Porous organic molecular materials(POMMs)are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks,mainly held by non-covalent interactions.POMMs represent a varie...Porous organic molecular materials(POMMs)are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks,mainly held by non-covalent interactions.POMMs represent a variety of chemical families,such as hydrogen-bonded organic frameworks,porous organic salts,porous organic cages,C-H···πmicroporous crystals,supramolecular organic frameworks,π-organic frameworks,halogen-bonded organic framework,and intrinsically porous molecular materials.In some porous materials such as zeolites and metal organic frameworks,the integration of multiscale has been adopted to build materials with multifunctionality and optimized properties.Therefore,considering the significant role of hierarchy in porous materials and the growing importance of POMMs in the realm of synthetic porous materials,we consider it appropriate to dedicate for the first time a critical review covering both topics.Herein,we will provide a summary of literature examples showcasing hierarchical POMMs,with a focus on their main synthetic approaches,applications,and the advantages brought forth by introducing hierarchy.展开更多
Organic solar cells(OSCs)have gained conspicuous progress during the past few decades due to the development of materials and upgrading of the device structure.The power conversion efficiency(PCE)of the single-junctio...Organic solar cells(OSCs)have gained conspicuous progress during the past few decades due to the development of materials and upgrading of the device structure.The power conversion efficiency(PCE)of the single-junction device had surpassed 19%.The cathode interface layer(CIL),by optimizing the connection between the active layer and the cathode electrode,has become a momentous part to strengthen the performances of the OSCs.Simultaneously,CIL is also indispensable to illustrating the working mechanism of OSCs and enhancing the stability of the OSCs.In this essay,hybrid CILs in OSCs have been summarized.Firstly,the advancement and operating mechanism of OSCs,and the effects and relevant design rules of CIL are briefly concluded;secondly,the significant influence of CIL on enhancing the stability and PCE of OSCs is presented;thirdly,the characteristics of organic hybrid CIL and organic-inorganic hybrid CIL are introduced.Finally,the conclusion and outlook of CIL are summarized.展开更多
Ploughing and fertilization practices in rice-wheat system have deteriorated the soil carbon (C) pools. Conservation agriculture (CA) based management approaches have proven to enhance C sequestration and reverse the ...Ploughing and fertilization practices in rice-wheat system have deteriorated the soil carbon (C) pools. Conservation agriculture (CA) based management approaches have proven to enhance C sequestration and reverse the loss of soil-organic-carbon (SOC), which further enhances soil fertility. Different fractions of SOC pools react to the alterations in management practices and indicate changes in SOC dynamics as compared to total C in the soil. Higher SOC levels in soil have been observed in case of reduced/no-till (NT) practices than conventional tillage (CT). However, between CT and zero tillage/NT, total SOC stocks diminished with an increase in soil depth, which demonstrated that the benefits of SOC are more pronounced in the topsoil under NT. Soil aggregation provides physical protection to C associated with different-sized particles, thus, the improvement in soil aggregation through CA is an effective way to mitigate soil C loss. Along with less soil disturbance, residual management, suitable crop rotation, rational application of manures and fertilizers, and integrated nutrient management have been found to be effective in not only improving soil C stock but also enhancing the soil health and productivity. Thus, CA can be considered as a potential method in the build-up of SOC of soil in rice-wheat system.展开更多
Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore mic...Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.展开更多
This paper is intended to explore soil organic matter and carbon isotope fractionation at three locations of the Passaic River to determine if microbial degradation of organic contaminants in soil is correlated to the...This paper is intended to explore soil organic matter and carbon isotope fractionation at three locations of the Passaic River to determine if microbial degradation of organic contaminants in soil is correlated to the surrounding physical environment. Microbial degradation of organic contaminants is important for the detoxification of toxic substances thereby minimizing stagnation in the environment and accumulating in the food chain. Since organic contaminants are not easily dissolved in water, they will penetrate sediment and end up enriching the adjacent soil. The hypothesis that we are testing is microbial activity and carbon isotope fractionation will be greater in preserved soils than urban soils. The reason why this is expected to be the case is the expectation of higher microbial activity in preserved environments due to less exposure to pollutants, better soil structure, higher organic matter content, and more favorable conditions for microbial growth. This is contrasted with urban soils, which are impacted by pollutants and disturbances, potentially inhibiting microbial activity. We wish to collect soil samples adjacent to the Passaic River at a pristine location, Great Swamp Wildlife Refuge, a suburban location, Goffle Brook Park, Hawthorne NJ, and an urban location, Paterson NJ. These soil samples will be weighed for soil organic matter (SOM) and weighed for isotope ratio mass spectrometry (IRMS) to test organic carbon isotopes. High SOM and δ13C depletion activity indicate microbial growth based on the characteristics of the soil horizon rather than the location of the soil sample which results in degradation of organic compounds.展开更多
