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Meiling Shui Chao Huang Peiyu Ma Wenjie Li Qun He Wenlong Wu Yisheng Tan Jun Bao 《中国化学快报》2021,32(7):2203-2206
With regard to the reaction of higheralcohol synthesis(HAS),the optimizations of activity and selectivity towards C_(2+) alcohol are restricted by the improper equilibrium in two different CO activation pathways and chain growth capacity.Herein,we find that delibrately controlling the compositions of catalysts is an effective strategy to achieve the equilibrium of CO activation pathways and promote the chain growth.As a result,the optimized Cu_(0.25)Co_(0.75) alloy catalyst can achieve a large proportion of higher alcohol in alcohol products(C_(2+)OH/MeOH=4.40),together with high CO conversion of 71.27% and space-time-yield of 147.65 g kg~(-1) h~(-1).The mechanistic studies suggest that the good performance of Cu_(0.25)Co_(0.75) catalyst is attributed to the synergistic effect between alloyed Cu and Co. 相似文献
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以纳米η-Al2O3粉和工业铬绿为原料,以摩尔比1:1配比制备Al2O3-Cr2O3固溶体,以TiO2为烧结助剂,在还原气氛下经1400 ℃、1500 ℃和1600 ℃固相烧结.研究了TiO2的加入对纳米η-Al2O3制备Al2O3-Cr2O3固溶体的致密度、线收缩率、相组成、晶胞参数、互扩散程度和微观结构的影响.结果表明:TiO2的加入能促进Al2O3-Cr2O3固溶体的致密化;当温度为1600 ℃,TiO2的添加量为2wt;时,试样的体积密度最大为4.57 g·cm-3,线收缩率为19.8;;TiO2的加入能使Al2O3-Cr2O3固溶体中Al3+和Cr3+的互扩散程度增加;微观结构表明,TiO2的加入能使Al2O3-Cr2O3固溶体晶粒之间结合更紧密,实验温度范围内,随着TiO2添加量的增加晶粒从沿晶断裂向穿晶断裂转变,只在晶间和晶内存在极少量气孔,当温度为1600 ℃,TiO2的添加量为2wt;时,晶粒大小较均匀,平均晶粒尺寸约10μm. 相似文献
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针对欠定卷积混合的语音信号模型,提出一种基于声源方位信息和非线性时频掩蔽的语音盲提取算法。首先对低频段混合语音信号进行时频分析估计瞬时相对时延(ITD)并采用势函数聚类分析方法估计出声源个数及其ITD,接着锁定目标提取准确的目标语音方位信息,最后利用独立语音在时频域上的近似W一分离正交性,采用非线性时频掩蔽的方法提取目标语音。仿真实验表明,该方法能锁定任意感兴趣目标方位,能有效提取目标语音,文中实验条件下信噪比增益平均达9.5 dB。 相似文献
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Neither the modified Bingham model nor the Herschel–Bulkley model can be used to characterize and calculate the performance of shear thickening of highly flowable mortar because of their incalculability of the rheological parameters. A new exponential rheological model was established to solve the characterization and calculation of shear thickening of the lubrication layer (highly flowable mortar) during the pumping of concrete in this paper. This new exponential rheological model has three rheological parameters, namely, yield stress, consistency coefficient, and consistency exponent. They can quantitatively describe the yield stress, differential viscosity, and shear thickening degree of highly flowable mortar. The calculating results of the rheological parameters of the newly established model for the mortars with different compositions showed that the consistency exponent of mortar decreased with the increase of its sand-binder ratio or the dosage of fly ash in the binder. This indicates that the shear thickening degree of mortar decreases. The consistency exponent of mortar initially decreases and subsequently increases with the increase in silica fume content or the dosage of the superplasticizer. It illustrates that the degree of the shear thickening of mortar initially decreased and subsequently increased. These varying patterns were confirmed by the rheological experiment of mortars. 相似文献
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Ge P Scanlon MD Peljo P Bian X Vubrel H O'Neill A Coleman JN Cantoni M Hu X Kontturi K Liu B Girault HH 《Chemical communications (Cambridge, England)》2012,48(52):6484-6486
The activities of a series of MoS(2)-based hydrogen evolution catalysts were studied by biphasic reactions monitored by UV/Vis spectroscopy. Carbon supported MoS(2) catalysts performed best due to an abundance of catalytic edge sites and strong electronic coupling of catalyst to support. 相似文献
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Olaya AJ Ge P Gonthier JF Pechy P Corminboeuf C Girault HH 《Journal of the American Chemical Society》2011,133(31):12115-12123
The four-electron reduction of oxygen by tetrathiafulvalene (TTF) in acidified 1,2-dichloroethane and at the acidified water/1,2-dichloroethane interface has been observed. Spectroscopy and ion transfer voltammetry results suggest that the reaction proceeds by the fast protonation of TTF followed by the 4-electron reduction of oxygen to form water. Electronic structure computations give evidence of the formation of a helical tetramer assembly ([TTF(4)H(2)](2+)) of two protonated TTF and two neutral TTF molecules. The protonated tetramer is potentially able to deliver the four electrons needed for the oxygen reduction. The production of water was corroborated by (1)H NMR analysis. 相似文献
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Ge Zhan Liding Wang Dr. Zifeng Zhao Peiyu Fang Prof. Dr. Zuqiang Bian Prof. Dr. Zhiwei Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(43):19173-19177
Luminescent EuII complexes with a characteristic 5d–4f transition have potential applications in many fields. However, their instability in ambient conditions impedes further exploration and application. Herein, we report two new EuII complexes, bis[hydrotris(3-trifluoromethylpyrazolyl)borate]europium(II) ( Eu-1 ) and bis[hydrotris(3-methylpyrazolyl)borate]europium(II) ( Eu-2 ). Intriguingly, the blue emissive Eu-1 showed high air stability arising from fluorine protection and close molecular packing, as maintaining a photoluminescence quantum yield (PLQY) of 91 % (initial 96 %) upon exposure to air over 2200 hours. While the orange emissive Eu-2 showed a maximum luminance of 30620 cd m−2, and a maximum external quantum efficiency (EQE) of 6.5 %, corresponding to an exciton utilization efficiency around 100 % in organic light-emitting diodes (OLEDs). These results could inspire further research on stable and efficient EuII complexes and their application in OLEDs. 相似文献
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Mihan Jin Bing Li Linlin Hu Peiyu Zhao Qilu Zhang Jiangxuan Song 《Journal of Energy Chemistry》2021,(9):156-161
Nickel-rich layered oxide LiNi1-x-yCoxAlyO2(NCA)with high theoretical capacity is a promising cathode material for the next-generation high-energy batteries.How... 相似文献