With the high dimensionality of data, the method of tensor decomposition has attracted much attention in the field of data research and analysis. The tensor decomposition is well reflected in the study of high-dimensi...With the high dimensionality of data, the method of tensor decomposition has attracted much attention in the field of data research and analysis. The tensor decomposition is well reflected in the study of high-dimensional data. The existing research uses the results of tensor decomposition to conduct community discovery. Based on the existing research, this paper presents a method to study community evolution using the results of tensor decomposition. The feature matrix obtained by the tensor decomposition algorithm was analyzed, and the real-time activity of the community with the feature matrix with time slice direction was studied to obtain the event process of community evolution. Experimental results in real data sets show that this method can well analyze dynamic events in the dataset and community evolution events.展开更多
A continuous flow bioreactor was operated for 300 days to investigate partial nitritation(PN)of mature landfill leachate,establishing the long-term performance of the system in terms of the microbial community composi...A continuous flow bioreactor was operated for 300 days to investigate partial nitritation(PN)of mature landfill leachate,establishing the long-term performance of the system in terms of the microbial community composition,evolution,and interactions.The stable operation phase(31-300 d)began after a 30 days of start-up period,reaching an average nitrite accumulation ratio(NAR)of 94.43%and a ratio of nitrite nitrogen to ammonia nitrogen(NO_(2)^(−)-N/NH_(4)^(+)-N)of 1.16.Some fulvic-like and humic-like compounds and proteins were effectively degraded in anaerobic and anoxic tanks,which was consistent with the corresponding abundance of methanogens and syntrophic bacteria in the anaerobic tank,and organic matter degrading bacteria in the anoxic tank.The ammonia-oxidizing bacteria(AOB)Nitrosomonas was found to be the key functional bacteria,exhibiting an increase in abundance from 0.27%to 6.38%,due to its collaborative interactions with organic matter degrading bacteria.In-situ inhibition of nitrite-oxidizing bacteria(NOB)was achieved using a combination of free ammonia(FA)and free nitrous acid(FNA),low dissolved oxygen(DO)with fewer bioavailable organics conditions were employed to maintain stable PN and a specific ratio of NO_(2)^(−)-N/NH_(4)^(+)-N,without an adverse impact on AOB.The synergistic relationships between AOB and both denitrifying bacteria and organic matter degrading bacteria,were found to contribute to the enhanced PN performance and microbial community structure stability.These findings provide a theoretical guidance for the effective application of PN-Anammox for mature landfill leachate treatment.展开更多
Globally,various types of pollution affect coastal waters as a result of human activities.Bioaugmentation and biostimulation are effective methods for treating water pollution.However,few studies have explored the res...Globally,various types of pollution affect coastal waters as a result of human activities.Bioaugmentation and biostimulation are effective methods for treating water pollution.However,few studies have explored the response of coastal prokaryotic and eukaryotic communities to bioaugmentation and biostimulation.Here,a 28-day outdoor mesocosm experiment with two treatments(bioaugmentation-A and combined treatment of bioaugmentation and biostimulation-AS)and a control(untreated-C)were carried out.The experiment was conducted in Meishan Bay to explore the composition,dynamics,and co-occurrence patterns of prokaryotic and eukaryotic communities in response to the A and AS using 16S rRNA and 18S rRNA gene amplicon sequencing.After treatment,Gammaproteobacteria and Epsilonproteobacteria were significantly increased in group AS compared to group C,while Flavobacteriia and Saprospirae were significantly reduced.Dinoflagellata was significantly reduced in AS compared to C,while Chrysophyta was significantly reduced in both AS and A.Compared to C,the principal response curve analyses of the prokaryotic and eukaryotic communities both showed an increasing trend followed by a decreasing trend for AS.Furthermore,the trends of prokaryotic and eukaryotic communities in group A were similar to those in group AS compared with group C,but AS changed them more than A did.According to the species weight table on principal response curves,a significant increase was observed in beneficial bacteria in prokaryotic communities,such as Rhodobacterales and Oceanospirillales,along with a decrease in autotrophs in eukaryotic communities,such as Chrysophyta and Diatom.Topological properties of network analysis reveal that A and AS complicate the interactions between the prokaryotic and eukaryotic communities.Overall,these findings expand our understanding of the response pattern of the bioaugmentation and biostimulation on coastal prokaryotic and eukaryotic communities.展开更多
Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent year...Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.展开更多
Parameterization is a critical step in modelling ecosystem dynamics.However,assigning parameter values can be a technical challenge for structurally complex natural plant communities;uncertainties in model simulations...Parameterization is a critical step in modelling ecosystem dynamics.However,assigning parameter values can be a technical challenge for structurally complex natural plant communities;uncertainties in model simulations often arise from inappropriate model parameterization.Here we compared five methods for defining community-level specific leaf area(SLA)and leaf C:N across nine contrasting forest sites along the North-South Transect of Eastern China,including biomass-weighted average for the entire plant community(AP_BW)and four simplified selective sampling(biomass-weighted average over five dominant tree species[5DT_BW],basal area weighted average over five dominant tree species[5DT_AW],biomass-weighted average over all tree species[AT_BW]and basal area weighted average over all tree species[AT_AW]).We found that the default values for SLA and leaf C:N embedded in the Biome-BGC v4.2 were higher than the five computational methods produced across the nine sites,with deviations ranging from 28.0 to 73.3%.In addition,there were only slight deviations(<10%)between the whole plant community sampling(AP_BW)predicted NPP and the four simplified selective sampling methods,and no significant difference between the predictions of AT_BW and AP_BW except the Shennongjia site.The findings in this study highlights the critical importance of computational strategies for community-level parameterization in ecosystem process modelling,and will support the choice of parameterization methods.展开更多
