Immune checkpoint inhibitors(ICIs)are used to relieve and refuel anti-tumor immunity by blocking the interaction,transcription,and translation of co-inhibitory immune checkpoints or degrading co-inhibitory immune chec...Immune checkpoint inhibitors(ICIs)are used to relieve and refuel anti-tumor immunity by blocking the interaction,transcription,and translation of co-inhibitory immune checkpoints or degrading co-inhibitory immune checkpoints.Thousands of small molecule drugs or biological materials,especially antibody-based ICIs,are actively being studied and antibodies are currently widely used.Limitations,such as anti-tumor efficacy,poor membrane permeability,and unneglected tolerance issues of antibody-based ICIs,remain evident but are thought to be overcome by small molecule drugs.Recent structural studies have broadened the scope of candidate immune checkpoint molecules,as well as innovative chemical inhibitors.By way of comparison,small molecule drug-based ICIs represent superior oral bioavailability and favorable pharmacokinetic features.Several ongoing clinical trials are exploring the synergetic effect of ICIs and other therapeutic strategies based on multiple ICI functions,including immune regulation,anti-angiogenesis,and cell cycle regulation.In this review we summarized the current progression of small molecule ICIs and the mechanism underlying immune checkpoint proteins,which will lay the foundation for further exploration.展开更多
As H-and J-aggregation receive more and more attention in the research of organic solar cells(OSCs),especially in small molecular systems,deep understanding of aggregation behavior is needed to guide the design of con...As H-and J-aggregation receive more and more attention in the research of organic solar cells(OSCs),especially in small molecular systems,deep understanding of aggregation behavior is needed to guide the design of conjugated small molecular structure and the fabrication process of OSC device.For this end,this review is written.Here,the review firstly introduced the basic information about H-and J-aggregation of conjugated small molecules in OSCs.Then,the characteristics of H-and J-aggregation and the methods to identify them were summarized.Next,it reviewed the research progress of H-and J-aggregation of conjugated small molecules in OSCs,including the factors influencing H-and J-aggregation in thin film and the effects of H-and J-aggregation on OPV performance.展开更多
We present an optimal and robust quantum control method for efficient population transfer in asymmetric double quantum-dot molecules.We derive a long-duration control scheme that allows for highly efficient population...We present an optimal and robust quantum control method for efficient population transfer in asymmetric double quantum-dot molecules.We derive a long-duration control scheme that allows for highly efficient population transfer by accurately controlling the amplitude of a narrow-bandwidth pulse.To overcome fluctuations in control field parameters,we employ a frequency-domain quantum optimal control theory method to optimize the spectral phase of a single pulse with broad bandwidth while preserving the spectral amplitude.It is shown that this spectral-phase-only optimization approach can successfully identify robust and optimal control fields,leading to efficient population transfer to the target state while concurrently suppressing population transfer to undesired states.The method demonstrates resilience to fluctuations in control field parameters,making it a promising approach for reliable and efficient population transfer in practical applications.展开更多
Aqueous potassium-ion batteries(APIBs),recognized as safe and reliable new energy devices,are considered as one of the alternatives to traditional batteries.Layered MnO_(2),serving as the main cathode,exhibits a lower...Aqueous potassium-ion batteries(APIBs),recognized as safe and reliable new energy devices,are considered as one of the alternatives to traditional batteries.Layered MnO_(2),serving as the main cathode,exhibits a lower specific capacity in aqueous electrolytes compared to organic systems and operates through a different reaction mechanism.The application of highly conductive graphene may effectively enhance the capacity of APIBs but could complicate the potassium storage environment.In this study,a MnO_(2) cathode pre-intercalated with K~+ions and grown on graphene(KMO@rGO) was developed using the microwave hydrothermal method for APIBs.KMO@rGO achieved a specific capacity of 90 mA h g^(-1) at a current density of 0.1 A g^(-1),maintaining a capacity retention rate of>90% after 5000 cycles at 5 A g^(-1).In-situ and exsitu characterization techniques revealed the energy-storage mechanism of KMO@rGO:layered MnO_(2)traps a large amount of "dead" water molecules during K~+ions removal.However,the introduction of graphene enables these water molecules to escape during K~+ ions insertion at the cathode.The galvanostatic intermittent titration technique and density functional theory confirmed that KMO@rGO has a higher K~+ions migration rate than MnO_(2).Therefore,the capacity of this cathode depends on the interaction between dead water and K~+ions during the energy-storage reaction.The optimal structural alignment between layered MnO_(2) and graphene allows electrons to easily flow into the external circuit.Rapid charge compensation forces numerous low-solvent K~+ions to displace interlayer dead water,enhancing the capacity.This unique reaction mechanism is unprecedented in other aqueous battery studies.展开更多
Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited b...Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.展开更多
Aqueous Zn-ion batteries(AZIBs)have attracted increasing attention in next-generation energy storage systems due to their high safety and economic.Unfortunately,the side reactions,dendrites and hydrogen evolution effe...Aqueous Zn-ion batteries(AZIBs)have attracted increasing attention in next-generation energy storage systems due to their high safety and economic.Unfortunately,the side reactions,dendrites and hydrogen evolution effects at the zinc anode interface in aqueous electrolytes seriously hinder the application of aqueous zinc-ion batteries.Here,we report a critical solvation strategy to achieve reversible zinc electrochemistry by introducing a small polar molecule acetonitrile to form a“catcher”to arrest active molecules(bound water molecules).The stable solvation structure of[Zn(H_(2)O)_(6)]^(2+)is capable of maintaining and completely inhibiting free water molecules.When[Zn(H_(2)O)_(6)]^(2+)is partially desolvated in the Helmholtz outer layer,the separated active molecules will be arrested by the“catcher”formed by the strong hydrogen bond N-H bond,ensuring the stable desolvation of Zn^(2+).The Zn||Zn symmetric battery can stably cycle for 2250 h at 1 mAh cm^(-2),Zn||V_(6)O_(13) full battery achieved a capacity retention rate of 99.2%after 10,000 cycles at 10 A g^(-1).This paper proposes a novel critical solvation strategy that paves the route for the construction of high-performance AZIBs.展开更多
