The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter per...The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter persistent dendrite growth and parasitic reactions,driven by the inhomogeneous charge distribution and water-dominated environment within the EDL.Compounding this,classical EDL theory,rooted in meanfield approximations,further fails to resolve molecular-scale interfacial dynamics under battery-operating conditions,limiting mechanistic insights.Herein,we established a multiscale theoretical calculation framework from single molecular characteristics to interfacial ion distribution,revealing the EDL’s structure and interactions between different ions and molecules,which helps us understand the parasitic processes in depth.Simulations demonstrate that water dipole and sulfate ion adsorption at the inner Helmholtz plane drives severe hydrogen evolution and by-product formation.Guided by these insights,we engineered a“water-poor and anion-expelled”EDL using 4,1’,6’-trichlorogalactosucrose(TGS)as an electrolyte additive.As a result,Zn||Zn symmetric cells with TGS exhibited stable cycling for over 4700 h under a current density of 1 mA cm^(−2),while NaV_(3)O_(8)·1.5H_(2)O-based full cells kept 90.4%of the initial specific capacity after 800 cycles at 5 A g^(−1).This work highlights the power of multiscale theoretical frameworks to unravel EDL complexities and guide high-performance ARZB design through integrated theory-experiment approaches.展开更多
Soft X-ray detectors play a vital role in materials science,high-energy physics and medical imaging.Cs_(2)AgBiBr_(6),a lead-free double perovskite,has gained attention for its excellent optoelectronic properties,stabi...Soft X-ray detectors play a vital role in materials science,high-energy physics and medical imaging.Cs_(2)AgBiBr_(6),a lead-free double perovskite,has gained attention for its excellent optoelectronic properties,stability,and nontoxicity.However,its fast crystallization and requirement for high-temperature annealing(>250℃)often lead to inferior film quality,limiting its application in flexible devices.This study introduces an alloying strategy that significantly improves the quality of Cs_(2)AgBiBr_(6)thin films annealed at a reduced temperature of 150℃.Devices based on the alloyed thin films exhibit an ultra-low dark current of 0.32 nA·cm^(-2)and a quantum efficiency of 725%.Furthermore,the first successful integration of Cs_(2)AgBiBr_(6)with a thinfilm transistor backplane demonstrates its superior imaging performance,indicating that Cs_(2)AgBiBr_(6)is a promising material for next-generation soft X-ray sensors.展开更多
Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen ba...Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.展开更多
Abiotic oxygen formation predates photosynthesis,sustaining early chemical evolution,yet its elementary mechanisms remain contested.Here,we show the production pathways for molecular oxygen from doubly ionized carbon ...Abiotic oxygen formation predates photosynthesis,sustaining early chemical evolution,yet its elementary mechanisms remain contested.Here,we show the production pathways for molecular oxygen from doubly ionized carbon dioxide upon electron-impact.Through fragment ions and electron coincidence momentum imaging,we unambiguously determine the ionization mechanism by measuring the projectile energy loss in association with the C^(+) +O_(2)^(+) channel.Further potential energy and trajectory calculations enable us to elucidate the dynamical details of this fragmentation process,in which a bond rearrangement pathway is found to proceed via the structural deformation to a triangular intermediate.Moreover,we demonstrate a further roaming pathway for the formation of O_(2)^(+) from CO_(2)^(+) 2,in which a frustrated C-O bond cleavage leaves the O atom without sufficient energy to escape.The O atom then wanders around varied configuration spaces of the flat potential energy regions and forms a C-O-O_(2)^(+) intermediate prior to the final products C^(+) +O_(2)^(+).Considering the large quantities of free electrons in interstellar space,the processes revealed here are expected to be significant and should be incorporated into atmospheric evolution models.展开更多
We reported a type of strong and highly directional non-covalent interactions based on the dimerization of single-stranded helix to double-stranded helix that can achieve supramolecular polymerization, giving rise to ...We reported a type of strong and highly directional non-covalent interactions based on the dimerization of single-stranded helix to double-stranded helix that can achieve supramolecular polymerization, giving rise to the formation of linear supramolecular polymers.展开更多
In our previous study, complete single DNA strands which were obtained from nuclei, chloroplasts and plant mitochondria obeyed Chargaff’s second parity rule, although those which were obtained from animal mitochondri...In our previous study, complete single DNA strands which were obtained from nuclei, chloroplasts and plant mitochondria obeyed Chargaff’s second parity rule, although those which were obtained from animal mitochondria deviated from the rule. On the other hand, plant mitochondria obeyed another different rule after their classification. Complete single DNA strand sequences obtained from chloroplasts, plant mitochondria, and animal mitochondria, were divided into the coding and non-coding regions. The non-coding region, which was the complementary coding region on the reverse strand, was incorporated as a coding region in the forward strand. When the nucleotide contents of the coding region or non-coding regions were plotted against the composition of the four nucleotides in the complete single DNA strand, it was determined that chloroplast and plant mitochondrial DNA obeyed Chargaff’s second parity rule in both the coding and non-coding regions. However, animal mitochondrial