Synthetic nitrogen(N)fertilizer has made a great contribution to the improvement of soil fertility and productivity,but excessive application of synthetic N fertilizer may cause agroecosystem risks,such as soil acidif...Synthetic nitrogen(N)fertilizer has made a great contribution to the improvement of soil fertility and productivity,but excessive application of synthetic N fertilizer may cause agroecosystem risks,such as soil acidification,groundwater contamination and biodiversity reduction.Meanwhile,organic substitution has received increasing attention for its ecologically and environmentally friendly and productivity benefits.However,the linkages between manure substitution,crop yield and the underlying microbial mechanisms remain uncertain.To bridge this gap,a three-year field experiment was conducted with five fertilization regimes:i)Control,non-fertilization;CF,conventional synthetic fertilizer application;CF_(1/2)M_(1/2),1/2 N input via synthetic fertilizer and 1/2 N input via manure;CF_(1/4)M_(3/4),1/4 N input synthetic fertilizer and 3/4 N input via manure;M,manure application.All fertilization treatments were designed to have equal N input.Our results showed that all manure substituted treatments achieved high soil fertility indexes(SFI)and productivities by increasing the soil organic carbon(SOC),total N(TN)and available phosphorus(AP)concentrations,and by altering the bacterial community diversity and composition compared with CF.SOC,AP,and the soil C:N ratio were mainly responsible for microbial community variations.The co-occurrence network revealed that SOC and AP had strong positive associations with Rhodospirillales and Burkholderiales,while TN and C:N ratio had positive and negative associations with Micromonosporaceae,respectively.These specific taxa are implicated in soil macroelement turnover.Random Forest analysis predicted that both biotic(bacterial composition and Micromonosporaceae)and abiotic(AP,SOC,SFI,and TN)factors had significant effects on crop yield.The present work strengthens our understanding of the effects of manure substitution on crop yield and provides theoretical support for optimizing fertilization strategies.展开更多
Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibili...Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibility in Malus plants.In this experiment,88 Malus germplasm resources,such as Aihuahong,Xishuhaitang,and Reguanzi,were used as materials.Seven gene-specific primer combinations were used in the genotype identification.PCR amplification using leaf DNA produced a single S-RNase gene fragment in all materials.The results revealed that 70 of the identified materials obtained a complete S-RNase genotype,while only one S-RNase gene was found in 18 of them.Through homology comparison and analysis,13 S-RNase genotypes were obtained:S_(1)S_(2)(Aihuahong,etc.),S_(1)S_(28)(Xixian Haitang,etc.),S_(1)S_(51)(Hebei Pingdinghaitang),S_(1)S_(3)(Xiangyangcun Daguo,etc.),S_(2)S_(3)(Zhaiyehaitang,etc.),S_(3)S_(51)(Xishan 1),S_(3)S_(28)(Huangselihaerde,etc.),S_(2)S_(28)(Honghaitang,etc.),S_(4)S_(28)(Bo 11),S_(7)S_(28)(Jiuquan Shaguo),S_(10)S_e(Dongchengguan 13),S_(10)S_(21)(Dongxiangjiao)and S_(3)S_(51)(Xiongyue Haitang).Simultaneously,the frequency of the S gene in the tested materials was analyzed.The findings revealed that different S genes had varying frequencies in Malus resources,as well as varying frequencies between intraspecific and interspecific.S_(3) had the highest frequency of 68.18%,followed by S_(1)(42.04%).In addition,the phylogenetic tree and origin evolution analysis revealed that the S gene differentiation was completed prior to the formation of various apple species,that cultivated species also evolved new S genes,and that the S_(50) gene is the oldest S allele in Malus plants.The S_(1),S_(29),and S_(33) genes in apple-cultivated species,on the other hand,may have originated in M.sieversii,M.hupehensis,and M.kansuensis,respectively.In addition to M.sieversii,M.kansuensis and M.sikkimensis may have also played a role in the origin and evolution of some Chinese apples.展开更多
By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the im...By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the improvement in synchronization control between two-stage light gas gun and the transient Raman spectra acquisition,as well as the sample preparation,the Raman peak of the N-O mode of TATB was firstly observed under shock pressure up to 13.6 GPa,noticeably higher than the upper limit of 8.5 GPa reported in available literatures.By taking into account of the continuous shift of the main peak and other observed Raman peaks,we did not distinguish any structural transition or any new species.Moreover,both the present Raman spectra and the time-resolved radiation of TATB during shock loading showed that TATB exhibits higher chemical stability than previous declaration.To reveal the detailed structural response and evolution of TATB under compression,the density functional theoretical calculations were conducted,and it was found that the pressure make N-O bond lengths shorter,nitro bond angles larger,and intermolecular and intra-molecular hydrogen bond interactions enhanced.The observed red shift of Raman peak was ascribed to the abnormal enhancement of H-bound effect on the scissor vibration mode of the nitro group.展开更多
The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide incl...The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.展开更多
Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performan...Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.展开更多
The complex and volatile international landscape has significantly impacted global grain supply security. This study uses a complex network analysis model to examine the evolution and trends of the global major grain ...The complex and volatile international landscape has significantly impacted global grain supply security. This study uses a complex network analysis model to examine the evolution and trends of the global major grain trade from 1990 to 2020, focusing on network topology, centrality ranking, and community structure. There are three major findings. First, the global major grain trade network has expanded in scale, with a growing emphasis on diversification and balance. During the study period, the United States, Canada, China, and Brazil were the core nodes of the network. Grain-exporting countries were mainly situated in Asia, the Americas, and Europe, and importing countries in Asia, Africa, and Europe. Second, a significant increase in the number of high centrality countries with high export capacity occurred, benefiting from natural advantages such as fertile land and favorable climates. Third, the main global grain trade network is divided into four communities, with the Americas-Europe community being the largest and most widespread. The formation of the community pattern was influenced by geographic proximity, driven by the core exporting countries. Therefore, the world needs to enhance the existing trade model, promote the multi-polarization of the grain trade network, and establish a global vision for the future community. Countries and regions should participate actively in global grain trade security governance and institutional reform, expand trade links with other countries, and optimize import and export policies to reduce trade risks.展开更多
A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high lumines...A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transfo...With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transformation and realizing rural revitalization and sustainable rural development.Based on the traceability analysis of spatial production theory,this paper constructed an analytical framework for the spatial production evolution of traditional villages,analyzed the spatial evolution process and characteristics of traditional villages by using buffer analysis,spatial syntax,and other research methods,and revealed the characteristics of the spatial production evolution of traditional villages and the driving mechanism.The results show that:(1)The village spatial formation and development follow the village life cycle theory and usually develop from embryonic villages to diversified and integrated villages;(2)The evolution of village spatial production is characterized by the diversity of material space,the sublimation of daily life space,and the integration of social system space and generalization of emotional space;(3)The evolution of village spatial production from backward and poor village to ecologically well-off village is influenced by a combination of factors;(4)The village has formed a spatial structure of"people-land-scape-culture-industry",realized comprehensive reconstruction and spatial reproduction.The study results reflect the spatial evolution characteristics of traditional villages in mountainous areas in a more comprehensive way,which helps to promote the protection and development of traditional villages in mountainous areas and,to a certain extent,provides a reference for the development of rural revitalization.展开更多
Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy...Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.展开更多
To deepen the understanding in the effect of potassium lactate on the sensory quality and safety of Rugao ham,sensory attributes,physicochemical parameters,total volatile basic nitrogen(TVBN),microorganism community a...To deepen the understanding in the effect of potassium lactate on the sensory quality and safety of Rugao ham,sensory attributes,physicochemical parameters,total volatile basic nitrogen(TVBN),microorganism community and biogenic amines of Rugao ham manufactured with different potassium lactate levels(0%,0.5%,1%,2%)were investigated;the relationship between microbial community and the formation of TVBN and biogenic amines was further evaluated.With the increase of potassium lactate from 0%to 2%,the increased sensory scores and the decreased total aerobic bacterial count and TVBN were observed;the abundance of Staphylococcus increased,while the content of Halomonas decreased.LDA effect size(LEf Se)and correlations analysis showed that Staphylococcus equorum and Lactobacillus fermentum could be the key species to improve sensory scores and decrease biogenic amines and TVBN.Metabolic pathway analysis further showed that amino acids metabolism and nitrogen metabolism were mainly involved in decreasing TVBN and biogenic amines in the treatment of 2%potassium lactate.展开更多
The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional ...The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.展开更多
Popular fermented golden pomfret(Trachinotus ovatus)is prepared via spontaneous fermentation;however,the mechanisms underlying the regulation of its flavor development remain unclear.This study shows the roles of the ...Popular fermented golden pomfret(Trachinotus ovatus)is prepared via spontaneous fermentation;however,the mechanisms underlying the regulation of its flavor development remain unclear.This study shows the roles of the complex microbiota and the dynamic changes in microbial community and flavor compounds during fish fermentation.Single-molecule real-time sequencing and molecular networking analysis revealed the correlations among different microbial genera and the relationships between microbial taxa and volatile compounds.Mechanisms underlying flavor development were also elucidated via KEGG based functional annotations.Clostridium,Shewanella,and Staphylococcus were the dominant microbial genera.Forty-nine volatile compounds were detected in the fermented fish samples,with thirteen identified as characteristic volatile compounds(ROAV>1).Volatile profiles resulted from the interactions among the microorganisms and derived enzymes,with the main metabolic pathways being amino acid biosynthesis/metabolism,carbon metabolism,and glycolysis/gluconeogenesis.This study demonstrated the approaches for distinguishing key microbiota associated with volatile compounds and monitoring the industrial production of high-quality fermented fish products.展开更多
Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will ben...Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts.Herein,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−2.Additionally,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,Raman spectroscopy revealed the transformation process of CoOOH.Calculations using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials.Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.展开更多
The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clu...The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.展开更多
文摘With the high dimensionality of data, the method of tensor decomposition has attracted much attention in the field of data research and analysis. The tensor decomposition is well reflected in the study of high-dimensional data. The existing research uses the results of tensor decomposition to conduct community discovery. Based on the existing research, this paper presents a method to study community evolution using the results of tensor decomposition. The feature matrix obtained by the tensor decomposition algorithm was analyzed, and the real-time activity of the community with the feature matrix with time slice direction was studied to obtain the event process of community evolution. Experimental results in real data sets show that this method can well analyze dynamic events in the dataset and community evolution events.
基金financially supported by the National Natural Science Foundation of China(No.52170049).
文摘A continuous flow bioreactor was operated for 300 days to investigate partial nitritation(PN)of mature landfill leachate,establishing the long-term performance of the system in terms of the microbial community composition,evolution,and interactions.The stable operation phase(31-300 d)began after a 30 days of start-up period,reaching an average nitrite accumulation ratio(NAR)of 94.43%and a ratio of nitrite nitrogen to ammonia nitrogen(NO_(2)^(−)-N/NH_(4)^(+)-N)of 1.16.Some fulvic-like and humic-like compounds and proteins were effectively degraded in anaerobic and anoxic tanks,which was consistent with the corresponding abundance of methanogens and syntrophic bacteria in the anaerobic tank,and organic matter degrading bacteria in the anoxic tank.The ammonia-oxidizing bacteria(AOB)Nitrosomonas was found to be the key functional bacteria,exhibiting an increase in abundance from 0.27%to 6.38%,due to its collaborative interactions with organic matter degrading bacteria.In-situ inhibition of nitrite-oxidizing bacteria(NOB)was achieved using a combination of free ammonia(FA)and free nitrous acid(FNA),low dissolved oxygen(DO)with fewer bioavailable organics conditions were employed to maintain stable PN and a specific ratio of NO_(2)^(−)-N/NH_(4)^(+)-N,without an adverse impact on AOB.The synergistic relationships between AOB and both denitrifying bacteria and organic matter degrading bacteria,were found to contribute to the enhanced PN performance and microbial community structure stability.These findings provide a theoretical guidance for the effective application of PN-Anammox for mature landfill leachate treatment.
基金supported by the National Natural Science Foundation of China(No.42077219)the Ningbo Municipal Natural Science Foundation(No.2019A610443)+1 种基金the Hangzhou Municipal Agriculture and Social Development Project(No.2020ZDSJ0697)the Fundamental Research Funds for the Provincial Universities of Zhejiang(No.SJLY2020011)
文摘Globally,various types of pollution affect coastal waters as a result of human activities.Bioaugmentation and biostimulation are effective methods for treating water pollution.However,few studies have explored the response of coastal prokaryotic and eukaryotic communities to bioaugmentation and biostimulation.Here,a 28-day outdoor mesocosm experiment with two treatments(bioaugmentation-A and combined treatment of bioaugmentation and biostimulation-AS)and a control(untreated-C)were carried out.The experiment was conducted in Meishan Bay to explore the composition,dynamics,and co-occurrence patterns of prokaryotic and eukaryotic communities in response to the A and AS using 16S rRNA and 18S rRNA gene amplicon sequencing.After treatment,Gammaproteobacteria and Epsilonproteobacteria were significantly increased in group AS compared to group C,while Flavobacteriia and Saprospirae were significantly reduced.Dinoflagellata was significantly reduced in AS compared to C,while Chrysophyta was significantly reduced in both AS and A.Compared to C,the principal response curve analyses of the prokaryotic and eukaryotic communities both showed an increasing trend followed by a decreasing trend for AS.Furthermore,the trends of prokaryotic and eukaryotic communities in group A were similar to those in group AS compared with group C,but AS changed them more than A did.According to the species weight table on principal response curves,a significant increase was observed in beneficial bacteria in prokaryotic communities,such as Rhodobacterales and Oceanospirillales,along with a decrease in autotrophs in eukaryotic communities,such as Chrysophyta and Diatom.Topological properties of network analysis reveal that A and AS complicate the interactions between the prokaryotic and eukaryotic communities.Overall,these findings expand our understanding of the response pattern of the bioaugmentation and biostimulation on coastal prokaryotic and eukaryotic communities.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51902101 and 21875203)the Natural Science Foundation of Hunan Province(Nos.2021JJ40044 and 2023JJ50287)Natural Science Foundation of Jiangsu Province(No.BK20201381).
