基于平面度的燃料电池电化学性能模拟

 固体氧化物燃料电池的翘曲会影响电极-盖板界面的接触情况，从而影响电化学性能，对相关制造工艺提出了很大的挑战．为了分析燃料电池平面度对放电过程的影响，揭示其潜在的风险，我们建立了两个基于有限元法的仿真模型，对考虑平面度缺陷的燃料电池封装和放电进行分析．在对固体氧化物燃料电池进行平面度测量的基础上，首先建立了具有真实燃料电池翘曲特性的几何模型，分析封装过程中接触压力的分布情况．然后将接触电阻的仿真结果导入到三维多物理场耦合模型中，模拟具有平面度缺陷的燃料电池电化学性能．计算结果展示了燃料电池两侧封装过程中接触压力的分布情况．通过对比有接触电阻和无接触电阻的燃料电池电流密度，分析了电池与盖板的接触对放电过程的影响．结果表明，燃料电池的凹陷面较难达到满意的接触状态，需要比凸起面更大的封装压力．燃料电池表面接触电阻的变化将引起电流传导路径的变化，产生局部高电流或低电流．这项工作强调了在燃料电池中保持均匀分布的接触电阻的重要性，为今后的优化工作奠定了基础．     

环境规制强度影响能源效率的门槛效应研究——基于PSTR模型

利用非径向-SBM和CCR模型测算了我国30个省市(暂不包括西藏和港澳台地区)2007-2016年间的环境规制强度以及能源效率,构建面板平滑转移回归模型(PSTR),分析了环境规制强度对我国能源效率的连续非线性变化的影响.研究结果显示,全国环境规制强度对我国能源效率存在非线性效应,二者之间呈倒“U”型关系.环境规制强度小于门槛值0.6376时,环境规制对能源效率产生创新补偿效应,当环境规制强度高于门槛值0.6376时,环境规制对能源效率产生遵循成本效应.而我国东西部地区的环境规制强度与地区能源效率间却存在着与之相反的“U”型效应.     

Sterically Facilitated Intramolecular Nucleophilic NMe2 Group Substitution in the Synthesis of Fused Isoxazoles: Theoretical Study

The influence of steric repulsion between the NMe₂ group and a second ortho-(peri-)substituent in the series of 1-dimethylaminonaphthalene and N,N-dimethylanilene ortho-oximes on the ease of the NMe₂ group’s intramolecular nucleophilic substitution is studied. Possible reaction intermediates for three mechanisms are calculated (ωB97xd/def-2-TZVP), and their free Gibbs energies are compared to model reaction profiles. Supporting experiments have proved the absence of studied reactivity in the case of simple 2-dimethylaminobenzaldoxime, which allowed us to establish reactivity limits. The significant facilitation of NMe₂ group displacement in the presence of bulky substituents is demonstrated. The possibility of fused isoxazoles synthesis via the intramolecular nucleophilic substitution of a protonated NMe₂ group in the aniline and naphthalene series is predicted.     

Alkyl‐Chain‐Regulated Charge Transfer in Fluorescent Inorganic CsPbBr3 Perovskite Solar Cells

Improved charge extraction and wide spectral absorption promote power conversion efficiency of perovskite solar cells (PSCs). The state‐of‐the‐art carbon‐based CsPbBr₃ PSCs have an inferior power output capacity because of the large optical band gap of the perovskite film and the high energy barrier at perovskite/carbon interface. Herein, we use alkyl‐chain regulated quantum dots as hole‐conductors to reduce charge recombination. By precisely controlling alkyl‐chain length of ligands, a balance between the surface dipole induced charge coulomb repulsive force and quantum tunneling distance is achieved to maximize charge extraction. A fluorescent carbon electrode is used as a cathode to harvest the unabsorbed incident light and to emit fluorescent light at 516 nm for re‐absorption by the perovskite film. The optimized PSC free of encapsulation achieves a maximum power conversion efficiency up to 10.85 % with nearly unchanged photovoltaic performances under 80 %RH, 80 °C, or light irradiation in air.     

