During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure o...During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure of phytoplankton community,resulting in algal blooms and seriously threatening the ecological security of the reservoir.It is of great significance to understand the continuous changes of phytoplankton in the initial impoundment period for the protection of reservoir water quality.Therefore,a two-year in-situ monitoring study was conducted on water quality and phytoplankton in a representative canyonshaped reservoir named Sanhekou and the interannual changes of phytoplankton community and its response to environmental changes during the initial impoundment period were discussed at taxonomic versus functional classification levels.The results showed that the total nitrogen and permanganate index levels were relatively high in the first year due to rapid water storage and heavy rainfall input,and the more stable hydrological conditions in the second year promoted the increase of algae density and the transformation of community,and the proportion of cyanobacteria increased significantly.The succession order of phytoplankton in the first year of the initial impoundment periodwas Chlorophyta-Bacillariophyta-Chlorophyta,or J/F/X1-P/MP/W1-A/X1/MP,respectively.And the succession order in the second year was Cyanobacteria/Chlorophyta-Bacillariophyta-Chlorophyta,or L_(M)/G/P-P/A/X1-X1/J/G.Water temperature,relativewater column stability,mixing depth,and pHwere crucial factors affecting phytoplankton community succession.This study revealed the interannual succession law and driving factors of phytoplankton in the initial impoundment period and provided an important reference for the operation management and ecological protection of canyon-shaped reservoirs.展开更多
Difunctionalization of unsaturated hydrocarbons is a pivotal synthetic strategy enabling the conversion of alkenes and alkynes into high value-added compounds.It allows for the introduction of two functional groups in...Difunctionalization of unsaturated hydrocarbons is a pivotal synthetic strategy enabling the conversion of alkenes and alkynes into high value-added compounds.It allows for the introduction of two functional groups into the unsaturated bond in a single step,facilitating the efficient construction of complex molecular architectures,which has been widely utilized in material chemistry,pharmaceutical and fine chemical synthesis.Recently,significant progress has been made via free radical-mediated difunctionalization due to the extensive application of photocatalysis.However,highly selective difunc-tionalization reactions still remain challenging.The research progress of selective difunctionalization of unsaturated hydro-carbons using a free radical addition/functional group migration strategy over the past decade is summarized,and synthetic strategies and key reaction steps are systematically elaborated.展开更多
Amyloid-like proteins are critical for interfacial adhesion across various marine organisms and bacteria.However,the specific contributions of different functional residues remain unclear.Herein,we introduce an approa...Amyloid-like proteins are critical for interfacial adhesion across various marine organisms and bacteria.However,the specific contributions of different functional residues remain unclear.Herein,we introduce an approach to deconstruct and mimic these residues using synthetic homopolymers and random copolymers with phenyl,amino,carboxyl,and hydroxyl functional groups using reversible addition-fragmentation chain transfer(RAFT)polymerization.The resulting polymers,designed with comparable molecular weights(M_(n):10–20 kDa)and narrow dispersities(PDI<1.3),mimic the diverse surface chemistry of amyloid-like proteins,enabling systematic investigation of their adhesive properties.The interfacial adhesion forces of different polymer films were quantified using atomic force microscopy(AFM)with a colloidal probe.Remarkably copolymers with multiple functional groups demonstrated significantly enhanced adhesion compared to homopolymers,a trend corroborated by macroscopic shear strength and stability tests.These results highlight that the synergistic effects of multiple functional groups are crucial for achieving universal interfacial adhesion of macromolecules,offering insights into protein adhesion mechanisms,and guiding polymer-based interfacial modifications.展开更多
As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC...As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC)were synthesized as CDI electrode material for removing Na^(+)and Cl^(−)in salty water.Results showed that the average diameter of HC was approximately 180 nm,and the infrared spectrum showed that its surface was successfully modified with sulfonic and amino groups,respectively.The sulfonic acid functionalized HC(HC-S)showed better electrochemical and desalting performance than the amino-functionalized HC(HC–N),with a maximum Faradic capacity of 287.4 F/g and an adsorptive capacity of 112.97 mg/g for NaCl.Additionally,92.63%capacity retention after 100 adsorption/desorption cycles demonstrates the excellent stability of HC-S.The main findings prove that HC-S is viable as an electrodematerial for desalination by high-performance CDI applications.展开更多
Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional g...Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional groups of different types and occurrences of organic matter.Combined with the quantitative evaluation of pore development via scanning electron microscopy(SEM),the response of organic pore formation and evolution mechanisms to chemical composition and structural evolution of organic matter in overmature marine shale is investigated.The results indicate that the AFM-IR spectra of graptolite periderms and pyrobitumen in shale are dominated by the stretching vibrations of conjugated C=C bonds in aromatic compounds at approximately 1600 cm-1,with weak absorption peaks near 1375,1450 and 1720 cm-1,corresponding to aliphatic chains and carbonyl/carboxyl functional groups.Overall,the AFM-IR structural indices(A and C factors)of organic matter show a strong correlation with visible porosity in shales of equivalent maturity.Lower A and C factor values correlate with enhanced development of organic pores,which is associated with the detachment of more aliphatic chains and oxygen-containing functional groups during thermal evolution.Pyrobitumen-clay mineral composites generally exhibit superior pore development,likely attributable to clay mineral dehydration participating in hydrocarbon generation reactions that promote the removal of more functional groups.Additionally,hydrocarbon generation within organic-clay composites during high-over mature stages may induce volumetric expansion,resulting in microfracturing and hydrocarbon expulsion.The associated higher hydrocarbon expulsion rates promote the formation of larger pores and fracture-shaped pores along the flake-shaped clay minerals.This study highlights that the research of submicron-scale molecular functional groups provides a deeper understanding of organic matter evolution and pores development mechanisms in overmature shales,thereby offering critical theoretical parameters for reservoir evaluation in shale oil and gas exploration.展开更多
