摘要：氨是一种很有前途的能源载体,由于其高氢含量和无碳的特点,可用于燃料电池,并可作为电解水制氢装置中水的替代氧化底物.然而,人们对氨电氧化反应(AOR)的机理认识不足,且缺乏廉价、高效的AOR催化剂,因而阻碍了氨基能源系统的发展.在这项工作中,我们通过光诱导化学沉淀法合成的新型Ni和Cu共掺杂的多孔FeOOH纳米棒(NiCu-FeOOH)可以作为AOR催化剂,其具有高效的催化活性(阳极电流密度达到10 mA cm^(-2)时执行电压为1.41 V)和在氨碱溶液中优异的稳定性.实验数据和理论计算结果表明,异质的Ni和Cu原子的协同作用使得NiCu-FeOOH表面的Ni和Fe位点表现出更合适的电子结构,他们可以共同吸附含氮中间产物和羟基,并使其吸附自由能位于火山形曲线的顶部,从而加速AOR脱氢.决速步骤的后移(*NH_(2)+*OH形成步骤移至*N_(2)H_(3)+*OH形成步骤)和决速步骤较低的能垒(0.86 eV)揭示了Ni和Cu的共掺策略使FeOOH晶体对催化AOR更具活性.本文创新地提出了涉及含氮中间物和羟基的共吸附反应途径,以更好地描述和模拟AOR过程,这为设计低成本和稳定的AOR催化剂开辟了新的路径.

摘要：Sodium ions(Na+) and ether electrolyte coinserted graphite possesses a considerable volume expansion effect. However, the mechanism fails to clearly explain its stability. In response to this deficiency, the co-inserted reaction is proposed, which is affected by the Lorentz force of the applied electric field under the high-current condition. The Na^(+) ions are separated out, while the ethylene glycol dimethyl ether molecules remain between the graphite layers. This insight provides a reasonable explanation for the extraordinary stability of this material. In situ X-ray diffraction and density functional theory calculations confirm the separation and release of Na+. On the basis of this result, unmodified commercial graphite was stably cycled 6400 times at a current density of up to 10 A g^(-1), and the capacity retention rate was as high as 97.2%. The full battery assembled in the laboratory has a maximum output power of 14,846 W kg^(-1)and an output energy density of 103 W h kg^(-1)(relative to the weight of anodic and cathodic active materials). The new mechanism provides innovative ideas for the design of large-scale energy storage devices.

摘要：Single-atom catalysts(SACs) with well-defined and specific single-atom dispersion on supports offer great potential for achieving both high catalytic activity and selectivity. Covalent organic frameworks(COFs) with tailormade crystalline structures and designable atomic composition is a class of promising supports for SACs. Herein, we have studied the binding sites and stability of Pd single atoms(SAs)dispersed on triazine COF(Pd1/trzn-COF) and the reaction mechanism of CO oxidation using the density functional theory(DFT). By evaluating different adsorption sites, including the nucleophilic sp2C atoms, heteroatoms and the conjugated π-electrons of aromatic ring and triazine, it is found that Pd SAs can stably combine with trzn-COF with a binding energy around-5.0 eV, and there are two co-existing dynamic Pd1/trzn-COFs due to the adjacent binding sites on trzn-COF. The reaction activities of CO oxidation on Pd1/trzn-COF can be regulated by the anion–π interaction between a +δ phenyl center and the related-δ moieties as well as the electron-withdrawing feature of imine in the specific complexes. The Pd1/trzn-COF catalyst is found to have a high catalytic activity for CO oxidation via a plausible tri-molecular Eley-Rideal(TER) reaction mechanism. This work provides insights into the d–π interaction between Pd SAs and trznCOF, and helps to better understand and design new SACs supported on COF nanomaterials.

摘要：nanopore 分析的概念，使用形成毛孔的蛋白质 -hemolysin 在单个分子的水平检测单个 nucleic 酸，首先在 1996 被建议。在过去的二十年，巨大的进步在 nanopore 地里被取得了，并且 nanopore 分析为与单个分子的敏感探查 biomolecules 和另外的 analytes 成为了一个没有标签、高产量的方法，特别保持为定序的第三产生 DNA 答应。然而，挑战在试验性的策略和整个基于 nanopore 的仪器的设计尚待。这里，我们骄傲地介绍奉献给 Nanopore 分析的话题的一个特殊话题，与 8 提供试验性的策略，理论计算和模拟的最新的范围的评论 / 文章，和仪器设计。试验性的策略上的评论和文章盖住划分成 nanopore，目标 DNA 的察觉，和基于 nanopore 的 DNA seq 的优点的 DNA 的控制……

摘要：The photoreduction of greenhouse gas CO_(2) using photocatalytic technologies not only benefits en-vironmental remediation but also facilitates the production of raw materials for ***-er,the efficiency of CO_(2) photoreduction remains generally low due to the challenging activation of CO_(2) and the limited light absorption and separation of *** engineering of catalysts rep-resents a pivotal strategy to enhance the photocatalytic activity for CO_(2),with most research on met-al oxide catalysts focusing on the creation of anionic *** exploration of metal vacancies and their effects,however,is still *** this study,we prepared an In2O3 catalyst with indium vacancies(VIn)through defect engineering for CO_(2) *** and theo-retical calculations results demonstrate that VIn not only facilitate light absorption and charge sepa-ration in the catalyst but also enhance CO_(2) adsorption and reduce the energy barrier for the for-mation of the key intermediate*COOH during CO_(2) *** metal vacancy engineering,the activity of the catalyst was 7.4 times,reaching an outstanding rate of 841.32μmol g(-1)h^(-1).This work unveils the mechanism of metal vacancies in CO_(2) photoreduction and provides theoretical guidance for the development of novel CO_(2) photoreduction catalysts.