Organic contaminants have posed a direct and substantial risk to human wellness and the environment.In recent years,piezo-electric catalysis has evolved as a novel and effective method for decomposing these contaminan...Organic contaminants have posed a direct and substantial risk to human wellness and the environment.In recent years,piezo-electric catalysis has evolved as a novel and effective method for decomposing these contaminants.Although piezoelectric materials offer a wide range of options,most related studies thus far have focused on inorganic materials and have paid little attention to organic materi-als.Organic materials have advantages,such as being lightweight,inexpensive,and easy to process,over inorganic materials.Therefore,this paper provides a comprehensive review of the progress made in the research on piezoelectric catalysis using organic materials,high-lighting their catalytic efficiency in addressing various pollutants.In addition,the applications of organic materials in piezoelectric cata-lysis for water decomposition to produce hydrogen,disinfect bacteria,treat tumors,and reduce carbon dioxide are presented.Finally,fu-ture developmental trends regarding the piezoelectric catalytic potential of organic materials are explored.展开更多
Colored rice is a type of high-quality,high-added-value rice that has attracted increasing attention in recent years.The use of large amounts of inorganic nitrogen fertilizer in rice fields results in low fertilizer u...Colored rice is a type of high-quality,high-added-value rice that has attracted increasing attention in recent years.The use of large amounts of inorganic nitrogen fertilizer in rice fields results in low fertilizer use efficiency and high environmental pollution.Organic fertilizer is a promising way to improve soil quality and sustain high yields.However,most studies focus on the effect of animal-based organic fertilizers.The effects of different ratios of plantbased organic fertilizer and inorganic fertilizer on the grain yield and quality of colored rice have rarely been reported.Therefore,a two-year field experiment was conducted in 2020 and 2021 to study the effects of replacing inorganic N fertilizers with plant-based organic fertilizers on the yield,nitrogen use efficiency(NUE),and anthocyanin content of two colored rice varieties in a tropical region in China.The experimental treatments included no nitrogen fertilization(T1),100% inorganic nitrogen fertilizer(T2),30%inorganic nitrogen fertilizer substitution with plant-based organic fertilizer(T3),60%inorganic nitrogen fertilizer substitution with plant-based organic fertilizer(T4),and 100% plantbased organic fertilizer(T5).The total nitrogen provided to all the treatments except T1 was the same at 120 kg ha-1.Our results showed that the T3 treatment enhanced the grain yield and anthocyanin content of colored rice by increasing nitrogen use efficiency compared with T2.On average,grain yields were increased by 9 and 8%,while the anthocyanin content increased by 16 and 10% in the two colored rice varieties under T3 across the two years,respectively,as compared with T2.Further study of the residual effect of partial substitution of inorganic fertilizers showed that the substitution of inorganic fertilizer with plant-based organic fertilizer improved the soil physiochemical properties,and thus increased the rice grain yield,in the subsequent seasons.The highest grain yield of the subsequent rice crop was observed under the T5 treatment.Our results suggested that the application of plantbased organic fertilizers can sustain the production of colored rice with high anthocyanin content in tropical regions,which is beneficial in reconciling the relationship between rice production and environmental protection.展开更多
SR-AOP(sulfate radical advanced oxidation process)is a novel water treatment method able to eliminate refractory organic pollutants.Hydrodynamic cavitation(HC)is a novel green technology,that can effectively produce s...SR-AOP(sulfate radical advanced oxidation process)is a novel water treatment method able to eliminate refractory organic pollutants.Hydrodynamic cavitation(HC)is a novel green technology,that can effectively produce strong oxidizing sulfate radicals.This paper presents a comprehensive review of the research advancements in these fields and a critical discussion of the principal factors influencing HC-enhanced SR-AOP and the mechanisms of synergistic degradation.Furthermore,some insights into the industrial application of HC/PS are also provided.Current research shows that this technology is feasible at the laboratory stage,but its application on larger scales requires further understanding and exploration.In this review,some attention is also paid to the design of the hydrodynamic cavitation reactor and the related operating parameters.展开更多
Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in superca...Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.展开更多
Phenazine-based non-fullerene acceptors(NFAs)have demonstrated great potential in improving the power conversion efficiency(PCE)of organic solar cells(OSCs).Halogenation is known to be an effective strategy for increa...Phenazine-based non-fullerene acceptors(NFAs)have demonstrated great potential in improving the power conversion efficiency(PCE)of organic solar cells(OSCs).Halogenation is known to be an effective strategy for increasing optical absorption,refining energy levels,and improving molecular packing in organic semiconductors.Herein,a series of NFAs(Pz IC-4H,Pz IC-4F,Pz IC-4Cl,Pz IC-2Br)with phenazine as the central core and with/without halogen-substituted(dicyanomethylidene)-indan-1-one(IC)as the electron-accepting end group were synthesized,and the effect of end group matched phenazine central unit on the photovoltaic performance was systematically studied.Synergetic photophysical and morphological analyses revealed that the PM6:Pz IC-4F blend involves efficient exciton dissociation,higher charge collection and transfer rates,better crystallinity,and optimal phase separation.Therefore,OSCs based on PM6:Pz IC-4F as the active layer exhibited a PCE of 16.48%with an open circuit voltage(Voc)and energy loss of 0.880 V and 0.53 e V,respectively.Accordingly,this work demonstrated a promising approach by designing phenazine-based NFAs for achieving high-performance OSCs.展开更多
