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1.
Through a facile hydrothermal method, we have successfully prepared Ti3C2/Bi2.15WO6 (TC/BWO) composite, and systematically investigated their reactivity for the photocatalytic reduction of Cr(VI) under visible light. X-ray diffraction and Raman analysis confirm the formation of heterostructure between Bi2.15WO6 and Ti3C2. The resultant 7TC/BWO composite exhibits enhanced photoactivity toward Cr(VI) reduction. After 120 min irradiation, the conversion of Cr(VI) reaches 92.5% with the quasi-first-order kinetic constant of k = 0.0145 min?1, which is higher than that of pure BWO (30% and k = 0.0005 min?1). The electrochemical and photoluminescent characterization confirm that the introduction of Ti3C2 is conducive to the separation of carriers, thus significantly improves the photocatalytic performance of TC/BWO. Furthermore, the radical capture experiments verify that the electrons are important for enhancing reduction of Cr(VI) to Cr(III). As a result, this research provides a comprehensive understanding of the reduction of Cr(VI) by TC/BWO composite under visible light.  相似文献   
2.
The H2 storage properties of isoreticular metal-organic framework materials (IRMOFs), MOF-5 and IRMOF-10, impregnated with different numbers and types of heterogeneous C48B12 molecules were investigated using density functional theory and grand canonical Monte Carlo (GCMC) calculations. The excess hydrogen adsorption isotherms of IRMOFs at 77 K within 20 bar indicate that suitable number and type of C48B12 molecules play a crucial role in improving the H2 storage properties of IRMOFs. Among the studied pure and nC48B12 (n = 1, 2, 4, 8) in Ci symmetry impregnating into MOF-5, at 77 K under 6 bar, MOF-5-4C48B12 with a 3.5 wt% and 29.9 g/L hydrogen storage density, and at 77 K under 12 bar, the pure MOF-5 with a 4.9 wt% and 31.0 g/L hydrogen storage density has the best hydrogen storage properties. Whereas, among the studied pure and nC48B12 (n = 1, 2, 4, 8) in S6 symmetry impregnating into IRMOF-10, IRMOF-10-8C48B12 always shows the best hydrogen storage properties among the pure and C48B12-impregnated IRMOF-10 at 77 K within 20 bar. IRMOF-10-8C48B12 has a 6.0 wt% and 34.6 g/L hydrogen storage density at 77 K under 6 bar, and has a 7.1 wt% and 41.4 g/L hydrogen storage density at 77 K under 12 bar. The confinement effect of IRMOFs on C48B12 molecules, and steric hindrance effect of C48B12 molecules on IRMOFs mainly affects the H2 uptake capacity by comparing the absolute H2 molecules in individual IRMOFs units, C48B12 molecules, and IRMOFs-nC48B12 compounds. The absolute hydrogen adsorption profiles show that eight C48B12 molecules impregnating into MOF-5 can exert obvious steric effects for H2 adsorption. The saturated gravimetric and volumetric H2 densities of IRMOF-10-8C48B12 higher than those of MOF-5-8C48B12 due to with larger free volume.  相似文献   
3.
A high-throughput (105.5 g/h) passive four-stage asymmetric oscillating feedback microreactor using chaotic mixing mechanism was developed to prepare aggregated Barium sulfate (BaSO4) particles of high primary nanoparticle size uniformity. Three-dimensional unsteady simulations showed that chaotic mixing could be induced by three unique secondary flows (i.e., vortex, recirculation, and oscillation), and the fluid oscillation mechanism was examined in detail. Simulations and Villermaux–Dushman experiments indicate that almost complete mixing down to molecular level can be achieved and the prepared BaSO4 nanoparticles were with narrow primary particle size distribution (PSD) having geometric standard deviation, σg, less than 1.43 when the total volumetric flow rate Qtotal was larger than 10 ml/min. By selecting Qtotal and reactant concentrations, average primary particle size can be controlled from 23 to 109 nm as determined by microscopy. An average size of 26 nm with narrow primary PSD (σg = 1.22) could be achieved at Qtotal of 160 ml/min.  相似文献   
4.
甫沙4井位于塔里木盆地塔西南坳陷昆仑山前冲断带的柯东构造带上,北部和东部分别发育有柯克亚和柯东1井油气田。为研究甫沙4井原油来源与充注过程,对原油样品和连续抽提后的含油砂样各组分(游离态、束缚态、包裹体)进行GC、GC?MS和 GC?IRMS分析,与柯克亚凝析油气田油样进行油—油对比。结果表明:甫沙4井晚期充注原油组分具有C29?32重排藿烷、重排甾烷和Ts相对含量高,C27?29甾烷ααα 20R分布呈反“L”型,以及正构烷烃单体碳同位素值较低等特征,与柯克亚凝析油气田来源于二叠系普司格组(P2?3p)烃源岩的主体原油(I类)地球化学特征一致。而早期充注的原油组分具有重排藿烷、重排甾烷和Ts相对含量较低,C27?29甾烷ααα 20R分布呈“V”型,以及正构烷烃单体碳同位素值较高等特征,与柯克亚凝析油气田来源于中—下侏罗统湖相泥岩的II类原油地球化学特征一致。甫沙4井经历3个阶段成藏过程:①在上新世,二叠系烃源岩于生油晚期阶段生成的I类原油运移至柯克亚构造带或柯东构造带深部形成油藏;②在更新世早期,侏罗系烃源岩于生油早—中期生成的II类原油运移至甫沙4井白垩系储层;③在第四纪,强烈的构造作用使深部I类原油沿断裂调整进入甫沙4井白垩系储层。最终造成甫沙4井白垩系储层II类原油先充注,I类原油后充注的特殊现象。  相似文献   
5.
