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1.
Minh Nguyen Vo Jonathan P. Ruffley J. Karl Johnson 《American Institute of Chemical Engineers》2021,67(3):e17156
Metal organic frameworks (MOFs) containing zirconium secondary building units (SBUs) in UiO-67 and related MOFs, are highly active for neutralizing both the chemical warfare agents and simulants, such as dimethyl methylphosphonate (DMMP). However, two recent publications gave conflicting reports of DMMP reaction with UiO-67 under ultra high vacuum (UHV) conditions, with one reporting chemisorption and reaction (Wang et al., J Phys Chem C, 2017, 121, 11261–11272) and the other reporting only physisorption and reversible desorption (Ruffley et al., J Phys Chem C, 2019, 123, 19748–19758) from very similar temperature programmed desorption experiments. We show that the discrepancy between these experiments may be explained by different levels of missing linker defects in the UiO-67 samples. We present density functional theory calculations showing that SBU sites having two-adjacent missing linkers exhibit reaction barriers that are about 30 kJ/mol lower than SBU sites having a single missing linker. We also show that topology of the undercoordinated sites plays an important role in the reaction barrier under UHV conditions. 相似文献
2.
Babak Jaleh Mahmoud Nasrollahzadeh Bahareh Feizi Mohazzab Mahtab Eslamipanah Mohaddeseh Sajjadi Hossein Ghafuri 《Ceramics International》2021,47(8):10389-10425
In both developing and industrialized/developed countries, various hazardous/toxic environmental pollutants are entering water bodies from organic and inorganic compounds (heavy metals and specifically dyes). The global population is growing whereas the accessibility of clean, potable and safe drinking water is decreasing, leading to world deterioration in human health and limitation of agricultural and/or economic development. Treatment of water/wastewater (mainly industrial water) via catalytic reduction/degradation of environmental pollutants is extremely critical and is a major concern/issue for public health. Light and/or laser ablation induced photocatalytic processes have attracted much attention during recent years for water treatment due to their good (photo)catalytic efficiencies in the reduction/degradation of organic/inorganic pollutants. Pulsed laser ablation (PLA) is a rather novel catalyst fabrication approach for the generation of nanostructures with special morphologies (nanoparticles (NPs), nanocrystals, nanocomposites, nanowires, etc.) and different compositions (metals, alloys, oxides, core-shell, etc.). Laser ablation in liquid (LAL) is generally considered a quickly growing approach for the synthesis and modification of nanomaterials for practical applications in diverse fields. LAL-synthesized nanomaterials have been identified as attractive nanocatalysts or valuable photocatalysts in (photo)catalytic reduction/degradation reactions. In this review, the laser ablation/irradiation strategies based on LAL are systematically described and the applications of LAL synthesized metal/metal oxide nanocatalysts with highly controlled nanostructures in the degradation/reduction of organic/inorganic water pollutants are highlighted along with their degradation/reduction mechanisms. 相似文献
3.
Understanding the mechanisms leading to the rise and dissemination of antimicrobial resistance (AMR) is crucially important for the preservation of power of antimicrobials and controlling infectious diseases. Measures to monitor and detect AMR, however, have been significantly delayed and introduced much later after the beginning of industrial production and consumption of antimicrobials. However, monitoring and detection of AMR is largely focused on bacterial pathogens, thus missing multiple key events which take place before the emergence and spread of AMR among the pathogens. In this regard, careful analysis of AMR development towards recently introduced antimicrobials may serve as a valuable example for the better understanding of mechanisms driving AMR evolution. Here, the example of evolution of tet(X), which confers resistance to the next-generation tetracyclines, is summarised and discussed. Initial mechanisms of resistance to these antimicrobials among pathogens were mostly via chromosomal mutations leading to the overexpression of efflux pumps. High-level resistance was achieved only after the acquisition of flavin-dependent monooxygenase-encoding genes from the environmental microbiota. These genes confer resistance to all tetracyclines, including the next-generation tetracyclines, and thus were termed tet(X). ISCR2 and IS26, as well as a variety of conjugative and mobilizable plasmids of different incompatibility groups, played an essential role in the acquisition of tet(X) genes from natural reservoirs and in further dissemination among bacterial commensals and pathogens. This process, which took place within the last decade, demonstrates how rapidly AMR evolution may progress, taking away some drugs of last resort from our arsenal. 相似文献
4.