DNA deviated from this rule. In chloroplast and plant mitochondrial DNA, which obey Chargaff’s second parity rule, the lines of regression for G (purine) and C (pyrimidine) intersected with regression lines for A (purine) and T (pyrimidines), respectively, at around 0.250 in all cases. On the other hand, in animal mitochondrial DNA, which deviates from Chargaff’s second parity rule, only regression lines due to the content of homonucleotides or their analogs in the coding or non-coding region against those in the complete single DNA strand intersected at around 0.250 at the horizontal axis. Conversely, the intersection of the two lines of regression (G and A or C and T) against the contents of heteronucleotides or their analogs shifted from 0.25 in both coding and non-coding regions. Nucleotide alternations in chloroplasts and plant mitochondria are strictly regulated, not only by the proportion of homonucleotides and their analogs, but also by the heteronucleotides and their analogs. They are strictly regulated in animal mitochondria only by the content of homonucleotides and their analogs.展开更多
In microcantilever-based label-free biodetection technologies, deflection changes induced by adsorptions of double-stranded DNA （dsDNA） molecules on Au-layer surface are greatly affected by the mechanical, thermal a...In microcantilever-based label-free biodetection technologies, deflection changes induced by adsorptions of double-stranded DNA （dsDNA） molecules on Au-layer surface are greatly affected by the mechanical, thermal and electrical properties of DNA biofilm. In this paper, the elastic properties of dsDNA biofilm are studied. First, the Parsegian＇s empirical potential based on a mesoscopic liq- uid crystal theory is employed to describe the interaction energy among coarse-grained DNA cylinders. Then, con- sidering a Gaussian distribution of DNA interaxial distance, the thought experiment method is used to derive an analyti- cal expression for Young＇s modulus of DNA biofilm with a stochastic packing pattern for the first time. Results show that Young＇s modulus of DNA biofilm is on the order of 10 MPa. These findings could provide a simple and effective method to evaluate the mechanical properties of soft biofilm on snbstrate.展开更多
The double-stranded DNA (dsDNA) probe contains two different protein binding sites. One is for DNA- binding proteins to be detected and the other is for a DNA restriction enzyme. The two sites were arranged together w...The double-stranded DNA (dsDNA) probe contains two different protein binding sites. One is for DNA- binding proteins to be detected and the other is for a DNA restriction enzyme. The two sites were arranged together with no base interval. The working principle of the capturing dsDNA probe is described as follows: the capturing probe can be cut with the DNA restriction enzyme (such as EcoR I) to cause a sticky terminal, if the probe is not bound with a target protein, and the sticky terminal can be extended and labeled with Cy3-dUTP by DNA polymerase. When the probe is bound with a target protein, the probe is not capable to be cut by the restriction enzyme because of space obstruction. The amount of the target DNA binding proteins can be measured according to the variations of fluorescent signals of the corresponding probes.展开更多
Objective： To describe the characteristics of short interfering double stranded RNA （dsRNA） against hepatitis C virus （HCV） and to fred out the determining factors in design for desirable inhibitory efficacy. Met...Objective： To describe the characteristics of short interfering double stranded RNA （dsRNA） against hepatitis C virus （HCV） and to fred out the determining factors in design for desirable inhibitory efficacy. Methods： The data were collected and analyzed by retrieval of 229 published short dsRNAs designed for degradation ofHCV RNA. Results： Statistical analyses showed that the most frequently involved short dsRNAs were directing against 5＇NTR/core and genotype lb, accounting for 64.2% and 69.9%, respectively. Inhibitory efficacy varied with the structural characteristics of short dsRNAs, of which the most potential were those directed against HCV core region with inhibitory efficacy of 70.2%. Moreover, the mean inhibitory efficacy of short dsRNAs with GC contents from 30% to 52% was higher than that of those with GC contents out of this range. Conclusion： Based on this pooled data in a relatively large sample, the present results provided clues to design for short dsRNAs with more potent inhibitory efficacy.展开更多
The unzipping process of double-stranded DNA is analysed using a discrete model at the base level [Chin. Phys. Lett. 22 （2005）1540]. The numerical results are consistent with the experimental observations on the for...The unzipping process of double-stranded DNA is analysed using a discrete model at the base level [Chin. Phys. Lett. 22 （2005）1540]. The numerical results are consistent with the experimental observations on the force-displacement behaviour including the sequence-dependence. We find that the hydrogen bond interaction in a base pair is crucially important to the force-displacement profile.展开更多
Using nonequilibrium molecular dynamics simulations, we study the thermal conductivity of asymmetric double chains. We couple two different single chains through interchain coupling to build three kinds of asymmetric ...Using nonequilibrium molecular dynamics simulations, we study the thermal conductivity of asymmetric double chains. We couple two different single chains through interchain coupling to build three kinds of asymmetric double- stranded chain system： intrachain interaction, external potential, and mass asymmetric double chains. It is reported that asymmetry is helpful in improving the thermal conductivity of the system. We first propose double-heat flux channels to explain the influence of asymmetric structures on the thermal conductivity. The phonon spectral behaviour and finite size effect are also included.展开更多
