Enriched Surface Oxygen Vacancies of Photoanodes by Photoetching with Enhanced Charge Separation

A facile photoetching approach is described that alleviates the negative effects from bulk defects by confining the oxygen vacancy (O_vac) at the surface of BiVO₄ photoanode, by 10‐minute photoetching. This strategy could induce enriched O_vac at the surface of BiVO₄, which avoids the formation of excessive bulk defects. A mechanism is proposed to explain the enhanced charge separation at the BiVO₄ /electrolyte interface, which is supported by density functional theory (DFT) calculations. The optimized BiVO₄ with enriched surface O_vac presents the highest photocurrent among undoped BiVO₄ photoanodes. Upon loading FeOOH/NiOOH cocatalysts, photoetched BiVO₄ photoanode reaches a considerable water oxidation photocurrent of 3.0 mA cm^?2 at 0.6 V vs. reversible hydrogen electrode. An unbiased solar‐to‐hydrogen conversion efficiency of 3.5 % is realized by this BiVO₄ photoanode and a Si photocathode under 1 sun illumination.     

Experimental study on the smoke temperature evolution in a polyethylene (PE)-lined compartment on fire

Smoke temperature evolution in the upper layer of compartment fire, which is critical for the prediction of potential flashover, was experimentally investigated in a real building. Three-millimeter polyethylene (PE) slabs attached on the internal walls were employed as the lining material to address the effect of the melting and combustion of the lining material on the smoke temperature. A corner gasoline pool fire was utilized as the fire source. Two thermocouple trees, mounted vertically at the center and the open door, and a high-definition camera were utilized to record the smoke temperature history and experimental video. Meanwhile, some furniture was loaded to study its enhancement feature on fire intensity. Heat release rates (HRRs) at different stages were analyzed based on MQH method (McCaffrey, Quintiere and Harkleroad) and pool fire theory. Smoke temperature was estimated through an improved MQH correlation considering the melting of the PE slabs and an empirical model, BFD curve (Barnett in Fire Saf J 37: 437–463, 2002) combined. The results show that both the maximum HRR and smoke temperature, 925.91 kW and 491.7 °C, are lower than the critical values of flashover. The PE lining greatly intensifies the fire power and the resulting smoke temperature compared with the ones in noncombustible wall scenario. Combustion of the molten PE flowing down from the walls would lead to a secondary peak in smoke temperature curve, which is rarely considered in previous work.

     

Bridge Bonded Oxygen Ligands between Approximated FeN4 Sites Confer Catalysts with High ORR Performance

The applications of the most promising Fe—N–C catalysts are prohibited by their limited intrinsic activities. Manipulating the Fe energy level through anchoring electron‐withdrawing ligands is found effective in boosting the catalytic performance. However, such regulation remains elusive as the ligands are only uncontrollably introduced oweing to their energetically unstable nature. Herein, we report a rational manipulation strategy for introducing axial bonded O to the Fe sites, attained through hexa‐coordinating Fe with oxygen functional groups in the precursor. Moreover, the O modifier is stabilized by forming the Fe?O?Fe bridge bond, with the approximation of two FeN₄ sites. The energy level modulation thus created confers the sites with an intrinsic activity that is over 10 times higher than that of the normal FeN₄ site. Our finding opens a novel strategy to manage coordination environments at an atomic level for high activity ORR catalysts.     

Shape memory behaviors of crosslinked copolymers containing stearyl acrylate

Shape memory polymers were prepared by copolymerizing stearyl acrylate and methyl acrylate. The principle of this shape memory effect is based on reversible order-disorder transition of crystalline aggregates of stearyl moieties. A specific feature of this type of shape memory copolymer is that the transition temperature at which the polymer abruptly becomes soft and deforms can be controlled by changing the monomer composition, which enables one to adjust the shape memory effect at a desired temperature. Mechanism and process of the shape memory behaviors were discussed.     

