摘要：Fluorescent labels are widely used in the characterizations of DNA-based reaction network *** systematically studied the effects of commonly used fluorescent pairs on thermal stabilities of signal-substrate duplex and the strand displacement *** is demonstrated that the modifications of duplex with fluorescent pairs stabilize DNA duplex by up to 3.5℃,and the kinetics of DNA strand displacement circuit is also evidently slowed *** results highlight the importance of fluorescent pairs towards the kinetic modulation in designing nucleic acid probes and complex DNA dynamic circuits.

摘要：Developing highly active alloy catalysts that surpass the performance of platinum group metals in the oxygen reduction reaction(ORR)is critical in ***-based single-atom alloy(AuSAA)clusters are gaining recognition as promising alternatives due to their potential for high ***,enhancing its activity of AuSAA clusters remains challenging due to limited insights into its actual active site in alkaline ***,we studied a variety of Au_(54)M_(1) SAA cluster catalysts and revealed the operando formed MO_(x)(OH)_(y) complex acts as the crucial active site for catalyzing the ORR under the basic solution *** observed volcano plot indicates that Au_(54)Co_(1),Au_(54)M_(1),and Au_(54)Ru_(1) clusters can be the optimal Au_(54)M_(1) SAA cluster catalysts for the *** findings offer new insights into the actual active sites of AuSAA cluster catalysts,which will inform rational catalyst design in experimental settings.

摘要：Responsive soft materials capable of complex,reversible,and rapid geometric deformations under external stimuli hold significant potential for applications in minimally invasive medicine,wearable devices,and soft *** this study,we present a novel approach for designing reconfigurable three dimensional(3D)deformable magnetic soft materials through photothermal *** embedding hard magnetic particles within a polymer matrix composed of fibrous polypyrrole(PPy)and semi-crystalline polymer,we develop magnetic composites that can be remotely controlled to achieve precise,programmable deformations under an external magnetic *** key innovation lies in utilizing the photothermal effect of PPy,which temporarily alters the viscosity of the composite when irradiated with infrared light,allowing dynamic orientation of the magnetic *** cooling,the magnetic anisotropy is solidified,enabling rapid and reversible geometric *** method allows for intricate control over the magnetization distribution,leading to the development of multifunctional devices with various potential applications such as complex 3D deformations for soft robotics,multimodal electrical switches,rewritable quick response codes,and shape-adaptable *** study not only enhances the understanding of magnetic moment programming in soft materials but also opens new avenues for the design of adaptive and responsive materials for advanced technological applications.

摘要：The dynamic adsorption of possible intermediates on single-atom catalysts(SACs)under working condition plays a key role in the electrocatalytic performance by the oxygen evolution reaction(OER),and therefore the performance of the dynamic adsorption should be fully considered in the theoretical screening of potential *** on density functional theory calculations,the OER performance of 27 types of C_(2)N-supported single transition metal atoms(TM@C_(2)N)is systematically investigated without and with considering the dynamic adsorption of possible *** considering dynamic adsorption,only Rh@C_(2)N and Ni@C_(2)N are screened out as good ***,by further considering the dynamic adsorption configurations of possible intermediates,more promising TM@C_(2)N SACs including Fe(Co,Ni,Ru,Rh,Ir)@C_(2)N toward the OER are screened *** presence of the intermediates(*HO,*O)on SACs could shift their d band center toward lower energy level,which makes the interaction between the adsorbate and SACs moderate and thus enhances their OER *** present work is instructive for further screening and designing of efficient single-atom catalysts for the oxygen evolution reaction.

摘要：Carbon monoxide(CO)is recognized as a diffusible and biologically membrane-permeable ***,the question of whether extracellular and intracellular CO delivery would yield similar or distinct biological functions remains *** this study,utilizing nonmetallic CO-releasing micelles as a platform for localized CO delivery,we present evidence suggesting that selective antibacterial effects against Staphylococcus aureus(***)are exclusively evident upon intracellular CO release,even in cases of extracellular release with higher CO concentrations showing no comparable *** substantiate this assertion,we systematically design micellar nanoparticles with varying sizes,monomer sequences,and shell *** these variants,only the micelles taken up by *** and capable of intracellular CO release exhibit efficient bacteria-killing *** further demonstrate that the selective bactericidal effect is closely linked to the production of hydroxyl radicals after intracellular CO ***,intracellular CO release proves to be an efficient treatment for ***-induced skin abscesses without the need for additional antibiotics,showcasing synergistic antibacterial and anti-inflammatory *** findings underscore the pivotal role of the spatial location of CO release,significantly enhancing our understanding of the pathophysiological functions of gasotransmitters.

