Portschinskia Semenov is a rare genus of bot fies whose larvae are obligate parasites of pikas and murine rodents,crucial for understanding the evolutionary biology of Oestridae.However,limited information on their ad...Portschinskia Semenov is a rare genus of bot fies whose larvae are obligate parasites of pikas and murine rodents,crucial for understanding the evolutionary biology of Oestridae.However,limited information on their adult biology and early immature stages has hindered the progress.Here,we provided the frst documentation of adult oviposition,behavior,and morphology of newly hatched frst instars of P.magnifca Pleske.Using confocal laser scanning microscopy and scanning electron microscopy,we characterized the ultrastructure of egg and frst-instar larva,identifying key traits facilitating attachment.Eggs were deposited individually or in groups,and glued on non-host surfaces with white adhesive substances,without specialized attachment organ.Newly hatched frst instars were circled with an anterior spinose band on each body segment except the anal division,awaited hosts in an upright position,and anchored to the egg shell by their anal division,likely supported by curved spines originating from the peritreme of the posterior spiracles.Evolutionary analyses of reproductive behavior across the 4 bot fy subfamilies reveal at least 3 times independent evolution of oviposition on non-host surfaces in Portschinskia or the Hypodermatinae clade as a sister group to Ochotonia,Gasterophilus pecorum(Fabricius)(Gasterophilinae),and Cuterebrinae.In contrast,species in the Oestrinae are larviparous,depositing frst instars directly onto hosts.Our fndings shed light on oviposition behavior and early immature morphology of the rare genus Portschinskia,offering insights into reproductive strategies and evolutionary adaptations of bot fies.展开更多
Chromosomal rearrangements(CRs)often cause phenotypic variations.Although several major rearrangements have been identified in Triticeae,a comprehensive study of the order,timing,and breakpoints of CRs has not been co...Chromosomal rearrangements(CRs)often cause phenotypic variations.Although several major rearrangements have been identified in Triticeae,a comprehensive study of the order,timing,and breakpoints of CRs has not been conducted.Here,we reconstruct high-quality ancestral genomes for the most recent common ancestor(MRCA)of the Triticeae,and the MRCA of the wheat lineage(Triticum and Aegilops).The protogenes of MRCA of the Triticeae and the wheat lineage are 22,894 and 29,060,respectively,which were arranged in their ancestral order.By partitioning modern Triticeae chromosomes into sets of syntenic regions and linking each to the corresponding protochromosomes,we revisit the rye chromosome structural evolution and propose alternative evolutionary routes.The previously identified 4L/5L reciprocal translocation in rye and Triticum urartu is found to have occurred independently and is unlikely to be the result of chromosomal introgression following distant hybridization.We also clarify that the 4AL/7BS translocation in tetraploid wheat was a bidirectional rather than unidirectional translocation event.Lastly,we identify several breakpoints in protochromosomes that independently reoccur following Triticeae evolution,representing potential CR hotspots.This study demonstrates that these reconstructed ancestral genomes can serve as special comparative references and facilitate a better understanding of the evolution of structural rearrangements in Triticeae.展开更多
The Malvaceae family,the most diverse family in the order Malvales,consists of nine subfamilies.Within the Firmiana genus of the Sterculioideae subfamily,most species are considered globally vulnerable,yet their genom...The Malvaceae family,the most diverse family in the order Malvales,consists of nine subfamilies.Within the Firmiana genus of the Sterculioideae subfamily,most species are considered globally vulnerable,yet their genomes remain unexplored.Here,we present a chromosome-level genome assembly for a representative Firmiana species,F.hainanensis,2n=40,totaling 1536 Mb.Phylogenomic analysis shows that F.hainanensis and Durio zibethinus have the closest evolutionary relationship,with an estimated divergence time of approximately 21 millions of years ago(MYA)and distinct polyploidization events in their histories.Evolutionary trajectory analyses indicate that fissions and fusions may play a crucial role in chromosome number variation(2n=14 to 2n=96).Analysis of repetitive elements among Malvaceae reveals that the Tekay subfamily(belonging to the Gypsy group)contributes to variation in genome size(ranging from 324 Mb to 1620 Mb).Additionally,genes associated with P450,peroxidase,and microtubules,and thereby related to cell wall biosynthesis,are significantly contracted in F.hainanensis,potentially leading to its lower wood density relative to Hopea hainanensis.Overall,our study provides insights into the evolution of chromosome number,genome size,and the genetic basis of cell wall biosynthesis in Malvaceae species.展开更多