A new coordination compound, [（CuI）（Btd）]n （1, Btd = 2,1,3-benzothiadiazole）, was obtained at room temperature by the reaction of 2,1,3-benzothiadiazole with CuI and KI saturated aqueous solution. It was charact...A new coordination compound, [（CuI）（Btd）]n （1, Btd = 2,1,3-benzothiadiazole）, was obtained at room temperature by the reaction of 2,1,3-benzothiadiazole with CuI and KI saturated aqueous solution. It was characterized by elemental analysis, IR spectroscopy, single-crystal X-ray diffraction analysis and photoluminescence. The complex crystallizes in the triclinic Pi space group, with a = 4.1620（6）, b = 10.4590（15）, c = 10.5052（15） A, a = 69.310（2）, β = 83.608（2）, γ = 78.873（2）°, V = 419.30（10） A3, Z = 2, C6H4N2SCuI, Mr = 326.61, Dc = 2.587 g/cm^3, F（000） = 304 and/^（MoKa） = 6.464 mm-1. The final R = 0.0418 and wR = 0.0936 for 1451 observed reflections with 1 〉 2σ（I） and R = 0.0422 and wR = 0.0939 for all data. In the complex, the Cu atoms are coordinated by one nitrogen atom and three iodine atoms to form a double-stranded stair, and such stairs are further linked to build a 2D framework via C-H…I interactions.展开更多
Inflammasomes function as intracellular sensors of pathogen infection or cellular perturbation and thereby play a central role in numerous diseases.Given the high abundance of NLRP1 in epithelial barrier tissues,we sc...Inflammasomes function as intracellular sensors of pathogen infection or cellular perturbation and thereby play a central role in numerous diseases.Given the high abundance of NLRP1 in epithelial barrier tissues,we screened a diverse panel of viruses for inflammasome activation in keratinocytes.We identified Semliki Forest virus(SFV),a positive-strand RNA virus,as a potent activator of human,but not murine NLRP1.SFV replication and the associated formation of double-stranded(ds)RNA was required to engage the NLRP1 inflammasome.Moreover,delivery of long dsRNA was sufficient to trigger activation.Biochemical studies revealed that NLRP1 binds dsRNA via its LRR,resulting in its NACHT domain gaining ATPase activity.Altogether,these results establish human NLRP1 as a direct sensor for dsRNA and thus RNA virus infection.展开更多
The genomes of eukaryotic cells are under continuous assault by environmental agents and endogenous metabolic byproducts. Damage induced in DNA usually leads to a cascade of cellular events, the DNA damage response. F...The genomes of eukaryotic cells are under continuous assault by environmental agents and endogenous metabolic byproducts. Damage induced in DNA usually leads to a cascade of cellular events, the DNA damage response. Failure of the DNA damage response can lead to development of malignancy by reducing the efficiency and fidelity of DNA repair. The NBS1 protein is a component of the MRE11/RAD50/NBS 1 complex （MRN） that plays a critical role in the cellular response to DNA damage and the maintenance of chromosomal integrity. Mutations in the NBS1 gene are responsible for Nijmegen breakage syndrome （NBS）, a hereditary disorder that imparts an increased predisposition to development of malignancy. The phenotypic characteristics of cells isolated from NBS patients point to a deficiency in the repair of DNA double strand breaks. Here, we review the current knowledge of the role of NBS1 in the DNA damage response. Emphasis is placed on the role of NBS1 in the DNA double strand repair, modulation of the DNA damage sensing and signaling, cell cycle checkpoint control and maintenance oftelomere stability.展开更多
Lanthanide ions(Ln^(3+))doping provides a potential strategy to control over the luminescent properties of lead-free halide double perovskite nanocrystals(DP NCs).However,due to the low energy transfer efficiency betw...Lanthanide ions(Ln^(3+))doping provides a potential strategy to control over the luminescent properties of lead-free halide double perovskite nanocrystals(DP NCs).However,due to the low energy transfer efficiency between self-trapped exciton(STE)and Ln^(3+)ions,the characteristic emissions of Ln^(3+)ions are not prominent.Furthermore,the energy transfer mechanism between STE and Ln^(3+)ions is also elusive and requires in-depth study.We chose trace Bi^(3+)-doped Cs_(2)Ag_(0.6)Na_(0.4)InCl_(6-x)Br_(x) as a representative DP matrix to demonstrate that by tuning the bromide concentration,the Ln^(3+)emission can be greatly enhanced.Such enhanced STE and Ln^(3+)ions energy transfer originates from the high covalency of Ln-Br bond,which contributes to improve ment of the characteristic emission of Ln^(3+)ions.Furthermo re,optical spectroscopy reveals that the energy transfer mechanism from DP to Eu^(3+)ions is different from all the other doped Ln^(3+)ions.The energy transfer from DP to Eu^(3+)ions is mostly through Eu-Br charge transfer while the other Ln^(3+)ions are excited by energy transfer from STE.The distinct energy transfer mechanism has resulted from the energy separation between the excited energy level of Ln^(3+)ions and the bottom of conduction band of DP.With increasing the energy separation,the energy transfer from STE to Ln^(3+)ions is less efficient because of the generation of a larger number of phonons and finally becomes impossible for Eu^(3+)ions.Our results provide new insight into tuning the energy transfer of Ln^(3+)-doped DP NCs.展开更多