Parasitic plants and their hosts communicate through haustorial connections.Nutrient deficiency is a common stress for plants,yet little is known about whether and how host plants and parasites communicate during adap...Parasitic plants and their hosts communicate through haustorial connections.Nutrient deficiency is a common stress for plants,yet little is known about whether and how host plants and parasites communicate during adaptation to such nutrient stresses.In this study,we used transcriptomics and proteomics to analyze how soybean(Glycine max)and its parasitizing dodder(Cuscuta australis)respond to nitrate and phosphate deficiency(-N and-P).After-N and-P treatment,the soybean and dodder plants exhibited substantial changes of transcriptome and proteome,although soybean plants showed very few transcriptional responses to-P and dodder did not show any transcriptional changes to either-N or-P.Importantly,large-scale interplant transport of mRNAs and proteins was detected.Although the mobile mRNAs only comprised at most 0.2%of the transcriptomes,the foreign mobile proteins could reach 6.8%of the total proteins,suggesting that proteins may be the major forms of interplant communications.Furthermore,the interplant mobility of macromolecules was specifically affected by the nutrient regimes and the transport of these macromolecules was very likely independently regulated.This study provides new insight into the communication between host plants and parasites under stress conditions.展开更多
Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"...Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed irreversibly.We further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)molecules.The IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water clusters.Such facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule frame.Further exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C electrocatalyst.The density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water molecules.Such results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.展开更多
The internal microbial diversity and small molecular metabolites of Nuodeng ham in different processing years(the first,second and third year sample)were analyzed by high-throughput sequencing technology and gas chrom...The internal microbial diversity and small molecular metabolites of Nuodeng ham in different processing years(the first,second and third year sample)were analyzed by high-throughput sequencing technology and gas chromatography-time of flight mass spectrography(GC-TOF-MS)to study the effects of microorganisms and small molecular metabolites on the quality of ham in different processing years.The results showed that the dominant bacteria phyla of Nuodeng ham in different processing years were Proteobacteria and Firmicutes,the dominant fungi phyla were Ascomycota and Basidiomycota,while Staphylococcus and Aspergillus were the dominant bacteria and fungi of Nuodeng ham,respectively.Totally,252 kinds of small molecular metabolites were identified from Nuodeng ham in different processing years,and 12 different metabolites were screened through multivariate statistical analysis.Further metabolic pathway analysis showed that 23 metabolic pathways were related to ham fermentation,of which 8 metabolic pathways had significant effects on ham fermentation(Impact>0.01,P<0.05).The content of L-proline,phenyllactic acid,L-lysine,carnosine,taurine,D-proline,betaine and creatine were significantly positively correlated with the relative abundance of Staphylococcus and Serratia,but negatively correlated with the relative abundance of Halomonas,Aspergillus and Yamadazyma.展开更多
The 21^(st) century has started with several innovations in the medical sciences,with wide applications in health care management.This development has taken in the field of medicines(newer drugs/molecules),various too...The 21^(st) century has started with several innovations in the medical sciences,with wide applications in health care management.This development has taken in the field of medicines(newer drugs/molecules),various tools and technology which has completely changed the patient management including abdominal surgery.Surgery for abdominal diseases has moved from maximally invasive to minimally invasive(laparoscopic and robotic)surgery.Some of the newer medicines have its impact on need for surgical intervention.This article focuses on the development of these emerging molecules,tools,and technology and their impact on present surgical form and its future effects on the surgical intervention in gastroenterological diseases.展开更多
Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,spec...Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,specifi cally fl uorenone-triphenylamine(FO-TPA)-x-Cl[x=para,meta,and ortho(p,m,and o)],with diff erent chlorine-substituent positions,as dopant-free HTMs for PSCs.These chlorinated molecules feature a symmetrical donor-acceptor-donor structure and ideal intramolecular charge transfer properties,allowing for self-doping and the establishment of built-in potentials for improving charge extraction.Highly effi cient hole-transfer interfaces are constructed between perovskites and these HTMs by strategi-cally modifying the chlorine substitution.Thus,the chlorinated HTM-derived inverted PSCs exhibited superior effi ciencies and air stabilities.Importantly,the dopant-free HTM FO-TPA-o-Cl not only attains a power conversion effi ciency of 20.82% but also demonstrates exceptional stability,retaining 93.8%of its initial effi ciency even after a 30-day aging test conducted under ambient air conditions in PSCs without encapsulation.These fi ndings underscore the critical role of chlorine-substituent regulation in HTMs in ensuring the formation and maintenance of effi cient and stable PSCs.展开更多
The process of neurite outgrowth and branching is a crucial aspect of neuronal development and regeneration.Axons and dendrites,sometimes referred to as neurites,are extensions of a neuron's cellular body that are...The process of neurite outgrowth and branching is a crucial aspect of neuronal development and regeneration.Axons and dendrites,sometimes referred to as neurites,are extensions of a neuron's cellular body that are used to start networks.Here we explored the effects of diethyl(3,4-dihydroxyphenethylamino)(quinolin-4-yl)methylphosphonate(DDQ)on neurite developmental features in HT22 neuronal cells.In this work,we examined the protective effects of DDQ on neuronal processes and synaptic outgrowth in differentiated HT22cells expressing mutant Tau(mTau)cDNA.To investigate DDQ chara cteristics,cell viability,biochemical,molecular,western blotting,and immunocytochemistry were used.Neurite outgrowth is evaluated through the segmentation and measurement of neural processes.These neural processes can be seen and measured with a fluorescence microscope by manually tracing and measuring the length of the neurite growth.These neuronal processes can be observed and quantified with a fluorescent microscope by manually tracing and measuring the length of the neuronal HT22.DDQ-treated mTau-HT22 cells(HT22 cells transfected with cDNA mutant Tau)were seen to display increased levels of synaptophysin,MAP-2,andβ-tubulin.Additionally,we confirmed and noted reduced levels of both total and p-Tau,as well as elevated levels of microtubule-associated protein 2,β-tubulin,synaptophysin,vesicular acetylcholine transporter,and the mitochondrial biogenesis protein-pe roxisome prolife rator-activated receptor-gamma coactivator-1α.In mTa u-expressed HT22 neurons,we observed DDQ enhanced the neurite characteristics and improved neurite development through increased synaptic outgrowth.Our findings conclude that mTa u-HT22(Alzheimer's disease)cells treated with DDQ have functional neurite developmental chara cteristics.The key finding is that,in mTa u-HT22 cells,DDQ preserves neuronal structure and may even enhance nerve development function with mTa u inhibition.展开更多