文摘Deformable catalytic material with excellent flexible structure is a new type of catalyst that has been applied in various chemical reactions,especially electrocatalytic hydrogen evolution reaction(HER).In recent years,deformable catalysts for HER have made great progress and would become a research hotspot.The catalytic activities of deformable catalysts could be adjustable by the strain engineering and surface reconfiguration.The surface curvature of flexible catalytic materials is closely related to the electrocatalytic HER properties.Here,firstly,we systematically summarized self-adaptive catalytic performance of deformable catalysts and various micro–nanostructures evolution in catalytic HER process.Secondly,a series of strategies to design highly active catalysts based on the mechanical flexibility of lowdimensional nanomaterials were summarized.Last but not least,we presented the challenges and prospects of the study of flexible and deformable micro–nanostructures of electrocatalysts,which would further deepen the understanding of catalytic mechanisms of deformable HER catalyst.
基金This research was funded by the National Natural Science Foundation of China(Grant Nos.31870426).
文摘Parameterization is a critical step in modelling ecosystem dynamics.However,assigning parameter values can be a technical challenge for structurally complex natural plant communities;uncertainties in model simulations often arise from inappropriate model parameterization.Here we compared five methods for defining community-level specific leaf area(SLA)and leaf C:N across nine contrasting forest sites along the North-South Transect of Eastern China,including biomass-weighted average for the entire plant community(AP_BW)and four simplified selective sampling(biomass-weighted average over five dominant tree species[5DT_BW],basal area weighted average over five dominant tree species[5DT_AW],biomass-weighted average over all tree species[AT_BW]and basal area weighted average over all tree species[AT_AW]).We found that the default values for SLA and leaf C:N embedded in the Biome-BGC v4.2 were higher than the five computational methods produced across the nine sites,with deviations ranging from 28.0 to 73.3%.In addition,there were only slight deviations(<10%)between the whole plant community sampling(AP_BW)predicted NPP and the four simplified selective sampling methods,and no significant difference between the predictions of AT_BW and AP_BW except the Shennongjia site.The findings in this study highlights the critical importance of computational strategies for community-level parameterization in ecosystem process modelling,and will support the choice of parameterization methods.
基金supported by the National Key Research and Development Program of China(2022YFD2301403-2)the Major Special Project of Anhui Province,China(2021d06050003)+2 种基金the Postdoctoral Foundation of Anhui Province,China(2022B638)the Special Project of Zhongke Bengbu Technology Transfer Center,China(ZKBB202103)the Grant of the President Foundation of Hefei Institutes of Physical Science of Chinese Academy of Sciences(YZJJ2023QN37)。
文摘Synthetic nitrogen(N)fertilizer has made a great contribution to the improvement of soil fertility and productivity,but excessive application of synthetic N fertilizer may cause agroecosystem risks,such as soil acidification,groundwater contamination and biodiversity reduction.Meanwhile,organic substitution has received increasing attention for its ecologically and environmentally friendly and productivity benefits.However,the linkages between manure substitution,crop yield and the underlying microbial mechanisms remain uncertain.To bridge this gap,a three-year field experiment was conducted with five fertilization regimes:i)Control,non-fertilization;CF,conventional synthetic fertilizer application;CF_(1/2)M_(1/2),1/2 N input via synthetic fertilizer and 1/2 N input via manure;CF_(1/4)M_(3/4),1/4 N input synthetic fertilizer and 3/4 N input via manure;M,manure application.All fertilization treatments were designed to have equal N input.Our results showed that all manure substituted treatments achieved high soil fertility indexes(SFI)and productivities by increasing the soil organic carbon(SOC),total N(TN)and available phosphorus(AP)concentrations,and by altering the bacterial community diversity and composition compared with CF.SOC,AP,and the soil C:N ratio were mainly responsible for microbial community variations.The co-occurrence network revealed that SOC and AP had strong positive associations with Rhodospirillales and Burkholderiales,while TN and C:N ratio had positive and negative associations with Micromonosporaceae,respectively.These specific taxa are implicated in soil macroelement turnover.Random Forest analysis predicted that both biotic(bacterial composition and Micromonosporaceae)and abiotic(AP,SOC,SFI,and TN)factors had significant effects on crop yield.The present work strengthens our understanding of the effects of manure substitution on crop yield and provides theoretical support for optimizing fertilization strategies.