To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation betwe...To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.展开更多
Global warming has caused an increase in the frequency and duration of droughts worldwide.Droughts could trigger large changes in physico-chemical conditions and phytoplankton community in waterbodies,resulting in a s...Global warming has caused an increase in the frequency and duration of droughts worldwide.Droughts could trigger large changes in physico-chemical conditions and phytoplankton community in waterbodies,resulting in a shift in the phytoplankton community.Spring diatom blooms in reservoirs have been increasingly observed in the past decade in the Taihu Lake basin.The aim of the present study is to elucidate the impacts of droughts on aquatic environment and to determine the driving factors for the succession of the phytoplankton functional groups based on the analysis of data collected during spring from 2009 to 2020 in the Daxi Reservoir.The unimodal relationship between 1-month aggregated precipitation index and phytoplankton species richness indicated the competitive exclusion occurred in extremely drought period.The structural equation modeling indicated that drought-related low water level conditions intensified sediment resuspension,and increased the phosphorus-enriched nonalgal turbidity in the Daxi Reservoir.Concurrently,a steady shift in the Reynolds phytoplankton functional groups from L 0,TD,J,X 2,and A(phytoplankton taxa preferring low turbidity and nutrient conditions)to TB(pennate diatoms being adapt to turbid and nutrient-rich conditions)was observed.The increased TP and non-algal turbidity in addition to the lowered disturbance contribute to the prevalence of Group TB.Considering the difficulties in nutrient control,timely water replenishment is often a feasible method of controlling the dominance of harmful algae for reservoir management.Finally,alternative water sources are in high demand for ensuring ecological safety and water availability when dealing with drought.展开更多
Anthropogenic disturbances are widespread in tropical forests and influence the species composition in the overstory.However,the impacts of historical disturbance on tropical forest overstory recovery are unclear due ...Anthropogenic disturbances are widespread in tropical forests and influence the species composition in the overstory.However,the impacts of historical disturbance on tropical forest overstory recovery are unclear due to a lack of disturbance data,and previous studies have focused on understory species.In this study,the purpose was to deter-mine the influence of historical disturbance on the diver-sity,composition and regeneration of overstory species in present forests.In the 20-ha Xishuangbanna tropical sea-sonal rainforest dynamics plot in southwestern China,the historical disturbance boundaries were delineated based on panchromatic photographs from 1965.Factors that drove species clustering in the overstory layer(DBH≥40 cm)were analyzed and the abundance,richness and composition of these species were compared among different tree groups based on multiple regression tree analysis.The coefficient of variation of the brightness value in historical panchro-matic photographs from 1965 was the primary driver of spe-cies clustering in the overstory layer.The abundance and richness of overstory species throughout the regeneration process were similar,but species composition was always different.Although the proportion of large-seeded and vigorous-sprouting species showed no significant differ-ence between disturbed and undisturbed forests in the tree-let layer(DBH<20 cm),the difference became significant when DBH increased.The findings highlight that historical disturbances have strong legacy effects on functional group composition in the overstory and the recovery of overstory species was multidimensional.Functional group composi-tion can better indicate the dynamics of overstory species replacement during secondary succession.展开更多
To understand the distribution of phytoplankton functional groups(PFGs)and key factors on their compositions in different watersheds of the Huanghe(Yellow)River basin,25 river sites and 25 lake-reservoirs sites were s...To understand the distribution of phytoplankton functional groups(PFGs)and key factors on their compositions in different watersheds of the Huanghe(Yellow)River basin,25 river sites and 25 lake-reservoirs sites were selected.The contents of nephelometric turbidity(NTU),total nitrogen(TN),and total phosphorus(TP)were significantly higher in rivers than that in lakes or reservoirs,whereas the pH and CODMn(chemical oxygen demand or potassium permanganate index)were lower.Results show that,27 PFGs,namely,assemblages A,B,C,D,E,F,G,H,J,K,LM,Lo,M,MP,N,P,S1,S2,T,TC,W1,W2,X1,X2,X3,XPh,and Y,were identified.Additionally,ANOSIM correlation analysis demonstrated significant differences in PFG composition between the riverine and lake-reservoir sections in the Huanghe River basin.In the riverine watersheds,the group MP was dominant,while assemblages B and J were prevalent in lakes and reservoirs.The Mantel correlation tests and RDA analysis showed that environmental variables,such as NTU,water temperature(WT),conductivity(Cond),and TP,were key driving factors of shaping the dominant PFGs of the study area.Using the Venn diagram based on variation partitioning analysis,PFGs were mainly influenced by WT and TP in lake-reservoir sites,while in the river sites were affected mainly by geo-climatic variables.This study helps understanding the PFGs in river ecosystems,and unraveling the key driving factors in different watersheds,which shall be important for the protection and management of entire Huanghe River basin.展开更多
In order to study the differences in algae species and their biomass in water bodies in a region, three reservoirs and two lakes at the center of Guanzhong Plain were chosen to identify algae functional groups, measur...In order to study the differences in algae species and their biomass in water bodies in a region, three reservoirs and two lakes at the center of Guanzhong Plain were chosen to identify algae functional groups, measure biomass, and assess water quality, from January2013 to December 2014. The water bodies represented different trophic levels： one oligotrophic, three mesotrophic, and one eutrophic. Based on the Reynolds’ functional groups, they had 10 groups in common—B, P, D, X1, M, MP, F, S1, J, and G, but the algae biomasses and proportions were different. In the oligotrophic reservoir, functional group B reached a peak biomass of 576 × 104 L-1, which accounted for 31.27%. In the eutrophic lake,functional group D reached a peak biomass of 3227 × 104 L-1, which accounted for only13.38%. When samples collected from other water bodies with similar trophic levels were compared, we found differences in the algae species functional groups. The potential reasons for the differences in algae functional group characteristics in the different water bodies in the region were water temperature and nutritional states.展开更多