Chalcopyrite is a common copper-bearing mineral with antiferromagnetic properties.However,this property has rarely been considered in previous studies for detailed adsorption behaviors of molecules on chalcopyrite.Bas...Chalcopyrite is a common copper-bearing mineral with antiferromagnetic properties.However,this property has rarely been considered in previous studies for detailed adsorption behaviors of molecules on chalcopyrite.Based on density functional theory(DFT),new adsorption pathways by H_(2)O and O_(2)on the chalcopyrite metal terminated(112)surface((112)-M)is found in this work.First,through simulating the adsorption of an isolated water molecule and monolayer water molecules,it is confirmed that H_(2)O molecules tend to adsorb on the surface Fe atoms more than on the surface Cu atoms.Then,we studied various adsorption behaviors of the O_(2)molecule.It is found that the adsorption on the hollow FeAFe site is the most stable case;however,O_(2)is undissociated.Two adsorption cases will happen when H_(2)OAO_(2)adsorb simultaneously on the surface.For the S site,the H_(2)O molecule thoroughly dissociated and formed SAO species,and the other case is H_(2)O undissociated adsorbing at the Cu site.For the former case,it is interesting that H_(2)O is dissociated before O_(2).展开更多
Advances in experimental and computational technologies continue to grow rapidly to provide novel avenues for the treatment of neurodegenerative disorders. Despite this, there remain only a handful of drugs that have ...Advances in experimental and computational technologies continue to grow rapidly to provide novel avenues for the treatment of neurodegenerative disorders. Despite this, there remain only a handful of drugs that have shown success in late-stage clinical trials for Tau-associated neurodegenerative disorders. The most commonly prescribed treatments are symptomatic treatments such as cholinesterase inhibitors and N-methyl-D-aspartate receptor blockers that were approved for use in Alzheimer's disease. As diagnostic screening can detect disorders at earlier time points, the field needs pre-symptomatic treatments that can prevent, or significantly delay the progression of these disorders(Koychev et al., 2019). These approaches may be different from late-stage treatments that may help to ameliorate symptoms and slow progression once symptoms have become more advanced should early diagnostic screening fail. This mini-review will highlight five key avenues of academic and industrial research for identifying therapeutic strategies to treat Tau-associated neurodegenerative disorders. These avenues include investigating(1) the broad class of chemicals termed “small molecules”;(2) adaptive immunity through both passive and active antibody treatments;(3) innate immunity with an emphasis on microglial modulation;(4) synaptic compartments with the view that Tau-associated neurodegenerative disorders are synaptopathies. Although this mini-review will focus on Alzheimer's disease due to its prevalence, it will also argue the need to target other tauopathies, as through understanding Alzheimer's disease as a Tau-associated neurodegenerative disorder, we may be able to generalize treatment options. For this reason, added detail linking back specifically to Tau protein as a direct therapeutic target will be added to each topic.展开更多
The advent of biologics and small molecules in inflammatory bowel disease(IBD)has marked a significant turning point in the prognosis of IBD,decreasing the rates of corticosteroid dependence,hospitalizations and impro...The advent of biologics and small molecules in inflammatory bowel disease(IBD)has marked a significant turning point in the prognosis of IBD,decreasing the rates of corticosteroid dependence,hospitalizations and improving overall quality of life.The introduction of biosimilars has also increased affordability and enhanced access to these otherwise costly targeted therapies.Biologics do not yet represent a complete panacea:A subset of patients do not respond to first-line anti-tumor necrosis factor(TNF)-alpha agents or may subsequently demonstrate a secondary loss of response.Patients who fail to respond to anti-TNF agents typically have a poorer response rate to second-line biologics.It is uncertain which patient would benefit from a different sequencing of biologics or even a combination of biologic agents.The introduction of newer classes of biologics and small molecules may provide alternative therapeutic targets for patients with refractory disease.This review examines the therapeutic ceiling in current treatment strategies of IBD and the potential paradigm shifts in the future.展开更多
Neural progenitor cells(NPCs) capable of self-renewal and differentiation into neural cell lineages offer broad prospects for cell therapy for neurodegenerative diseases. However, cell therapy based on NPC transplanta...Neural progenitor cells(NPCs) capable of self-renewal and differentiation into neural cell lineages offer broad prospects for cell therapy for neurodegenerative diseases. However, cell therapy based on NPC transplantation is limited by the inability to acquire sufficient quantities of NPCs. Previous studies have found that a chemical cocktail of valproic acid, CHIR99021, and Repsox(VCR) promotes mouse fibroblasts to differentiate into NPCs under hypoxic conditions. Therefore, we used VCR(0.5 mM valproic acid, 3 μM CHIR99021, and 1 μM Repsox) to induce the reprogramming of rat embryonic fibroblasts into NPCs under a hypoxic condition(5%). These NPCs exhibited typical neurosphere-like structures that can express NPC markers, such as Nestin, SRY-box transcription factor 2, and paired box 6(Pax6), and could also differentiate into multiple types of functional neurons and astrocytes in vitro. They had similar gene expression profiles to those of rat brain-derived neural stem cells. Subsequently, the chemically-induced NPCs(ciNPCs) were stereotactically transplanted into the substantia nigra of 6-hydroxydopamine-lesioned parkinsonian rats. We found that the ciNPCs exhibited long-term survival, migrated long distances, and differentiated into multiple types of functional neurons and glial cells in vivo. Moreover, the parkinsonian behavioral defects of the parkinsonian model rats grafted with ciNPCs showed remarkable functional recovery. These findings suggest that rat fibroblasts can be directly transformed into NPCs using a chemical cocktail of VCR without introducing exogenous factors, which may be an attractive donor material for transplantation therapy for Parkinson’s disease.展开更多