A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and...A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and Mo2S3 nanoparticles were integrated at the edges of Co3O4 nanosheets,creating a rich,heterogeneous interface that enhances the synergistic effects of each component.In an alkaline electrolyte,the synthesized CoMoNiO-S/NF-110 exhibited superior electrocatalytic performance for oxygen evolution reaction(OER),achieving current densities of 100 and 200 mA·cm^(-2) with low overpotentials of 199.4 and 224.4 mV,respectively,outperforming RuO2 and several high-performance Mo and Ni-based catalysts.This excellent performance is attributed to the rich interface formed between the components and active sites exposed by the defect structure.展开更多
The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecul...The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.展开更多
The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor ...The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.展开更多
Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a fo...Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.展开更多
Background:Tandem gene repeats naturally occur as important genomic features and determine many traits in living organisms,like human diseases and microbial productivities of target bioproducts.Methods:Here,we develop...Background:Tandem gene repeats naturally occur as important genomic features and determine many traits in living organisms,like human diseases and microbial productivities of target bioproducts.Methods:Here,we developed a bacterial type-II toxin-antitoxin-mediated method to manipulate genomic integration of tandem gene repeats in Saccharomyces cerevisiae and further visualised the evolutionary trajectories of gene repeats.We designed a tri-vector system to introduce toxin-antitoxin-driven gene amplification modules.Results:This system delivered multi-copy gene integration in the form of tandem gene repeats spontaneously and independently from toxin-antitoxin-mediated selection.Inducing the toxin(RelE)expressing via a copper(II)-inducible CUP1 promoter successfully drove the in-situ gene amplification of the antitoxin(RelB)module,resulting in~40 copies of a green fluorescence reporter gene per copy of genome.Copy-number changes,copy-number increase and copy-number decrease,and stable maintenance were visualised using the green fluorescence protein and blue chromoprotein AeBlue as reporters.Copy-number increases happened spontaneously and independent on a selection pressure.Increased copy number was quickly enriched through toxin-antitoxin-mediated selection.Conclusion:In summary,the bacterial toxin-antitoxin systems provide a flexible mechanism to manipulate gene copy number in eukaryotic cells and can be exploited for synthetic biology and metabolic engineering applications.展开更多
Hydrogen production by electrolysis of water is a key technology to achieve green hydrogen energy economy,but it relies on advanced catalyst materials with high efficiency,stability,and wide pH adaptability.In this st...Hydrogen production by electrolysis of water is a key technology to achieve green hydrogen energy economy,but it relies on advanced catalyst materials with high efficiency,stability,and wide pH adaptability.In this study,Ni,Ru,and Pt ternary metals were embedded into nitrogen-doped hollow carbon spheres(NHCSs)by hydrothermal tandem heat treatment to form ternary supported metal nanoparticles with high dispersion and ultra-small particle size(~1.3 nm),which realized efficient hydrogen evolution from multi-scenario electrocatalytic water splitting.In the whole pH range,the performance of NiRuPt/NHCSs is better than that of commercial Pt/C catalyst,and the overpotentials under alkaline,neutral,and acidic conditions are as low as 15.5,20.0,and 29.5 mV,respectively.Under industrial conditions,NiRuPt/NHCSs also have excellent hydrogen evolution reaction(HER)performance,achieving efficient electrolysis of seawater for hydrogen production,and achieving Ampere-level hydrogen production at low voltage(~1.76 V)on integrated membrane electrode assemblies.Density functional theory(DFT)calculations show that in the NiRuPt ternary metal,the Pt site is conducive to promoting the desorption of*H to form H_(2),the Ru site is conducive to promoting the capture of H_(2)O,and the Ni site is conducive to promoting the dissociation of H_(2)O.Therefore,the formed NiRuPt ternary metal synergistically promotes multi-scenario efficient electrolysis of water to produce hydrogen.This study provides a new idea for the design of multi-component metal/carbon-based composite catalysts,and promotes the development of non-noble metal/noble metal composite catalysts in hydrogen production by electrolysis of water.展开更多