[Objective]The aim was to carry out stoichiometry on the early-spring herbs functional group in subtropical artificial wetland.[Method]UV-Vis spectrophotometer was used for the determination of nitrate-nitrogen,ammoni...[Objective]The aim was to carry out stoichiometry on the early-spring herbs functional group in subtropical artificial wetland.[Method]UV-Vis spectrophotometer was used for the determination of nitrate-nitrogen,ammonium nitrogen and phosphorus concentrations.Potassium persulfate absorptiometry was used for the measurement of total N content,while the flame photometer was used to detect the potassium and sodium concentration in plants.All the nutrient determination of plant samples were repeated for four times.[Result]The four nutrient concentrations in almost all samples were in the normal range of natural plant nutrition concentrations;in early-spring herbs functional groups,different species showed diversity on the nutrient concentrations;plant height had no significant effect on the nutrient concentrations in plants;the nutrient concentrations of non-grass group plants were higher than that of grass group plants;the nutrient concentrations of the annual herb were higher than that of perennial herbs.[Conclusion]The study had provided basis for the understanding of the effects of changes in nutritional conditions on species diversity,community structure and succession of the system.展开更多
Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary...Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary greatly due to their complex chemical constituents and different preparation processes and are reflected in the values of parameters such as the specific surface area(SSA),pore volume/size,and surface functional groups(SFGs).The effects of SSA and pore volume/size on the adsorption of aromatics have been widely reported.However,the corresponding mechanisms of BC SFGs towards aromatics adsorption remains unclear as the compositions of the SFGs are usually complex and hard to determine.To address in this gap in the literature,this review introduces a new perspective on the adsorption mechanisms of aromatics.Through collecting previously-reported results,the parameters log P(logarithm of the Kow),polar surface area,and the positive/negative charges were carefully calculated using Chem Draw3D,which allowed the hydrophobicity/hydrophilicity properties,electron donor-acceptor interactions,Hbonding,and electrostatic interactions between SFGs and aromatics-based contaminates to be inferred intuitively.These predictions were consistent with the reported results and showed that tailor-made BCs can be designed according to the molecular weights,chemical structures,and polarities of the target aromatics.Overall,this review provides new insight into predicting the physicochemical properties of BCs through revealing the relationship between SFGs and adsorbates,which may provide useful guidance for the preparing of highly-efficient,functional BCs for the adsorption of aromatics.展开更多
The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and a...The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and after modification was analyzed based on the nitrogen adsorption isotherms.The morphology of those activated carbons was characterized using scanning electronic microscopy （SEM）.The surface functional groups were determined by Fourier transform infrared spectroscopy （FTIR）.The quantity of those groups was measured by the Boehm titration method.Cr（VI） removal by the activated carbons from aqueous solution was investigated at different pH values.The results show that compared with H2SO4,HNO3 destructs the original pore of the activated carbon more seriously and induces more acidic surface functional groups on the activated carbon.The pH value of the solution plays a key role in the Cr（VI） removal.The ability of reducing Cr（VI） to Cr（III） by the activated carbons is relative to the acidic surface functional groups.At higher pH values,the Cr（VI） removal ratio is improved by increasing the acidic surface functional groups of the activated carbons.At lower pH values,however,the acidic surface functional groups almost have no effect on the Cr（VI） removal by the activated carbon from aqueous solution.展开更多
Variations in the fractions of biomass allocated to functional components are widely considered as plant responses to resource availability for grassland plants. Observations indicated shoots isometrically relates to ...Variations in the fractions of biomass allocated to functional components are widely considered as plant responses to resource availability for grassland plants. Observations indicated shoots isometrically relates to roots at the community level but allometrically at the species level in Tibetan alpine grasslands. These differences may result from the specific complementarity of functional groups between functional components, such as leaf, root, stem and reproductive organ. To test the component complementary responses to regional moisture variation, we conducted a multi-site transect survey to measure plant individual size and component biomass fractions of common species belonging to the functional groups： forbs, grasses, legumes and sedges on the Northern Tibetan Plateau in peak growing season in 2010. Along the mean annual precipitation （MAP） gradient, we sampled 7o species, in which 2o are in alpine meadows, 20 in alpine steppes, 15 in alpine desert-steppes and 15 in alpine deserts, respectively. Our results showed that the size of alpine plants is small with individual biomass mostly lower than 1.0 g. Plants keep relative conservative component individual responses moisture functional fractions across alpine grasslands at the level. However, the complementary between functional components to variations specifically differ among groups. These results indicate that functional group diversity may be an effective tool for scaling biomass allocation patterns from individual up to community level. Therefore, it is necessary andvaluable to perform intensive and systematic studies on identification and differentiation the influences of compositional changes in functional groups on ecosystem primary services and processes.展开更多