Investigating the characteristics and transformation of water-soluble carbonaceous matter in the cryosphere regions is important for understanding biogeochemical process in the earth system.Water-soluble carbonaceous ...Investigating the characteristics and transformation of water-soluble carbonaceous matter in the cryosphere regions is important for understanding biogeochemical process in the earth system.Water-soluble carbonaceous matter is a heterogeneous mixture of organic compounds that is soluble in aquatic environments.Despite its importance,we still lack systematic understanding for dissolved organic carbon(DOC)in several aspects including exact chemical composition and physical interactions with microorganisms,glacier meltwater.This review presents the chemical composition and physical properties of glacier DOC deposited through anthropogenic emission,terrestrial,and biogenic sources.We present the molecular composition of DOC and its effect over snow albedo and associated radiative forcings.Results indicate that DOC in snow/ice is made up of aromatic protein-like species,fulvic acid-like materials,and humic acid-like materials.Light-absorbing impurities in surface snow and glacier ice cause considerable albedo reduction and the associated radiative forcing is definitely positive.Water-soluble carbonaceous matter dominated the carbon transport in the high-altitude glacial area.Owing to prevailing global warming and projected increase in carbon emission,the glacial DOC is expected to release,which will have strong underlying impacts on cryosphere ecosystem.The results of this work have profound implications for better understanding the carbon cycle in high altitude cryosphere regions.A new compilation of globally distributed work is required,including large-scale measurements of glacial DOC over high-altitude cryosphere regions,to overcome and address the scientific challenges to constrain climate impacts of light-absorbing impurities related processes in Earth system and climate models.展开更多
Biochar is widely used to improve soil physical properties and carbon sequestration. However, few studies focuse on the impact of maize stalk biochar on labile organic carbon(LOC) pool and the relationship between phy...Biochar is widely used to improve soil physical properties and carbon sequestration. However, few studies focuse on the impact of maize stalk biochar on labile organic carbon(LOC) pool and the relationship between physical properties and LOC fractions. A field positioning experiment was performed in Mollisols region of Northeast China to evaluate the influence of maize stalk biochar on the spatial distribution and temporal changes of physical properties and LOC fractions. Maize stalk biochar treatments included C1(1.5 kg·hm^(-2)), C2(3 kg·hm^(-2)), C3(15 kg·hm^(-2)), C4(30 kg·hm^(-2)), and CK(0). The results showed that maize stalk biochar increased soil water contents(SWC) and soil porosity(SP), but reduced bulk density(BD). Maize stalk biochar reduced dissolved organic carbon(DOC) contents in the 0-20 cm soil layer, ranging from 0.25 g·kg^(-1) to 0.31 g·kg^(-1) in harvest period, while increased in the 20-40 cm soil layer. In addition, the application of biochar had a significant impact on the spatial distribution and temporal change of SWC, BD, SP, DOC, hot-water extractable carbon(HWC), acid hydrolyzed organic carbon(AHC Ⅰ, Ⅱ), and readily oxidized organic carbon(ROC). High amounts of maize stalk biochar up-regulated the contents of soil organic carbon SOC, HWC, AHC Ⅰ, AHC Ⅱ, and ROC. In addition, SWC and SP were the key physical factors to affect LOC fractions. In conclusions, maize stalk biochar could improve physical properties, and then influence LOC fractions, and maize stalk biochar could be used as an organic amendment for restoring degraded soils governed by their rates of addition.展开更多
Designing novel nonfullerene acceptors(NFAs)is of vital importance for the development of organic solar cells(OSC).Modification on the side chain and end group are two powerful tools to construct efficient NFAs.Here,b...Designing novel nonfullerene acceptors(NFAs)is of vital importance for the development of organic solar cells(OSC).Modification on the side chain and end group are two powerful tools to construct efficient NFAs.Here,based on the high-performance L8BO,we selected 3-ethylheptyl to substitute the inner chain of 2-ethylhexyl,obtaining the backbone of BON3.Then we introduced different halogen atoms of fluorine and chlorine on 2-(3-oxo-2,3-dihydro-1Hinden-1-ylidene)malononitrile end group(EG)to construct efficient NFAs named BON3-F and BON3-Cl,respectively.Polymer donor D18 was chosen to combine with two novel NFAs to construct OSC devices.Impressively,D18:BON3-Cl-based device shows a remarkable power conversion efficiency(PCE)of 18.57%,with a high open-circuit voltage(V_(OC))of 0.907 V and an excellent fill factor(FF)of 80.44%,which is one of the highest binary PCE of devices based on D18 as the donor.However,BON3-F-based device shows a relatively lower PCE of 17.79%with a decreased FF of 79.05%.The better photovoltaic performance is mainly attributed to the red-shifted absorption,higher electron and hole mobilities,reduced charge recombination,and enhanced molecular packing in the D18:BON3-Cl films.Also,we performed stability tests on two binary systems;the D18:BON3-Cl and D18:BON3-F devices maintain 88.1%and 85.5%of their initial efficiencies after 169 h of storage at 85°C in an N2-filled glove box,respectively.Our work demonstrates the importance of selecting halogen atoms on EG and provides an efficient binary system of D18:BON3-Cl for further improvement of PCE.展开更多
Lacustrine shale oil and gas are important fields for unconventional exploration and development in China,and organic-rich shale deposition lays down the critical foundation for hydrocarbon generation.There are two se...Lacustrine shale oil and gas are important fields for unconventional exploration and development in China,and organic-rich shale deposition lays down the critical foundation for hydrocarbon generation.There are two sets of shale,the Dongyuemiao and Da’anzhai Members,in the Ziliujing Formation in the Sichuan Basin.To identify the differential enrichment characteristics of organic matter and clarify its controlling factors,geochemical analyses of organic and inorganic geochemical analyses were performed.The results showed that the total organic carbon content of the Dongyuemiao shale(1.36%)is slightly higher than that of the Da’anzhai shale(0.95%).The enrichment of organic matter in the two shales resulted from the comprehensive controls of paleoproductivity,paleoenvironment,and terrigenous input,but different factors have different effects.In addition,driven by climate,the change in the sulfate concentration in the bottom water further led to the different intensities of bacterial sulfate reduction in early diagenesis.This made a great difference regarding organic matter accumulation in the two members.In general,climate may have played a dominant role in organic matter enrichment in the two sets of shale.展开更多
