析氢反应动力的交流阻抗法研究

利用交流阻抗法测定析氢电化学动力参数，得到与极化曲线法一致的结果，为确定复杂析氢过程速决定步骤提供了判据。     

Approximate Controllability for a Class of Abstract Second-Order Functional Evolution Equations

Results providing sufficient conditions for the approximate controllability of a class of second-order abstract functional evolution equations governed by the generator of a strongly continuous cosine family of linear operators, together with nonlocal initial conditions, are developed. This work extends results included in recent work by Naito, Park, Zhou, and others. The abstract theory is then applied to a parabolic partial integrodifferential equation.     

一般变换下的Jacobi椭圆函数展开法及应用

将在行波变换下的Jacobi椭圆函数展开法推广到范围非常广泛的一般函数变换下进行，利用这一方法求得了一些非线性发展方程的精确周期解，这些解包括了在行波变换下所求得的周期解. 证明了一些非线性发展方程的周期解一定是行波解. 关键词： 非线性发展方程 周期解 行波解 Jacobi椭圆函数     

Structural Evolution of a Formamide Modified Sol—Spectroscopic Study

We investigated the influence of formamide on the acid-catalyzed sol-gel process at 40°C, by Fourier transformed infrared spectroscopy. Two silica sols were studied: one containing formamide and one without. Following the time evolution of both the Si−O(H) stretching vibration at around 950 cm⁻¹ and the Si−O(−Si) vibration between 1080 and 1200 cm⁻¹, we were able to describe the structural evolution of each sol. We thus observed, in the case of the formamide containing sol, a peculiar two-step structural evolution which eventually resulted in a highly interconnected gel.     

氢气在贮氢合金电极上析出反应机理的研究

贮氢合金电极上氢气的析出反应分为水分子的放电和吸附氢原子复合脱附两个步骤，即反应按Ｖｏｌｍｅｒ－Ｔａｆｅｌ机理进行，反应的超电势η可以区分为η１和η２两个组成部分，反映了Ｖｏｌｍｅｒ和Ｔａｆｅｌ反应的极化特征。析氢反应的速度由二者混合控制，在高超电势区，主要则由Ｖｏｌｍｅｒ反应所控制。     

Screening of Clenbuterol Hydrochloride Aptamers Based on Capillary Electrophoresis

Capillary electrophoresis based systematic evolution of ligands via exponential enrichment (CE-SELEX) was reported as a homogeneous efficient method for high-affinity selection of aptamer, with several merits involving screening in free solution without nonspecific binding, capable of high-efficient separation, low-sample consumption, and saving money. There are few studies regarding the aptamer selection against small molecule using CE-SELEX, resulting from the aspects of less binding sites and the negligible variety of its complex with nucleic acid in the electrophoretic mobility. In this study, we performed the aptamer selection towards a small molecule target of clenbuterol hydrochloride (Clen) by CE-SELEX. In brief, Clen were first incubated with an 80 nt ssDNA library, and CZE-UV approach was used to separate complex and random ssDNA. The complex was then collected into a vial followed by PCR amplification. Through three round selections, the third library was selected to clone and ten sequences were finally obtained. The dissociation constant (K_d) of three potential candidates (Apt 4, Apt 7 and Apt 12) were determined by CE-LIF, and showed high affinities of 9.315 × 10^?7 M, 1.040 × 10^?6 M and 1.143 × 10^?5 M, respectively. The result of m-Fold software analysis showed that the above three sequences could form stem-loop structure, and the Apt 4 gave the lowest free energy and the most stable structure. Using salbutamol as a control, three selected aptamers were verified with high specificity.     

Gold/monolayer graphitic carbon nitride plasmonic photocatalyst for ultrafast electron transfer in solar-to-hydrogen energy conversion

Gold (Au) plasmonic nanoparticles were grown evenly on monolayer graphitic carbon nitride (g-C₃N₄) nanosheets via a facile oil-bath method. The photocatalytic activity of the Au/monolayer g-C₃N₄ composites under visible light was evaluated by photocatalytic hydrogen evolution and environmental treatment. All of the Au/monolayer g-C₃N₄ composites showed better photocatalytic performance than that of monolayer g-C₃N₄ and the 1% Au/monolayer g-C₃N₄ composite displayed the highest photocatalytic hydrogen evolution rate of the samples. The remarkable photocatalytic activity was attributed largely to the successful introduction of Au plasmonic nanoparticles, which led to the surface plasmon resonance (SPR) effect. The SPR effect enhanced the efficiency of light harvesting and induced an efficient hot electron transfer process. The hot electrons were injected from the Au plasmonic nanoparticles into the conduction band of monolayer g-C₃N₄. Thus, the Au/monolayer g-C₃N₄ composites possessed higher migration and separation efficiencies and lower recombination probability of photogenerated electron-hole pairs than those of monolayer g-C₃N₄. A photocatalytic mechanism for the composites was also proposed.     