基金financially supported by the Agricultural Science and Technology Innovation Program(CAASASTIP-2021-RIP-02)。
文摘Identification of the S genotype of Malus plants will greatly promote the discovery of new genes,the cultivation and production of apple,the breeding of new varieties,and the origin and evolution of self-incompatibility in Malus plants.In this experiment,88 Malus germplasm resources,such as Aihuahong,Xishuhaitang,and Reguanzi,were used as materials.Seven gene-specific primer combinations were used in the genotype identification.PCR amplification using leaf DNA produced a single S-RNase gene fragment in all materials.The results revealed that 70 of the identified materials obtained a complete S-RNase genotype,while only one S-RNase gene was found in 18 of them.Through homology comparison and analysis,13 S-RNase genotypes were obtained:S_(1)S_(2)(Aihuahong,etc.),S_(1)S_(28)(Xixian Haitang,etc.),S_(1)S_(51)(Hebei Pingdinghaitang),S_(1)S_(3)(Xiangyangcun Daguo,etc.),S_(2)S_(3)(Zhaiyehaitang,etc.),S_(3)S_(51)(Xishan 1),S_(3)S_(28)(Huangselihaerde,etc.),S_(2)S_(28)(Honghaitang,etc.),S_(4)S_(28)(Bo 11),S_(7)S_(28)(Jiuquan Shaguo),S_(10)S_e(Dongchengguan 13),S_(10)S_(21)(Dongxiangjiao)and S_(3)S_(51)(Xiongyue Haitang).Simultaneously,the frequency of the S gene in the tested materials was analyzed.The findings revealed that different S genes had varying frequencies in Malus resources,as well as varying frequencies between intraspecific and interspecific.S_(3) had the highest frequency of 68.18%,followed by S_(1)(42.04%).In addition,the phylogenetic tree and origin evolution analysis revealed that the S gene differentiation was completed prior to the formation of various apple species,that cultivated species also evolved new S genes,and that the S_(50) gene is the oldest S allele in Malus plants.The S_(1),S_(29),and S_(33) genes in apple-cultivated species,on the other hand,may have originated in M.sieversii,M.hupehensis,and M.kansuensis,respectively.In addition to M.sieversii,M.kansuensis and M.sikkimensis may have also played a role in the origin and evolution of some Chinese apples.
基金supported by the National Natural Science Foundation of China(Grant Nos.12072299,11902276)the Natural Science Foundation of Sichuan Province(Grant No.2022NSFSC1802)+1 种基金the Basic Research Project of Southwest Jiaotong University(Grant No.2682023ZTPY009)the National Key Laboratory for Shock Wave and Detonation Physics of China(Grant No.JCKYS2019212007)。
文摘By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the improvement in synchronization control between two-stage light gas gun and the transient Raman spectra acquisition,as well as the sample preparation,the Raman peak of the N-O mode of TATB was firstly observed under shock pressure up to 13.6 GPa,noticeably higher than the upper limit of 8.5 GPa reported in available literatures.By taking into account of the continuous shift of the main peak and other observed Raman peaks,we did not distinguish any structural transition or any new species.Moreover,both the present Raman spectra and the time-resolved radiation of TATB during shock loading showed that TATB exhibits higher chemical stability than previous declaration.To reveal the detailed structural response and evolution of TATB under compression,the density functional theoretical calculations were conducted,and it was found that the pressure make N-O bond lengths shorter,nitro bond angles larger,and intermolecular and intra-molecular hydrogen bond interactions enhanced.The observed red shift of Raman peak was ascribed to the abnormal enhancement of H-bound effect on the scissor vibration mode of the nitro group.
基金Agency for Science,Technology and Research(A*STAR),under the RIE2020 Advanced Manufacturing and Engineering(AME)Programmatic Grant(Grant no.A18B1b0061)。
文摘The corrosion rates of additive-manufactured Mg alloys are higher than their as-cast counterparts,possibly due to increased kinetics for the hydrogen evolution reaction on secondary phases,which may include oxide inclusions.Scanning Kelvin Probe Force Microscopy demonstrated that MgO inclusions could act as cathodes for Mg corrosion,but their low conductivity likely precludes this.However,the density of state calculations through density functional theory using hybrid HSE06 functional revealed overlapping electronic states at the Mg/MgO interface,which facilitates electron transfers and participates in redox reactions.Subsequent determination of the hydrogen absorption energy at the Mg/MgO interface reveals it to be an excellent catalytic site,with HER being found to be a factor of 23x more efficient at the interface than on metallic Mg.The results not only support the plausibility of the Mg/MgO interface being an effective cathode to the adjacent anodic Mg matrix during corrosion but also contribute to the understanding of the enhanced cathodic activities observed during the anodic dissolution of magnesium.
