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31.
Theoretical investigation of solvent effects on the selective hydrogenation of furfural over Pt(111)
Jian Wang Cun-Qin Lv Jian-Hong Liu Rong-Rong Ren Gui-Chang Wang 《International Journal of Hydrogen Energy》2021,46(2):1592-1604
It was well known that solvent effect plays a very important role in the catalytic reaction. There are many theoretical studies on the solvent effect in homogeneous catalysis while there are few theoretical studies on the solvent effect in the heterogeneous catalytic reaction and there has been no work to investigate the solvent effect on furfural transformation in heterogeneous catalysis. In the present work, both the density functional calculations and the microkinetic analysis were performed to study the selective hydrogenation of furfural over Pt(111) in the presence of methanol as well as toluene and compared with that in the gas condition. The present results indicated that the methanol can enhance the adsorption strength of furfural and other oxygen-containing reaction species due to its relatively strong polarity properties and this can be a main reason for solvent-induced high activity and selectivity. Another reason is that reaction paths study showed that the presence of methanol solvent makes the dehydrogenation of furfural less thermochemical due to the fact that furfural is more stabilized than that of dehydrogenation species, and methanol also has an inhibition effect on the dehydrogenation of furfural in the kinetic aspect, and further energetic span theory proves highest activity and selectivity for hydrogenation in methanol solvent of vapor, methanol and toluene. Moreover, microkinetic model simulation demonstrated that the activity and selectivity of hydrogenation in methanol is both higher than that in vapor and toluene. The much higher activity in methanol is due to the stabilized adsorbed reactants in the surface, which leads to a higher surface coverage of furfural. It might be proposed based on the present work that a solvent with relatively strong polarity may be favorable for the high selective hydrogenation of furfural. 相似文献
32.
多井评价是建立在单井精细解释对比分析基础上的预测储层及含油气性平面分布规律的技术方法,而常规测井资料无法区分碳酸盐岩岩溶储层,因而利用多井评价结果确定岩溶发育程度在平面上的分布规律就显得十分重要。为此,在岩心标定成像测井的基础上,对四川盆地高石梯—磨溪地区15口井的成像测井岩溶发育特征进行分析,建立了中二叠统茅口组岩溶发育各分带的标准成像图版,利用交会图及直方图分析各分带的常规测井响应特征,在此基础上形成了电成像测井刻度常规测井识别岩溶发育带的新方法。研究结果表明:①高石梯—磨溪地区茅口组岩溶带自上而下可划分为风化壳残积带、垂直渗流岩溶带、水平潜流岩溶带以及受岩溶作用较弱的基岩;②风化壳残积带在成像测井图像显示为"暗—亮—暗"条带状模式,垂直渗流岩溶带为垂直线状与暗色斑状组合模式,水平潜流岩溶带为水平线状—层状与斑状组合模式,基岩整体显示为亮色块状模式偶见线状或斑状特征;③有效储层主要发育在垂直渗流带和水平潜流带的顶部;④该区茅口组岩溶发育主要受裂缝发育控制,而裂缝发育又与断层关系密切。结论认为,该新方法对碳酸盐岩岩溶储层的多井评价具有普遍适用性,为四川盆地中二叠统风险探井的部署提供了技术支撑。 相似文献
33.
本实验采用4D-非标记蛋白质组学技术研究秦川牛肉贮藏过程中(0~8 d)肌红蛋白含量及其衍生物的转化情况,阐释冷却秦川牛肉中肌红蛋白含量及其衍生物转化的分子机制。结果表明:贮藏过程中,肌红蛋白表达量在宰后0~4 d上升、4~8 d下降,利用非标记蛋白质组学技术鉴定出与肌红蛋白及其衍生物相关的差异蛋白14 种,具体包括代谢酶、氧化还原酶、过氧化物酶、伴侣蛋白4 类,这4 类蛋白的表达共同调控贮藏过程中肌红蛋白含量的变化及其3 种衍生物之间的转化,具体表现为贮藏过程中肌红蛋白表达量整体呈下降趋势,氧合肌红蛋白相对含量持续下降,脱氧肌红蛋白、高铁肌红蛋白相对含量逐渐增加,导致肉色发生褐变。本研究结果有利于理解秦川牛肉贮藏过程肉类变色的复杂生化变化机制。 相似文献
34.