Reservoirs are an important water source in many densely populated areas in southwest China.Phytoplankton play an essential role in maintaining the structure and function of reservoir ecosystems.Understanding the succ...Reservoirs are an important water source in many densely populated areas in southwest China.Phytoplankton play an essential role in maintaining the structure and function of reservoir ecosystems.Understanding the succession in phytoplankton communities and the factors driving it are essential for eff ective water quality management in drinking water reservoirs.In this study,water samples were collected monthly at the surface layers from March 2016 to December 2019 in Hongfeng Reservoir,southwest China.The relationship between functional group succession was analyzed based on nonmetric multidimensional scaling analysis(NMDS),redundancy analysis(RDA),succession rate,and other analysis methods.The results showed distinct shifts in the community structure of phytoplankton functional groups within study period.The Cyclotella sp.was dominant in 2016 and 2017,and Pseudanabaena limnetica was the dominant group in 2018 and 2019.It appears that the phytoplankton composition and biomass are closely related to the water temperature and nutrient status in this reservoir.The results clearly showed that the permanganate index(COD_(Mn))was the key factor of dramatic phytoplankton functional group succession,and the change in succession rates was closely caused by total nitrogen concentration(TN).Therefore,the succession pattern and key factors of Hongfeng Reservoir revealed in this study were important guidance for the management of drinking water reservoirs in southwest China.A reasonable limit on exogenous nutrient input should be a priority,especially in high water temperature period.展开更多
The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) i...The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) ion adsorption onto AC-T.The modified activated carbon is characterized by scanning electron microscopy,Fourier transform infrared spectroscopy(FT-IR) and X-ray photoelectron spectroscopy(XPS).The results of batch experiments indicate that the maximal adsorption could be achieved over the broad pH range of 4.5 to 6.5.Adsorption isotherms and kinetic study suggest that the sorption of Cd(Ⅱ) onto AC-T produces monolayer coverage and that adsorption is controlled by chemical adsorption.And the adsorbent has a good reusability.According to the FT-IR and XPS analyses,electrostatic attraction and cation exchange between Cd(Ⅱ) and oxygen-containing functional groups on AC-T are dominant mechanisms for Cd(Ⅱ) adsorption.展开更多
The relationship between trace elements in coal and organic functional groups of coal, also some of aromatic structure, was investigated by using curve fitting of infrared spectra. Cluster analysis was also performed ...The relationship between trace elements in coal and organic functional groups of coal, also some of aromatic structure, was investigated by using curve fitting of infrared spectra. Cluster analysis was also performed according to the degree of affinity of organic groups to the trace elements. The results show that there is a possibility that trace elements, especially LREE, were bound to peripheral organic functional groups of middle rank coal macromolecule. The most possible functional group that binds trace element is the hydroxyl, and to the less degree, the asymmetric -CH3 and 〉CH2 stretching, -CH3 stretching, etc. The degree of affinity of trace elements to different functional groups varies. The tendency obeys the natural structural changing law of trace elements-- the periodic law. The deviation of some trace elements from this regular trend is attributed to the deviation of intrinsic ＂confusion degree＂ （conventional molar entropy） of the matter system of coal basin, which is affected by the inner and outer factors during the evolution.展开更多
Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were ...Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were prepared by using the fresh urea and the urea kept for five years,respectively,for the first time.Experimental results show that the H2 production rate of the C-GCN is 39.06μmol/h,which is about 5 times of the Y-GCN.Meantime,in terms of apparent quantum efficiency(AQ.E)at 420 nm,C-GCN has a value of 6.3%and nearly 7.3 times higher than that of Y-GCN(0.86%).The results of XRD,IR,DRS,and NMR show,different from Y-GCN,a new kind of functional group of—N=CH—was firstly in-situ introduced into the C-GCN,resulting in good visible light absorption,and then markedly improving the photocatalytic performance.DFT calculation also confirms the effect of the—N=CH—group band structure of g-C3N4.Furthermore,XPS results demonstrate that the existence of—N=CH—groups in C-GCN results in tight interaction between C-GCN and Pt nanoparticles,and then improves the charge separation and photocatalytic performance.The present work demonstrates a good example of"defect engineering"to modify the intrinsic molecular structure of g-C3N4 and provides a new avenue to enhance the photocatalytic activity of g-C3N4 via facile and environmental-friendly method.展开更多
In order to explore the influence of modification sites of functional groups on landfill gas （CO2/CH4） separation performance of metal-organic frameworks （MOFs）, six types of or- ganic linkers and three types of f...In order to explore the influence of modification sites of functional groups on landfill gas （CO2/CH4） separation performance of metal-organic frameworks （MOFs）, six types of or- ganic linkers and three types of functional groups （i.e. -F, -NH2, -CH3） were used to construct 36 MOFs of pcu topology based on copper paddlewheel. Grand canonical Monte Carlo sim- ulations were performed in this work to evaluate the separation performance of MOFs at low （vacuum swing adsorption） and high （pressure swing adsorption） pressures, respectively. Simulation results demonstrated that CO2 working capacity of the unfunctionalized MOFs generally exhibits pore-size dependence at 1 bar, which increases with the decrease in pore sizes. It was also found that -NH2 funetionalized MOFs exhibit the highest CO2 uptake due to the enhanced Coulombic interactions between the polar -NH2 groups and the quadrupole moment of CO2 molecules, which is followed by -CH3 and -F functionalized ones. Moreover, positioning the functional groups -NH2 and -CH3 at sites far from the metal node （site b） exhibits more significant enhancement on CO2/CH4 separation performance compared to that adjacent to the metal node （site a）.展开更多
MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their p...MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their practical application in lithium-ion batteries.In this work,a robust strategy is developed to control the functional groups of Nb_2 CT_x MXene.The capacity of pristine Nb_2 CT_x MXene can be significantly increased by Li~+ intercalation and surface modification.The specific capacity of the treated Nb_2 CT_x is up to 448 mAh g^(-1) at 0.05 A g^(-1),and at a large current density of 2 A g^(-1) remains a high reversible capacity retention rate of 75% after an ultra-long cycle of 2000 cycles.These values exceed most of the reported pristine MXenes(including the most studied Ti_3 C_2 T_x) and carbon-based materials.It demonstrates that this strategy has great help to improve the electrochemical performance of pristine MXene,and the results enhance the promise of MXenes in the application of lithium-ion batteries.展开更多
基金supported by the National Key R&D Program of China(No.2022YFC3203602)the Natural Science Foundation of China(No.52370018)+1 种基金Shaanxi Provincial Youth Innovation Team Project(No.22JP040)Shaanxi Provincial Key Scientific and Technological Innovation Team(No.2023-CX-TD-32).