Zhichuan Shen Jiawei Zhong Wenhao Xie Jinbiao Chen Xi Ke Jianmin Ma Zhicong Shi 《金属学报(英文版)》2021,34(3):359-372
All-solid-state lithium batteries(ASSLB) are promising candidates for next-generation energy storage devices.Nevertheless,the large-scale commercial application of high energy density AS S LB with the polymer electrolyte still faces challenges.In this study,a thin solid polymer composite electrolyte(SPCE) is prepared through a facile and cost-effective strategy with an infiltration of thermoplastic polyurethane(TPU),lithium salt(LiTFSI or LiFSI),and halloysite nanotubes(HNTs) in a porous framework of polyethylene separator(PE)(TPU-HNTs-LiTFSI-PE or TPU-HNTs-LiFSI-PE).The composition,electrochemical performance,and especially the effect of anions(TFSI~-and FSI~-) on cycling performance are investigated.The results reveal that the flexible TPU-HNTs-LiTFSI-PE and TPU-HNTs-LiFSI-PE with a thickness of 34 μm exhibit wide electrochemical windows of 4.9 and 5.1 V(vs.Li+/Li) at 60℃,respectively.Reduction in FSI~-tends to form more LiF and sulfur compounds at the interface between TPU-HNTs-LiFSI-PE and Li metal anode,thus enhancing the interfacial stability.As a result,cell composed of TPU-HNTs-LiFSI-PE exhibits a smaller increase in interfacial resistance of solid electrolyte interphase(SEI) with a distinct decrease in charge-transfer resistance during cycling.Li|Li symmetric cell with TPU-HNTs-LiFSI-PE could keep its stable overpotential profile for nearly 1300 h with a low hysteresis of approximately39 mV at a current density of 0.1 mA cm~(-2),while a sudden voltage rise with internal cell impedance-surge signals was observed within 600 h for cell composed of TPU-HNTs-LiTFSI-PE.The initial capacities of NCMITPU-HNTs-LiTFSIPEILi and NCMITPU-HNTs-LiFSI-PEILi cells were 149 and 114 mAh g~(-1),with capacity retention rates of 83.52% and89.99% after 300 cycles at 0.5 C,respectively.This study provides a valuable guideline for designing flexible SPCE,which shows great application prospect in the practice of ASSLB. 相似文献
5.
Bin Feng Xin Jiang Guisheng Zou Wengan Wang Tianming Sun Heng Yang Guanlei Zhao Mingye Dong Yu Xiao Hongwei Zhu Lei Liu 《Advanced functional materials》2021,31(29):2102359
The realization of liquid metal-based wearable systems will be a milestone toward high-performance, integrated electronic skin. However, despite the revolutionary progress achieved in many other components of electronic skin, liquid metal-based flexible sensors still suffer from poor sensitivity due to the insufficient resistance change of liquid metal to deformation. Herein, a nacre-inspired architecture composed of a biphasic pattern (liquid metal with Cr/Cu underlayer) as “bricks” and strain-sensitive Ag film as “mortar” is developed, which breaks the long-standing sensitivity bottleneck of liquid metal-based electronic skin. With 2 orders of magnitude of sensitivity amplification while maintaining wide (>85%) working range, for the first time, liquid metal-based strain sensors rival the state-of-art counterparts. This liquid metal composite features spatially regulated cracking behavior. On the one hand, hard Cr cells locally modulate the strain distribution, which avoids premature cut-through cracks and prolongs the defect propagation in the adjacent Ag film. On the other hand, the separated liquid metal cells prevent unfavorable continuous liquid-metal paths and create crack-free regions during strain. Demonstrated in diverse scenarios, the proposed design concept may spark more applications of ultrasensitive liquid metal-based electronic skins, and reveals a pathway for sensor development via crack engineering. 相似文献
6.