Lead-free hybrid double perovskites(LFHDPs) have received a lot of attention due to their environmental friendliness and promising attributes. However, studying the effect of film thickness on LFHDPs optoelectronic pr...Lead-free hybrid double perovskites(LFHDPs) have received a lot of attention due to their environmental friendliness and promising attributes. However, studying the effect of film thickness on LFHDPs optoelectronic properties has not yet been investigated. Herein, we synthesized two new Ruddlesden–Popper LFHDPs, namely(C_(5)H_(12)N)_(4)AgBiI_(8)(CAB-1) and(C_(6)H_(14)N)_(4)Ag Bi I8(CAB-2) using cyclopentylamine and cyclohexylamine as monoamine ligands. Indeed, these two Ag(Ⅰ)-Bi(Ⅲ) LFHDPs form smooth and uniform films ranging in thickness from 250 nm to 1 μm, with preferred orientations. Notably, the studies on the optical properties showed that the direct band gap value decreased from 2.17 e V to 1.91 e V for CAB-1 and from 2.05 e V to 1.86 e V for CAB-2 with increasing thickness. Accordingly, photo-current response using a xenon lamp revealed a significant difference of over 1000 n A between light and dark conditions for1 μm-thickness films, suggesting potential for light harvesting. Other than that, thicker films of CAB-1and CAB-2 exhibit high stability for 90 days in a relatively humid environment(RH of 55%), paving the way for promising optoelectronic applications.展开更多
The increased demand for personalized customization calls for new production modes to enhance collaborations among a wide range of manufacturing practitioners who unnecessarily trust each other.In this article,a block...The increased demand for personalized customization calls for new production modes to enhance collaborations among a wide range of manufacturing practitioners who unnecessarily trust each other.In this article,a blockchain-enabled manufacturing collaboration framework is proposed,with a focus on the production capacity matching problem for blockchainbased peer-to-peer(P2P)collaboration.First,a digital model of production capacity description is built for trustworthy and transparent sharing over the blockchain.Second,an optimization problem is formulated for P2P production capacity matching with objectives to maximize both social welfare and individual benefits of all participants.Third,a feasible solution based on an iterative double auction mechanism is designed to determine the optimal price and quantity for production capacity matching with a lack of personal information.It facilitates automation of the matching process while protecting users'privacy via blockchainbased smart contracts.Finally,simulation results from the Hyperledger Fabric-based prototype show that the proposed approach increases social welfare by 1.4%compared to the Bayesian game-based approach,makes all participants profitable,and achieves 90%fairness of enterprises.展开更多
Reconfigurable intelligent surface(RIS)is a novel meta-material which can form a smart radio environment by dynamically altering reflection directions of the impinging electromagnetic waves.In the prior literature,the...Reconfigurable intelligent surface(RIS)is a novel meta-material which can form a smart radio environment by dynamically altering reflection directions of the impinging electromagnetic waves.In the prior literature,the inter-RIS links which also contribute to the performance of the whole system are usually neglected when multiple RISs are deployed.In this paper we investigate a general double-RIS assisted multiple-input multiple-output(MIMO)wireless communication system under spatially correlated non line-of-sight propagation channels,where the cooperation of the double RISs is also considered.The design objective is to maximize the achievable ergodic rate based on full statistical channel state information(CSI).Specifically,we firstly present a closedform asymptotic expression for the achievable ergodic rate by utilizing replica method from statistical physics.Then a full statistical CSI-enabled optimal design is proposed which avoids high pilot training overhead compared to instantaneous CSI-enabled design.To further reduce the signal processing overhead and lower the complexity for practical realization,a common-phase scheme is proposed to design the double RISs.Simulation results show that the derived asymptotic ergodic rate is quite accurate even for small-sized antenna arrays.And the proposed optimization algorithm can achieve substantial gain at the expense of a low overhead and complexity.Furthermore,the cooperative double-RIS assisted MIMO framework is proven to achieve superior ergodic rate performance and high communication reliability under harsh propagation environment.展开更多
基金supported by the National Natural Science Foundation of China(52471240)the Natural Science Foundation of Zhejiang Province(LZ23B030003)+2 种基金the Fundamental Research Funds for the Central Universities(226-2024-00075)support from the Engineering and Physical Sciences Research Council(EPSRC,UK)RiR grant-RIR18221018-1EU COST CA23155。
文摘The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter persistent dendrite growth and parasitic reactions,driven by the inhomogeneous charge distribution and water-dominated environment within the EDL.Compounding this,classical EDL theory,rooted in meanfield approximations,further fails to resolve molecular-scale interfacial dynamics under battery-operating conditions,limiting mechanistic insights.Herein,we established a multiscale theoretical calculation framework from single molecular characteristics to interfacial ion distribution,revealing the EDL’s structure and interactions between different ions and molecules,which helps us understand the parasitic processes in depth.Simulations demonstrate that water dipole and sulfate ion adsorption at the inner Helmholtz plane drives severe hydrogen evolution and by-product formation.Guided by these insights,we engineered a“water-poor and anion-expelled”EDL using 4,1’,6’-trichlorogalactosucrose(TGS)as an electrolyte additive.As a result,Zn||Zn symmetric cells with TGS exhibited stable cycling for over 4700 h under a current density of 1 mA cm^(−2),while NaV_(3)O_(8)·1.5H_(2)O-based full cells kept 90.4%of the initial specific capacity after 800 cycles at 5 A g^(−1).This work highlights the power of multiscale theoretical frameworks to unravel EDL complexities and guide high-performance ARZB design through integrated theory-experiment approaches.