Wenjia Jing Baoqiang Hou Jinxiao Wang Qiang Zhi Jianfeng Yang Bo Wang 《Journal of the American Ceramic Society》2022,105(5):3141-3146
Photocatalysts often show excellent performances on the basis of their surface state of exposed faces with high reactivity, but unfortunately surfaces of this type are usually concealed into the interior of crystals for their high surface energy. We report here a possibility that for fluorine-terminated surfaces of monoclinic ZrO2, these higher-energy surfaces could be retained and exposed. Urchin-like ZrO2 hollow microspheres (UZHS) composed of nanoribbons with exposed (010) facets are obtained through a fluoride mediately solvothermal method. We prove the stabilization effect of fluorine adsorption on (010) facets by density functional theory calculations. More interestingly, UZHS exhibit tunable photocatalytic selectivity in dye degradation. The fluorinated UZHS exhibit good performances both on decomposing Congo red (CR) and methylene blue, while the surface-modified UZHS by calcination only favor decomposition of CR. 相似文献
35.
Yuhuan Sun Hongshuang Qin Zhengqing Yan Chuanqi Zhao Jinsong Ren Xiaogang Qu 《Advanced functional materials》2019,29(14)
Recently, quorum sensing (QS) inhibitors (QSIs) have been combined with antibiotics to enhance antibiofilm efficacy in vitro and in vivo. However, targeting QS signals alone is not enough to prevent bacterial infections. Drug resistance and recurrence of biofilms makes it difficult to eradicate. Herein, photodynamic therapy (PDT) is selected to unite QSIs and antibiotics. A synergistically antibiofilm system, which combines QSIs, antibiotics, and PDT based on hollow carbon nitride spheres (HCNSs) is envisaged. First, HCNS provides the multidrug delivering ability, enabling QSIs and antibiotics to be released in sequence. Subsequently, multistage releases sensitize bacteria effectively, potentiating the chemotherapeutic effects of the antibiotics. Finally, the integration of QSIs and PDT not only minimizes the possibility of drug resistance, but also overcomes the problem of limited mass and extension of PDT. Even after 48 h of incubation, the bacterial biofilm is obviously inhibited. And its biofilm disperse efficiency exceeds 48% (compared with QSI‐potentiated chemotherapy group) and 40% (compared with PDT group). Besides, the inhibition of the QS system influences phenotypes related to virulence factor production and surface hydrophobicity, which weaken biofilm invasion and formation. Eventually, this system is applied to disperse bacterial biofilm in vivo. Overall, PDT and QS modulation are devoted to eradicate drug resistance and recurrence of the biofilm. 相似文献
36.
Xiaohu Ren Xilou Pu Hongfeng Yin Yun Tang Hudie Yuan Huiqing Fan 《Ceramics International》2021,47(9):12122-12129
Hexagonal barium ferries is a promising and efficient microwave (MW) absorbing material, but the low dielectric loss and poor conductivity have limited their extensive applications. In this work, a simple tactic of coating conductive polymer PANI on hexaferrite BaCo2Fe16O27 is presented, wherein the dielectric properties are customized, and more significantly, the electromagnetic loss is greatly enhanced. As displayed from structural characterizations, PANI were coated equably on the surface of hexaferrite grains by an in-situ polymerization process. The outcomes exhibit the as-prepared PANI@hexaferrite composite has remarkable electromagnetic wave absorption capacity. When the thickness is 6.0 mm, the minimal RL of ?40.4 dB was achieved at 2.9 GHz. The effective absorption bandwidth (RL < ?20 dB) of 0.65 GHz, 0.53 GHz, 0.65 GHz, 0.52 GHz, 0.46 GHz and 0.39 GHz was achieved separately when the thickness ranges from 4 to 9 mm. The highly efficient MW absorbing performance of PANI@hexaferrite composite were the consequence of multiple loss mechanisms and perfect impedance matching. It is demonstrated that the PANI@hexaferrite composite with excellent MW absorption performance is expected to be potential MW absorbers for extensive applications. 相似文献
37.
