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1.
Efficient,robust and cost-effective electrocatalysts that catalyze hydrogen evolution/oxidation reaction(HER/HOR)in alkaline media are highly demanded.Recently,single-atom catalysts(SACs)have emerged as new promising candidates;however,the rational design of supports and the optimization of coordination environment between supports and metal atoms are challenging.In this work,we successfully fabricate atomically dispersed ruthenium(Ru)species,which are strongly coordinated by N and S dual heteroatoms on holey graphene(RuSA/NSG),as an excellent bifunctional catalyst for HER/HOR.In alkaline media,the developed catalyst exhibits high catalytic performance with a low overpotential of 57.3 mV to drive a current density of 10 mA cm-1 for HER,and its mass activity is about 5.8 times higher than that of commercial Pt/C and Ru/C catalysts at an overpotential of 100 mV.Similarly,considerable HOR performance of Ru SA/NSG is verified to be superior to Pt/C and Ru/C.Furthermore,X-ray-based spectroscopy measurements and density-functional theory calculations have confirmed that,compared with Ru–N4,the tailored Ru–N4–S2 with nearby S dopants can act as more active centers to greatly accelerate the sluggish HER/HOR kinetics in alkaline media.The present work provides a new atomic-level engineering strategy to modulate catalytic activities of SACs via the coordination design using dual heteroatoms on the carbon support.  相似文献   
2.
Constructing molecular switches based on supramolecular assembly strategy is a research hotspot. In this work, we constructed an all visible-light-regulated supramolecular photo-switch based on pyridinium-modified diarylethene derivative (DTE-Me) and cucurbit[8]uril (CB[8]). CB[8] not only accelerated the photochromic process under 365 nm ultraviolet light but also shifted the absorption of open formed DTE-Me to the visible region, which led to efficient photocyclization under 450 nm visible light irradiation, while DTE-Me and DTE-Me/CB[7] remained unchanged under the same irradiating condition. Moreover, the complexation with CB[8] could induce the strong thermally activated delayed fluorescence (TADF) of guest molecular at 550 nm, which further shifted to 670 nm through two-step sequential energy transfer with sulforhodamine B (SRB) and Cy5. This energy transfer process could also be regulated with visible light, and the application for information encryption was also demonstrated. This assembly provides a convenient approach to construct all visible light-regulated TADF photo-switch.  相似文献   
3.
The surface charge is a key concept in electrochemistry. Mathematically, the surface charge is obtained from a spatial integration of the volume charge along a particular direction. Ambiguities thus arise in choosing the starting and ending points of the integration. As for electrocatalytic interfaces, the presence of chemisorbates further complicates the situation. In this minireview, I adopt a definition of the surface charge within a continuum picture of the electric double layer. I will introduce surface charging behaviors of firstly ordinary electrochemical interfaces and then electrocatalytic interfaces featuring partially charged chemisorbates. Particularly, the origin of nonmonotonic surface charging behaviors of electrocatalytic interfaces is explained using a primitive model. Finally, a brief account of previous studies on the nonmonotonic surface charging behavior is presented, as a subline of the spectacular history of electric double layer.  相似文献   
4.
Supercapacitors (SCs) with high energy density and power density are a research hotspot. Herein, we report a flexible porous carbon membrane supercapacitor prepared by electrospinning polyacrylonitrile (PAN) with γ-cyclodextrin-MOF (γ-CD-MOF) and then carbonizing at 900 °C. BET results showed that the supercapacitor retained the skeleton of γ-CD, γ-CD-MOF and the pores formed by the spun-fibers, which were 0.73, 1.09 and 23–186 nm, respectively, showing a high specific surface area of 134.7 m2/g. The hierarchically porous structures ensure rapid charge transfer and ion diffusion, resulting in the PAN/γ-CD-MOF carbon electrode with a high capacity of 283.3 F/g. Moreover, the supercapacitor had a high energy density up to 17.5 Wh/kg and power density up to 6 kW/kg. Significantly, it showed excellent cycle stability with a capacitance retention of 97.5% after 6000 cycles. This work provides a supramolecular strategy to construct a flexible porous carbon membrane, which has potential for supercapacitor applications.  相似文献   
5.