Design,Synthesis, and Structure–Activity Relationship Study of Potent MAPK11 Inhibitors

Huntington’s disease (HD) is a rare single-gene neurodegenerative disease, which can only be treated symptomatically. Currently, there are no approved drugs for HD on the market. Studies have found that MAPK11 can serve as a potential therapeutic target for HD. Regrettably, no MAPK11 small molecule inhibitors have been approved at present. This paper presents three series of compounds that were designed and synthesized based on the structure of skepinone-L, a known MAPK14 inhibitor. Among the synthesized compounds, 13a and 13b, with IC₅₀ values of 6.40 nM and 4.20 nM, respectively, displayed the best inhibitory activities against MAPK11. Furthermore, the structure–activity relationship (SAR) is discussed in detail, which is constructive in optimizing the MAPK11 inhibitors for better activity and effect against HD.     

高压下β-InSe弹性常数、电子结构的第一性原理研究

基于密度泛函理论的第一性原理计算方法,本文研究了高压对β-InSe弹性常数、机械性能和电子结构的影响.在0～20 GPa范围内,随着压力的增大,β-InSe的晶格常数、晶胞体积逐渐减小,结构参数a/a_0、c/c_0、V/V_0单调减小.在0～12 GPa范围内,弹性模量G、E、B和泊松比v随着压力增大而增大,在16 GPa时大幅减小,G、E、B分别减小了34.9%、53.3%、82.9%.随着压力增大,Se-In和In-In原子之间的电荷密度增大,Se-In原子之间的共价键增强,层间距减小.而且,β-InSe在20 GPa时带隙消失,发生了半导体向半金属的相变.     

Theoretical investigation of the crystallographic structure,anisotropic elastic response,and electronic properties of the major borides in Ni-based superalloys

ABSTRACT

In Ni-based superalloys, it is usually found that borides can strengthen the grain boundaries, thereby resulting in an increase in mechanical strength and high-temperature creep properties. Due to their importance and prevalence in Ni-based superalloys, this study employs first-principles methods to investigate the crystallographic structure, anisotropic elastic response, and electronic properties of the major borides, such as M₂B, M₅B₃ and M₃B₂ (M: Cr, Mo, W), respectively, which is necessary for the assessment of complex mechanical responses of Ni-based superalloys. The results demonstrate that the studied borides are all thermodynamically and mechanically stable. Among the M _x B _y binary borides analysed, Cr _x B _y exhibits the largest shear modulus, Young’s modulus, and Vicker hardness values, and these properties increase with the increase of B contents. The studied borides display nearly isotropic elastic properties except for W₅B₃ and W₃B₂. The electronic structure analysis of M _x B _y shows that the strong hybridisation between M-d and B-p orbitals leads to these borides exhibiting higher theoretical hardness, and the overlapping peaks of M-d and B-p orbitals move to a lower energy area with the increase of B contents, which leads to the increase of shear and Young’s moduli of M _x B _y . Furthermore, for M₃B₂ borides, the Cr-B bonds and Cr–Cr bonds are much stronger than the W-B & Mo-B bonds, and W-W & Mo-Mo bonds, respectively, which leads to Cr _x B _y yielding the largest values of elastic moduli.     

石榴石固体电解质Li3BO3界面改性研究

石榴石固体电解质由于其高的离子电导率,对锂金属稳定等优点成为了下一代高性能锂电池的重要研究方向之一.但锂金属负极界面浸润性与锂枝晶问题限制了其应用.本文通过简单的液相沉积结合高温烧结的方法,在石榴石固体电解质片表面构建了一层稳定的硼酸三锂(Li3BO3)修饰层.研究表明,Li3BO3 修饰层可以有效改善石榴石固体电解质...     

Structural Entropy of the Stochastic Block Models

With the rapid expansion of graphs and networks and the growing magnitude of data from all areas of science, effective treatment and compression schemes of context-dependent data is extremely desirable. A particularly interesting direction is to compress the data while keeping the “structural information” only and ignoring the concrete labelings. Under this direction, Choi and Szpankowski introduced the structures (unlabeled graphs) which allowed them to compute the structural entropy of the Erdős–Rényi random graph model. Moreover, they also provided an asymptotically optimal compression algorithm that (asymptotically) achieves this entropy limit and runs in expectation in linear time. In this paper, we consider the stochastic block models with an arbitrary number of parts. Indeed, we define a partitioned structural entropy for stochastic block models, which generalizes the structural entropy for unlabeled graphs and encodes the partition information as well. We then compute the partitioned structural entropy of the stochastic block models, and provide a compression scheme that asymptotically achieves this entropy limit.