广泛应用。本文对常温合成铬铁矿的可行性进行全面研究。考查了关键因素对出水水质、合成产物结晶行为和稳定性的影响。结果表明，经过常温铁氧体法处理后，废水中铬的去除率超过99.0%，上清液中铬的浓度达到污水排放标准。提高充气速率、搅拌速率和反应时间有利于稳定铬铁矿的形成。通过常温铁氧体法获得的颗粒结构致密，最大粒径可达52 μm。在合成过程中，铬逐渐地进入尖晶石晶体结构，合成铬铁矿的分子式为Fe_3-xCr_xO₄，其中x约0.30。为阐明常温环境下铬铁矿的合成机理，提出了微观反应路径。本研究为铁氧体法在含铬废水净化和综合利用方面的工业应用奠定了基础。

关键词：含铬废水铬铁矿合成常温结晶行为稳定性

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A modified zone model for estimating equivalent room thermal capacity

Hua CHEN, Xiaolin WANG

《能源前沿（英文）》 2013年第7卷第3期页码 351-357 doi: 10.1007/s11708-013-0254-x

摘要： The zone model has been widely applied in control analysis of heating, ventilation and air conditioning (HVAC) systems to achieve a high building efficiency. This paper proposed a modified zone model which is much simpler in the HVAC system simulation and has the similar accuracy to the complicated simulation model. The proposed model took into consideration the effect of envelop heat reservoir on the room indoor temperature by introducing the thermal admittance of the inner surfaces of the building enclosure. The thermal admittance for the building enclosure was developed based on the building thermal network analytical theory and transfer function method. The efficacy of the proposed model was demonstrated by comparing it with the complicated model — heat balance method (HTB2 program). The predicted results from the proposed model well agreed with those from the complicated simulation. The proposed model can then make the HVAC system dynamic simulation much faster and more acceptable for control design due to its simplicity and efficiency.

关键词： room model thermal network analysis transfer function heating ventilation and air conditioning (HVAC) system simulation

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Room temperature oxidation of acetone by ozone over alumina-supported manganese and cobalt mixed oxides

Mehraneh Ghavami, Mostafa Aghbolaghy, Jafar Soltan, Ning Chen

《化学科学与工程前沿（英文）》 2020年第14卷第6期页码 937-947 doi: 10.1007/s11705-019-1900-6

摘要： Volatile organic compounds (VOCs) are among the major sources of air pollution. Catalytic ozonation is an efficient process for removing VOCs at lower reaction temperature compared to catalytic oxidation. In this study, a series of alumina supported single and mixed manganese and cobalt oxides catalysts were used for ozonation of acetone at room temperature. The influence of augmenting the single Mn and Co catalysts were investigated on the performance and structure of the catalyst. The manganese and cobalt single and mixed oxides catalysts of the formula Mn10%-CoX and Co10%-MnX (where X= 0, 2.5%, 5%, or 10%) were prepared. It was found that addition of Mn and Co at lower loading levels (2.5% or 5%) to single metal oxide catalysts enhanced the catalytic activity. The mixed oxides catalysts of (Mn10%-Co2.5%) and (Mn10%-Co5%) led to acetone conversion of about 84%. It is concluded that lower oxidation state of the secondary metal improves ozone decomposition and oxidation of acetone.

关键词： ozone VOC manganese oxides cobalt oxides alumina support

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Room temperature preparation of hydrazine-linked covalent organic frameworks coated capillaries for

《化学科学与工程前沿（英文）》 2023年第17卷第5期页码 548-556 doi: 10.1007/s11705-022-2252-1

摘要： Covalent organic frameworks (COFs) have been increasingly used in capillary electrochromatography due to their excellent characteristics. In this work, hydrazine-linked TFPB-DHzDS (TFPB: 1,3,5-tris(4-formylphenyl)benzene; DHzDS: 2,5-bis(3-(ethylthio)propoxy)terephthalohydrazide) was first synthesized by a simpler and easier method at room temperature and introduced into capillary electrochromatography as coating material. The TFPB-DHzDS coated capillaries were prepared by an in-situ growth process at room temperature. After optimizing the coating concentration and experimental conditions of capillary electrochromatography, baseline separation of two groups of polycyclic aromatic hydrocarbons was achieved based on the TFPB-DHzDS coated capillary. And the established method was used successfully to determine PAHs in natural water and soil samples. The spiked recoveries of polycyclic aromatic hydrocarbons in these samples ranged from 90.01% to 111.0%, indicating that the method is reliable and could detect polycyclic aromatic hydrocarbons in natural samples. Finally, molecular simulation was applied to study and visualize the interaction between the analytes and coating COF materials to investigate the molecular level separation mechanism further.