Due to the solution processable nature,the prepared perovskite films are polycrystalline with considerable number of defects.These defects,especially defects at interface accelerate the carrier recombination and reduc...Due to the solution processable nature,the prepared perovskite films are polycrystalline with considerable number of defects.These defects,especially defects at interface accelerate the carrier recombination and reduce the carrier collection.Besides,the surface defects also affect the long-term stability of the perovskite solar cells(PVSCs).To solve this problem,surface passivation molecules are introduced at selective interface(the interface between perovskite and carrier selective layer).This review summarizes recent progress of small molecules used in PVSCs.Firstly,different types of defect states in perovskite films are introduced and their effects on device performance are discussed.Subsequently,surface passivation molecules are divided into four categories,and the interaction between the functional groups of the surface passivation molecules and selective defect states in perovskite films are highlighted.Finally,we look into the prospects and challenges in design noble small molecules for PVSCs applications.展开更多
Soliton molecules(SMs)of the(2+1)-dimensional generalized KonopelchenkoDubrovsky-Kaup-Kupershmidt(gKDKK)equation are found by utilizing a velocity resonance ansatz to N-soliton solutions,which can transform to asymmet...Soliton molecules(SMs)of the(2+1)-dimensional generalized KonopelchenkoDubrovsky-Kaup-Kupershmidt(gKDKK)equation are found by utilizing a velocity resonance ansatz to N-soliton solutions,which can transform to asymmetric solitons upon assigning appropriate values to some parameters.Furthermore,a double-peaked lump solution can be constructed with breather degeneration approach.By applying a mixed technique of a resonance ansatz and conjugate complexes of partial parameters to multisoliton solutions,various kinds of interactional structures are constructed;There include the soliton molecule(SM),the breather molecule(BM)and the soliton-breather molecule(SBM).Graphical investigation and theoretical analysis show that the interactions composed of SM,BM and SBM are inelastic.展开更多
Using quantum chemical calculations,we model the pathways for synthesizing two purine nucleobases,adenine and guanine,in the gas-phase interstellar environment,surrounded by neutral atomic hydrogen(H I).H I is found a...Using quantum chemical calculations,we model the pathways for synthesizing two purine nucleobases,adenine and guanine,in the gas-phase interstellar environment,surrounded by neutral atomic hydrogen(H I).H I is found active in facilitating a series of fundamental proton transfer processes of organic synthesis,including bond formation,cyclization,dehydrogenation,and H migration.The reactive potential barriers were significantly reduced in the alternative pathways created by H I,leading to a remarkable increase in the reaction rate.The presence of H I also lowered the reactive activation temperature from 757.8 K to 131.5–147.0 K,indicating the thermodynamic feasibility of these pathways in star-forming regions where some of the reactants have been astronomically detected.Our findings suggest that H I may serve as an effective catalyst for interstellar organic synthesis.展开更多
Photo-responsive slippery lubricant-infused porous surface(SLIPS) for droplet manipulation is flexible, noncontact and non-destructive in droplet manipulation, which has promising applications in flexible robotics, mi...Photo-responsive slippery lubricant-infused porous surface(SLIPS) for droplet manipulation is flexible, noncontact and non-destructive in droplet manipulation, which has promising applications in flexible robotics, microfluidics,biomedicine, and chemical analysis. However, the repeated manipulations for droplets of SLIPSs are quite limited in the works reported so far, the poor durability of droplet manipulation severely limits the practical application of the surfaces. In this paper, an Fe3O4-doped polydimethylsiloxane(PDMS)-based SLIPS is proposed and implemented to achieve ultra-high repeated droplet manipulation numbers under near-infrared ray(NIR) laser irradiation. Firstly, a micron columnar array structure with micro-pits on the top side, as well as, a wall structure out of the array is designed on SLIPS to reserve the lubricant. Secondly, the prototype of the SLIPS is fabricated by a 3-step ultraviolet(UV) lithography, and subsequently immersed in silicone oil for more than 96 h to obtain the ultra-high durability slippery lubricant-infused porous surface(UD-SLIPS). With a power of 25 m W–85 m W NIR laser, the repeated manipulation of microdroplets(≤ 5 μL) in the scale of 1 cm can exceed more than 3000 times which is far beyond that in previous reports. Finally, the droplet manipulation performance of this photo-responsive UD-SLIPS and the influence of infusion time on durability are investigated. The mechanism of the PDMS swelling effect is found to be the key factor in improving the droplet manipulation durability of SLIPS. The findings of this work would be of great significance for the development of highly durable photo-responsive functional surfaces for droplet manipulation.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.82203539 and 92259102)Provincial Cooperation Project of Science and Technology Department of Sichuan Province(Grant No.2023YFSY0043)the National Key Research and Development Program of China(Grant No.2023YFC3402100).
文摘Immune checkpoint inhibitors(ICIs)are used to relieve and refuel anti-tumor immunity by blocking the interaction,transcription,and translation of co-inhibitory immune checkpoints or degrading co-inhibitory immune checkpoints.Thousands of small molecule drugs or biological materials,especially antibody-based ICIs,are actively being studied and antibodies are currently widely used.Limitations,such as anti-tumor efficacy,poor membrane permeability,and unneglected tolerance issues of antibody-based ICIs,remain evident but are thought to be overcome by small molecule drugs.Recent structural studies have broadened the scope of candidate immune checkpoint molecules,as well as innovative chemical inhibitors.By way of comparison,small molecule drug-based ICIs represent superior oral bioavailability and favorable pharmacokinetic features.Several ongoing clinical trials are exploring the synergetic effect of ICIs and other therapeutic strategies based on multiple ICI functions,including immune regulation,anti-angiogenesis,and cell cycle regulation.In this review we summarized the current progression of small molecule ICIs and the mechanism underlying immune checkpoint proteins,which will lay the foundation for further exploration.