摘要：The ternary cobalt-nickel-iron phosphide nanocubes (P-Co0.9Ni0.9Fe1.2 NCs) with high intrinsic activity, conductivity, defect concentration and optimized ratio have been realized through a facile phosphorization treatment using ternary cobalt-nickel-iron nanocubes of Prussian blue analogs (PBA) as a precursor. The scanning electron microscopy and transmission electron microscopy results show that the P-Co0.9Ni0.9Fe1.2 NCs maintain a cubic structure with a rough surface, implying the rich surface defects as exposed active sites. The thermal phosphorization of the ternary PBA precursor not only provids carbon doping but also leads to the in situ construction of surface defects on the NCs. The carbon doping from the PBA precursor lowers the charge transfer resistance and optimizes the electronic transformation. The synergistic effect among the ternary metal ions and rich defects contributes to the enhanced electrocatalytic performance . The P-Co0.9Ni0.9Fe1.2NCs achieve low overpotentials of -200.7 and 273.1 mV at a current density of 10 mA cm^-2 for the hydrogen evolution reaction and the oxygen evolution reaction, respectively. The potential of overall water splitting reaches 1.52 V at a current density of 10 mA cm^-2. The longterm stability of the electrocatalysts was also evaluated. This work provides a facile method to design efficient transitionmetal- based bifunctional electrocatalysts for overall water splitting.

摘要：Regulating the selectivity of catalysts in selective hydrogenation reactions at the atomic level is highly desirable but remains a grand challenge. Here we report a simple and practical strategy to synthesize a monolithic single-atom catalyst(SAC) with isolated Pd atoms supported on bulk nitrogen-doped carbon foams(Pd-SAs/CNF). Moreover, we demonstrate that the single-atom Pd sites with unique electronic structure endow Pd-SAs/CNF with an isolated site effect, leading to excellent activity and selectivity in 4-nitrophenylacetylene semi-hydrogenation reaction. In addition, benefiting from the great integrity and excellent mechanical strength, monolithic Pd-SAs/CNF catalyst is easy to separate from the reaction system for conducting the subsequent recycling. The cyclic test demonstrates the excellent reusability and stability of monolithic Pd-SAs/CNF *** discovery of isolated site effect provides a new approach to design highly selective catalysts. And the development of monolithic SACs provides new opportunities to advance the practical applications of single-atom catalysts.

摘要：The development of new proton-pump inhibitors (PPIs) with less adverse effects by lowering the pKa values of nitrogen atoms in pyrimidine rings has been previously suggested by our group. In this work, we proposed that new PPIs should have the following features:(1) number of ring II = number of ring I+ 1;(2) preferably five, six, or seven-membered heteroatomic ring for stability;and (3) 1<pKa1<4. Six molecular scaffolds based on the aforementioned criteria were constructed, and R groups were extracted from compounds in extensive data sources. A virtual molecule dataset was established, and the pKa values of specific atoms on the molecules in the dataset were calculated to select the molecules with required pKa values. Drug-likeness screening was further conducted to obtain the candidates that significantly reduced the adverse effects of long-term PPI use. This study provided insights and tools for designing targeted molecules in silico that are suitable for practical applications.

摘要：Azimuthal electromagnetic(EM)logging while drilling(LWD)has been extensively used in high-angle and horizontal(HA/HZ)***,due to the effects of formation anisotropy,accurate geosteering decision and formation evaluations have become increasingly *** quantitatively analyze the effect of anisotropy on tool responses and data processing,this paper investigates the sensitivity of EM LWD measurements to electric anisotropy and inversion accuracy via forward modeling and ***,a sensitivity factor is defined to quantitatively analyze the sensitivity of the magnetic field components and synthetic signals to electric ***,azimuthal EM LWD responses in anisotropic layered formations are simulated,and the sensitivities to formation parameters for compensated and uncompensated tool configurations are comparatively ***,we discuss the effects of the inversion model on bed boundary inversion in anisotropic *** simulation and inversion results show that azimuthal EM LWD can be significantly affected by electric ***,by using a symmetrical compensation configuration,the sensitivity of the geosignals to electric anisotropy can be suppressed,and the boundary detection capability can be further *** normally gives rise to separated resistivity curves and abnormal"horns";moreover,complicated nonlinear distortion can also arise in geosignals as the tool approaches a bed *** anisotropy effects are ignored in the inversion process,the estimated bed boundary and formation resistivity are usually unreliable,which may mislead geosteering decisions.

摘要：在电解水制氢过程中,为了在低电位下获得超高电流密度,其关键在于打破氧生成反应的标度关系.本文中,我们设计了一种新型异质界面功能化的NiFe(OH)_(x)/Ni_(3)S_(2)电催化剂,成功地规避了析氧反应(OER)的标度关系,使ΔGHOO*-ΔGHO*的差值从3.20 eV降低到2.38 eV.所制备的NiFe(OH)_(x)/Ni_(3)S_(2)电催化剂仅需要310 mV的过电位即可获得2000 mA cm^(-2)的超高电流密度, Tafel斜率仅为20.8 mV dec^(-1).此外,在1000 mA cm^(-2)的电流密度下,稳定运行100小时后无明显的活性损失,该性能优于目前报道的OER催化剂.进一步利用密度泛函理论计算和实验结果揭示了并联催化作用机制,发现多种中间体吸附能均一化能够优化OER反应路径,从而提升超高电流密度下的OER催化性能.本文的研究结果对开发工业级高性能水分解电催化剂具有重要的指导意义.