Customizing catalysts from the electronic structure, such as spin state, is an effective but challenging strategy for oxygen evolution reaction (OER). Herein, an ultrafine Co–Fe material highly dispersed on nitrogen carbide matrix is fabricated by coordination polymer and self-templating method to scrutinize the impact of spin state of Co on OER through Fe doping. The optimized catalyst shows boosted OER performance, which only requires overpotential of 333 mV at 10 mA cm?2, outperforming other control samples and commercial RuO2. The elevated local spin states of Co by Fe doping lead to charge transfer acceleration and fast generation of oxygenated intermediates, which is proved to account for the OER elevation. In addition, the long-term stability of Co–Fe material is guaranteed by the strong coordination of Co/Fe to the melamine-formaldehyde resin, which is used to adsorb metal ions, contributing to the high dispersion of active sites during the OER process.  相似文献   
6.
The study of steels which guarantee safety and reliability throughout their service life in hydrogen-rich environments has increased considerably in recent years. Their mechanical behavior in terms of hydrogen embrittlement is of utmost importance. This work aims to assess the effects of hydrogen on the tensile properties of quenched and tempered 42CrMo4 steels. Tensile tests were performed on smooth and notched specimens under different conditions: pre-charged in high pressure hydrogen gas, electrochemically pre-charged, and in-situ hydrogen charged in an acid aqueous medium. The influence of the charging methodology on the corresponding embrittlement indexes was assessed. The role of other test variables, such as the applied current density, the electrolyte composition, and the displacement rate was also studied. An important reduction of the strength was detected when notched specimens were subjected to in-situ charging. When the same tests were performed on smooth tensile specimens, the deformation results were reduced. This behavior is related to significant changes in the operative failure micromechanisms, from ductile (microvoids coalescence) in absence of hydrogen or under low hydrogen contents, to brittle (decohesion of martensite lath interfaces) under the most stringent conditions.  相似文献   
7.
8.
Conjugated polymers have emerged as a promising class of organic photocatalysts for photocatalytic hydrogen evolution from water splitting due to their adjustable chemical structures and electronic properties. However, developing highly efficient organic polymer photocatalysts with high photocatalytic activity for hydrogen evolution remains a significant challenge. Herein, we present an efficient approach to enhance the photocatalytic performance of linear conjugated polymers by modifying the surface chemistry via introducing a hydrophilic adenine group into the side chain. The adenine unit with five nitrogen atoms could enhance the interaction between the surface of polymer photocatalyst and water molecules through the formation of hydrogen bonding, which improves the hydrophilicity and dispersity of the resulting polymer photocatalyst in the photocatalytic reaction solution. In addition, the strong electron-donating ability of adenine group with plentiful nitrogen atoms could promote the separation of light-induced electrons and holes. As a result, the adenine-functionalized conjugated polymer PF6A-DBTO2 shows a high photocatalytic activity with a hydrogen evolution rate (HER) of 25.21 mmol g?1 h?1 under UV-Vis light irradiation, which is much higher than that of its counterpart polymer PF6-DBTO2 without the adenine group (6.53 mmol g?1 h?1). More importantly, PF6A-DBTO2 without addition of a Pt co-catalyst also exhibits an impressive HER of 21.93 mmol g?1 h?1 under visible light (λ > 420 nm). This work highlights that it is an efficient strategy to improve the photocatalytic activity of conjugated polymer photocatalysts by the modification of surface chemistry.  相似文献   
9.
Solar steam generation has attracted considerable interest due to its easy accessibility and sustainability. However, dye molecules were gradually concentrated on bulk water or the surface of solar absorbers during the disposal of dye wastewater. Herein, LaB6/g-C3N4 composites were immobilized on porous cotton cloth, served as a solar absorber resistant to dye clogging. The optimal solar absorber possessed solar harvesting of 92.3% and showed great application potential in the field of the treatment of dye wastewater. This study presented a new approach for the treatment of dye wastewater.  相似文献   
10.
CD4+ T cells orchestrate adaptive immune responses through their capacity to recruit and provide help to multiple immune effectors, in addition to exerting direct effector functions. CD4+ T cells are increasingly recognized as playing an essential role in the control of chronic viral infections. In this review, we present recent advances in understanding the nature of CD4+ T cell help provided to antiviral effectors. Drawing from our studies of natural human immunodeficiency virus (HIV) control, we then focus on the role of high-affinity T cell receptor (TCR) clonotypes in mediating antiviral CD4+ T cell responses. Last, we discuss the role of TCR affinity in determining CD4+ T cell differentiation, reviewing the at times divergent studies associating TCR signal strength to the choice of a T helper 1 (Th1) or a T follicular helper (Tfh) cell fate.  相似文献   
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