基金funded by the National Natural Science Foundation of China (NSFC) (Nos. 22221001, 22201115, 21931001, and 21922105)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province (2019ZX–04)+3 种基金the 111 Project (B20027)by the Fundamental Research Funds for the Central Universities (lzujbky-2023-eyt03)support Natural Science Foundation of Gansu Providence (22JR5RA540)Gansu Province Youth Science and Technology Talent Promotion Project (GXH202220530-02)。
文摘Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.
基金funded by the National Natural Science Foundation of China(42271313)the Chinese Academy of Agricultural Sciences Innovation Project(CAAS-ASTIP2021-AII)the Central Public-interest Scientific Institution Basal Research Fund,China(JBYW-AII-2022-06,JBYWAII-2022-40)。
文摘The complex and volatile international landscape has significantly impacted global grain supply security. This study uses a complex network analysis model to examine the evolution and trends of the global major grain trade from 1990 to 2020, focusing on network topology, centrality ranking, and community structure. There are three major findings. First, the global major grain trade network has expanded in scale, with a growing emphasis on diversification and balance. During the study period, the United States, Canada, China, and Brazil were the core nodes of the network. Grain-exporting countries were mainly situated in Asia, the Americas, and Europe, and importing countries in Asia, Africa, and Europe. Second, a significant increase in the number of high centrality countries with high export capacity occurred, benefiting from natural advantages such as fertile land and favorable climates. Third, the main global grain trade network is divided into four communities, with the Americas-Europe community being the largest and most widespread. The formation of the community pattern was influenced by geographic proximity, driven by the core exporting countries. Therefore, the world needs to enhance the existing trade model, promote the multi-polarization of the grain trade network, and establish a global vision for the future community. Countries and regions should participate actively in global grain trade security governance and institutional reform, expand trade links with other countries, and optimize import and export policies to reduce trade risks.
基金supported by the Natural Science Foundation of Hebei Province(Grant No.E2022209039)Key Research Project of North China University of Science and Technology(Grant No.ZD-YG-202301)Tangshan Talent Funding Project(Grant No.A202202007).
文摘A series of carbon nitride(CN)materials represented by graphitic carbon nitride(g-C3N4)have been widely used in bioimaging,biosensing,and other fields in recent years due to their nontoxicity,low cost,and high luminescent quantum efficiency.What is more attractive is that the luminescent properties such as wavelength and intensity can be regulated by controlling the structure at the molecular level.Hence,it is time to summarize the related research on CN structural evolution and make a prospect on future developments.In this review,we first summarize the research history and multiple structural evolution of CN.Then,the progress of improving the luminescence performance of CN through structural evolution was discussed.Significantly,the relationship between CN structure evolution and energy conversion in the forms of photoluminescence,chemiluminescence,and electrochemiluminescence was reviewed.Finally,key challenges and opportunities such as nanoscale dispersion strategy,luminous efficiency improving methods,standardization evaluation,and macroscopic preparation of CN are highlighted.
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金supported by the National Natural Science Foundation of China(Grant No.42061035)the Guizhou Provincial Program on Commercialization of Scientific and Technological Achievements([2022]010).
文摘With the rapid urbanization process,the space of traditional villages in China is undergoing significant changes.Studying the spatial evolution of traditional villages is significant in promoting rural spatial transformation and realizing rural revitalization and sustainable rural development.Based on the traceability analysis of spatial production theory,this paper constructed an analytical framework for the spatial production evolution of traditional villages,analyzed the spatial evolution process and characteristics of traditional villages by using buffer analysis,spatial syntax,and other research methods,and revealed the characteristics of the spatial production evolution of traditional villages and the driving mechanism.The results show that:(1)The village spatial formation and development follow the village life cycle theory and usually develop from embryonic villages to diversified and integrated villages;(2)The evolution of village spatial production is characterized by the diversity of material space,the sublimation of daily life space,and the integration of social system space and generalization of emotional space;(3)The evolution of village spatial production from backward and poor village to ecologically well-off village is influenced by a combination of factors;(4)The village has formed a spatial structure of"people-land-scape-culture-industry",realized comprehensive reconstruction and spatial reproduction.The study results reflect the spatial evolution characteristics of traditional villages in mountainous areas in a more comprehensive way,which helps to promote the protection and development of traditional villages in mountainous areas and,to a certain extent,provides a reference for the development of rural revitalization.
基金supported by the National Natural Sci-ence Foundation of China(22272081),Jiangsu Provincial Specially Appointed Professors Foundation.
文摘Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.