Ningyu Chen Jintang Zhou Zhengjun Yao Yiming Lei Ruiyang Tan Yuxin Zuo Wenjian Zheng Zibao Jiao 《Ceramics International》2021,47(8):10545-10554
The electromagnetic materials are featured by good magnetic permeability and dielectric constant characteristics, which are of significant importance in solving the pollution problem of electromagnetic. In this study, after the complete of the use of sol-gel method, argon gas was then introduced for calcination, and eventually a new type of MWCNTs/Ni0.5Zn0.5Nd0.04Fe1.96O4 composites was synthesized after the above mentioned procedures. The synthesized MWCNTs were able to be adsorbed on the surface of Ni0.5Zn0.5Nd0.04Fe1.96O4 and could form a good conductive work of 3D. Also, the effect of additional MWCNTs on microwave absorption properties of MWCNTs/Ni0.5Zn0.5Nd0.04Fe1.96O4 composites were also observed in this study. The results indicate that the additional MWCNTs function to significantly improve the microwave absorption property of MWCNTs/Ni0.5Zn0.5Nd0.04Fe1.96O4. Through altering the amount of MWCNTs, the microwave attenuation performance and impedance matching coefficient of this electromagnetic materials can be effectively improved. The S2 sample presented a minimum reflection loss of ?35.05 dB when its thickness reached 1.6 mm, meanwhile, the effective absorption bandwidth achieved 4.55 GHz. The prepared composites perform well in microwave absorption, which can attribute to the reasonable ratio of composites as well as its interaction with both of the magnetic and dielectric components. This research paved the way for novel ideas to be put in the electromagnetic absorption materials with high-efficient. 相似文献
7.
In this study, a kind of Ni-based superalloy specially designed for additive manufacturing (AM) was investigated. Thermo-Calc simulation and differential scanning calorimetry (DSC) analysis were used to determine phases and their transformation temperature. Experimental specimens were prepared by laser metal deposition (LMD) and traditional casting method. Microstructure, phase constitution and mechanical properties of the alloy were characterized by scanning electron microscopy (SEM), transmission scanning electron microscopy (TEM), X-ray diffraction (XRD) and tensile tests. The results show that this alloy contains two basic phases, γ/γ', in addition to these phases, at least two secondary phases may be present, such as MC carbides and Laves phases. Furthermore, the as-deposited alloy has finer dendrite, its mean primary dendrite arm space (PDAS) is about 30-45 μm, and the average size of γ' particles is 100-150 nm. However, the dendrite size of the as-cast alloy is much larger and its PDAS is 300-500 μm with secondary and even third dendrite arms. Correspondingly, the alloy displays different tensile behavior with different processing methods, and the as-deposited specimen shows better ultimate tensile stress (1,085.7±51.7 MPa), yield stress (697±19.5 MPa) and elongation (25.8%±2.2%) than that of the as-cast specimen. The differences in mechanical properties of the alloy are due to the different morphology and size of dendrites, γ', and Laves phase, and the segregation of elements, etc. Such important information would be helpful for alloy application as well as new alloy development. 相似文献
8.