基金financially supported by the National Natural Science Foundation of China(52203024,22225504)the Shandong Provincial Natural Science Foundation(ZR2022QE135)+2 种基金the Youth Innovation Team Project of Shandong Provincial University(2023KJ330)the Qilu University of Technology strong base plan(2023PY001)Guangdong Provincial Key Laboratory of Catalysis(2020B121201002)。
文摘As H-and J-aggregation receive more and more attention in the research of organic solar cells(OSCs),especially in small molecular systems,deep understanding of aggregation behavior is needed to guide the design of conjugated small molecular structure and the fabrication process of OSC device.For this end,this review is written.Here,the review firstly introduced the basic information about H-and J-aggregation of conjugated small molecules in OSCs.Then,the characteristics of H-and J-aggregation and the methods to identify them were summarized.Next,it reviewed the research progress of H-and J-aggregation of conjugated small molecules in OSCs,including the factors influencing H-and J-aggregation in thin film and the effects of H-and J-aggregation on OPV performance.
基金This work was supported by the National Natural Science Foundations of China(Grant Nos.12275033,61973317,and 12274470)the Natural Science Foundation of Hunan Province for Distinguished Young Scholars(Grant No.2022JJ10070)+1 种基金the Natural Science Foundation of Hunan Province(Grant No.2022JJ30582)the Scientific Research Fund of Hunan Provincial Education Department(Grant No.20A025).
文摘We present an optimal and robust quantum control method for efficient population transfer in asymmetric double quantum-dot molecules.We derive a long-duration control scheme that allows for highly efficient population transfer by accurately controlling the amplitude of a narrow-bandwidth pulse.To overcome fluctuations in control field parameters,we employ a frequency-domain quantum optimal control theory method to optimize the spectral phase of a single pulse with broad bandwidth while preserving the spectral amplitude.It is shown that this spectral-phase-only optimization approach can successfully identify robust and optimal control fields,leading to efficient population transfer to the target state while concurrently suppressing population transfer to undesired states.The method demonstrates resilience to fluctuations in control field parameters,making it a promising approach for reliable and efficient population transfer in practical applications.
基金financially supported by the Scientific and Technological Plan Project of Guizhou Province (Grant No. [2021]060)the Industry and Education Combination Innovation Platform of Intelligent Manufacturing and the Graduate Joint Training Base at Guizhou University (Grant No. 2020-520000-83-01-324061)the Guizhou Engineering Research Center for smart services (Grant No. 2203-520102-04-04-298868)。
文摘Aqueous potassium-ion batteries(APIBs),recognized as safe and reliable new energy devices,are considered as one of the alternatives to traditional batteries.Layered MnO_(2),serving as the main cathode,exhibits a lower specific capacity in aqueous electrolytes compared to organic systems and operates through a different reaction mechanism.The application of highly conductive graphene may effectively enhance the capacity of APIBs but could complicate the potassium storage environment.In this study,a MnO_(2) cathode pre-intercalated with K~+ions and grown on graphene(KMO@rGO) was developed using the microwave hydrothermal method for APIBs.KMO@rGO achieved a specific capacity of 90 mA h g^(-1) at a current density of 0.1 A g^(-1),maintaining a capacity retention rate of>90% after 5000 cycles at 5 A g^(-1).In-situ and exsitu characterization techniques revealed the energy-storage mechanism of KMO@rGO:layered MnO_(2)traps a large amount of "dead" water molecules during K~+ions removal.However,the introduction of graphene enables these water molecules to escape during K~+ ions insertion at the cathode.The galvanostatic intermittent titration technique and density functional theory confirmed that KMO@rGO has a higher K~+ions migration rate than MnO_(2).Therefore,the capacity of this cathode depends on the interaction between dead water and K~+ions during the energy-storage reaction.The optimal structural alignment between layered MnO_(2) and graphene allows electrons to easily flow into the external circuit.Rapid charge compensation forces numerous low-solvent K~+ions to displace interlayer dead water,enhancing the capacity.This unique reaction mechanism is unprecedented in other aqueous battery studies.
基金supported by the National Natural Science Foundation of China(Grant Nos.62321166653,22090044,and 12350410372).Calculations were performed in part at the high-performance computing center of Jilin University.
文摘Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.
基金supported by the National Natural Science Foundation of China(No.52272198 and 52002122)the Project funded by China Postdoctoral Science Foundation(No.2021M690947).
文摘Aqueous Zn-ion batteries(AZIBs)have attracted increasing attention in next-generation energy storage systems due to their high safety and economic.Unfortunately,the side reactions,dendrites and hydrogen evolution effects at the zinc anode interface in aqueous electrolytes seriously hinder the application of aqueous zinc-ion batteries.Here,we report a critical solvation strategy to achieve reversible zinc electrochemistry by introducing a small polar molecule acetonitrile to form a“catcher”to arrest active molecules(bound water molecules).The stable solvation structure of[Zn(H_(2)O)_(6)]^(2+)is capable of maintaining and completely inhibiting free water molecules.When[Zn(H_(2)O)_(6)]^(2+)is partially desolvated in the Helmholtz outer layer,the separated active molecules will be arrested by the“catcher”formed by the strong hydrogen bond N-H bond,ensuring the stable desolvation of Zn^(2+).The Zn||Zn symmetric battery can stably cycle for 2250 h at 1 mAh cm^(-2),Zn||V_(6)O_(13) full battery achieved a capacity retention rate of 99.2%after 10,000 cycles at 10 A g^(-1).This paper proposes a novel critical solvation strategy that paves the route for the construction of high-performance AZIBs.