摘要：Layered inorganic materials provide an essential platform for constructing new structural configurations of materials with exceptional ***,precise control over the interlayer molecular arrangement remains a significant challenge,impeding in-depth exploration in physics and chemistry ***,we demonstrated a new layered organic-inorganic superlattice composed of a S-Ta-S inorganic lattice and bilayer linear molecules,providing superhigh heat insulation.A series of interlayer-confined intercalations of alkylamines with increasing chain length in the layered inorganic materials were achieved through precisely ordered molecule design(TaS_(2)-Cn,n=3,6,8,12).Systematic spectral analysis reveals that as the length of the intercalated alkyl chain increases,the alkyl chain between layers becomes more ordered and linear,and the gauche conformation ***,the more linear and ordered alkyl chain conformation results in lower thermal *** thermal conductivity of TaS_(2)-C12 is 0.426 W m^(−1) K^(−1),which is only one-third that of the pristine TaS_(2) *** anticipate that this layered organic-inorganic superlattice design will pave a new avenue for developing new organic-inorganic functional materials and probing the limits of ultralow thermal conductivity materials.

摘要：将不同金属元素通过合金化形成二维材料(金属烯)对基础研究和纳米电子器件的实际应用具有重要意义,但目前鲜有金属烯材料是具有本征带隙的半导体.受离子晶体成键特征的启发,通过结构搜索、成键分析和高通量第一性原理计算,本文从2500多个双金属烯中筛选出一系列具有晶格动力学稳定和碱金属-金离子键的二维碱金属金化物双金属烯半导体.由于碱金属和金之间的大电负性差,其中32个碱金属金化物双金属烯是带隙范围为0.97~5.20 eV的半导体材料,而锂金双金属烯由于电负性差减小呈现出金属性.Bohn-Oppenheimer分子动力学模拟表明19个双金属烯在室温下结构稳定有利于实际应用.这项研究为设计双金属烯半导体提供了指导,并揭示了二维金属合金中成键行为和电子结构性质间的关联.

摘要：Dissociative adsorption of HCl on Au(111)has become one of unsolved puzzles in surface *** tremendous efforts in the past years,varioustheoretical models still greatly overestimate the zero-coverage initial sticking probabilities(So).To find the origin of the large experiment-theory discrepancy,we have revisited the dissociative adsorption of HCl on Au(111)with a newly designed molecular beam-surface *** zero-coverage So derived from Cl-coverage measurements with varying HCl doses agree well with previous ***,we notice a sharp change of the coverage/dose slope with the HCl dosage at the low coverage regime,which may result in some uncertainties to the fitted So *** seems consistent with a coverage-dependence of the dissociation barrier predicted by density functional theory at low *** results reveal the potential inconsistency of utilizing simulations with finite coverage to compare against experimental data with zero coverage in this system,and provide guidance for improving both experiment and theory in this regard.

摘要：层状无机材料的弱层间耦合和大面积表面为构建低导热性无机固体材料提供了基本框架.合成具有足够散射和非谐波性的稳定层状材料,从而降低热导率,仍是一项挑战.本文在层状无机FeOCl材料体系中,通过一步氧化还原反应成功获得了一种结构稳定的富含Fe^(2+)的层状材料,实现了表面和界面的同步改性,并实现了超低的热导率.具体而言,系统的X射线吸收精细结构(XAFS)分析和电子能量损失光谱(EELS)分析表明,碱金属原子的层间插层和表面缺陷的引入诱导了大量Fe^(2+)的存在,从而增强了其非谐波性和声子散射.此外,声子态密度(PDOS)分布也提供了确凿的证据,证明了散射概率的提高和声子模式整体的软化.所制得的层状无机材料Fe(III)_(1−n)Fe(II)_(n)O_(1−x)Cl[K^(+)]_(m)不仅结构稳定,而且在298 K时的热导率比原始FeOCl降低了近60%,低至0.29 W m^(−1) K^(−1),这在层状无机材料中是极低的.这项研究为低导热层状材料的设计提供了新的视角.

摘要：The achievement of electrical spin control is highly *** promising strategy involves electrically mod-ulating the Rashba spin orbital coupling effect in materials.A semiconductor with high sensitivity in its Rashba constant to external electric fields holds great potential for short channel lengths in spin field-effect transistors,which is crucial for preserving spin coherence and enhancing integration ***,two-dimensional(2D)Rashba semiconductors with large Rashba constants and significant electric field responses are highly ***,by employing first-principles calculations,we design a thermodynamically stable 2D Rashba semiconductor,YSbTe_(3),which possesses an indirect band gap of 1.04 eV,a large Rashba constant of 1.54 eV·Åand a strong electric field response of up to 4.80 e·Å^(2).In particular,the Rashba constant dependence on the electric field shows an unusual nonlinear *** the same time,YSbTe_(3)has been identified as a 2D ferroelectric material with a moderate polarization switching energy barrier(~0.33 eV per formula).By changing the electric polarization direction,the Rashba spin texture of YSbTe_(3)can be *** out-standing properties make the ferroelectric Rashba semiconductor YSbTe_(3)quite promising for spintronic applications.