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881.
Anti-plane deformation of square lattices containing interphases is analyzed. It is assumed that lattices are linear elastic but not necessarily isotropic, whereas interphases exhibit non-linear elastic behavior. It is demonstrated that such problems can be treated effectively using Green’s functions, which allow to eliminate the degrees of freedom outside of the interphase. Illustrative numerical examples focus on the determination of applied stresses leading to lattice instability. 相似文献
882.
We introduce a mixed network coupling mechanism and study its effects on how cooperation evolves in interdependent networks. This mechanism allows some players (conservative-driven) to establish a fixed-strength coupling, while other players (radical-driven) adjust their coupling strength through the evolution of strategy. By means of numerical simulation, a hump-like relationship between the level of cooperation and conservative participant density is revealed. Interestingly, interspecies interactions stimulate polarization of the coupling strength of radical-driven players, promoting cooperation between two types of players. We thus demonstrate that a simple mixed network coupling mechanism substantially expands the scope of cooperation among structured populations. 相似文献
883.
本文从几个不同方面回顾了何泽慧先生的学术成长经历。她继承了蔡元培等老一辈学者科学救国的理念,接受了前沿的科学教育和训练,在国际交流与合作中做出创新工作,并参与创建我国核科学事业,汇聚和培养了大批人才。科学的创新离不开优良的传统,我们纪念何泽慧先生百年诞辰,既缅怀她的创新成就和对科学事业的贡献,也要发扬她的科学精神和传统。 相似文献
884.
Yiming Sui Prof. Xiulei Ji 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(2):e202312585
The narrow electrochemical stability window of water poses a challenge to the development of aqueous electrolytes. In contrast to non-aqueous electrolytes, the products of water electrolysis do not contribute to the formation of a passivation layer on electrodes. As a result, aqueous electrolytes require the reactions of additional components, such as additives and co-solvents, to facilitate the formation of the desired solid electrolyte interphase (SEI) on the anode and cathode electrolyte interphase (CEI) on the cathode. This review highlights the fundamental principles and recent advancements in generating electrolyte interphases in aqueous batteries. 相似文献
885.
Dr. Delilah Jewel Dr. Rachel E. Kelemen Rachel L. Huang Dr. Zeyu Zhu Bharathi Sundaresh Kaitlin Malley Quan Pham Conor Loynd Zeyi Huang Prof. Tim van Opijnen Prof. Abhishek Chatterjee 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(9):e202316428
Heterologous tRNAs used for noncanonical amino acid (ncAA) mutagenesis in mammalian cells typically show poor activity. We recently introduced a virus-assisted directed evolution strategy (VADER) that can enrich improved tRNA mutants from naïve libraries in mammalian cells. However, VADER was limited to processing only a few thousand mutants; the inability to screen a larger sequence space precluded the identification of highly active variants with distal synergistic mutations. Here, we report VADER2.0, which can process significantly larger mutant libraries. It also employs a novel library design, which maintains base-pairing between distant residues in the stem regions, allowing us to pack a higher density of functional mutants within a fixed sequence space. VADER2.0 enabled simultaneous engineering of the entire acceptor stem of M. mazei pyrrolysyl tRNA (tRNAPyl), leading to a remarkably improved variant, which facilitates more efficient incorporation of a wider range of ncAAs, and enables facile development of viral vectors and stable cell-lines for ncAA mutagenesis. 相似文献
886.
政企关系是理解中国长期经济增长和经济转型的微观基础,也是转型经济中最重要的关系之一。然而,目前学术界关于政企关系类型和决定因素的研究总体上显得比较笼统,或者难以验证。为此,有必要提出一个初步的动态政企关系分析框架。从政府对企业是否干预以及如何干预两个维度,可将世界各国或地区的政企关系分为四种类型:政企合作、政企合谋、政企分治和政企伤害。由此得出了决定政企关系类型的三个主要因素:政府能力、产业规模和监督力量,三者分别代表政府、企业和第三方力量,通过在不同国家(或地区)、不同阶段的博弈决定了政企关系的性质以及动态变迁过程。在此基础上,提出了四个可检验的基本命题,并通过国内外的案例加以佐证。应用动态政企关系框架可以解释“中国奇迹”以及相关的重要现象,为我们理解真实世界的政企关系和改善政企关系提供了一套可识别和可操作的分析工具。 相似文献
887.