基金supported by the National Natural Science Foundation of China (31970274 (J.W.), 32170272 (X.W.), 32100251 (J.Z.), 32000179 (Y.X.))the Special Research Assistant of Chinese Academy of Sciences (J.Z. and Y.X.), China Postdoctoral Science Foundation (2022M713224 (J.Z.))+6 种基金the Strategic Priority Research Program of Chinese Academy of Sciences (XDPB16 (J.W.))the Yunnan Innovation Team Project (202105AE160013 (J.W.))CAS “Light of West China” Program (G.S.)Yunnan Revitalization Talent Support Program “Young Talents” Project (XDYC-QNRC-2022-0301 (J.Z.), XDYC-QNRC-2022-0001 (G.S.))the General and Key Project of the Applied Basic Research Program of Yunnan (202001AS070021(J.W.))Yunnan Fundamental Research Projects-General Project (202101AT070457 (S.L.))Yunnan Fundamental Research Projects-Youth Talent Project (202101AU070021(S.L.))
文摘Parasitic plants and their hosts communicate through haustorial connections.Nutrient deficiency is a common stress for plants,yet little is known about whether and how host plants and parasites communicate during adaptation to such nutrient stresses.In this study,we used transcriptomics and proteomics to analyze how soybean(Glycine max)and its parasitizing dodder(Cuscuta australis)respond to nitrate and phosphate deficiency(-N and-P).After-N and-P treatment,the soybean and dodder plants exhibited substantial changes of transcriptome and proteome,although soybean plants showed very few transcriptional responses to-P and dodder did not show any transcriptional changes to either-N or-P.Importantly,large-scale interplant transport of mRNAs and proteins was detected.Although the mobile mRNAs only comprised at most 0.2%of the transcriptomes,the foreign mobile proteins could reach 6.8%of the total proteins,suggesting that proteins may be the major forms of interplant communications.Furthermore,the interplant mobility of macromolecules was specifically affected by the nutrient regimes and the transport of these macromolecules was very likely independently regulated.This study provides new insight into the communication between host plants and parasites under stress conditions.
基金funded by the Key Research and Development Program sponsored by the Ministry of Science and Technology(MOST)(2022YFA1203400)National Natural Science Foundation of China(21925205,22072145,21372155,22005294,and 22102172)。
文摘Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed irreversibly.We further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)molecules.The IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water clusters.Such facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule frame.Further exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C electrocatalyst.The density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water molecules.Such results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.
基金supported by Major Science and Technology Projects of Yunnan Science and Technology Plan(2019ZG003)Yunnan Young and Middle-aged Academic and Technical Leader Reserve Talent Project(202105AC160068)。
文摘The internal microbial diversity and small molecular metabolites of Nuodeng ham in different processing years(the first,second and third year sample)were analyzed by high-throughput sequencing technology and gas chromatography-time of flight mass spectrography(GC-TOF-MS)to study the effects of microorganisms and small molecular metabolites on the quality of ham in different processing years.The results showed that the dominant bacteria phyla of Nuodeng ham in different processing years were Proteobacteria and Firmicutes,the dominant fungi phyla were Ascomycota and Basidiomycota,while Staphylococcus and Aspergillus were the dominant bacteria and fungi of Nuodeng ham,respectively.Totally,252 kinds of small molecular metabolites were identified from Nuodeng ham in different processing years,and 12 different metabolites were screened through multivariate statistical analysis.Further metabolic pathway analysis showed that 23 metabolic pathways were related to ham fermentation,of which 8 metabolic pathways had significant effects on ham fermentation(Impact>0.01,P<0.05).The content of L-proline,phenyllactic acid,L-lysine,carnosine,taurine,D-proline,betaine and creatine were significantly positively correlated with the relative abundance of Staphylococcus and Serratia,but negatively correlated with the relative abundance of Halomonas,Aspergillus and Yamadazyma.
文摘The 21^(st) century has started with several innovations in the medical sciences,with wide applications in health care management.This development has taken in the field of medicines(newer drugs/molecules),various tools and technology which has completely changed the patient management including abdominal surgery.Surgery for abdominal diseases has moved from maximally invasive to minimally invasive(laparoscopic and robotic)surgery.Some of the newer medicines have its impact on need for surgical intervention.This article focuses on the development of these emerging molecules,tools,and technology and their impact on present surgical form and its future effects on the surgical intervention in gastroenterological diseases.
基金This study was supported by the National Nat-ural Science Foundation of China(No.22379105)the Natural Sci-ence Foundation of Shanxi Province(Nos.20210302123110 and 202303021211059)the Open Fund Project of Ningxia Sinostar Display Material Co.,Ltd.
文摘Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,specifi cally fl uorenone-triphenylamine(FO-TPA)-x-Cl[x=para,meta,and ortho(p,m,and o)],with diff erent chlorine-substituent positions,as dopant-free HTMs for PSCs.These chlorinated molecules feature a symmetrical donor-acceptor-donor structure and ideal intramolecular charge transfer properties,allowing for self-doping and the establishment of built-in potentials for improving charge extraction.Highly effi cient hole-transfer interfaces are constructed between perovskites and these HTMs by strategi-cally modifying the chlorine substitution.Thus,the chlorinated HTM-derived inverted PSCs exhibited superior effi ciencies and air stabilities.Importantly,the dopant-free HTM FO-TPA-o-Cl not only attains a power conversion effi ciency of 20.82% but also demonstrates exceptional stability,retaining 93.8%of its initial effi ciency even after a 30-day aging test conducted under ambient air conditions in PSCs without encapsulation.These fi ndings underscore the critical role of chlorine-substituent regulation in HTMs in ensuring the formation and maintenance of effi cient and stable PSCs.