Serbisütherapy(ST)is a distinctive external treatment modality within traditional Mongolian medicine(TMM),historically developed within a nomadic cultural framework.This study presents a comprehensive philologica...Serbisütherapy(ST)is a distinctive external treatment modality within traditional Mongolian medicine(TMM),historically developed within a nomadic cultural framework.This study presents a comprehensive philological and historical analysis of ST,tracing its evolution from early battlefield applications to contemporary clinical use.By critically examining classical Mongolian medical texts alongside modern case studies,we aim to systematize ST’s therapeutic methods,indications,and limitations,while exploring its mechanisms of action through both traditional theory and modern biomedical perspectives.ST has undergone significant transformation,shifting from whole-body cavity immersion in the 13th century to targeted,organ-specific applications in modern practice.Its four primary methods–Covering,Mounted,Organ Placement,and Suction–demonstrate efficacy in treating cold-natured diseases,musculoskeletal disorders,gynecological conditions,and certain emergencies.ST embodies the core principles of TMM,particularly the balance of the“Three Roots”and the correction of cold-induced pathologies through heat.Despite challenges related to standardization,cultural translation,and regulatory acceptance,ST holds translational potential for integrative medicine.Future research should prioritize mechanistic validation,clinical standardization,and the development of biocompatible thermal technologies to bridge traditional practice with modern healthcare systems.展开更多
Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the...Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the preparation of a series of novel copper iridium nanocatalysts with heterostructures and low iridium content for OER.The electrochemical tests revealed higher OER of Cu@Ir_(0.3) catalyst under acidic conditions with a generated current density of 10 mA/cm^(2) at only 284 mV overpotential.The corresponding OER mass activity was estimated to be 1.057 A/mgIr,a value 8.39-fold higher than that of the commercial IrO_(2).After 50 h of endurance testing,the Cu@Ir_(0.3) catalyst preserved excellent catalytic activity with a negligible rise in overpotential and maintained a good heterostructures.Cu@Ir_(0.3) The excellent OER activity can be attributed to its heterostructure,as con-firmed by density functional theory(DFT)calculations,indicating that Cu@Ir The coupling between isoquanta causes charge redistribution,optimizing the adsorption energy of unsaturated Ir sites for oxygen intermediates and reducing the energy barrier of OER free energy determining the rate step.In summary,this method provides a new approach for designing efficient,stable,and low iridium content OER catalysts.展开更多
Deep insights into electrocatalytic mechanisms are vital for the rational design of catalysts for oxygen evolution reaction(OER).Mechanistically,the OER driven by adsorbate evolution mechanism(AEM)is limited by the li...Deep insights into electrocatalytic mechanisms are vital for the rational design of catalysts for oxygen evolution reaction(OER).Mechanistically,the OER driven by adsorbate evolution mechanism(AEM)is limited by the linear scaling relationship,thereby exhibiting large overpotentials.In the lattice oxygen mechanism(LOM),the OER can be enhanced by enabling direct O_(2)formation.However,this enhancement is accompanied by the generation of oxygen vacancies,which presents a significant challenge to the long-term stability of LOMOER,particularly when operating at high current densities.Recently,the*O-*O coupling mechanism(OCM)has emerged as a promising alternative;it not only breaks the linear scaling relationship but also ensures catalytic stability.This review encapsulates the cutting-edge advancements in electrocatalysts that are grounded in the OCM,offering a detailed interpretation on the foundational principles guiding the design of OCM-OER catalysts.It also highlights recent theoretical investigations combining machine learning(ML)with density functional theory(DFT)calculations to reveal OER mechanisms.At the end of this review,the challenges and opportunities associated with OCM-OER electrocatalysts are discussed.展开更多
基金supported by the National Natural Science Foundation of China(grant numbers 32170450 and 31872964)Science&Technology Fundamental Resources Investigation Program(grant number 2022FY202100).