Dr. Fabrizio Creazzo Prof. Sandra Luber 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(68):17024-17037
Notwithstanding that RuO2 is a promising catalyst for the oxygen evolution reaction (OER), a plethora of fundamental details on its catalytic properties are still elusive, severely limiting its large-scale deployment. It is also established experimentally that corrosion and wettability of metal oxides can, in fact, enhance the catalytic activity for OER owing to the formation of a hydrated surface layer. However, the mechanistic interplay between surface wettability, interfacial water dynamics and OER across RuO2, and what degree these processes are correlated are still debated. Herein, spin-polarized Density Functional Theory Molecular Dynamics (DFT-MD) simulations, coupled with advanced enhanced sampling methods in the well-tempered metadynamics framework, are applied to gain a global understanding of RuO2 aqueous interface (explicit water solvent) in catalyzing the OER, and hence possibly help in the design of novel catalysts in the context of photochemical water oxidation. The present study quantitatively assesses the free-energy barriers behind the OER at the (110)-RuO2 catalyst surface revealing plausible pathways composing the reaction network of the O2 evolution. In particular, OER is investigated at room temperature when such a surface is exposed to both gas-phase and liquid-phase water. Albeit a unique efficient pathway has been identified in the gas-phase OER, a surprisingly lowest-free-energy-requiring reaction route is possible when (110)-RuO2 is in contact with explicit liquid water. By estimating the free-energy surfaces associated to these processes, we reveal a noticeable water-assisted OER mechanism which involves a crucial proton-transfer-step assisted by the local water environment. These findings pave the way toward the systematic usage of DFT-MD coupled with metadynamics techniques for the fine assessment of the activity of catalysts, considering finite-temperature and explicit-solvent effects. 相似文献
888.
Lilin Feng Liang Gao Volkan Besirlioglu Khalil Essani Malte Wittwer Tetiana Kurkina Yu Ji Prof. Ulrich Schwaneberg 《Angewandte Chemie (International ed. in English)》2023,62(22):e202214999
Oxidases are of interest to chemical and pharmaceutical industries because they catalyze highly selective oxidations. However, oxidases found in nature often need to be re-engineered for synthetic applications. Herein, we developed a versatile and robust flow cytometry-based screening platform “FlOxi” for directed oxidase evolution. FlOxi utilizes hydrogen peroxide produced by oxidases expressed in E. coli to oxidize Fe2+ to Fe3+ (Fenton reaction). Fe3+ mediates the immobilization of a His6-tagged eGFP (eGFPHis) on the E. coli cell surface, ensuring the identification of beneficial oxidase variants by flow cytometry. FlOxi was validated with two oxidases—a galactose oxidase (GalOx) and a D-amino acid oxidase (D-AAO)—yielding a GalOx variant (T521A) with a 4.4-fold lower Km value and a D-AAO variant (L86M/G14/A48/T205) with a 4.2-fold higher kcat than their wildtypes. Thus, FlOxi can be used for the evolution of hydrogen peroxide-producing oxidases and applied for non-fluorescent substrates. 相似文献
889.
Byeong Su Gu Dr. Soumen Dutta Yu-Rim Hong Dr. Odongo Francis Ngome Okello Hyeonae Im Seungil Ahn Prof. Dr. Si-Young Choi Prof. Dr. Jeong Woo Han Prof. Dr. Sunmin Ryu Prof. Dr. In Su Lee 《Angewandte Chemie (International ed. in English)》2023,62(31):e202307816
The performance of nanocrystal (NC) catalysts could be maximized by introducing rationally designed heterointerfaces formed by the facet- and spatio-specific modification with other materials of desired size and thickness. However, such heterointerfaces are limited in scope and synthetically challenging. Herein, we applied a wet chemistry method to tunably deposit Pd and Ni on the available surfaces of porous 2D−Pt nanodendrites (NDs). Using 2D silica nanoreactors to house the 2D-PtND, an 0.5-nm-thick epitaxial Pd or Ni layer ( e - Pd or e -Ni ) was exclusively formed on the flat {110} surface of 2D−Pt, while a non-epitaxial Pd or Ni layer ( n - Pd or n -Ni ) was typically deposited at the {111/100} edge in absence of nanoreactor. Notably, these differently located Pd/Pt and Ni/Pt heterointerfaces experienced distinct electronic effect to influence unequally in electrocatalytic synergy for hydrogen evolution reaction (HER). For instance, an enhanced H2 generation on the Pt{110} facet with 2D-2D interfaced e -Pd deposition and faster water dissociation on the edge-located n -Ni overpowered their facet-located counterparts in respective HER catalysis. Therefore, a feasible assembling of the valuable heterointerfaces in the optimal 2D n -Ni/e-Pd/Pt catalyst overcame the sluggish alkaline HER kinetics, with a catalytic activity 7.9 times higher than that of commercial Pt/C. 相似文献