基金supported by the NSFC under Grant No.62474169the National Key Research and Development Program of China under Grant No.2024YFB3212200the funding from USTC under Grant Nos.WK2100000025,KY2190000003,and KY2190000006。
文摘Soft X-ray detectors play a vital role in materials science,high-energy physics and medical imaging.Cs_(2)AgBiBr_(6),a lead-free double perovskite,has gained attention for its excellent optoelectronic properties,stability,and nontoxicity.However,its fast crystallization and requirement for high-temperature annealing(>250℃)often lead to inferior film quality,limiting its application in flexible devices.This study introduces an alloying strategy that significantly improves the quality of Cs_(2)AgBiBr_(6)thin films annealed at a reduced temperature of 150℃.Devices based on the alloyed thin films exhibit an ultra-low dark current of 0.32 nA·cm^(-2)and a quantum efficiency of 725%.Furthermore,the first successful integration of Cs_(2)AgBiBr_(6)with a thinfilm transistor backplane demonstrates its superior imaging performance,indicating that Cs_(2)AgBiBr_(6)is a promising material for next-generation soft X-ray sensors.
基金financially supported by the National Natural Science Foundation of China(U21A20311,U24A2040,52171141,52272117)the Natural Science Foundation of Shandong Province(ZR2022JQ19)+3 种基金the Key Technology Research Project of Shandong Province(2023CXGC010202)the Taishan Industrial Experts Program(TSCX202306142)the Core Facility Sharing Platform of Shandong Universitythe Foundation of Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University。
文摘Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.
基金supported by the National Natural Science Foundation of China (Grant Nos.12325406,92261201,12404305,and W2512072)the Shaanxi Province Natural Science Fundamental Research Project (Grant Nos.2023JC-XJ-03 and23JSQ013)the China Postdoctoral Science Foundation (Grant Nos.BX20240286 and 2024M7625)。
文摘Abiotic oxygen formation predates photosynthesis,sustaining early chemical evolution,yet its elementary mechanisms remain contested.Here,we show the production pathways for molecular oxygen from doubly ionized carbon dioxide upon electron-impact.Through fragment ions and electron coincidence momentum imaging,we unambiguously determine the ionization mechanism by measuring the projectile energy loss in association with the C^(+) +O_(2)^(+) channel.Further potential energy and trajectory calculations enable us to elucidate the dynamical details of this fragmentation process,in which a bond rearrangement pathway is found to proceed via the structural deformation to a triangular intermediate.Moreover,we demonstrate a further roaming pathway for the formation of O_(2)^(+) from CO_(2)^(+) 2,in which a frustrated C-O bond cleavage leaves the O atom without sufficient energy to escape.The O atom then wanders around varied configuration spaces of the flat potential energy regions and forms a C-O-O_(2)^(+) intermediate prior to the final products C^(+) +O_(2)^(+).Considering the large quantities of free electrons in interstellar space,the processes revealed here are expected to be significant and should be incorporated into atmospheric evolution models.
基金financially supported by the National Natural Science Foundation of China(Nos.21574054,21722403,and 21420102007)
文摘We reported a type of strong and highly directional non-covalent interactions based on the dimerization of single-stranded helix to double-stranded helix that can achieve supramolecular polymerization, giving rise to the formation of linear supramolecular polymers.