文摘During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure of phytoplankton community,resulting in algal blooms and seriously threatening the ecological security of the reservoir.It is of great significance to understand the continuous changes of phytoplankton in the initial impoundment period for the protection of reservoir water quality.Therefore,a two-year in-situ monitoring study was conducted on water quality and phytoplankton in a representative canyonshaped reservoir named Sanhekou and the interannual changes of phytoplankton community and its response to environmental changes during the initial impoundment period were discussed at taxonomic versus functional classification levels.The results showed that the total nitrogen and permanganate index levels were relatively high in the first year due to rapid water storage and heavy rainfall input,and the more stable hydrological conditions in the second year promoted the increase of algae density and the transformation of community,and the proportion of cyanobacteria increased significantly.The succession order of phytoplankton in the first year of the initial impoundment periodwas Chlorophyta-Bacillariophyta-Chlorophyta,or J/F/X1-P/MP/W1-A/X1/MP,respectively.And the succession order in the second year was Cyanobacteria/Chlorophyta-Bacillariophyta-Chlorophyta,or L_(M)/G/P-P/A/X1-X1/J/G.Water temperature,relativewater column stability,mixing depth,and pHwere crucial factors affecting phytoplankton community succession.This study revealed the interannual succession law and driving factors of phytoplankton in the initial impoundment period and provided an important reference for the operation management and ecological protection of canyon-shaped reservoirs.
文摘Difunctionalization of unsaturated hydrocarbons is a pivotal synthetic strategy enabling the conversion of alkenes and alkynes into high value-added compounds.It allows for the introduction of two functional groups into the unsaturated bond in a single step,facilitating the efficient construction of complex molecular architectures,which has been widely utilized in material chemistry,pharmaceutical and fine chemical synthesis.Recently,significant progress has been made via free radical-mediated difunctionalization due to the extensive application of photocatalysis.However,highly selective difunc-tionalization reactions still remain challenging.The research progress of selective difunctionalization of unsaturated hydro-carbons using a free radical addition/functional group migration strategy over the past decade is summarized,and synthetic strategies and key reaction steps are systematically elaborated.
基金supported by the National Natural Science Foundation of China(Nos.22375122 and 22105065)the National Science Fund for Distinguished Young Scholars(No.52225301)+3 种基金the National Key R&D Program of China(Nos.2020YFA0710400 and 2020YFA0710402)the 111 Project(No.B14041)Fundamental Research Funds for Central Universities(No.GK202304040)Open Project of the State Key Laboratory of Supramolecular Structure and Materials(No.sklssm2024023)。
文摘Amyloid-like proteins are critical for interfacial adhesion across various marine organisms and bacteria.However,the specific contributions of different functional residues remain unclear.Herein,we introduce an approach to deconstruct and mimic these residues using synthetic homopolymers and random copolymers with phenyl,amino,carboxyl,and hydroxyl functional groups using reversible addition-fragmentation chain transfer(RAFT)polymerization.The resulting polymers,designed with comparable molecular weights(M_(n):10–20 kDa)and narrow dispersities(PDI<1.3),mimic the diverse surface chemistry of amyloid-like proteins,enabling systematic investigation of their adhesive properties.The interfacial adhesion forces of different polymer films were quantified using atomic force microscopy(AFM)with a colloidal probe.Remarkably copolymers with multiple functional groups demonstrated significantly enhanced adhesion compared to homopolymers,a trend corroborated by macroscopic shear strength and stability tests.These results highlight that the synergistic effects of multiple functional groups are crucial for achieving universal interfacial adhesion of macromolecules,offering insights into protein adhesion mechanisms,and guiding polymer-based interfacial modifications.
基金supported by the National Science Foundation of China(No.21606191)the Natural Science Foundation of Shandong Province(No.ZR2020ME024).
文摘As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC)were synthesized as CDI electrode material for removing Na^(+)and Cl^(−)in salty water.Results showed that the average diameter of HC was approximately 180 nm,and the infrared spectrum showed that its surface was successfully modified with sulfonic and amino groups,respectively.The sulfonic acid functionalized HC(HC-S)showed better electrochemical and desalting performance than the amino-functionalized HC(HC–N),with a maximum Faradic capacity of 287.4 F/g and an adsorptive capacity of 112.97 mg/g for NaCl.Additionally,92.63%capacity retention after 100 adsorption/desorption cycles demonstrates the excellent stability of HC-S.The main findings prove that HC-S is viable as an electrodematerial for desalination by high-performance CDI applications.
基金Supported by the National Natural Science Foundation of China(42172148,42172142)。
文摘Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional groups of different types and occurrences of organic matter.Combined with the quantitative evaluation of pore development via scanning electron microscopy(SEM),the response of organic pore formation and evolution mechanisms to chemical composition and structural evolution of organic matter in overmature marine shale is investigated.The results indicate that the AFM-IR spectra of graptolite periderms and pyrobitumen in shale are dominated by the stretching vibrations of conjugated C=C bonds in aromatic compounds at approximately 1600 cm-1,with weak absorption peaks near 1375,1450 and 1720 cm-1,corresponding to aliphatic chains and carbonyl/carboxyl functional groups.Overall,the AFM-IR structural indices(A and C factors)of organic matter show a strong correlation with visible porosity in shales of equivalent maturity.Lower A and C factor values correlate with enhanced development of organic pores,which is associated with the detachment of more aliphatic chains and oxygen-containing functional groups during thermal evolution.Pyrobitumen-clay mineral composites generally exhibit superior pore development,likely attributable to clay mineral dehydration participating in hydrocarbon generation reactions that promote the removal of more functional groups.Additionally,hydrocarbon generation within organic-clay composites during high-over mature stages may induce volumetric expansion,resulting in microfracturing and hydrocarbon expulsion.The associated higher hydrocarbon expulsion rates promote the formation of larger pores and fracture-shaped pores along the flake-shaped clay minerals.This study highlights that the research of submicron-scale molecular functional groups provides a deeper understanding of organic matter evolution and pores development mechanisms in overmature shales,thereby offering critical theoretical parameters for reservoir evaluation in shale oil and gas exploration.
基金funding of the National Key Research and Development Plan(Grant 2017YFB0306600)the Project of SINOPEC(NO.117006).
文摘To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.
