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排序方式: 共有4619条查询结果,搜索用时 15 毫秒
1.
Benjamin De Bari Alexandra Paxton Dilip K. Kondepudi Bruce A. Kay James A. Dixon 《Entropy (Basel, Switzerland)》2021,23(5)
Coordination within and between organisms is one of the most complex abilities of living systems, requiring the concerted regulation of many physiological constituents, and this complexity can be particularly difficult to explain by appealing to physics. A valuable framework for understanding biological coordination is the coordinative structure, a self-organized assembly of physiological elements that collectively performs a specific function. Coordinative structures are characterized by three properties: (1) multiple coupled components, (2) soft-assembly, and (3) functional organization. Coordinative structures have been hypothesized to be specific instantiations of dissipative structures, non-equilibrium, self-organized, physical systems exhibiting complex pattern formation in structure and behaviors. We pursued this hypothesis by testing for these three properties of coordinative structures in an electrically-driven dissipative structure. Our system demonstrates dynamic reorganization in response to functional perturbation, a behavior of coordinative structures called reciprocal compensation. Reciprocal compensation is corroborated by a dynamical systems model of the underlying physics. This coordinated activity of the system appears to derive from the system’s intrinsic end-directed behavior to maximize the rate of entropy production. The paper includes three primary components: (1) empirical data on emergent coordinated phenomena in a physical system, (2) computational simulations of this physical system, and (3) theoretical evaluation of the empirical and simulated results in the context of physics and the life sciences. This study reveals similarities between an electrically-driven dissipative structure that exhibits end-directed behavior and the goal-oriented behaviors of more complex living systems. 相似文献
2.
Dr. Deepak Gupta Dr. Alae E. Lakraychi Dr. Buddha D. Boruah Simon De Kreijger Dr. Ludovic Troian-Gautier Prof. Benjamin Elias Prof. Michael De Volder Prof. Alexandru Vlad 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(42):e202201220
Controlling redox activity of judiciously appended redox units on a photo-sensitive molecular core is an effective strategy for visible light energy harvesting and storage. The first example of a photosensitizer - electron donor coordination compound in which the photoinduced electron transfer step is used for light to electrical energy conversion and storage is reported. A photo-responsive Ru-diimine module conjugated with redox-active catechol groups in [Ru(II)(phenanthroline-5,6-diolate)3]4− photosensitizer can mediate photoinduced catechol to dione oxidation in the presence of a sacrificial electron acceptor or at the surface of an electrode. Under potentiostatic condition, visible light triggered current density enhancement confirmed the light harvesting ability of this photosensitizer. Upon implementation in galvanostatic charge-discharge of a Li battery configuration, the storage capacity was found to be increased by 100 %, under 470 nm illumination with output power of 4.0 mW/cm−2. This proof-of-concept molecular system marks an important milestone towards a new generation of molecular photo-rechargeable materials. 相似文献
3.
古代食谱重建是目前国际考古学研究的热点之一。随着研究的深入,传统基于骨骼提取出骨胶原蛋白进行分析的方法逐渐凸显出一定的局限性。尤其是在考察先民食物结构和营养等级等方面,针对蛋白大分子获得的同位素信息,无法排除一些内在或外在因素的影响,因而常会引导我们做出错误的判断。因此,发展一种能进一步提高古代食谱研究准确率和分辨率的新方法,是当前科技考古研究的迫切需求。不同于大分子蛋白,氨基酸能在更细微的层面提供有机体和生态环境中有机代谢过程中多方面的信息,在生物考古领域内具有极大的应用潜力。以北非突尼斯迦太基凡达里奇墓地出土的人和动物样品为例(遗址年代约在公元5世纪中期至6世纪早期),进行基于骨胶原和单分子氨基酸的稳定同位素分析工作。对10个人和4具动物考古样品提取骨胶原,并进一步进行酸水解、衍生化等操作,通过气相色谱(GC)与同位素质谱(IRMS)串联技术,开展特定化合物同位素分析。研究结果揭示了该遗址先民的食谱特征,以C3类食物为主。重点考察了该遗址先民饮食中的蛋白摄入情况,结果表明该遗址先民饮食摄入有大量的动物蛋白,且不同个体存在较大差异。最后,通过对骨胶原和氨基酸分析结果所得结论的比较,证实基于单分子氨基酸的氮同位素分析对个体营养级位置的准确判断具有较大的优势。研究结果为深入研究我国古代先民食物结构差异和人群分化等问题提供了新的思路和依据。研究证实基于单分子氨基酸的同位素分析,将是显著提高古代食谱重建分辨率的有力手段,呼吁未来在我国考古材料中开展大量相关研究。 相似文献
4.