文摘In our previous study, complete single DNA strands which were obtained from nuclei, chloroplasts and plant mitochondria obeyed Chargaff’s second parity rule, although those which were obtained from animal mitochondria deviated from the rule. On the other hand, plant mitochondria obeyed another different rule after their classification. Complete single DNA strand sequences obtained from chloroplasts, plant mitochondria, and animal mitochondria, were divided into the coding and non-coding regions. The non-coding region, which was the complementary coding region on the reverse strand, was incorporated as a coding region in the forward strand. When the nucleotide contents of the coding region or non-coding regions were plotted against the composition of the four nucleotides in the complete single DNA strand, it was determined that chloroplast and plant mitochondrial DNA obeyed Chargaff’s second parity rule in both the coding and non-coding regions. However, animal mitochondrial DNA deviated from this rule. In chloroplast and plant mitochondrial DNA, which obey Chargaff’s second parity rule, the lines of regression for G (purine) and C (pyrimidine) intersected with regression lines for A (purine) and T (pyrimidines), respectively, at around 0.250 in all cases. On the other hand, in animal mitochondrial DNA, which deviates from Chargaff’s second parity rule, only regression lines due to the content of homonucleotides or their analogs in the coding or non-coding region against those in the complete single DNA strand intersected at around 0.250 at the horizontal axis. Conversely, the intersection of the two lines of regression (G and A or C and T) against the contents of heteronucleotides or their analogs shifted from 0.25 in both coding and non-coding regions. Nucleotide alternations in chloroplasts and plant mitochondria are strictly regulated, not only by the proportion of homonucleotides and their analogs, but also by the heteronucleotides and their analogs. They are strictly regulated in animal mitochondria only by the content of homonucleotides and their analogs.
基金supported by the National Natural Science Foundation of China(11272193 and 10872121)the Shanghai Leading Academic Discipline Project(S30106)
文摘In microcantilever-based label-free biodetection technologies, deflection changes induced by adsorptions of double-stranded DNA （dsDNA） molecules on Au-layer surface are greatly affected by the mechanical, thermal and electrical properties of DNA biofilm. In this paper, the elastic properties of dsDNA biofilm are studied. First, the Parsegian＇s empirical potential based on a mesoscopic liq- uid crystal theory is employed to describe the interaction energy among coarse-grained DNA cylinders. Then, con- sidering a Gaussian distribution of DNA interaxial distance, the thought experiment method is used to derive an analyti- cal expression for Young＇s modulus of DNA biofilm with a stochastic packing pattern for the first time. Results show that Young＇s modulus of DNA biofilm is on the order of 10 MPa. These findings could provide a simple and effective method to evaluate the mechanical properties of soft biofilm on snbstrate.
文摘The double-stranded DNA (dsDNA) probe contains two different protein binding sites. One is for DNA- binding proteins to be detected and the other is for a DNA restriction enzyme. The two sites were arranged together with no base interval. The working principle of the capturing dsDNA probe is described as follows: the capturing probe can be cut with the DNA restriction enzyme (such as EcoR I) to cause a sticky terminal, if the probe is not bound with a target protein, and the sticky terminal can be extended and labeled with Cy3-dUTP by DNA polymerase. When the probe is bound with a target protein, the probe is not capable to be cut by the restriction enzyme because of space obstruction. The amount of the target DNA binding proteins can be measured according to the variations of fluorescent signals of the corresponding probes.
基金Supported by Grants from the Committee of Science and Technology of Shanghai, China (No.10ZR1413100, and No.114119a1400)
文摘Objective： To describe the characteristics of short interfering double stranded RNA （dsRNA） against hepatitis C virus （HCV） and to fred out the determining factors in design for desirable inhibitory efficacy. Methods： The data were collected and analyzed by retrieval of 229 published short dsRNAs designed for degradation ofHCV RNA. Results： Statistical analyses showed that the most frequently involved short dsRNAs were directing against 5＇NTR/core and genotype lb, accounting for 64.2% and 69.9%, respectively. Inhibitory efficacy varied with the structural characteristics of short dsRNAs, of which the most potential were those directed against HCV core region with inhibitory efficacy of 70.2%. Moreover, the mean inhibitory efficacy of short dsRNAs with GC contents from 30% to 52% was higher than that of those with GC contents out of this range. Conclusion： Based on this pooled data in a relatively large sample, the present results provided clues to design for short dsRNAs with more potent inhibitory efficacy.
基金Supported by the National Natural Science Foundation of China under Grant No 10474109, the 100 Persons Project of Chinese Academy of sciences, the Foundation of Ministry of Personnel of China, and Shanghai Supercomputer Center of China.
文摘The unzipping process of double-stranded DNA is analysed using a discrete model at the base level [Chin. Phys. Lett. 22 （2005）1540]. The numerical results are consistent with the experimental observations on the force-displacement behaviour including the sequence-dependence. We find that the hydrogen bond interaction in a base pair is crucially important to the force-displacement profile.
基金supported in part by the National Natural Science Foundation of China (Grant No. 11004082)the Natural Science Foundation of Guangdong Province of China (Grant No. 01005249)the Fundamental Research Funds for the Central Universities of China (Grant No. 21609305)
文摘Using nonequilibrium molecular dynamics simulations, we study the thermal conductivity of asymmetric double chains. We couple two different single chains through interchain coupling to build three kinds of asymmetric double- stranded chain system： intrachain interaction, external potential, and mass asymmetric double chains. It is reported that asymmetry is helpful in improving the thermal conductivity of the system. We first propose double-heat flux channels to explain the influence of asymmetric structures on the thermal conductivity. The phonon spectral behaviour and finite size effect are also included.