基金Supported by the National Natural Science Foundation of China(Nos.U22A20616,32071573)。
文摘Global warming has caused an increase in the frequency and duration of droughts worldwide.Droughts could trigger large changes in physico-chemical conditions and phytoplankton community in waterbodies,resulting in a shift in the phytoplankton community.Spring diatom blooms in reservoirs have been increasingly observed in the past decade in the Taihu Lake basin.The aim of the present study is to elucidate the impacts of droughts on aquatic environment and to determine the driving factors for the succession of the phytoplankton functional groups based on the analysis of data collected during spring from 2009 to 2020 in the Daxi Reservoir.The unimodal relationship between 1-month aggregated precipitation index and phytoplankton species richness indicated the competitive exclusion occurred in extremely drought period.The structural equation modeling indicated that drought-related low water level conditions intensified sediment resuspension,and increased the phosphorus-enriched nonalgal turbidity in the Daxi Reservoir.Concurrently,a steady shift in the Reynolds phytoplankton functional groups from L 0,TD,J,X 2,and A(phytoplankton taxa preferring low turbidity and nutrient conditions)to TB(pennate diatoms being adapt to turbid and nutrient-rich conditions)was observed.The increased TP and non-algal turbidity in addition to the lowered disturbance contribute to the prevalence of Group TB.Considering the difficulties in nutrient control,timely water replenishment is often a feasible method of controlling the dominance of harmful algae for reservoir management.Finally,alternative water sources are in high demand for ensuring ecological safety and water availability when dealing with drought.
基金supported by the Natural Science Foundation of Yunnan Province(Grant No:202301AT070356)the Open Fund of the Key Laboratory of Tropical Forest Ecology,Chinese Academy of Sciences,National Science Foundation of China(Grant No.32061123003)+1 种基金the Joint Fund of the National Natural Science Foundation of China-Yunnan Province(Grant No.U1902203)the Field Station Foundation of the Chinese Academy of Sciences.
文摘Anthropogenic disturbances are widespread in tropical forests and influence the species composition in the overstory.However,the impacts of historical disturbance on tropical forest overstory recovery are unclear due to a lack of disturbance data,and previous studies have focused on understory species.In this study,the purpose was to deter-mine the influence of historical disturbance on the diver-sity,composition and regeneration of overstory species in present forests.In the 20-ha Xishuangbanna tropical sea-sonal rainforest dynamics plot in southwestern China,the historical disturbance boundaries were delineated based on panchromatic photographs from 1965.Factors that drove species clustering in the overstory layer(DBH≥40 cm)were analyzed and the abundance,richness and composition of these species were compared among different tree groups based on multiple regression tree analysis.The coefficient of variation of the brightness value in historical panchro-matic photographs from 1965 was the primary driver of spe-cies clustering in the overstory layer.The abundance and richness of overstory species throughout the regeneration process were similar,but species composition was always different.Although the proportion of large-seeded and vigorous-sprouting species showed no significant differ-ence between disturbed and undisturbed forests in the tree-let layer(DBH<20 cm),the difference became significant when DBH increased.The findings highlight that historical disturbances have strong legacy effects on functional group composition in the overstory and the recovery of overstory species was multidimensional.Functional group composi-tion can better indicate the dynamics of overstory species replacement during secondary succession.
基金Supported by the Young Backbone Teachers Project of Henan Province (No. 2020GGJS064)the Key Scientific and Technological Project of Henan Province (No. 232102321056)+1 种基金the Scientific Fund of Henan Normal University (No. 2020QK02)the Project of Huanghe River Fisheries Resources and Environment Investigation from the MARA,China,and the Observation and Research Station on Water Ecosystem in Danjiangkou Reservoir of Henan Province
文摘To understand the distribution of phytoplankton functional groups(PFGs)and key factors on their compositions in different watersheds of the Huanghe(Yellow)River basin,25 river sites and 25 lake-reservoirs sites were selected.The contents of nephelometric turbidity(NTU),total nitrogen(TN),and total phosphorus(TP)were significantly higher in rivers than that in lakes or reservoirs,whereas the pH and CODMn(chemical oxygen demand or potassium permanganate index)were lower.Results show that,27 PFGs,namely,assemblages A,B,C,D,E,F,G,H,J,K,LM,Lo,M,MP,N,P,S1,S2,T,TC,W1,W2,X1,X2,X3,XPh,and Y,were identified.Additionally,ANOSIM correlation analysis demonstrated significant differences in PFG composition between the riverine and lake-reservoir sections in the Huanghe River basin.In the riverine watersheds,the group MP was dominant,while assemblages B and J were prevalent in lakes and reservoirs.The Mantel correlation tests and RDA analysis showed that environmental variables,such as NTU,water temperature(WT),conductivity(Cond),and TP,were key driving factors of shaping the dominant PFGs of the study area.Using the Venn diagram based on variation partitioning analysis,PFGs were mainly influenced by WT and TP in lake-reservoir sites,while in the river sites were affected mainly by geo-climatic variables.This study helps understanding the PFGs in river ecosystems,and unraveling the key driving factors in different watersheds,which shall be important for the protection and management of entire Huanghe River basin.
基金supported by the Ministry of Human Resources and Social Security of the People's Republic of China,Shaanxi Youth Science and Technology Star Project(No.2012KJXX-32)the National Natural Science Youth Fund(No.51008242)
文摘In order to study the differences in algae species and their biomass in water bodies in a region, three reservoirs and two lakes at the center of Guanzhong Plain were chosen to identify algae functional groups, measure biomass, and assess water quality, from January2013 to December 2014. The water bodies represented different trophic levels： one oligotrophic, three mesotrophic, and one eutrophic. Based on the Reynolds’ functional groups, they had 10 groups in common—B, P, D, X1, M, MP, F, S1, J, and G, but the algae biomasses and proportions were different. In the oligotrophic reservoir, functional group B reached a peak biomass of 576 × 104 L-1, which accounted for 31.27%. In the eutrophic lake,functional group D reached a peak biomass of 3227 × 104 L-1, which accounted for only13.38%. When samples collected from other water bodies with similar trophic levels were compared, we found differences in the algae species functional groups. The potential reasons for the differences in algae functional group characteristics in the different water bodies in the region were water temperature and nutritional states.