Gui-Jia Gao Mei-Qi Zeng En-Liang Zhang Rong-Chang Zeng Lan-Yue Cui Dao-kui Xu Feng-Qin Wang M.Bobby Kannan 《材料科学技术学报》2021,83(24):161-178
The microstructure and chemical compositions of the solid solution-treated Mg-3Nd-1Li-0.2Zn alloy were characterized using optical microscope,scanning electron microscope(SEM),transmission electron microscope(TEM),electron probe micro-analyzer(EPMA)and X-ray photoelectron spectroscopy(XPS).The corrosion behaviour of the alloy was investigated via electrochemical polarization,electrochemical impedance spectroscopy(EIS),hydrogen evolution test and scanning Kelvin probe(SKP).The results showed that the microstructure of the as-extruded Mg-3Nd-1Li-0.2Zn alloy contained α-Mg matrix and nanometric second phase Mg41 Nd5.The grain size of the alloy increased significantly with the increase in the heat-treatment duration,whereas the volume fraction of the second phase decreased after the solid solution treatment.The surface film was composed of oxides(Nd2O3,MgO,Li2O and ZnO)and carbonates(MgCO3 and Li2CO3),in addition to Nd.The as-extruded alloy exhibited the best corrosion resistance after an initial soaking of 10 min,whereas the alloy with 4h-solution-treatment possessed the lowest corrosion rate after a longer immersion(1 h).This can be attributed to the formation of Nd-containing oxide film on the alloys and a dense corrosion product layer.The dealloying corrosion of the second phase was related to the anodic Mg41Nd5 with a more negative Volta potential relative to α-Mg phase.The preferential corrosion of Mg41Nd5 is proven by in-situ observation and SEM.The solid solution treatment of Mg-3Nd-1Li-0.2Zn alloy led to a shift in corrosion type from pitting corrosion to uniform corrosion under long-term exposure. 相似文献
9.
Son Ha Daesin Kim Hyung-Kyu Lim Chong Min Koo Seon Joon Kim Young Soo Yun 《Advanced functional materials》2021,31(32):2101261
The positive effects of a lithiophilic substrate on the electrochemical performance of lithium metal anodes are confirmed in several reports, while the understanding of lithiophilic substrate-guided lithium metal nucleation and growth behavior is still insufficient. In this study, the effect of a lithiophilic surface on lithium metal nucleation and growth behaviors is investigated using a large-area Ti3C2Tx MXene substrate with a large number of oxygen and fluorine dual heteroatoms. The use of the MXene substrate results in a high lithium-ion concentration as well as the formation of uniform solid–electrolyte-interface (SEI) layers on the lithiophilic surface. The solid–solid interface (MXene-SEI layer) significantly affects the surface tension of the deposited lithium metal nuclei as well as the nucleation overpotential, resulting in the formation of uniformly dispersed lithium nanoparticles ( ≈ 10–20 nm in diameter) over the entire MXene surface. The primary lithium nanoparticles preferentially coalesce and agglomerate into larger secondary particles while retaining their primary particle shapes. Subsequently, they form close-packed structures, resulting in a dense metal layer composed of particle-by-particle microstructures. This distinctive lithium metal deposition behavior leads to highly reversible cycling performance with high Columbic efficiencies > 99.0% and long cycle lives of over 1000 cycles. 相似文献
10.
Sichen Gu Si-Wei Zhang Junwei Han Yaqian Deng Chong Luo Guangmin Zhou Yanbing He Guodan Wei Feiyu Kang Wei Lv Quan-Hong Yang 《Advanced functional materials》2021,31(28):2102128
Lithium metal anodes (LMAs) are promising for next-generation batteries but have poor compatibility with the widely used carbonate-based electrolytes, which is a major reason for their severe dendrite growth and low Coulombic efficiency (CE). A nitrate additive to the electrolyte is an effective solution, but its low solubility in carbonates is a problem that can be solved using a crown ether, as reported. A rubidium nitrate additive coordinated with 18-crown-6 crown ether stabilizes the LMA in a carbonate electrolyte. The coordination promotes the dissolution of NO3− ions and helps form a dense solid electrolyte interface that is Li3N-rich which guides uniform Li deposition. In addition, the Rb (18-crown-6)+ complexes are adsorbed on the dendrite tips, shielding them from Li deposition on the dendrite tips. A high CE of 97.1% is achieved with a capacity of 1 mAh cm−2 in a half cell, much higher than when using the additive-free electrolyte (92.2%). Such an additive is very compatible with a nickel-rich ternary cathode at a high voltage, and the assembled full battery with a cathode material loading up to 10 mg cm−2 shows an average CE of 99.8% over 200 cycles, indicating a potential for practical use. 相似文献