基金Supported by the National Natural Science Foundation of China (61205184)the Department of Education of Zhejiang Province (Y201122207)+1 种基金Open Foundation of Zhejiang Provincial Top Key Academic Discipline of Applied Chemistry and Eco-Dyeing & Finishing Engineering (YR2012013)the Young Researchers Foundation of Zhejiang Provincial Top Key Academic Discipline of Applied Chemistry and Eco-Dyeing & Finishing Engineering (ZYG2012003)
文摘A new coordination compound, [（CuI）（Btd）]n （1, Btd = 2,1,3-benzothiadiazole）, was obtained at room temperature by the reaction of 2,1,3-benzothiadiazole with CuI and KI saturated aqueous solution. It was characterized by elemental analysis, IR spectroscopy, single-crystal X-ray diffraction analysis and photoluminescence. The complex crystallizes in the triclinic Pi space group, with a = 4.1620（6）, b = 10.4590（15）, c = 10.5052（15） A, a = 69.310（2）, β = 83.608（2）, γ = 78.873（2）°, V = 419.30（10） A3, Z = 2, C6H4N2SCuI, Mr = 326.61, Dc = 2.587 g/cm^3, F（000） = 304 and/^（MoKa） = 6.464 mm-1. The final R = 0.0418 and wR = 0.0936 for 1451 observed reflections with 1 〉 2σ（I） and R = 0.0422 and wR = 0.0939 for all data. In the complex, the Cu atoms are coordinated by one nitrogen atom and three iodine atoms to form a double-stranded stair, and such stairs are further linked to build a 2D framework via C-H…I interactions.
文摘Inflammasomes function as intracellular sensors of pathogen infection or cellular perturbation and thereby play a central role in numerous diseases.Given the high abundance of NLRP1 in epithelial barrier tissues,we screened a diverse panel of viruses for inflammasome activation in keratinocytes.We identified Semliki Forest virus(SFV),a positive-strand RNA virus,as a potent activator of human,but not murine NLRP1.SFV replication and the associated formation of double-stranded(ds)RNA was required to engage the NLRP1 inflammasome.Moreover,delivery of long dsRNA was sufficient to trigger activation.Biochemical studies revealed that NLRP1 binds dsRNA via its LRR,resulting in its NACHT domain gaining ATPase activity.Altogether,these results establish human NLRP1 as a direct sensor for dsRNA and thus RNA virus infection.
文摘The genomes of eukaryotic cells are under continuous assault by environmental agents and endogenous metabolic byproducts. Damage induced in DNA usually leads to a cascade of cellular events, the DNA damage response. Failure of the DNA damage response can lead to development of malignancy by reducing the efficiency and fidelity of DNA repair. The NBS1 protein is a component of the MRE11/RAD50/NBS 1 complex （MRN） that plays a critical role in the cellular response to DNA damage and the maintenance of chromosomal integrity. Mutations in the NBS1 gene are responsible for Nijmegen breakage syndrome （NBS）, a hereditary disorder that imparts an increased predisposition to development of malignancy. The phenotypic characteristics of cells isolated from NBS patients point to a deficiency in the repair of DNA double strand breaks. Here, we review the current knowledge of the role of NBS1 in the DNA damage response. Emphasis is placed on the role of NBS1 in the DNA double strand repair, modulation of the DNA damage sensing and signaling, cell cycle checkpoint control and maintenance oftelomere stability.
基金Project supported by the Research Project of Mindu Innovation Laboratory(2021ZZ114)Natural Science Foundation of Xiamen(3502Z20227255)+1 种基金Major Research Project of Xiamen(3502Z20191015)the Science and Technology Major Project of Fujian Province(2021HZ021013)。
文摘Lanthanide ions(Ln^(3+))doping provides a potential strategy to control over the luminescent properties of lead-free halide double perovskite nanocrystals(DP NCs).However,due to the low energy transfer efficiency between self-trapped exciton(STE)and Ln^(3+)ions,the characteristic emissions of Ln^(3+)ions are not prominent.Furthermore,the energy transfer mechanism between STE and Ln^(3+)ions is also elusive and requires in-depth study.We chose trace Bi^(3+)-doped Cs_(2)Ag_(0.6)Na_(0.4)InCl_(6-x)Br_(x) as a representative DP matrix to demonstrate that by tuning the bromide concentration,the Ln^(3+)emission can be greatly enhanced.Such enhanced STE and Ln^(3+)ions energy transfer originates from the high covalency of Ln-Br bond,which contributes to improve ment of the characteristic emission of Ln^(3+)ions.Furthermo re,optical spectroscopy reveals that the energy transfer mechanism from DP to Eu^(3+)ions is different from all the other doped Ln^(3+)ions.The energy transfer from DP to Eu^(3+)ions is mostly through Eu-Br charge transfer while the other Ln^(3+)ions are excited by energy transfer from STE.The distinct energy transfer mechanism has resulted from the energy separation between the excited energy level of Ln^(3+)ions and the bottom of conduction band of DP.With increasing the energy separation,the energy transfer from STE to Ln^(3+)ions is less efficient because of the generation of a larger number of phonons and finally becomes impossible for Eu^(3+)ions.Our results provide new insight into tuning the energy transfer of Ln^(3+)-doped DP NCs.