基金Supported by National Natural Science Foundation of China(30370146)~~
文摘[Objective]The aim was to carry out stoichiometry on the early-spring herbs functional group in subtropical artificial wetland.[Method]UV-Vis spectrophotometer was used for the determination of nitrate-nitrogen,ammonium nitrogen and phosphorus concentrations.Potassium persulfate absorptiometry was used for the measurement of total N content,while the flame photometer was used to detect the potassium and sodium concentration in plants.All the nutrient determination of plant samples were repeated for four times.[Result]The four nutrient concentrations in almost all samples were in the normal range of natural plant nutrition concentrations;in early-spring herbs functional groups,different species showed diversity on the nutrient concentrations;plant height had no significant effect on the nutrient concentrations in plants;the nutrient concentrations of non-grass group plants were higher than that of grass group plants;the nutrient concentrations of the annual herb were higher than that of perennial herbs.[Conclusion]The study had provided basis for the understanding of the effects of changes in nutritional conditions on species diversity,community structure and succession of the system.
基金funded by the National Natural Science Foundation of China(No.51961165104)Project of Thousand Youth Talents(No.AUGA2160100917)+1 种基金University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2020050)Provincial Leading Talent Echelon Cultivation Project of Heilongjiang Institute of Technology(No.2020LJ04)。
文摘Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary greatly due to their complex chemical constituents and different preparation processes and are reflected in the values of parameters such as the specific surface area(SSA),pore volume/size,and surface functional groups(SFGs).The effects of SSA and pore volume/size on the adsorption of aromatics have been widely reported.However,the corresponding mechanisms of BC SFGs towards aromatics adsorption remains unclear as the compositions of the SFGs are usually complex and hard to determine.To address in this gap in the literature,this review introduces a new perspective on the adsorption mechanisms of aromatics.Through collecting previously-reported results,the parameters log P(logarithm of the Kow),polar surface area,and the positive/negative charges were carefully calculated using Chem Draw3D,which allowed the hydrophobicity/hydrophilicity properties,electron donor-acceptor interactions,Hbonding,and electrostatic interactions between SFGs and aromatics-based contaminates to be inferred intuitively.These predictions were consistent with the reported results and showed that tailor-made BCs can be designed according to the molecular weights,chemical structures,and polarities of the target aromatics.Overall,this review provides new insight into predicting the physicochemical properties of BCs through revealing the relationship between SFGs and adsorbates,which may provide useful guidance for the preparing of highly-efficient,functional BCs for the adsorption of aromatics.
文摘The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and after modification was analyzed based on the nitrogen adsorption isotherms.The morphology of those activated carbons was characterized using scanning electronic microscopy （SEM）.The surface functional groups were determined by Fourier transform infrared spectroscopy （FTIR）.The quantity of those groups was measured by the Boehm titration method.Cr（VI） removal by the activated carbons from aqueous solution was investigated at different pH values.The results show that compared with H2SO4,HNO3 destructs the original pore of the activated carbon more seriously and induces more acidic surface functional groups on the activated carbon.The pH value of the solution plays a key role in the Cr（VI） removal.The ability of reducing Cr（VI） to Cr（III） by the activated carbons is relative to the acidic surface functional groups.At higher pH values,the Cr（VI） removal ratio is improved by increasing the acidic surface functional groups of the activated carbons.At lower pH values,however,the acidic surface functional groups almost have no effect on the Cr（VI） removal by the activated carbon from aqueous solution.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB03030401 & XDA05060700)the National Natural Science Foundation of China (Grant Nos. 41171044, 31070391, 41271067)the General Financial Grant from the China Postdoctoral Science Foundation (Grant No. 2013M530716)
文摘Variations in the fractions of biomass allocated to functional components are widely considered as plant responses to resource availability for grassland plants. Observations indicated shoots isometrically relates to roots at the community level but allometrically at the species level in Tibetan alpine grasslands. These differences may result from the specific complementarity of functional groups between functional components, such as leaf, root, stem and reproductive organ. To test the component complementary responses to regional moisture variation, we conducted a multi-site transect survey to measure plant individual size and component biomass fractions of common species belonging to the functional groups： forbs, grasses, legumes and sedges on the Northern Tibetan Plateau in peak growing season in 2010. Along the mean annual precipitation （MAP） gradient, we sampled 7o species, in which 2o are in alpine meadows, 20 in alpine steppes, 15 in alpine desert-steppes and 15 in alpine deserts, respectively. Our results showed that the size of alpine plants is small with individual biomass mostly lower than 1.0 g. Plants keep relative conservative component individual responses moisture functional fractions across alpine grasslands at the level. However, the complementary between functional components to variations specifically differ among groups. These results indicate that functional group diversity may be an effective tool for scaling biomass allocation patterns from individual up to community level. Therefore, it is necessary andvaluable to perform intensive and systematic studies on identification and differentiation the influences of compositional changes in functional groups on ecosystem primary services and processes.
基金Supported by the National Natural Science Foundation of China(No.U1612442)the Science and Technology Foundation of Guizhou Province(Nos.[2020]6009,[2020]4Y009)Anton Brancelj was supported by Slovenian Research Agency(ARRS)(No.P1-0255)。
文摘Reservoirs are an important water source in many densely populated areas in southwest China.Phytoplankton play an essential role in maintaining the structure and function of reservoir ecosystems.Understanding the succession in phytoplankton communities and the factors driving it are essential for eff ective water quality management in drinking water reservoirs.In this study,water samples were collected monthly at the surface layers from March 2016 to December 2019 in Hongfeng Reservoir,southwest China.The relationship between functional group succession was analyzed based on nonmetric multidimensional scaling analysis(NMDS),redundancy analysis(RDA),succession rate,and other analysis methods.The results showed distinct shifts in the community structure of phytoplankton functional groups within study period.The Cyclotella sp.was dominant in 2016 and 2017,and Pseudanabaena limnetica was the dominant group in 2018 and 2019.It appears that the phytoplankton composition and biomass are closely related to the water temperature and nutrient status in this reservoir.The results clearly showed that the permanganate index(COD_(Mn))was the key factor of dramatic phytoplankton functional group succession,and the change in succession rates was closely caused by total nitrogen concentration(TN).Therefore,the succession pattern and key factors of Hongfeng Reservoir revealed in this study were important guidance for the management of drinking water reservoirs in southwest China.A reasonable limit on exogenous nutrient input should be a priority,especially in high water temperature period.