BACKGROUND Volatile organic compounds(VOCs)are a promising potential biomarker that may be able to identify the presence of cancers.AIM To identify exhaled breath VOCs that distinguish pancreatic ductal adenocar-cinom...BACKGROUND Volatile organic compounds(VOCs)are a promising potential biomarker that may be able to identify the presence of cancers.AIM To identify exhaled breath VOCs that distinguish pancreatic ductal adenocar-cinoma(PDAC)from intraductal papillary mucinous neoplasm(IPMN)and healthy volunteers.METHODS We collected exhaled breath from histologically proven PDAC patients,radiological diagnosis IPMN,and healthy volunteers using the ReCIVA®device between 10/2021-11/2022.VOCs were identified by thermal desorption-gas chromatography/field-asymmetric ion mobility spectrometry and compared between groups.RESULTS A total of 156 participants(44%male,mean age 62.6±10.6)were enrolled(54 PDAC,42 IPMN,and 60 controls).Among the nine VOCs identified,two VOCs that showed differences between groups were dimethyl sulfide[0.73 vs 0.74 vs 0.94 arbitrary units(AU),respectively;P=0.008]and acetone dimers(3.95 vs 4.49 vs 5.19 AU,respectively;P<0.001).After adjusting for the imbalance parameters,PDAC showed higher dimethyl sulfide levels than the control and IPMN groups,with adjusted odds ratio(aOR)of 6.98(95%CI:1.15-42.17)and 4.56(1.03-20.20),respectively(P<0.05 both).Acetone dimer levels were also higher in PDAC compared to controls and IPMN(aOR:5.12(1.80-14.57)and aOR:3.35(1.47-7.63),respectively(P<0.05 both).Acetone dimer,but not dimethyl sulfide,performed better than CA19-9 in PDAC diagnosis(AUROC 0.910 vs 0.796).The AUROC of acetone dimer increased to 0.936 when combined with CA19-9,which was better than CA19-9 alone(P<0.05).CONCLUSION Dimethyl sulfide and acetone dimer are VOCs that potentially distinguish PDAC from IPMN and healthy participants.Additional prospective studies are required to validate these findings.展开更多
With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices....With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.展开更多
Adjusting agronomic measures to alleviate the kernel position effect in maize is important for ensuring high yields.In order to clarify whether the combined application of organic fertilizer and chemical fertilizer(CA...Adjusting agronomic measures to alleviate the kernel position effect in maize is important for ensuring high yields.In order to clarify whether the combined application of organic fertilizer and chemical fertilizer(CAOFCF)can alleviate the kernel position effect of summer maize,field experiments were conducted during the 2019 and 2020 growing seasons,and five treatments were assessed:CF,100%chemical fertilizer;OFCF1,15%organic fertilizer+85%chemical fertilizer;OFCF2,30%organic fertilizer+70%chemical fertilizer;OFCF3,45%organic fertilizer+55%chemical fertilizer;and OFCF4,60%organic fertilizer+40%chemical fertilizer.Compared with the CF treatment,the OFCF1 and OFCF2 treatments significantly alleviated the kernel position effect by increasing the weight ratio of inferior kernels to superior kernels and reducing the weight gap between the superior and inferior kernels.These effects were largely due to the improved filling and starch accumulation of inferior kernels.However,there were no obvious differences in the kernel position effect among plants treated with CF,OFCF3,or OFCF4 in most cases.Leaf area indexes,post-silking photosynthetic rates,and net assimilation rates were higher in plants treated with OFCF1 or OFCF2 than in those treated with CF,reflecting an enhanced photosynthetic capacity and improved postsilking dry matter accumulation(DMA)in the plants treated with OFCF1 or OFCF2.Compared with the CF treatment,the OFCF1 and OFCF2 treatments increased post-silking N uptake by 66.3 and 75.5%,respectively,which was the major factor driving post-silking photosynthetic capacity and DMA.Moreover,the increases in root DMA and zeatin riboside content observed following the OFCF1 and OFCF2 treatments resulted in reduced root senescence,which is associated with an increased post-silking N uptake.Analyses showed that post-silking N uptake,DMA,and grain yield in summer maize were negatively correlated with the kernel position effect.In conclusion,the combined application of 15-30%organic fertilizer and 70-85%chemical fertilizer alleviated the kernel position effect in summer maize by improving post-silking N uptake and DMA.These results provide new insights into how CAOFCF can be used to improve maize productivity.展开更多
The Southern Ocean is an important carbon sink pool and plays a critical role in the global carbon cycling.The Amundsen Sea was reported to be highly productive in inshore area in the Southern Ocean.In order to invest...The Southern Ocean is an important carbon sink pool and plays a critical role in the global carbon cycling.The Amundsen Sea was reported to be highly productive in inshore area in the Southern Ocean.In order to investigate the influence of transparent exopolymer particles(TEP)on the behavior of dissolved organic carbon(DOC)in this region,a comprehensive study was conducted,encompassing both open water areas and highly productive polynyas.It was found that microbial heterotrophic metabolism is the primary process responsible for the production of humic-like fluorescent components in the open ocean.The relationship between apparent oxygen utilization and the two humic-like components can be accurately described by a power-law function,with a conversion rate consistent with that observed globally.The presence of TEP was found to have little impact on this process.Additionally,the study revealed the accumulation of DOC at the sea surface in the Amundsen Sea Polynya,suggesting that TEP may play a critical role in this phenomenon.These findings contribute to a deeper understanding of the dynamics and surface accumulation of DOC in the Amundsen Sea Polynya,and provide valuable insights into the carbon cycle in this region.展开更多
Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy...Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.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
基金the MICINN (Spain)(Projects PID2019-104778GB-I00, PID2020-115100GB-I00Excellence Unit “Maria de Maeztu” CEX2019-000919-M)+5 种基金the Royal Society of Chemistryfunded by Generalitat Valenciana(PROMETEU/2021/054 and SEJI/2020/034)the “Ramón y Cajal” program (RYC2019-027940-I)the Royal Society (RGSR1221390)Royal Society of Chemistry (R21-5119312833) for the funding.