文摘Portschinskia Semenov is a rare genus of bot fies whose larvae are obligate parasites of pikas and murine rodents,crucial for understanding the evolutionary biology of Oestridae.However,limited information on their adult biology and early immature stages has hindered the progress.Here,we provided the frst documentation of adult oviposition,behavior,and morphology of newly hatched frst instars of P.magnifca Pleske.Using confocal laser scanning microscopy and scanning electron microscopy,we characterized the ultrastructure of egg and frst-instar larva,identifying key traits facilitating attachment.Eggs were deposited individually or in groups,and glued on non-host surfaces with white adhesive substances,without specialized attachment organ.Newly hatched frst instars were circled with an anterior spinose band on each body segment except the anal division,awaited hosts in an upright position,and anchored to the egg shell by their anal division,likely supported by curved spines originating from the peritreme of the posterior spiracles.Evolutionary analyses of reproductive behavior across the 4 bot fy subfamilies reveal at least 3 times independent evolution of oviposition on non-host surfaces in Portschinskia or the Hypodermatinae clade as a sister group to Ochotonia,Gasterophilus pecorum(Fabricius)(Gasterophilinae),and Cuterebrinae.In contrast,species in the Oestrinae are larviparous,depositing frst instars directly onto hosts.Our fndings shed light on oviposition behavior and early immature morphology of the rare genus Portschinskia,offering insights into reproductive strategies and evolutionary adaptations of bot fies.
基金CAs Youth Interdisciplinary Team(JCTD-2022-06)the National Nature Science Foundation of China(31870209).
文摘Chromosomal rearrangements(CRs)often cause phenotypic variations.Although several major rearrangements have been identified in Triticeae,a comprehensive study of the order,timing,and breakpoints of CRs has not been conducted.Here,we reconstruct high-quality ancestral genomes for the most recent common ancestor(MRCA)of the Triticeae,and the MRCA of the wheat lineage(Triticum and Aegilops).The protogenes of MRCA of the Triticeae and the wheat lineage are 22,894 and 29,060,respectively,which were arranged in their ancestral order.By partitioning modern Triticeae chromosomes into sets of syntenic regions and linking each to the corresponding protochromosomes,we revisit the rye chromosome structural evolution and propose alternative evolutionary routes.The previously identified 4L/5L reciprocal translocation in rye and Triticum urartu is found to have occurred independently and is unlikely to be the result of chromosomal introgression following distant hybridization.We also clarify that the 4AL/7BS translocation in tetraploid wheat was a bidirectional rather than unidirectional translocation event.Lastly,we identify several breakpoints in protochromosomes that independently reoccur following Triticeae evolution,representing potential CR hotspots.This study demonstrates that these reconstructed ancestral genomes can serve as special comparative references and facilitate a better understanding of the evolution of structural rearrangements in Triticeae.
基金supported by the National Key R&D Program of China(2022YFF1001400)postdoctoral innovative talents support program(517000-X92308)+2 种基金the specific research fund of The Innovation Platform for Academicians of Hainan Province(YSPTZX202154,YSPTZX202139)the Research Startup Funding from Hainan Institute of Zhejiang University(0202-6602-A12201)the Distinguished Discipline Support Program of Zhejiang University(226-2024-00205,226-2022-00100).
文摘The Malvaceae family,the most diverse family in the order Malvales,consists of nine subfamilies.Within the Firmiana genus of the Sterculioideae subfamily,most species are considered globally vulnerable,yet their genomes remain unexplored.Here,we present a chromosome-level genome assembly for a representative Firmiana species,F.hainanensis,2n=40,totaling 1536 Mb.Phylogenomic analysis shows that F.hainanensis and Durio zibethinus have the closest evolutionary relationship,with an estimated divergence time of approximately 21 millions of years ago(MYA)and distinct polyploidization events in their histories.Evolutionary trajectory analyses indicate that fissions and fusions may play a crucial role in chromosome number variation(2n=14 to 2n=96).Analysis of repetitive elements among Malvaceae reveals that the Tekay subfamily(belonging to the Gypsy group)contributes to variation in genome size(ranging from 324 Mb to 1620 Mb).Additionally,genes associated with P450,peroxidase,and microtubules,and thereby related to cell wall biosynthesis,are significantly contracted in F.hainanensis,potentially leading to its lower wood density relative to Hopea hainanensis.Overall,our study provides insights into the evolution of chromosome number,genome size,and the genetic basis of cell wall biosynthesis in Malvaceae species.