基金Supported by the Fundamental Research Funds for the Central Universities(TD2013-2,2012LYB33)the National Natural Science Foundation of China(51278053,21373032)grant-in-aid from Kochi University of Technology and China Scholarship Council
文摘The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) ion adsorption onto AC-T.The modified activated carbon is characterized by scanning electron microscopy,Fourier transform infrared spectroscopy(FT-IR) and X-ray photoelectron spectroscopy(XPS).The results of batch experiments indicate that the maximal adsorption could be achieved over the broad pH range of 4.5 to 6.5.Adsorption isotherms and kinetic study suggest that the sorption of Cd(Ⅱ) onto AC-T produces monolayer coverage and that adsorption is controlled by chemical adsorption.And the adsorbent has a good reusability.According to the FT-IR and XPS analyses,electrostatic attraction and cation exchange between Cd(Ⅱ) and oxygen-containing functional groups on AC-T are dominant mechanisms for Cd(Ⅱ) adsorption.
基金supported by the National Science Foundation of China(Nos.41172143 and 40872101)Developmental Plan of Basic Research on Natural Science of Shanxi Province(20012JM5005)Science Research Plan of Shanxi education department(12JK0483)
文摘The relationship between trace elements in coal and organic functional groups of coal, also some of aromatic structure, was investigated by using curve fitting of infrared spectra. Cluster analysis was also performed according to the degree of affinity of organic groups to the trace elements. The results show that there is a possibility that trace elements, especially LREE, were bound to peripheral organic functional groups of middle rank coal macromolecule. The most possible functional group that binds trace element is the hydroxyl, and to the less degree, the asymmetric -CH3 and 〉CH2 stretching, -CH3 stretching, etc. The degree of affinity of trace elements to different functional groups varies. The tendency obeys the natural structural changing law of trace elements-- the periodic law. The deviation of some trace elements from this regular trend is attributed to the deviation of intrinsic ＂confusion degree＂ （conventional molar entropy） of the matter system of coal basin, which is affected by the inner and outer factors during the evolution.
基金financial support of the National Natural Science Foundation of China(NSFC,Nos.51622806,51878325,51868050,51378246 and 51720105001)the Natural Science Foundation of Jiangxi Province(Nos.20162BCB22017,20165BCB18008,20171ACB20017,20133ACB21001 and 20171BAB206049)。
文摘Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were prepared by using the fresh urea and the urea kept for five years,respectively,for the first time.Experimental results show that the H2 production rate of the C-GCN is 39.06μmol/h,which is about 5 times of the Y-GCN.Meantime,in terms of apparent quantum efficiency(AQ.E)at 420 nm,C-GCN has a value of 6.3%and nearly 7.3 times higher than that of Y-GCN(0.86%).The results of XRD,IR,DRS,and NMR show,different from Y-GCN,a new kind of functional group of—N=CH—was firstly in-situ introduced into the C-GCN,resulting in good visible light absorption,and then markedly improving the photocatalytic performance.DFT calculation also confirms the effect of the—N=CH—group band structure of g-C3N4.Furthermore,XPS results demonstrate that the existence of—N=CH—groups in C-GCN results in tight interaction between C-GCN and Pt nanoparticles,and then improves the charge separation and photocatalytic performance.The present work demonstrates a good example of"defect engineering"to modify the intrinsic molecular structure of g-C3N4 and provides a new avenue to enhance the photocatalytic activity of g-C3N4 via facile and environmental-friendly method.
基金supported by the National Natural Science Foundation of China(No.51606081)the Basic Research Foundation of Shenzhen(No.JCYJ20160506170043770)
文摘In order to explore the influence of modification sites of functional groups on landfill gas （CO2/CH4） separation performance of metal-organic frameworks （MOFs）, six types of or- ganic linkers and three types of functional groups （i.e. -F, -NH2, -CH3） were used to construct 36 MOFs of pcu topology based on copper paddlewheel. Grand canonical Monte Carlo sim- ulations were performed in this work to evaluate the separation performance of MOFs at low （vacuum swing adsorption） and high （pressure swing adsorption） pressures, respectively. Simulation results demonstrated that CO2 working capacity of the unfunctionalized MOFs generally exhibits pore-size dependence at 1 bar, which increases with the decrease in pore sizes. It was also found that -NH2 funetionalized MOFs exhibit the highest CO2 uptake due to the enhanced Coulombic interactions between the polar -NH2 groups and the quadrupole moment of CO2 molecules, which is followed by -CH3 and -F functionalized ones. Moreover, positioning the functional groups -NH2 and -CH3 at sites far from the metal node （site b） exhibits more significant enhancement on CO2/CH4 separation performance compared to that adjacent to the metal node （site a）.
基金Project supported by the National Science Foundation of China (No.51772070 and 51772069)。
文摘MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their practical application in lithium-ion batteries.In this work,a robust strategy is developed to control the functional groups of Nb_2 CT_x MXene.The capacity of pristine Nb_2 CT_x MXene can be significantly increased by Li~+ intercalation and surface modification.The specific capacity of the treated Nb_2 CT_x is up to 448 mAh g^(-1) at 0.05 A g^(-1),and at a large current density of 2 A g^(-1) remains a high reversible capacity retention rate of 75% after an ultra-long cycle of 2000 cycles.These values exceed most of the reported pristine MXenes(including the most studied Ti_3 C_2 T_x) and carbon-based materials.It demonstrates that this strategy has great help to improve the electrochemical performance of pristine MXene,and the results enhance the promise of MXenes in the application of lithium-ion batteries.
