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11.
Wenshu Chen Jiajun Gu Yongping Du Fang Song Fanxing Bu Jinghan Li Yang Yuan Ruichun Luo Qinglei Liu Di Zhang 《Advanced functional materials》2020,30(25)
Large‐scale production of hydrogen from water‐alkali electrolyzers is impeded by the sluggish kinetics of hydrogen evolution reaction (HER) electrocatalysts. The hybridization of an acid‐active HER catalyst with a cocatalyst at the nanoscale helps boost HER kinetics in alkaline media. Here, it is demonstrated that 1T–MoS2 nanosheet edges (instead of basal planes) decorated by metal hydroxides form highly active / heterostructures, which significantly enhance HER performance in alkaline media. Featured with rich / sites, the fabricated 1T–MoS2 QS/Ni(OH)2 hybrid (quantum sized 1T–MoS2 sheets decorated with Ni(OH)2 via interface engineering) only requires overpotentials of 57 and 112 mV to drive HER current densities of 10 and 100 mA cm?2, respectively, and has a low Tafel slope of 30 mV dec?1 in 1 m KOH. So far, this is the best performance for MoS2‐based electrocatalysts and the 1T–MoS2 QS/Ni(OH)2 hybrid is among the best‐performing non‐Pt alkaline HER electrocatalysts known. The HER process is durable for 100 h at current densities up to 500 mA cm?2. This work not only provides an active, cost‐effective, and robust alkaline HER electrocatalyst, but also demonstrates a design strategy for preparing high‐performance catalysts based on edge‐rich 2D quantum sheets for other catalytic reactions. 相似文献
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The effect of charge on the dihydrogen storage capacity of Sc2–C6H6 has been investigated at B3LYP-D3/6-311G(d,p) level. The neutral system Sc2–C6H6 can store 8H2 with gravimetric density of 8.76 wt %, and one H2 dissociates and bonds atomically on the scandium atom. The adsorption of 8H2 on Sc2–C6H6 is energetically favorable below 155 K. The atom-centered density matrix propagation (ADMP) molecular dynamics simulations show that Sc2–C6H6 can adsorb 3H2 within 1000 fs at 300K. Compared with Sc2–C6H6, the charged systems can adsorb more hydrogen molecules with higher gravimetric density, and all the H2 are adsorbed in the molecular form. The gravimetric densities of Sc2–C6H6+ and Sc2–C6H62+ are 9.75 and 10.71 wt%. Moreover, the maximum adsorption of charged systems are favorable in wider temperature range. Most importantly, the ADMP-MD simulations indicate that Sc2–C6H62+ can adsorb 6 hydrogen molecules within 1000 fs at 300K. It can be found that the gravimetric density (6.72 wt%) of Sc2–C6H62+ still exceeds the target of US Department of Energy (DOE) under ambient conditions. 相似文献
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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
16.
Solenn Percelay Jean-Marie Billard Thomas Freret Annie Andrieux Michel Boulouard Valentine Bouet 《International journal of molecular sciences》2021,22(5)
For a better translation from treatment designs of schizophrenia to clinical efficiency, there is a crucial need to refine preclinical animal models. In order to consider the multifactorial nature of the disorder, a new mouse model associating three factors (genetic susceptibility—partial deletion of the MAP6 gene, early-life stress—maternal separation, and pharmacological treatment—chronic Δ-9-tetrahydrocannabinol during adolescence) has recently been described. While this model depicts a schizophrenia-like phenotype, the neurobiological correlates remain unknown. Synaptic transmission and functional plasticity of the CA1 hippocampal region of male and female 3-hit mice were therefore investigated using electrophysiological recordings on the hippocampus slice. While basal excitatory transmission remained unaffected, NMDA receptor (NMDAr)-mediated long-term potentiation (LTP) triggered by theta-burst (TBS) but not by high-frequency (HFS) stimulation was impaired in 3-hit mice. Isolated NMDAr activation was not affected or even increased in female 3-hit mice, revealing a sexual dimorphism. Considering that the regulation of LTP is more prone to inhibitory tone if triggered by TBS than by HFS, the weaker potentiation in 3-hit mice suggests a deficiency of intrinsic GABA regulatory mechanisms. Indeed, NMDAr activation was increased by GABAA receptor blockade in wild-type but not in 3-hit mice. This electrophysiological study highlights dysregulations of functional properties and plasticity in hippocampal networks of 3-hit mice, one of the mechanisms suspected to contribute to the pathophysiology of schizophrenia. It also shows differences between males and females, supporting the sexual dimorphism observed in the disorder. Combined with the previously reported study, the present data reinforce the face validity of the 3-hit model that will help to consider new therapeutic strategies for psychosis. 相似文献
17.
针对谱聚类融合模糊C-means(FCM)聚类的蛋白质相互作用(PPI)网络功能模块挖掘方法准确率不高、执行效率较低和易受假阳性影响的问题,提出一种基于模糊谱聚类的不确定PPI网络功能模块挖掘(FSC-FM)方法。首先,构建一个不确定PPI网络模型,使用边聚集系数给每一条蛋白质交互作用赋予一个存在概率测度,克服假阳性对实验结果的影响;第二,利用基于边聚集系数流行距离(FEC)策略改进谱聚类中的相似度计算,解决谱聚类算法对尺度参数敏感的问题,进而利用谱聚类算法对不确定PPI网络数据进行预处理,降低数据的维数,提高聚类的准确率;第三,设计基于密度的概率中心选取策略(DPCS)解决模糊C-means算法对初始聚类中心和聚类数目敏感的问题,并对预处理后的PPI数据进行FCM聚类,提高聚类的执行效率以及灵敏度;最后,采用改进的边期望稠密度(EED)对挖掘出的蛋白质功能模块进行过滤。在酵母菌DIP数据集上运行各个算法可知,FSC-FM与基于不确定图模型的检测蛋白质复合物(DCU)算法相比,F-measure值提高了27.92%,执行效率提高了27.92%;与在动态蛋白质相互作用网络中识别复合物的方法(CDUN)、演化算法(EA)、医学基因或蛋白质预测算法(MGPPA)相比也有更高的F-measure值和执行效率。实验结果表明,在不确定PPI网络中,FSC-FM适合用于功能模块的挖掘。 相似文献
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Functional expression and synergistic cooperation of xylan‐degrading enzymes from Hypocrea orientalis and Aspergillus niger 下载免费PDF全文
20.
《Journal of the European Ceramic Society》2020,40(9):3437-3444
xBi2/3Cu3Ti4O12/(1-x)CaCu3Ti4O12 composites were prepared by traditional solid-state reaction method. Extremely high nonlinear coefficient of 25 and breakdown field of 18.92 kV·cm−1 were obtained in small current range of 0.1−1 mA·cm-2. In addition, reduced dielectric loss of 0.055 was achieved with high dielectric constant of 1369. Optimized nonlinear and dielectric properties were integrated to make the composites a promising dual-function varistor-capacitor candidate. Microstructure analysis discovered two areas with various Bi/Ca ratio, designated as Bi-H and Bi-L respectively. It was found that the maximum ratio of Bi-H/Bi-L heterogeneous interface corresponded to optimized nonlinear and dielectric performance, which was associated with elevated potential barrier height and huge grain boundary resistance. Combined with relaxation analysis, a core-shell structure was proposed to elaborate microstructure evolution in xBi2/3Cu3Ti4O12/(1-x)CaCu3Ti4O12 composite. According to the core-shell model, variation of heterogeneous interface was illustrated on how to influence nonlinear properties, which was well fitted to experimental results. 相似文献