关键词： hydrazine-linked TFPB-DHzDS in-situ growth method open-tubular capillary electrochromatography molecular simulations

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Hydrogenation of furfuryl alcohol to tetrahydrofurfuryl alcohol on NiB/SiO2 amorphous alloy catalyst

SONG Yun, LI Wei, ZHANG Minghui, TAO Keyi

《化学科学与工程前沿（英文）》 2007年第1卷第2期页码 151-154 doi: 10.1007/s11705-007-0028-2

摘要： NiB/SiO amorphous alloy catalyst was prepared by power electroless plating method and characterized by induction coupled plasma (ICP), Brunauer Emmett Teller method (BET), transmission electron microscope (TEM) and X-ray diffraction (XRD) techniques. The catalytic performance of NiB/SiO was investigated for the hydrogenation of furfuryl alcohol (FA) to tetrahydrofurfuryl alcohol (THFA). The effects of operational conditions, such as reaction temperature, pressure, and stirring rate were carefully studied. The proper conditions were determined as the following: pressure 2.0 MPa, temperature 120?C and stirring rate 550 r/min. A typical result with FA conversion of 99% and THFA selectivity of 100% was obtained under such conditions, which was close to that over Raney Ni.

关键词： following Brunauer electroless temperature transmission

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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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Prevention of surgical site infection under different ventilation systems in operating room environment

Zhijian Liu, Haiyang Liu, Hang Yin, Rui Rong, Guoqing Cao, Qihong Deng

《环境科学与工程前沿（英文）》 2021年第15卷第3期 doi: 10.1007/s11783-020-1327-9

摘要： Abstract • The effectiveness of four different ventilation systems was compared in depth. • Airflow and bacteria-carrying particles concentration were quantitatively analyzed. • Vertical laminar airflow with high airflow rate could not achieve desired effect. • Temperature-controlled airflow ventilation could guarantee air cleanliness. Biological particles in the operating room (OR) air environment can cause surgical site infections (SSIs). Various ventilation systems have been employed in ORs to ensure an ultraclean environment. However, the effect of different ventilation systems on the control of bacteria-carrying particles (BCPs) released from the surgical staff during surgery is unclear. In this study, the performance of four different ventilation systems (vertical laminar airflow ventilation (VLAF), horizontal laminar airflow ventilation (HLAF), differential vertical airflow ventilation (DVAF), and temperature-controlled airflow ventilation (TAF)) used in an OR was evaluated and compared based on the spatial BCP concentration. The airflow field in the OR was solved by the Renormalization Group (RNG) k-e turbulence model, and the BCP phase was calculated by Lagrangian particle tracking (LPT) and the discrete random walk (DRW) model. It was found that the TAF system was the most effective ventilation system among the four ventilation systems for ensuring air cleanliness in the operating area. This study also indicated that air cleanliness in the operating area depended not only on the airflow rate of the ventilation system but also on the airflow distribution, which was greatly affected by obstacles such as surgical lamps and surgical staff.

关键词： Operating room (OR) Bacteria-carrying particles (BCPs) Surgical site infections (SSIs) Ventilation

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NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

《化学科学与工程前沿（英文）》 2023年第17卷第12期页码 1973-1985 doi: 10.1007/s11705-023-2364-2

摘要： Ammonia is crucial in industry and agriculture, but its production is hindered by environmental concerns and energy-intensive processes. Hence, developing an efficient and environmentally friendly catalyst is imperative. In this study, we employed a straightforward and efficient impregnation technique to create various Cu-doped catalysts. Notably, the optimized 10Fe-8Cu/TiO₂ catalyst exhibited exceptional catalytic performance in converting NO to NH₃, achieving an NO conversion rate exceeding 80% and an NH₃ selectivity exceeding 98% at atmospheric pressure and 350 °C. We employed in situ diffuse reflectance Fourier transform infrared spectroscopy and conducted density functional theory calculations to investigate the intermediates and subsequent adsorption. Our findings unequivocally demonstrate that Cu doping enhances the rate-limiting hydrogenation step and lowers the energy barrier for NH₃ desorption, thereby resulting in improved NO conversion and enhanced selectivity toward ammonia. This study presents a pioneering approach toward energy-efficient ammonia synthesis and recycling of nitrogen sources.

关键词： NO hydrogenation synthetic ammonia 10Fe-xCu/TiO₂ high selectivity

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墙角火灾环境下钢构件温度分布及响应行为的实验研究

陈长坤,姚斌,杨昀,蔡昕,张和平,万玉田

《中国工程科学》 2005年第7卷第9期页码 70-75

摘要：

利用ISO9705标准火灾实验系统，模拟墙角火灾环境，以薄壁方管钢梁为研究对象，对钢构件在热、力耦合作用下的行为进行实验研究。对火灾的热释放速率与室内温度场，钢构件及其表面气体的温度、构件在火灾作用下的挠度进行测量，分析真实火灾下钢构件温升及温度分布的特点与火灾发展对构件挠度的影响。研究结果表明钢构件在长向上存在着很大的温差，而构件的挠度变化也并不对称，这说明以往研究中往往假设钢构件在长向上温度一致并不恰当，这种非均匀温度场对构件的行为有着重要影响，它使得构件高温区部分更易发生局部屈服而失效，在相同规模的火灾环境下，与均匀温度场相比，这种墙角火灾所导致的非均匀温度场更不利于钢构件的安全。

关键词： ISO标准火灾实验系统钢构件墙角火温度分布