Fuzzy Optimization and Decision Making - All existing methods to estimate unknown parameters in uncertain differential equations are based on difference scheme, and do not work when the time...  相似文献   
6.
In this paper, we investigate the existence of triple positive solutions of boundary value problems for high-order fractional differential equation at resonance with singularities by using the fixed point index theory and the Leggett-Williams theorem. The spectral theory and some new height functions are also employed to establish the existence of triple positive solutions. The nonlinearity involved is arbitrary fractional derivative, and permits singularity.  相似文献   
7.
Zheng  J.  Maharaj  C.  Liu  J.  Chai  H.  Liu  H.  Dear  J. P. 《Mechanics of Composite Materials》2022,58(1):125-140
Mechanics of Composite Materials - In this research, the maximum stress, Hashin, Puck, LaRC03, and Northwestern University (NU) criteria are analyzed based literature data, analytical results...  相似文献   
8.
物理教学离不开理想化模型的建构,简化的理想模型能够帮助中学生在现有知识层面的基础上,更好地理解相关知识并解决问题.但是在实际物理问题中,如果不充分考虑理想化条件,学生在解决问题时就容易产生认知矛盾,不知所措.以一个有趣的静电场问题为例,揭示理想化模型的局限性,强调"去理想化"思维习惯的重要性.探讨分析了教师如何帮助学生打破思维定势,让其对已掌握的物理知识活学活用,培养学生严谨的科学思维.  相似文献   
9.
主要基于紫外可见(UV-Vis)漫反射光谱首次对比研究了经过热处理、有机或无机染料改色或钴-60产生的γ射线辐照三种不同处理工艺对同为珍珠质的淡水与海水珍珠及贝壳珍珠层的漫反射光谱的影响机制。结果表明:(1)在不同颜色、淡海水属性的珍珠与贝壳珍珠层的UV-Vis反射光谱的紫外区皆存在约280 nm 处的吸收峰,上述吸收峰位归属于珍珠层中自身存在的有机质所致,而非珍珠的致色色素。(2)以上三种不同的处理工艺对上述280 nm处的吸收峰位存在一致的影响行为,即随着不同的处理工艺强度的增大,处理样品对应的反射谱图中约280 nm处吸收峰的强度逐渐降低直至消失。与此同时,珍珠的反射谱图中紫外区的反射主波长的反射强度也随之减弱,且反射主波长的峰位向可见光区发生显著红移。研究工作可为珍珠及珍珠的优化处理的鉴定筛选及其珍珠颜色的形成属性判定提供检测依据与理论支撑。  相似文献   
10.
Saxifraga atrata is an important traditional Tibetan medicine used to treat cough and pneumonia, and has tremendous medicinal potential. In this study, we devised a technique to separate 1,1-diphenyl-2-picrylhydrazyl inhibitors from a methanol extract of S. atrata. The material was first processed using MCI GEL CHP20P medium-pressure liquid chromatography, yielding 1.1 g of the target fraction Fr2. Subsequently, online hydrophilic interaction liquid chromatography-1,1-diphenyl-2-picrylhydrazyl assay was used to identify prospective 1,1-diphenyl-2-picrylhydrazyl inhibitors, and two 1,1-diphenyl-2-picrylhydrazyl inhibitor fractions (Fr24 and Fr25) were identified from Fr2. Then, medium-pressure preparation was continued using an XIon column to separate two 1,1-diphenyl-2-picrylhydrazyl inhibitor fractions (Fr24 and Fr25). The target compound was concentrated in fractions Fr24 and Fr25 using reverse-phase liquid chromatography during further separation procedures. Finally, the purity, structure, and 1,1-diphenyl-2-picrylhydrazyl inhibitory activity of the isolated 1,1-diphenyl-2-picrylhydrazyl inhibitors were determined. Two 1,1-diphenyl-2-picrylhydrazyl inhibitors (adenosine with the half maximal inhibitory concentration of 66.87 ± 14.33 μM and (-)-4-O-(E)-caffeoyl-l -threonic acid with the half maximal inhibitory concentration of 59.06 ± 5.02 μM) were isolated with purities exceeding 95%. The results showed that this technology is effective in the targeted separation of antioxidants from natural products.  相似文献   
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