文摘Porous organic molecular materials(POMMs)are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks,mainly held by non-covalent interactions.POMMs represent a variety of chemical families,such as hydrogen-bonded organic frameworks,porous organic salts,porous organic cages,C-H···πmicroporous crystals,supramolecular organic frameworks,π-organic frameworks,halogen-bonded organic framework,and intrinsically porous molecular materials.In some porous materials such as zeolites and metal organic frameworks,the integration of multiscale has been adopted to build materials with multifunctionality and optimized properties.Therefore,considering the significant role of hierarchy in porous materials and the growing importance of POMMs in the realm of synthetic porous materials,we consider it appropriate to dedicate for the first time a critical review covering both topics.Herein,we will provide a summary of literature examples showcasing hierarchical POMMs,with a focus on their main synthetic approaches,applications,and the advantages brought forth by introducing hierarchy.
基金supported by the National Natural Science Foundation of China(52263017,21965023,52173170,51973087,and22065025)the Science Fund for Distinguished Young Scholars of Jiangxi Province(20212ACB214009)+2 种基金the Natural Science Foundation of Jiangxi Province(20212ACB203010,20224BAB214007 and20212BAB204052)the Training Project of High-level and Highskilled Leading Talents of Jiangxi Province(2023)the Thousand Talents Plan of Jiangxi Province(jxsq2019201004 and jxsq2020101068)。
文摘Organic solar cells(OSCs)have gained conspicuous progress during the past few decades due to the development of materials and upgrading of the device structure.The power conversion efficiency(PCE)of the single-junction device had surpassed 19%.The cathode interface layer(CIL),by optimizing the connection between the active layer and the cathode electrode,has become a momentous part to strengthen the performances of the OSCs.Simultaneously,CIL is also indispensable to illustrating the working mechanism of OSCs and enhancing the stability of the OSCs.In this essay,hybrid CILs in OSCs have been summarized.Firstly,the advancement and operating mechanism of OSCs,and the effects and relevant design rules of CIL are briefly concluded;secondly,the significant influence of CIL on enhancing the stability and PCE of OSCs is presented;thirdly,the characteristics of organic hybrid CIL and organic-inorganic hybrid CIL are introduced.Finally,the conclusion and outlook of CIL are summarized.
文摘Ploughing and fertilization practices in rice-wheat system have deteriorated the soil carbon (C) pools. Conservation agriculture (CA) based management approaches have proven to enhance C sequestration and reverse the loss of soil-organic-carbon (SOC), which further enhances soil fertility. Different fractions of SOC pools react to the alterations in management practices and indicate changes in SOC dynamics as compared to total C in the soil. Higher SOC levels in soil have been observed in case of reduced/no-till (NT) practices than conventional tillage (CT). However, between CT and zero tillage/NT, total SOC stocks diminished with an increase in soil depth, which demonstrated that the benefits of SOC are more pronounced in the topsoil under NT. Soil aggregation provides physical protection to C associated with different-sized particles, thus, the improvement in soil aggregation through CA is an effective way to mitigate soil C loss. Along with less soil disturbance, residual management, suitable crop rotation, rational application of manures and fertilizers, and integrated nutrient management have been found to be effective in not only improving soil C stock but also enhancing the soil health and productivity. Thus, CA can be considered as a potential method in the build-up of SOC of soil in rice-wheat system.
基金This research was supported by Natural Science Foundation of Jiangsu Province(BK20220405)National Natural Science Foundation of China(21834004,22276100,22304086)+5 种基金Key Laboratory for Organic Electronics&Information Displays,NJUPT(GZR2022010010,GZR2023010045)Nanjing Science and Technology Innovation Project for Chinese Scholars Studying Abroad(NJKCZYZZ2022-01)Research Fund for Jiangsu Distinguished Professor(RK030STP22001)Natural Science Research Start-up Foundation of Recruiting Talents of NJUPT(NY221006,NY223051)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB150025)State Key Laboratory of Analytical Chemistry for Life Science,Nanjing University(SKLACLS2311).
文摘Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.