基金supported by NIH grants AG079264(to PHR)and AG071560(to APR)。
文摘The process of neurite outgrowth and branching is a crucial aspect of neuronal development and regeneration.Axons and dendrites,sometimes referred to as neurites,are extensions of a neuron's cellular body that are used to start networks.Here we explored the effects of diethyl(3,4-dihydroxyphenethylamino)(quinolin-4-yl)methylphosphonate(DDQ)on neurite developmental features in HT22 neuronal cells.In this work,we examined the protective effects of DDQ on neuronal processes and synaptic outgrowth in differentiated HT22cells expressing mutant Tau(mTau)cDNA.To investigate DDQ chara cteristics,cell viability,biochemical,molecular,western blotting,and immunocytochemistry were used.Neurite outgrowth is evaluated through the segmentation and measurement of neural processes.These neural processes can be seen and measured with a fluorescence microscope by manually tracing and measuring the length of the neurite growth.These neuronal processes can be observed and quantified with a fluorescent microscope by manually tracing and measuring the length of the neuronal HT22.DDQ-treated mTau-HT22 cells(HT22 cells transfected with cDNA mutant Tau)were seen to display increased levels of synaptophysin,MAP-2,andβ-tubulin.Additionally,we confirmed and noted reduced levels of both total and p-Tau,as well as elevated levels of microtubule-associated protein 2,β-tubulin,synaptophysin,vesicular acetylcholine transporter,and the mitochondrial biogenesis protein-pe roxisome prolife rator-activated receptor-gamma coactivator-1α.In mTa u-expressed HT22 neurons,we observed DDQ enhanced the neurite characteristics and improved neurite development through increased synaptic outgrowth.Our findings conclude that mTa u-HT22(Alzheimer's disease)cells treated with DDQ have functional neurite developmental chara cteristics.The key finding is that,in mTa u-HT22 cells,DDQ preserves neuronal structure and may even enhance nerve development function with mTa u inhibition.
基金The authors are grateful for the financial support provided by the National Natural Science Foundation of China(NSFC)(Nos.51974094,51964004,and U20A20269).
文摘Chalcopyrite is a common copper-bearing mineral with antiferromagnetic properties.However,this property has rarely been considered in previous studies for detailed adsorption behaviors of molecules on chalcopyrite.Based on density functional theory(DFT),new adsorption pathways by H_(2)O and O_(2)on the chalcopyrite metal terminated(112)surface((112)-M)is found in this work.First,through simulating the adsorption of an isolated water molecule and monolayer water molecules,it is confirmed that H_(2)O molecules tend to adsorb on the surface Fe atoms more than on the surface Cu atoms.Then,we studied various adsorption behaviors of the O_(2)molecule.It is found that the adsorption on the hollow FeAFe site is the most stable case;however,O_(2)is undissociated.Two adsorption cases will happen when H_(2)OAO_(2)adsorb simultaneously on the surface.For the S site,the H_(2)O molecule thoroughly dissociated and formed SAO species,and the other case is H_(2)O undissociated adsorbing at the Cu site.For the former case,it is interesting that H_(2)O is dissociated before O_(2).
基金the MRC Laboratory of Molecular Biology (to MR)。
文摘Advances in experimental and computational technologies continue to grow rapidly to provide novel avenues for the treatment of neurodegenerative disorders. Despite this, there remain only a handful of drugs that have shown success in late-stage clinical trials for Tau-associated neurodegenerative disorders. The most commonly prescribed treatments are symptomatic treatments such as cholinesterase inhibitors and N-methyl-D-aspartate receptor blockers that were approved for use in Alzheimer's disease. As diagnostic screening can detect disorders at earlier time points, the field needs pre-symptomatic treatments that can prevent, or significantly delay the progression of these disorders(Koychev et al., 2019). These approaches may be different from late-stage treatments that may help to ameliorate symptoms and slow progression once symptoms have become more advanced should early diagnostic screening fail. This mini-review will highlight five key avenues of academic and industrial research for identifying therapeutic strategies to treat Tau-associated neurodegenerative disorders. These avenues include investigating(1) the broad class of chemicals termed “small molecules”;(2) adaptive immunity through both passive and active antibody treatments;(3) innate immunity with an emphasis on microglial modulation;(4) synaptic compartments with the view that Tau-associated neurodegenerative disorders are synaptopathies. Although this mini-review will focus on Alzheimer's disease due to its prevalence, it will also argue the need to target other tauopathies, as through understanding Alzheimer's disease as a Tau-associated neurodegenerative disorder, we may be able to generalize treatment options. For this reason, added detail linking back specifically to Tau protein as a direct therapeutic target will be added to each topic.
文摘The advent of biologics and small molecules in inflammatory bowel disease(IBD)has marked a significant turning point in the prognosis of IBD,decreasing the rates of corticosteroid dependence,hospitalizations and improving overall quality of life.The introduction of biosimilars has also increased affordability and enhanced access to these otherwise costly targeted therapies.Biologics do not yet represent a complete panacea:A subset of patients do not respond to first-line anti-tumor necrosis factor(TNF)-alpha agents or may subsequently demonstrate a secondary loss of response.Patients who fail to respond to anti-TNF agents typically have a poorer response rate to second-line biologics.It is uncertain which patient would benefit from a different sequencing of biologics or even a combination of biologic agents.The introduction of newer classes of biologics and small molecules may provide alternative therapeutic targets for patients with refractory disease.This review examines the therapeutic ceiling in current treatment strategies of IBD and the potential paradigm shifts in the future.
基金supported by the National Natural Science Foundation of China,No. 81771381 (to CQL)Anhui Provincial Key Research and Development Project,Nos. 2022e07020030 (to CQL), 2022e07020032 (to YG)+2 种基金Science Research Project of Bengbu Medical College,No. 2021byfy002 (to CQL)the Natural Science Foundation of the Higher Education Institutions of Anhui Province,No. KJ2021ZD0085 (to CJW)the Undergraduate Innovative Training Program of China,Nos. 202110367043 (to CQL), 202110367044 (to YG)。
文摘Neural progenitor cells(NPCs) capable of self-renewal and differentiation into neural cell lineages offer broad prospects for cell therapy for neurodegenerative diseases. However, cell therapy based on NPC transplantation is limited by the inability to acquire sufficient quantities of NPCs. Previous studies have found that a chemical cocktail of valproic acid, CHIR99021, and Repsox(VCR) promotes mouse fibroblasts to differentiate into NPCs under hypoxic conditions. Therefore, we used VCR(0.5 mM valproic acid, 3 μM CHIR99021, and 1 μM Repsox) to induce the reprogramming of rat embryonic fibroblasts into NPCs under a hypoxic condition(5%). These NPCs exhibited typical neurosphere-like structures that can express NPC markers, such as Nestin, SRY-box transcription factor 2, and paired box 6(Pax6), and could also differentiate into multiple types of functional neurons and astrocytes in vitro. They had similar gene expression profiles to those of rat brain-derived neural stem cells. Subsequently, the chemically-induced NPCs(ciNPCs) were stereotactically transplanted into the substantia nigra of 6-hydroxydopamine-lesioned parkinsonian rats. We found that the ciNPCs exhibited long-term survival, migrated long distances, and differentiated into multiple types of functional neurons and glial cells in vivo. Moreover, the parkinsonian behavioral defects of the parkinsonian model rats grafted with ciNPCs showed remarkable functional recovery. These findings suggest that rat fibroblasts can be directly transformed into NPCs using a chemical cocktail of VCR without introducing exogenous factors, which may be an attractive donor material for transplantation therapy for Parkinson’s disease.