三维百合花状的CoNi2S4作为先进的双功能电催化剂用于氢析出和氧析出反应

为简化电解水催化剂的合成过程和优化电解水操作系统, 双功能电解水催化剂的研究, 特别是在碱性条件下同时具有优异催化氢析出和氧析出反应性能的双功能电催化剂的研究尤为重要. 其中, 过渡金属硫化物, 特别是 CoNi 硫化物, 被报道有与氢化酶类似的催化活性中心, 从而具有优异的催化氢析出和催化氧析出反应性能. 虽然有关对过渡金属硫化物的研究很多, 但主要集中在具有一维纳米线和二维纳米片形貌结构的过渡金属硫化物. 不幸的是, 这些形貌结构的过渡金属硫化物在电催化过程中容易聚集和受限于电荷传输能力. 三维纳米结构的材料具有较大的比表面积以分布更多的活性位点和拥有良好的电子传输能力, 所以, 开发三维纳米结构的过渡金属硫化物材料可能是改进其催化电解水性能的一个好途径. 本文采用简单的两步水热法, 通过硫化合成的 CoNi 前体得到了长于泡沫镍上的三维百合花状的 CoNi2S4(Co-Ni2S4/Ni). 它只需要 54 mV 的过电位即可获得 10 mA cm-2的催化氢析出反应电流, 是最好的碱性催化氢析出反应电极材料之一. 它在驱动 100 mA cm-2的催化氧析出反应电流时也只需要 328 mV 的过电位. 另外, 把 CoNi2S4/Ni 分别作为阴极和阳极组装成双电极碱性水电解槽时, 它只需要 1.56 V 的电压即可获取 10 mA cm-2的催化全电解水电流并具有良好的催化全电解水稳定性.扫描电子显微镜、透射电子显微镜和 N2吸脱附曲线测试结果表明, 该三维百合花状的 CoNi2S4/Ni 的表面粗糙度高和拥有多孔特性. 多孔结构的 CoNi2S4/Ni 可提供更多可接触的催化活性位点, 也有利于催化过程中的电解质和生成的气体的扩散与传递. 交流阻抗图谱测试结果表明, CoNi2S4/Ni 具有良好的电子传输能力. 另外, 不同于前期对尖晶石结构的硫化物 AB2S4的研究结果, XPS 结果表明, CoNi2S4/Ni 中含有 Niб+和 Sб-活性物种, 表明 CoNi2S4具有与活性氢化酶类似的活 性中心. Niδ+和 Sδ-可分别作为氢氧根和质子的接收体, 协助促进吸附的水分子的分离, 从而提高材料的催化性能. 所以, Niδ+和 Sδ-活性物种的出现, 大比表面积的三维百合花状多孔结构和良好的电荷传输能力等特性集合于 CoNi2S4/Ni 上使得CoNi2S4/Ni 具有优异的催化氢析出和催化氧析出反应性能.     

碳球担载二硫化钴纳米复合电催化剂的制备及其析氢性能研究

采用一步水热法,通过引入载体碳球(CSs)和表面活性剂CTAB,将二硫化钴(CoS_2)纳米颗粒均匀负载在CSs表面.相比于单独的CoS_2,改性后CSs担载的CoS_2(CoS_2/A-CSs)展现出了更好的电催化活性.在电解液为0.5mol/L H_2SO_4溶液中,电流密度为10 mA·cm~(-2)条件下,其析氢反应过电位仅为154 mV.经过12 h的稳定性测试,CoS_2/A-CSs析氢反应过电位为180 mV,这表明其仍具有良好的电化学催化析氢反应活性.这种复合电催化剂的优良性能主要归因于CSs的高导电性和其对CoS_2纳米颗粒的均匀分散;此外,CTAB的引入,促使CSs与CoS_2之间结合的更加紧密,进而加快了活性位点间的电子传导.