文摘This paper is intended to explore soil organic matter and carbon isotope fractionation at three locations of the Passaic River to determine if microbial degradation of organic contaminants in soil is correlated to the surrounding physical environment. Microbial degradation of organic contaminants is important for the detoxification of toxic substances thereby minimizing stagnation in the environment and accumulating in the food chain. Since organic contaminants are not easily dissolved in water, they will penetrate sediment and end up enriching the adjacent soil. The hypothesis that we are testing is microbial activity and carbon isotope fractionation will be greater in preserved soils than urban soils. The reason why this is expected to be the case is the expectation of higher microbial activity in preserved environments due to less exposure to pollutants, better soil structure, higher organic matter content, and more favorable conditions for microbial growth. This is contrasted with urban soils, which are impacted by pollutants and disturbances, potentially inhibiting microbial activity. We wish to collect soil samples adjacent to the Passaic River at a pristine location, Great Swamp Wildlife Refuge, a suburban location, Goffle Brook Park, Hawthorne NJ, and an urban location, Paterson NJ. These soil samples will be weighed for soil organic matter (SOM) and weighed for isotope ratio mass spectrometry (IRMS) to test organic carbon isotopes. High SOM and δ13C depletion activity indicate microbial growth based on the characteristics of the soil horizon rather than the location of the soil sample which results in degradation of organic compounds.
基金the National Natural Science Foundation of China(No.22179108)the Key Research and Development Projects of Shaanxi Province,China(No.2020GXLH-Z-032)+2 种基金the Doctoral Re-search Start-up Fund project of Xi’an Polytechnic University(No.107020589)the Shaanxi Provincial High-Level Talents Introduction Project(Youth Talent Fund)the Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province,China(No.22567627H).
文摘Organic contaminants have posed a direct and substantial risk to human wellness and the environment.In recent years,piezo-electric catalysis has evolved as a novel and effective method for decomposing these contaminants.Although piezoelectric materials offer a wide range of options,most related studies thus far have focused on inorganic materials and have paid little attention to organic materi-als.Organic materials have advantages,such as being lightweight,inexpensive,and easy to process,over inorganic materials.Therefore,this paper provides a comprehensive review of the progress made in the research on piezoelectric catalysis using organic materials,high-lighting their catalytic efficiency in addressing various pollutants.In addition,the applications of organic materials in piezoelectric cata-lysis for water decomposition to produce hydrogen,disinfect bacteria,treat tumors,and reduce carbon dioxide are presented.Finally,fu-ture developmental trends regarding the piezoelectric catalytic potential of organic materials are explored.
基金supported by the National Natural Science Foundation of China(32060430 and 31971840)the Research Initiation Fund of Hainan University,China(KYQD(ZR)19104)。
文摘Colored rice is a type of high-quality,high-added-value rice that has attracted increasing attention in recent years.The use of large amounts of inorganic nitrogen fertilizer in rice fields results in low fertilizer use efficiency and high environmental pollution.Organic fertilizer is a promising way to improve soil quality and sustain high yields.However,most studies focus on the effect of animal-based organic fertilizers.The effects of different ratios of plantbased organic fertilizer and inorganic fertilizer on the grain yield and quality of colored rice have rarely been reported.Therefore,a two-year field experiment was conducted in 2020 and 2021 to study the effects of replacing inorganic N fertilizers with plant-based organic fertilizers on the yield,nitrogen use efficiency(NUE),and anthocyanin content of two colored rice varieties in a tropical region in China.The experimental treatments included no nitrogen fertilization(T1),100% inorganic nitrogen fertilizer(T2),30%inorganic nitrogen fertilizer substitution with plant-based organic fertilizer(T3),60%inorganic nitrogen fertilizer substitution with plant-based organic fertilizer(T4),and 100% plantbased organic fertilizer(T5).The total nitrogen provided to all the treatments except T1 was the same at 120 kg ha-1.Our results showed that the T3 treatment enhanced the grain yield and anthocyanin content of colored rice by increasing nitrogen use efficiency compared with T2.On average,grain yields were increased by 9 and 8%,while the anthocyanin content increased by 16 and 10% in the two colored rice varieties under T3 across the two years,respectively,as compared with T2.Further study of the residual effect of partial substitution of inorganic fertilizers showed that the substitution of inorganic fertilizer with plant-based organic fertilizer improved the soil physiochemical properties,and thus increased the rice grain yield,in the subsequent seasons.The highest grain yield of the subsequent rice crop was observed under the T5 treatment.Our results suggested that the application of plantbased organic fertilizers can sustain the production of colored rice with high anthocyanin content in tropical regions,which is beneficial in reconciling the relationship between rice production and environmental protection.
文摘SR-AOP(sulfate radical advanced oxidation process)is a novel water treatment method able to eliminate refractory organic pollutants.Hydrodynamic cavitation(HC)is a novel green technology,that can effectively produce strong oxidizing sulfate radicals.This paper presents a comprehensive review of the research advancements in these fields and a critical discussion of the principal factors influencing HC-enhanced SR-AOP and the mechanisms of synergistic degradation.Furthermore,some insights into the industrial application of HC/PS are also provided.Current research shows that this technology is feasible at the laboratory stage,but its application on larger scales requires further understanding and exploration.In this review,some attention is also paid to the design of the hydrodynamic cavitation reactor and the related operating parameters.
基金We are grateful to National Natural Science Foundation of China(Grant No.22375056,52272163)the Key R&D Program of Hebei(Grant No.216Z1201G)+1 种基金Natural Science Foundation of Hebei Province(Grant No.E2022208066,B2021208014)Key R&D Program of Hebei Technological Innovation Center of Chiral Medicine(Grant No.ZXJJ20220105).
文摘Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.