基金support from Key Program of National Natural Science Foundation of China(22133006)the National Natural Science Foundation of China(ZX20210286)+1 种基金the Fundamental Research Funds for the Central Universities(20CX06004A)Talent Introduction Program of China University of Petroleum(East China)(ZX20190162)and the Post-Graduate Innovation Project of China University of Petroluem(East China)(YCX2021140)are acknowledged.We also thank the support from the Yankuang Group 2019 Science and Technology Program(YKKJ2019AJ05JG-R60).Prof.X.Li and Dr.T.Zhang thank the Taishan Scholar Programof Shandong Province(ts201712019,tsnq201909069)for financial support.
文摘Due to the solution processable nature,the prepared perovskite films are polycrystalline with considerable number of defects.These defects,especially defects at interface accelerate the carrier recombination and reduce the carrier collection.Besides,the surface defects also affect the long-term stability of the perovskite solar cells(PVSCs).To solve this problem,surface passivation molecules are introduced at selective interface(the interface between perovskite and carrier selective layer).This review summarizes recent progress of small molecules used in PVSCs.Firstly,different types of defect states in perovskite films are introduced and their effects on device performance are discussed.Subsequently,surface passivation molecules are divided into four categories,and the interaction between the functional groups of the surface passivation molecules and selective defect states in perovskite films are highlighted.Finally,we look into the prospects and challenges in design noble small molecules for PVSCs applications.
基金Supported by the National Natural Science Foundation of China(12001424)the Natural Science Basic Research Program of Shaanxi Province(2021JZ-21)the Fundamental Research Funds for the Central Universities(2020CBLY013)。
文摘Soliton molecules(SMs)of the(2+1)-dimensional generalized KonopelchenkoDubrovsky-Kaup-Kupershmidt(gKDKK)equation are found by utilizing a velocity resonance ansatz to N-soliton solutions,which can transform to asymmetric solitons upon assigning appropriate values to some parameters.Furthermore,a double-peaked lump solution can be constructed with breather degeneration approach.By applying a mixed technique of a resonance ansatz and conjugate complexes of partial parameters to multisoliton solutions,various kinds of interactional structures are constructed;There include the soliton molecule(SM),the breather molecule(BM)and the soliton-breather molecule(SBM).Graphical investigation and theoretical analysis show that the interactions composed of SM,BM and SBM are inelastic.
基金supported by the National Natural Science Foundation of China (11964002)。
文摘Using quantum chemical calculations,we model the pathways for synthesizing two purine nucleobases,adenine and guanine,in the gas-phase interstellar environment,surrounded by neutral atomic hydrogen(H I).H I is found active in facilitating a series of fundamental proton transfer processes of organic synthesis,including bond formation,cyclization,dehydrogenation,and H migration.The reactive potential barriers were significantly reduced in the alternative pathways created by H I,leading to a remarkable increase in the reaction rate.The presence of H I also lowered the reactive activation temperature from 757.8 K to 131.5–147.0 K,indicating the thermodynamic feasibility of these pathways in star-forming regions where some of the reactants have been astronomically detected.Our findings suggest that H I may serve as an effective catalyst for interstellar organic synthesis.
基金Project supported by the National Major Scientific Research Instrument Development Project of China (Grant No. 51927804)the National Natural Science Foundation of China (Grant No. 62275216)the Science and Technology Innovation Team Project of Shaanxi Province (Grant Nos. S2018-ZC-TD-0061 and 2023-CX-TD-06)。
文摘Photo-responsive slippery lubricant-infused porous surface(SLIPS) for droplet manipulation is flexible, noncontact and non-destructive in droplet manipulation, which has promising applications in flexible robotics, microfluidics,biomedicine, and chemical analysis. However, the repeated manipulations for droplets of SLIPSs are quite limited in the works reported so far, the poor durability of droplet manipulation severely limits the practical application of the surfaces. In this paper, an Fe3O4-doped polydimethylsiloxane(PDMS)-based SLIPS is proposed and implemented to achieve ultra-high repeated droplet manipulation numbers under near-infrared ray(NIR) laser irradiation. Firstly, a micron columnar array structure with micro-pits on the top side, as well as, a wall structure out of the array is designed on SLIPS to reserve the lubricant. Secondly, the prototype of the SLIPS is fabricated by a 3-step ultraviolet(UV) lithography, and subsequently immersed in silicone oil for more than 96 h to obtain the ultra-high durability slippery lubricant-infused porous surface(UD-SLIPS). With a power of 25 m W–85 m W NIR laser, the repeated manipulation of microdroplets(≤ 5 μL) in the scale of 1 cm can exceed more than 3000 times which is far beyond that in previous reports. Finally, the droplet manipulation performance of this photo-responsive UD-SLIPS and the influence of infusion time on durability are investigated. The mechanism of the PDMS swelling effect is found to be the key factor in improving the droplet manipulation durability of SLIPS. The findings of this work would be of great significance for the development of highly durable photo-responsive functional surfaces for droplet manipulation.