文摘A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and Mo2S3 nanoparticles were integrated at the edges of Co3O4 nanosheets,creating a rich,heterogeneous interface that enhances the synergistic effects of each component.In an alkaline electrolyte,the synthesized CoMoNiO-S/NF-110 exhibited superior electrocatalytic performance for oxygen evolution reaction(OER),achieving current densities of 100 and 200 mA·cm^(-2) with low overpotentials of 199.4 and 224.4 mV,respectively,outperforming RuO2 and several high-performance Mo and Ni-based catalysts.This excellent performance is attributed to the rich interface formed between the components and active sites exposed by the defect structure.
文摘The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.
文摘The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.
基金support from the National Natural Science Foundation of China(Nos.12305373 and 52276220)the Guangzhou Basic Research Program(No.SL2024A04J00234).
文摘Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.
基金supported partially by the Australian Government through the Australian Research Council Centres of Excellence funding scheme(project CE200100029)。
文摘Background:Tandem gene repeats naturally occur as important genomic features and determine many traits in living organisms,like human diseases and microbial productivities of target bioproducts.Methods:Here,we developed a bacterial type-II toxin-antitoxin-mediated method to manipulate genomic integration of tandem gene repeats in Saccharomyces cerevisiae and further visualised the evolutionary trajectories of gene repeats.We designed a tri-vector system to introduce toxin-antitoxin-driven gene amplification modules.Results:This system delivered multi-copy gene integration in the form of tandem gene repeats spontaneously and independently from toxin-antitoxin-mediated selection.Inducing the toxin(RelE)expressing via a copper(II)-inducible CUP1 promoter successfully drove the in-situ gene amplification of the antitoxin(RelB)module,resulting in~40 copies of a green fluorescence reporter gene per copy of genome.Copy-number changes,copy-number increase and copy-number decrease,and stable maintenance were visualised using the green fluorescence protein and blue chromoprotein AeBlue as reporters.Copy-number increases happened spontaneously and independent on a selection pressure.Increased copy number was quickly enriched through toxin-antitoxin-mediated selection.Conclusion:In summary,the bacterial toxin-antitoxin systems provide a flexible mechanism to manipulate gene copy number in eukaryotic cells and can be exploited for synthetic biology and metabolic engineering applications.
基金financially supported by the Yunnan Fundamental Research Projects(Nos.202401CF070026 and 202501AT070017)the Scientific Research Fund Project of Yunnan Provincial Education Department(No.2024J0134)+1 种基金the Xingdian Talent Program of Yunnan Province,and the Scientific and Technological Project of Yunnan Precious Metals Laboratory(No.YPML-20240502065)Xinjiang Key Laboratory of Novel Functional Materials Chemistry Open Science Project(No.XJLNFMC-202406).
文摘Hydrogen production by electrolysis of water is a key technology to achieve green hydrogen energy economy,but it relies on advanced catalyst materials with high efficiency,stability,and wide pH adaptability.In this study,Ni,Ru,and Pt ternary metals were embedded into nitrogen-doped hollow carbon spheres(NHCSs)by hydrothermal tandem heat treatment to form ternary supported metal nanoparticles with high dispersion and ultra-small particle size(~1.3 nm),which realized efficient hydrogen evolution from multi-scenario electrocatalytic water splitting.In the whole pH range,the performance of NiRuPt/NHCSs is better than that of commercial Pt/C catalyst,and the overpotentials under alkaline,neutral,and acidic conditions are as low as 15.5,20.0,and 29.5 mV,respectively.Under industrial conditions,NiRuPt/NHCSs also have excellent hydrogen evolution reaction(HER)performance,achieving efficient electrolysis of seawater for hydrogen production,and achieving Ampere-level hydrogen production at low voltage(~1.76 V)on integrated membrane electrode assemblies.Density functional theory(DFT)calculations show that in the NiRuPt ternary metal,the Pt site is conducive to promoting the desorption of*H to form H_(2),the Ru site is conducive to promoting the capture of H_(2)O,and the Ni site is conducive to promoting the dissociation of H_(2)O.Therefore,the formed NiRuPt ternary metal synergistically promotes multi-scenario efficient electrolysis of water to produce hydrogen.This study provides a new idea for the design of multi-component metal/carbon-based composite catalysts,and promotes the development of non-noble metal/noble metal composite catalysts in hydrogen production by electrolysis of water.
基金supported by The China Ethnic Medicine Association Research Grant(No.2023MY055-81)Science and Technology Program of the Joint Fund of Scientific Research for the Public Hospitals of Inner Mongolia Academy of Medical Sciences(2023GLLHD177,2023GLLH0174)Inner Mongolia Autonomous Region Regional Medical Center for Specialized Care(2025).