基金financially supported by the National Natural Science Foundation of China (22279152,U21A20331)the National Science Fund for Distinguished Young Scholars (21925506)+1 种基金the Ningbo key scientific and technological project (2022Z117)the Ningbo Natural Science Foundation (2021J192)。
文摘Phenazine-based non-fullerene acceptors(NFAs)have demonstrated great potential in improving the power conversion efficiency(PCE)of organic solar cells(OSCs).Halogenation is known to be an effective strategy for increasing optical absorption,refining energy levels,and improving molecular packing in organic semiconductors.Herein,a series of NFAs(Pz IC-4H,Pz IC-4F,Pz IC-4Cl,Pz IC-2Br)with phenazine as the central core and with/without halogen-substituted(dicyanomethylidene)-indan-1-one(IC)as the electron-accepting end group were synthesized,and the effect of end group matched phenazine central unit on the photovoltaic performance was systematically studied.Synergetic photophysical and morphological analyses revealed that the PM6:Pz IC-4F blend involves efficient exciton dissociation,higher charge collection and transfer rates,better crystallinity,and optimal phase separation.Therefore,OSCs based on PM6:Pz IC-4F as the active layer exhibited a PCE of 16.48%with an open circuit voltage(Voc)and energy loss of 0.880 V and 0.53 e V,respectively.Accordingly,this work demonstrated a promising approach by designing phenazine-based NFAs for achieving high-performance OSCs.
基金supported by the second Tibetan Plateau Scientific Expedition and Research Program(STEP)(2019QZKK0605)the National Natural Science Foundation of China(41971080)the support of Youth Innovation Promotion Association CAS(2021429)。
文摘Investigating the characteristics and transformation of water-soluble carbonaceous matter in the cryosphere regions is important for understanding biogeochemical process in the earth system.Water-soluble carbonaceous matter is a heterogeneous mixture of organic compounds that is soluble in aquatic environments.Despite its importance,we still lack systematic understanding for dissolved organic carbon(DOC)in several aspects including exact chemical composition and physical interactions with microorganisms,glacier meltwater.This review presents the chemical composition and physical properties of glacier DOC deposited through anthropogenic emission,terrestrial,and biogenic sources.We present the molecular composition of DOC and its effect over snow albedo and associated radiative forcings.Results indicate that DOC in snow/ice is made up of aromatic protein-like species,fulvic acid-like materials,and humic acid-like materials.Light-absorbing impurities in surface snow and glacier ice cause considerable albedo reduction and the associated radiative forcing is definitely positive.Water-soluble carbonaceous matter dominated the carbon transport in the high-altitude glacial area.Owing to prevailing global warming and projected increase in carbon emission,the glacial DOC is expected to release,which will have strong underlying impacts on cryosphere ecosystem.The results of this work have profound implications for better understanding the carbon cycle in high altitude cryosphere regions.A new compilation of globally distributed work is required,including large-scale measurements of glacial DOC over high-altitude cryosphere regions,to overcome and address the scientific challenges to constrain climate impacts of light-absorbing impurities related processes in Earth system and climate models.
基金Supported by the National Natural Science Foundation of China Project(31770582)。
文摘Biochar is widely used to improve soil physical properties and carbon sequestration. However, few studies focuse on the impact of maize stalk biochar on labile organic carbon(LOC) pool and the relationship between physical properties and LOC fractions. A field positioning experiment was performed in Mollisols region of Northeast China to evaluate the influence of maize stalk biochar on the spatial distribution and temporal changes of physical properties and LOC fractions. Maize stalk biochar treatments included C1(1.5 kg·hm^(-2)), C2(3 kg·hm^(-2)), C3(15 kg·hm^(-2)), C4(30 kg·hm^(-2)), and CK(0). The results showed that maize stalk biochar increased soil water contents(SWC) and soil porosity(SP), but reduced bulk density(BD). Maize stalk biochar reduced dissolved organic carbon(DOC) contents in the 0-20 cm soil layer, ranging from 0.25 g·kg^(-1) to 0.31 g·kg^(-1) in harvest period, while increased in the 20-40 cm soil layer. In addition, the application of biochar had a significant impact on the spatial distribution and temporal change of SWC, BD, SP, DOC, hot-water extractable carbon(HWC), acid hydrolyzed organic carbon(AHC Ⅰ, Ⅱ), and readily oxidized organic carbon(ROC). High amounts of maize stalk biochar up-regulated the contents of soil organic carbon SOC, HWC, AHC Ⅰ, AHC Ⅱ, and ROC. In addition, SWC and SP were the key physical factors to affect LOC fractions. In conclusions, maize stalk biochar could improve physical properties, and then influence LOC fractions, and maize stalk biochar could be used as an organic amendment for restoring degraded soils governed by their rates of addition.
基金supported by the National Natural Science Foundation of China(No.U21A20331)the National Science Fund for Distinguished Young Scholars(No.21925506)+3 种基金Zhejiang Provincial Natural Science Foundation of China(No.LQ22E030013)Ningbo Key Scientific and Technological Project(2022Z117)Ningbo Public Welfare Science and Technology Planning Project(2021S149)ZBTI Scientific Research Innovation Team(KYTD202105).