Information percolation and cutoff for the random‐cluster model

We consider the random‐cluster model (RCM) on with parameters p∈(0,1) and q ≥ 1. This is a generalization of the standard bond percolation (with edges open independently with probability p) which is biased by a factor q raised to the number of connected components. We study the well‐known Fortuin‐Kasteleyn (FK)‐dynamics on this model where the update at an edge depends on the global geometry of the system unlike the Glauber heat‐bath dynamics for spin systems, and prove that for all small enough p (depending on the dimension) and any q>1, the FK‐dynamics exhibits the cutoff phenomenon at with a window size , where λ_∞ is the large n limit of the spectral gap of the process. Our proof extends the information percolation framework of Lubetzky and Sly to the RCM and also relies on the arguments of Blanca and Sinclair who proved a sharp mixing time bound for the planar version. A key aspect of our proof is the analysis of the effect of a sequence of dependent (across time) Bernoulli percolations extracted from the graphical construction of the dynamics, on how information propagates.     

Comparison of the stability of thymine tautomers and the interaction of its tautomers with Na+, K+, Mg2+ and Ca2+ in gas and solvent phases

The present study compared the interactions among Na ⁺, K ⁺, Mg²⁺ and Ca²⁺, thymine and its tautomers in the gas and solvent phase, an interaction dependent upon the electronic construction of the tautomers. Three types of cation interaction with thymine and its tautomers were observed. In the first one, the metal cations interacted with a lone pair of nitrogen or oxygen of the tautomers. In the second type, there was an interaction among the cations, nitrogen and oxygen at the same time; the last one was that of cations with the electron density of thymine π-system, where the cations were perpendicular to the ring of thymine. The interaction of metals cation with tautomers was studied in the gas and solvent phases; a comparison was then made between interactions in two phases. The interaction energy for all complexes indicated the stability of complexes, an energy which was higher in Ca²⁺ and Mg²⁺ compared with Na⁺ and K⁺. Concerning K⁺ and Na⁺, the stability of all complexes of tautomers was greater than that of thymine complexes; however, the stability of certain Ca²⁺ and Mg²⁺ complexes was lower than the complexes of thymine.     

An improved evaluation of the neutron background in the PandaX-Ⅱ experiment

In dark matter direct detection experiments,neutron is a serious source of background,which can mimic the dark matter-nucleus scattering signals.In this paper,we present an improved evaluation of the neutron background in the PandaX-II dark matter experiment by a novel approach.Instead of fully relying on the Monte Carlo simulation,the overall neutron background is determined from the neutron-induced high energy signals in the data.In addition,the probability of producing a dark-matter-like background per neutron is evaluated with a complete Monte Carlo generator,where the correlated emission of neutron(s)andγ(s)in the(α,n)reactions and spontaneous fissions is taken into consideration.With this method,the neutron backgrounds in the Run 9(26-ton-day)and Run 10(28-ton-day)data sets of PandaX-II are estimated to be(0.66±0.24)and(0.47±0.25)events,respectively.     

Quantum to classical crossover under dephasing effects in a two-dimensional percolation model

Scaling theory predicts complete localization in d = 2 in quantum systems belonging to the orthogonal class(i.e., with timereversal symmetry and spin-rotation symmetry). The conductance g behaves as g^exp(-L/l) with system size L and localization length l in the strong disorder limit. However, classical systems can always have metallic states in which Ohm’s law shows a constant g in d=2. We study a two-dimensional quantum percolation model by controlling dephasing effects. The numerical investigation of g aims at simulating a quantum-to-classical percolation evolution. An unexpected metallic phase, where g increases with L, generates immense interest before the system becomes completely classical. Furthermore, the analysis of the scaling plot of g indicates a metal-insulator crossover.     

密度泛函理论研究MN@H_2O (M=Ga,Ge, In,Sn, Sb; N=M,Al)团簇的特性

采用密度泛函理论的B3LYP, B3P86, B1B95, P3PW91和PBE1PBE方法结合SDD, LANL2DZ和CEP-121G基组计算了d~(10)组态二聚物MN(M=Ga, Ge, In, Sn和Sb; N=M和Al)的几何结构.采用B3P86/SDD进一步研究了MN@H_2O团簇的几何结构及吸附能.结果表明,水分子结合在二聚物M_2上时,对二聚物影响较大,对水分子自身影响较小.将M_2中Ga, Ge, In, Sn或Sb替换一个原子为Al时,水分子在GeAl和SnAl上的吸附能变化较大,而在GaAl, InAl和SbAl上吸附能变化较小.另外, H_2O吸附在Ga, Ge, In, Sn和Sb上时,与吸附在Al上时,吸附能的变化不大.