文摘Serbisütherapy(ST)is a distinctive external treatment modality within traditional Mongolian medicine(TMM),historically developed within a nomadic cultural framework.This study presents a comprehensive philological and historical analysis of ST,tracing its evolution from early battlefield applications to contemporary clinical use.By critically examining classical Mongolian medical texts alongside modern case studies,we aim to systematize ST’s therapeutic methods,indications,and limitations,while exploring its mechanisms of action through both traditional theory and modern biomedical perspectives.ST has undergone significant transformation,shifting from whole-body cavity immersion in the 13th century to targeted,organ-specific applications in modern practice.Its four primary methods–Covering,Mounted,Organ Placement,and Suction–demonstrate efficacy in treating cold-natured diseases,musculoskeletal disorders,gynecological conditions,and certain emergencies.ST embodies the core principles of TMM,particularly the balance of the“Three Roots”and the correction of cold-induced pathologies through heat.Despite challenges related to standardization,cultural translation,and regulatory acceptance,ST holds translational potential for integrative medicine.Future research should prioritize mechanistic validation,clinical standardization,and the development of biocompatible thermal technologies to bridge traditional practice with modern healthcare systems.
基金supported by the Major Science and Technology Special Plan of Yunnan Province(Nos.202302AB080012 and 202402AB080004)the National Natural Science Foundation of China(No.22264025)+1 种基金the Basic Research Foundation of Yunnan Province(Nos.202401AS070033 and 202501AT070055)the Reserve talents for young and middleaged academic and technical leaders project of Yunnan Province(No.202405AC350071).
文摘Oxygen evolution reaction(OER)is a key step in hydrogen production by water electrolysis technology.How-ever,developing efficient,stable,and low-cost OER electrocatalysts is still challenging.This article presents the preparation of a series of novel copper iridium nanocatalysts with heterostructures and low iridium content for OER.The electrochemical tests revealed higher OER of Cu@Ir_(0.3) catalyst under acidic conditions with a generated current density of 10 mA/cm^(2) at only 284 mV overpotential.The corresponding OER mass activity was estimated to be 1.057 A/mgIr,a value 8.39-fold higher than that of the commercial IrO_(2).After 50 h of endurance testing,the Cu@Ir_(0.3) catalyst preserved excellent catalytic activity with a negligible rise in overpotential and maintained a good heterostructures.Cu@Ir_(0.3) The excellent OER activity can be attributed to its heterostructure,as con-firmed by density functional theory(DFT)calculations,indicating that Cu@Ir The coupling between isoquanta causes charge redistribution,optimizing the adsorption energy of unsaturated Ir sites for oxygen intermediates and reducing the energy barrier of OER free energy determining the rate step.In summary,this method provides a new approach for designing efficient,stable,and low iridium content OER catalysts.
基金supported by the National Natural Science Foundation of China(Nos.22373063 and 22302005)Fundamental Research Funds for the Central Universities of China(No.GK202203002)+1 种基金China Postdoctoral Science Foundation(No.2023M730044)Technology Innovation Leading Program of Shaanxi(Program No.2023KXJ-007).
文摘Deep insights into electrocatalytic mechanisms are vital for the rational design of catalysts for oxygen evolution reaction(OER).Mechanistically,the OER driven by adsorbate evolution mechanism(AEM)is limited by the linear scaling relationship,thereby exhibiting large overpotentials.In the lattice oxygen mechanism(LOM),the OER can be enhanced by enabling direct O_(2)formation.However,this enhancement is accompanied by the generation of oxygen vacancies,which presents a significant challenge to the long-term stability of LOMOER,particularly when operating at high current densities.Recently,the*O-*O coupling mechanism(OCM)has emerged as a promising alternative;it not only breaks the linear scaling relationship but also ensures catalytic stability.This review encapsulates the cutting-edge advancements in electrocatalysts that are grounded in the OCM,offering a detailed interpretation on the foundational principles guiding the design of OCM-OER catalysts.It also highlights recent theoretical investigations combining machine learning(ML)with density functional theory(DFT)calculations to reveal OER mechanisms.At the end of this review,the challenges and opportunities associated with OCM-OER electrocatalysts are discussed.