Wei Lai Lihong Ge Huaming Li Yilin Deng Bin Xu Bo Ouyang Erjun Kan 《International Journal of Hydrogen Energy》2021,46(53):26861-26872
The electrochemical water splitting to produce H2 in high efficiency with earth-abundant-metal catalysts remains a challenge. Here, we describe a simple “cyclic voltammetry + ageing” protocol at room temperature to activate Ni electrode (AC-Ni/NF) for hydrogen evolution reaction (HER), by which Ni/Ni(OH)2 heterostructure is formed at the surface. In situ Raman spectroscopy reveals the gradual growth of Ni/Ni(OH)2 heterostructure during the first 30 min of the aging treatment and combined with polarization measurements, it suggests a positive relation between the Ni/Ni(OH)2 amount and HER performance of the electrode. The obtained AC-Ni/NF catalyst, with plentiful Ni–Ni(OH)2 interfaces, exhibits remarkable performance towards HER, with the low overpotential of only 30 mV at a H2-evolving current density of 10 mA/cm2 and 153 mV at 100 mA/cm2, as well as a small Tafel slope of 46.8 mV/dec in 1 M KOH electrolyte at ambient temperature. The excellent HER performance of the AC-Ni/NF could be maintained for at least 24 h without obvious decay. Ex situ experiments and in situ electrochemical-Raman spectroscopy along with density functional theory (DFT) calculations reveal that Ni/Ni(OH)2 heterostructure, although partially reduced, can still persist during HER catalysis and it is the Ni–Ni(OH)2 interface reducing the energy barrier of H1 adsorption thus promoting the HER performance. 相似文献
38.
对赤红球菌的组氨酸激酶基因进行密码子优化,将优化后的组氨酸激酶基因(rhks)构建重组表达质粒pGEX-4T-2-rhks。将此质粒导入到大肠杆菌BL21(DE3)中进行异源表达。在25 ℃和1 mmol/L异丙基-β-D-硫代吡喃半乳糖苷诱导条件下,组氨酸激酶融合蛋白(GST-RHK)获得成功表达,并具有催化活性。经谷胱甘肽琼脂糖亲和层析纯化,获得电泳纯的GST-RHK,其中纯化倍数为3.1,得率为19.5%。该蛋白大小约为72.75 kDa,Km、Vmax和Kcat值分别为20.92 μmol/L、0.17 μmol/(L·min)和1.4 min-1。野生型赤红球菌、组氨酸激酶基因增强株sdrhkE和组氨酸激酶基因敲减株sdrhkD在分别含有苯酚、甲苯、氯苯、异辛烷4 种有机溶剂的培养基中培养,菌株sdrhkD的生长情况都优于野生型赤红球菌,菌株sdrhkE的生长情况都低于野生型赤红球菌。本研究为进一步揭示赤红球菌SD3中组氨酸激酶涉及的信号转导途径与赤红球菌有机溶剂耐受性的关联机制提供一定参考依据。 相似文献
39.
Wang Hay Kan Chenxi Wei Dongchang Chen Tao Bo Bao‐Tian Wang Yan Zhang Yangchao Tian Jun‐Sik Lee Yijin Liu Guoying Chen 《Advanced functional materials》2019,29(17)
Lithium‐rich disordered rock‐salt oxides have attracted great interest owing to their promising performance as Li‐ion battery cathodes. While experimental and theoretical efforts are critical in advancing this class of materials, a fundamental understanding of key property changes upon Li extraction is largely missing. In the present study, single‐crystal synthesis of a new disordered rock‐salt cathode material, Li1.3Ta0.3Mn0.4O2 (LTMO), and its use as a model compound to investigate Li concentration–driven evolution of local cationic ordering, charge compensation, and chemical distribution are reported. Through the combined use of 2D and 3D X‐ray nanotomography, it is shown that Li removal accompanied by oxygen oxidation is correlated with the development of morphological defects such as particle cracking. Chemical heterogeneity, quantified by subparticle level distribution of Mn valence state, is minimal during Mn redox, which drastically increases upon the formation of cracks during oxygen redox. Density functional theory and bond valence sum mismatch calculations reveal the presence of local short‐range ordering in the pristine oxide, which gradually disappears along with the extraction of Li. The study suggests that with cycling the transformation into true cation–disordered state can be expected, which likely impacts the voltage profile and obtainable energy density of the oxide cathodes. 相似文献
40.
Xiao-Guang Yue Guang Zhang Qu Wu Fei Li Xian-Feng Chen Gao-Feng Ren Mei Li 《稀有金属(英文版)》2015,(2):125-132
In order to predict the wearing of stellite alloys,the related methods of rare metals data processing were discussed. The method of opposite degree(OD) algorithm was put forward to predict the wearing of stellite alloys.OD algorithm is based on prior numerical data, posterior numerical data and the opposite degree between numerical forecast data. To compare the performance of predicted results based on different algorithms, the back propagation(BP) and radial basis function(RBF) neural network methods were introduced. Predicted results show that the relative error of OD algorithm is smaller than those of BP and RBF neural network methods. OD algorithm is an effective method to predict the wearing of stellite alloys and it can be applied in practice. 相似文献