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1.
Dr. Yong-Sheng Wei Dr. Liming Sun Miao Wang Dr. Jinhua Hong Dr. Lianli Zou Hongwen Liu Dr. Yu Wang Dr. Mei Zhang Dr. Zheng Liu Prof. Yinwei Li Prof. Satoshi Horike Prof. Kazu Suenaga Prof. Qiang Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16147-16156
Understanding the thermal aggregation behavior of metal atoms is important for the synthesis of supported metal clusters. Here, derived from a metal–organic framework encapsulating a trinuclear FeIII2FeII complex (denoted as Fe3) within the channels, a well-defined nitrogen-doped carbon layer is fabricated as an ideal support for stabilizing the generated iron nanoclusters. Atomic replacement of FeII by other metal(II) ions (e.g., ZnII/CoII) via synthesizing isostructural trinuclear-complex precursors (Fe2Zn/Fe2Co), namely the “heteroatom modulator approach”, is inhibiting the aggregation of Fe atoms toward nanoclusters with formation of a stable iron dimer in an optimal metal–nitrogen moiety, clearly identified by direct transmission electron microscopy and X-ray absorption fine structure analysis. The supported iron dimer, serving as cooperative metal–metal site, acts as efficient oxygen evolution catalyst. Our findings offer an atomic insight to guide the future design of ultrasmall metal clusters bearing outstanding catalytic capabilities. 相似文献
2.
《自然科学进展(英文版)》2020,30(2):185-191
Metal-organic frameworks(MOFs) have been regarded as promising catalyst materials due to the richness of coordinately unsaturated metal sites on the surface,which can act as catalytic active centres.In this study,a hybrid MOF material composed of Fe-based MOF and Co-based MOF was prepared with the involvement of graphene oxide nanosheets as additive.It was demonstrated that the hybrid MOF materials showed much higher electro-catalytic activity towards oxygen evolution than the single-phase counterparts.To drive current density of 10 mA cm~(-2),the hybrid CoFe-based MOF only needed an over potential of 290 mV in 1 M KOH.The catalytic activity could sustain for a longer time with only slight current density decrease.During oxygen evolution operation,the MOF catalyst evolved into catalytic active species but kept well the microscale sheet-like structure.It is thus believed that this study will provide an avenue for the development of advanced electrocatalysts. 相似文献
3.
Hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) have been deemed as clean and sustainable strategies to solve the energy crisis and environmental problems. Various catalysts have been developed to promote the process of HER and OER. Among them, two-dimensional covalent organic frameworks (2D COFs) have received great attention due to their diverse and designable structure. In this minireview, we mainly summarize the diverse linkages of 2D COFs and strategies for enhancing the catalytic performance of 2D COFs for HER and OER, such as introducing active building blocks, metal ions and tailored linkages. Furthermore, a brief outlook for the development directions of COFs in the field of HER and OER is provided, expecting to stimulate new opportunities in future research. 相似文献
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In 1976 S. Hawking claimed that “Because part of the information about the state of the system is lost down the hole, the final situation is represented by a density matrix rather than a pure quantum state”. 1 This was the starting point of the popular “black hole (BH) information paradox”. 相似文献
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热运动对纳米级磁流变液系统的颗粒团聚行为和宏观流变特性扰动影响不可忽视.为研究施加外磁场后系统微结构与热运动间的关系,探讨在不同颗粒粒径情况下热运动能量在系统总能量中的占比.采用CCD设计方法,分析Monte Carlo仿真获取的颗粒位形信息,生成关于外磁场磁感应强度、颗粒粒径和体积分数的系统热耦合系数<λ>回归模型;成链团聚的临界颗粒粒径计算值比文献经验值高出约23%,证实在考虑系统内多因素的综合影响下,纳米级磁流变液具有更严格的流变现象临界发生条件. 相似文献
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本文通过组合数学和矩阵论的方法获得了完全图的特征多项式和谱,指出完全图的特征多项式的系数与图的结构之间的关系,并证明了邻接谱、拉谱拉斯谱和无符号拉谱拉斯谱三者之间的关系. 相似文献
9.
Sung Hwan Koo Dong Jun Li Taeyeong Yun Dong Sung Choi Kyung Eun Lee Gil Yong Lee Youngtak Oh Joonwon Lim Suchithra Padmajan Sasikala Ho Jin Lee In Ho Kim Hong Ju Jung Rishabh Jain Sang Ouk Kim 《Particle & Particle Systems Characterization》2019,36(7)
Efficient water electrolysis catalyst is highly demanded for the production of hydrogen as a sustainable energy fuel. It is reported that cobalt derived nanoparticle (CoS2, CoP, CoS|P) decorated reduced graphene oxide (rGO) composite aerogel catalysts for highly active and reliable hydrogen evolution reaction electrocatalysts. 7 nm level cobalt derived nanoparticles are synthesized over graphene aerogel surfaces with excellent surface coverage and maximal expose of active sites. CoS|P/rGO hybrid aerogel composites show an excellent catalytic activity with overpotential of ≈169 mV at a current density of ≈10 mA cm?2. Accordingly, efficient charge transfer is attained with Tafel slope of ≈52 mV dec?1 and a charge transfer resistance (Rct) of ≈12 Ω. This work suggests a viable route toward ultrasmall, uniform nanoparticles decorated graphene surfaces with well‐controlled chemical compositions, which can be generally useful for various applications commonly requiring large exposure of active surface area as well as robust interparticle charger transfer. 相似文献
10.
We give a sheaf theoretic interpretation of Potts models with external magnetic field, in terms of constructible sheaves and their Euler characteristics. We show that the polynomial countability question for the hypersurfaces defined by the vanishing of the partition function is affected by changes in the magnetic field: elementary examples suffice to see non-polynomially countable cases that become polynomially countable after a perturbation of the magnetic field. The same recursive formula for the Grothendieck classes, under edge-doubling operations, holds as in the case without magnetic field, but the closed formulae for specific examples like banana graphs differ in the presence of magnetic field. We give examples of computation of the Euler characteristic with compact support, for the set of real zeros, and find a similar exponential growth with the size of the graph. This can be viewed as a measure of topological and algorithmic complexity. We also consider the computational complexity question for evaluations of the polynomial, and show both tractable and NP-hard examples, using dynamic programming. 相似文献