Archiv der Mathematik - Motivated by recent results on the minimal base of a permutation group, we introduce a new local invariant attached to arbitrary finite groups. More precisely, a subset... 相似文献
5.
Journal of Algebraic Combinatorics - It is well known that linear rank-metric codes give rise to q-polymatroids. Analogously to matroid theory, one may ask whether a given q-polymatroid is... 相似文献
6.
We consider percolation on the Voronoi tessellation generated by a homogeneous Poisson point process on the hyperbolic plane. We show that the critical probability for the existence of an infinite cluster tends to 1/2 as the intensity of the Poisson process tends to infinity. This confirms a conjecture of Benjamini and Schramm [5]. 相似文献
7.
Lucas Schreyer Roberta Properzi Benjamin List 《Angewandte Chemie (International ed. in English)》2019,58(37):12761-12777
High acidity and structural confinement are pivotal elements in asymmetric acid catalysis. The recently introduced imidodiphosphorimidate (IDPi) Brønsted acids have met with remarkable success in combining those features, acting as powerful Brønsted acid catalysts and “silylium” Lewis acid precatalysts in numerous thus far inaccessible transformations. Substrates as challenging to activate as simple olefins were readily transformed, ketones were employed as acceptors in aldolizations allowing sub‐ppm level catalysis, whereas enolates of the smallest donor aldehyde, acetaldehyde, did not polymerize but selectively added a single time to a variety of acceptor aldehydes. 相似文献
8.
Gabrielle A. Leith Allison M. Rice Brandon J. Yarbrough Anna A. Berseneva Richard T. Ly Charles N. Buck III Dr. Denis Chusov Amy J. Brandt Prof. Dr. Donna A. Chen Benjamin W. Lamm Prof. Dr. Morgan Stefik Kenneth S. Stephenson Dr. Mark D. Smith Prof. Dr. Aaron K. Vannucci Dr. Perry J. Pellechia Prof. Dr. Sophya Garashchuk Prof. Dr. Natalia B. Shustova 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(15):6056-6062
The effect of donor (D)–acceptor (A) alignment on the materials electronic structure was probed for the first time using novel purely organic porous crystalline materials with covalently bound two- and three-dimensional acceptors. The first studies towards estimation of charge transfer rates as a function of acceptor stacking are in line with the experimentally observed drastic, eight-fold conductivity enhancement. The first evaluation of redox behavior of buckyball- or tetracyanoquinodimethane-integrated crystalline was conducted. In parallel with tailoring the D-A alignment responsible for “static” changes in materials properties, an external stimulus was applied for “dynamic” control of the electronic profiles. Overall, the presented D–A strategic design, with stimuli-controlled electronic behavior, redox activity, and modularity could be used as a blueprint for the development of electroactive and conductive multidimensional and multifunctional crystalline porous materials. 相似文献
9.
10.
Daniel Hernández-Valdés Ricardo Fernández-Terán Benjamin Probst Bernhard Spingler Roger Alberto 《Helvetica chimica acta》2020,103(10):e2000147
Reduction of CO2 to CO and H2O is a two electron/two proton process. For this process, multinuclear complexes offer advantages by concentrating reduction equivalents more efficiently than mononuclear systems. We present novel complexes with [Re(η6-C6H6)2]+ as scaffold conjugated to one or two catalytically active [Ru(dmbpy)(CO)2Cl2] subunits (dmbpy=5,5′-dimethyl-2,2′-bipyridine). The [Re(η6-C6H6)2]+ scaffold was chosen due to its very high photo- and chemical stability, as well as the multiple degrees of freedom it offers for any conjugated functionalities. High efficiency and selectivity for the reduction of CO2 to CO (over H2 or HCOOH) is reported. TONs and TOFs were found to be comparable or higher than for the catalyst subunit without the rhenium framework. Cooperativity in photo- and electrocatalysis is observed for the complex comprising two catalytic subunits. The synergistic communication between the two catalytic subunits is responsible for the observed enhancement in both photo- and electrocatalytic performance. Confirmation of electronic communication between the two [Ru(dmbpy)(CO)2Cl2] subunits as well as the elucidation of a possible mechanism was supported by electrochemistry, IR-spectroelectrochemistry and DFT studies. 相似文献