基金supported by National Natural Science Foundation of China(32022066,32101975)Zhejiang Province Natural Science Foundation(LQ22C200017)+1 种基金China Postdoctoral Foundation(2020M681806,2021T140348)Science and Technology Programs of Ningbo(202003N4130,202002N3067)。
文摘To deepen the understanding in the effect of potassium lactate on the sensory quality and safety of Rugao ham,sensory attributes,physicochemical parameters,total volatile basic nitrogen(TVBN),microorganism community and biogenic amines of Rugao ham manufactured with different potassium lactate levels(0%,0.5%,1%,2%)were investigated;the relationship between microbial community and the formation of TVBN and biogenic amines was further evaluated.With the increase of potassium lactate from 0%to 2%,the increased sensory scores and the decreased total aerobic bacterial count and TVBN were observed;the abundance of Staphylococcus increased,while the content of Halomonas decreased.LDA effect size(LEf Se)and correlations analysis showed that Staphylococcus equorum and Lactobacillus fermentum could be the key species to improve sensory scores and decrease biogenic amines and TVBN.Metabolic pathway analysis further showed that amino acids metabolism and nitrogen metabolism were mainly involved in decreasing TVBN and biogenic amines in the treatment of 2%potassium lactate.
基金financial support from the National Natural Science Foundation of China (52203070)the Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies (FZ2022005)+2 种基金the Open Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing (STRZ202203)the financial support provided by the China Scholarship Council (CSC)Visiting Scholar Programfinancial support from Institute for Sustainability,Energy and Resources,The University of Adelaide,Future Making Fellowship,Australia。
文摘The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.
基金supported by the National Natural Science Foundation of China(32001733)the Earmarked fund for CARS(CARS-47)+3 种基金Guangxi Natural Science Foundation Program(2021GXNSFAA196023)Guangdong Basic and Applied Basic Research Foundation(2021A1515010833)Young Talent Support Project of Guangzhou Association for Science and Technology(QT20220101142)the Special Scientific Research Funds for Central Non-profit Institutes,Chinese Academy of Fishery Sciences(2020TD69)。
文摘Popular fermented golden pomfret(Trachinotus ovatus)is prepared via spontaneous fermentation;however,the mechanisms underlying the regulation of its flavor development remain unclear.This study shows the roles of the complex microbiota and the dynamic changes in microbial community and flavor compounds during fish fermentation.Single-molecule real-time sequencing and molecular networking analysis revealed the correlations among different microbial genera and the relationships between microbial taxa and volatile compounds.Mechanisms underlying flavor development were also elucidated via KEGG based functional annotations.Clostridium,Shewanella,and Staphylococcus were the dominant microbial genera.Forty-nine volatile compounds were detected in the fermented fish samples,with thirteen identified as characteristic volatile compounds(ROAV>1).Volatile profiles resulted from the interactions among the microorganisms and derived enzymes,with the main metabolic pathways being amino acid biosynthesis/metabolism,carbon metabolism,and glycolysis/gluconeogenesis.This study demonstrated the approaches for distinguishing key microbiota associated with volatile compounds and monitoring the industrial production of high-quality fermented fish products.
基金The National Natural Science Foundation of China(Grant Nos.52072114 and 51922008)the 111 Project(Grant No.D17007),the Henan Center for Outstanding Overseas Scientists(Grant No.GZS2018003)+2 种基金Xinxiang Major Science and Technology Projects(Grant No.21ZD001)Guangdong Innovative and Entrepreneurial Research Team Program(2016ZT06N500)Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(2018B030322001)all provided financial support for this work.
文摘Transition-metal oxyhydroxides are attractive catalysts for oxygen evolution reactions(OERs).Further studies for developing transition-metal oxyhydroxide catalysts and understanding their catalytic mechanisms will benefit their quick transition to the next catalysts.Herein,Mo-doped CoOOH was designed as a high-performance model electrocatalyst with durability for 20 h at 10 mAcm−2.Additionally,it had an overpotential of 260 mV(glassy carbon)or 215 mV(nickel foam),which was 78 mV lower than that of IrO_(2)(338 mV).In situ,Raman spectroscopy revealed the transformation process of CoOOH.Calculations using the density functional theory showed that during OER,doped Mo increased the spin-up density of states and shrank the spin-down bandgap of the 3d orbits in the reconstructed CoOOH under the electrochemical activation process,which simultaneously optimized the adsorption and electron conduction of oxygen-related intermediates on Co sites and lowered the OER overpotentials.Our research provides new insights into the methodical planning of the creation of transition-metal oxyhydroxide OER catalysts.
基金supported by the National Natural Science Foundation of China(22205209,52202373 and U21A200972)China Postdoctoral Science Foundation(2022M722867)Key Research Project of Higher Education Institutions in Henan Province(23A530001)。
文摘The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation strategies.Hence,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum disulfide.The unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active sites.Among them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical calculation.Whereupon,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.