基金supported by the National Natural Science Foundation of China (Nos. 22375157 and W2433042)the Key Scientific and Technological Innovation Team of Shaanxi Province(No. 2020TD-001)+1 种基金the Fundamental Research Funds for Central Universities, State Key Laboratory of Electrical Insulation and Power Equipment (No. EIPE23409)the Instrument Analysis Center of Xi’an Jiaotong University for assistance。
文摘Lead-free hybrid double perovskites(LFHDPs) have received a lot of attention due to their environmental friendliness and promising attributes. However, studying the effect of film thickness on LFHDPs optoelectronic properties has not yet been investigated. Herein, we synthesized two new Ruddlesden–Popper LFHDPs, namely(C_(5)H_(12)N)_(4)AgBiI_(8)(CAB-1) and(C_(6)H_(14)N)_(4)Ag Bi I8(CAB-2) using cyclopentylamine and cyclohexylamine as monoamine ligands. Indeed, these two Ag(Ⅰ)-Bi(Ⅲ) LFHDPs form smooth and uniform films ranging in thickness from 250 nm to 1 μm, with preferred orientations. Notably, the studies on the optical properties showed that the direct band gap value decreased from 2.17 e V to 1.91 e V for CAB-1 and from 2.05 e V to 1.86 e V for CAB-2 with increasing thickness. Accordingly, photo-current response using a xenon lamp revealed a significant difference of over 1000 n A between light and dark conditions for1 μm-thickness films, suggesting potential for light harvesting. Other than that, thicker films of CAB-1and CAB-2 exhibit high stability for 90 days in a relatively humid environment(RH of 55%), paving the way for promising optoelectronic applications.
基金supported in part by the National Natural Science Foundation of China(62273310)the Natural Science Foundation of Zhejiang Province of China(LY22F030006,LZ24F030009)
文摘The increased demand for personalized customization calls for new production modes to enhance collaborations among a wide range of manufacturing practitioners who unnecessarily trust each other.In this article,a blockchain-enabled manufacturing collaboration framework is proposed,with a focus on the production capacity matching problem for blockchainbased peer-to-peer(P2P)collaboration.First,a digital model of production capacity description is built for trustworthy and transparent sharing over the blockchain.Second,an optimization problem is formulated for P2P production capacity matching with objectives to maximize both social welfare and individual benefits of all participants.Third,a feasible solution based on an iterative double auction mechanism is designed to determine the optimal price and quantity for production capacity matching with a lack of personal information.It facilitates automation of the matching process while protecting users'privacy via blockchainbased smart contracts.Finally,simulation results from the Hyperledger Fabric-based prototype show that the proposed approach increases social welfare by 1.4%compared to the Bayesian game-based approach,makes all participants profitable,and achieves 90%fairness of enterprises.
基金supported in part by the Xi’an Jiaotong-Liverpool University(XJTLU)Research Development Fund(2024–2027)under Grant RDF-23-02-010supported in part by the Guangdong Basic and Applied Basic Research Foundation under Grant 2023A1515110732+5 种基金supported in part by the National Natural Science Foundation of China(NSFC)under Grant 62071247supported in part by the Science and Technology Development Fund,Macao,China SAR under Grants 0087/2022/AFJ and 001/2024/SKLin part by the National Natural Science Foundation of China under Grant 62261160650in part by the Research Committee of University of Macao,Macao SAR,China under Grants MYRG-GRG2023-00116-FST-UMDF and MYRG2020-00095-FSTsupported in part by the NSFC under Grant 62261160576 and 62301148in part by the Fundamental Research Funds for the Central Universities under Grant 2242023K5003.
文摘Reconfigurable intelligent surface(RIS)is a novel meta-material which can form a smart radio environment by dynamically altering reflection directions of the impinging electromagnetic waves.In the prior literature,the inter-RIS links which also contribute to the performance of the whole system are usually neglected when multiple RISs are deployed.In this paper we investigate a general double-RIS assisted multiple-input multiple-output(MIMO)wireless communication system under spatially correlated non line-of-sight propagation channels,where the cooperation of the double RISs is also considered.The design objective is to maximize the achievable ergodic rate based on full statistical channel state information(CSI).Specifically,we firstly present a closedform asymptotic expression for the achievable ergodic rate by utilizing replica method from statistical physics.Then a full statistical CSI-enabled optimal design is proposed which avoids high pilot training overhead compared to instantaneous CSI-enabled design.To further reduce the signal processing overhead and lower the complexity for practical realization,a common-phase scheme is proposed to design the double RISs.Simulation results show that the derived asymptotic ergodic rate is quite accurate even for small-sized antenna arrays.And the proposed optimization algorithm can achieve substantial gain at the expense of a low overhead and complexity.Furthermore,the cooperative double-RIS assisted MIMO framework is proven to achieve superior ergodic rate performance and high communication reliability under harsh propagation environment.