文摘Designing novel nonfullerene acceptors(NFAs)is of vital importance for the development of organic solar cells(OSC).Modification on the side chain and end group are two powerful tools to construct efficient NFAs.Here,based on the high-performance L8BO,we selected 3-ethylheptyl to substitute the inner chain of 2-ethylhexyl,obtaining the backbone of BON3.Then we introduced different halogen atoms of fluorine and chlorine on 2-(3-oxo-2,3-dihydro-1Hinden-1-ylidene)malononitrile end group(EG)to construct efficient NFAs named BON3-F and BON3-Cl,respectively.Polymer donor D18 was chosen to combine with two novel NFAs to construct OSC devices.Impressively,D18:BON3-Cl-based device shows a remarkable power conversion efficiency(PCE)of 18.57%,with a high open-circuit voltage(V_(OC))of 0.907 V and an excellent fill factor(FF)of 80.44%,which is one of the highest binary PCE of devices based on D18 as the donor.However,BON3-F-based device shows a relatively lower PCE of 17.79%with a decreased FF of 79.05%.The better photovoltaic performance is mainly attributed to the red-shifted absorption,higher electron and hole mobilities,reduced charge recombination,and enhanced molecular packing in the D18:BON3-Cl films.Also,we performed stability tests on two binary systems;the D18:BON3-Cl and D18:BON3-F devices maintain 88.1%and 85.5%of their initial efficiencies after 169 h of storage at 85°C in an N2-filled glove box,respectively.Our work demonstrates the importance of selecting halogen atoms on EG and provides an efficient binary system of D18:BON3-Cl for further improvement of PCE.
基金This work was funded by the National Natural Science Foundation of China(Grant No.42002139 and U20B6001)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA14010404).
文摘Lacustrine shale oil and gas are important fields for unconventional exploration and development in China,and organic-rich shale deposition lays down the critical foundation for hydrocarbon generation.There are two sets of shale,the Dongyuemiao and Da’anzhai Members,in the Ziliujing Formation in the Sichuan Basin.To identify the differential enrichment characteristics of organic matter and clarify its controlling factors,geochemical analyses of organic and inorganic geochemical analyses were performed.The results showed that the total organic carbon content of the Dongyuemiao shale(1.36%)is slightly higher than that of the Da’anzhai shale(0.95%).The enrichment of organic matter in the two shales resulted from the comprehensive controls of paleoproductivity,paleoenvironment,and terrigenous input,but different factors have different effects.In addition,driven by climate,the change in the sulfate concentration in the bottom water further led to the different intensities of bacterial sulfate reduction in early diagenesis.This made a great difference regarding organic matter accumulation in the two members.In general,climate may have played a dominant role in organic matter enrichment in the two sets of shale.
基金The study protocol was reviewed and approved by the Institutional Research Committee,Faculty of Medicine,Chulalongkorn University(No.0482/65)registered in the Thai Clinical Trials Registry(TCTR20211109002).
文摘BACKGROUND Volatile organic compounds(VOCs)are a promising potential biomarker that may be able to identify the presence of cancers.AIM To identify exhaled breath VOCs that distinguish pancreatic ductal adenocar-cinoma(PDAC)from intraductal papillary mucinous neoplasm(IPMN)and healthy volunteers.METHODS We collected exhaled breath from histologically proven PDAC patients,radiological diagnosis IPMN,and healthy volunteers using the ReCIVA®device between 10/2021-11/2022.VOCs were identified by thermal desorption-gas chromatography/field-asymmetric ion mobility spectrometry and compared between groups.RESULTS A total of 156 participants(44%male,mean age 62.6±10.6)were enrolled(54 PDAC,42 IPMN,and 60 controls).Among the nine VOCs identified,two VOCs that showed differences between groups were dimethyl sulfide[0.73 vs 0.74 vs 0.94 arbitrary units(AU),respectively;P=0.008]and acetone dimers(3.95 vs 4.49 vs 5.19 AU,respectively;P<0.001).After adjusting for the imbalance parameters,PDAC showed higher dimethyl sulfide levels than the control and IPMN groups,with adjusted odds ratio(aOR)of 6.98(95%CI:1.15-42.17)and 4.56(1.03-20.20),respectively(P<0.05 both).Acetone dimer levels were also higher in PDAC compared to controls and IPMN(aOR:5.12(1.80-14.57)and aOR:3.35(1.47-7.63),respectively(P<0.05 both).Acetone dimer,but not dimethyl sulfide,performed better than CA19-9 in PDAC diagnosis(AUROC 0.910 vs 0.796).The AUROC of acetone dimer increased to 0.936 when combined with CA19-9,which was better than CA19-9 alone(P<0.05).CONCLUSION Dimethyl sulfide and acetone dimer are VOCs that potentially distinguish PDAC from IPMN and healthy participants.Additional prospective studies are required to validate these findings.
基金R.Ma thanks the support from PolyU Distinguished Postdoc Fellowship(1-YW4C)Z.Luo thanks the National Natural Science Foundation of China(NSFC,No.22309119)+7 种基金J.Wu thanks the Guangdong government and the Guangzhou government for funding(2021QN02C110)the Guangzhou Municipal Science and Technology Project(No.2023A03J0097 and 2023A03J0003)H.Yan appreciates the support from the National Key Research and Development Program of China(No.2019YFA0705900)funded by MOST,the Basic and Applied Research Major Program of Guangdong Province(No.2019B030302007)the Shen Zhen Technology and Innovation Commission through(Shenzhen Fundamental Research Program,JCYJ20200109140801751)the Hong Kong Research Grants Council(research fellow scheme RFS2021-6S05,RIF project R6021-18,CRF project C6023‐19G,GRF project 16310019,16310020,16309221,and 16309822)Hong Kong Innovation and Technology Commission(ITC‐CNERC14SC01)Foshan‐HKUST(Project NO.FSUST19‐CAT0202)Zhongshan Municipal Bureau of Science and Technology(NO.ZSST20SC02)and Tencent Xplorer Prize。
文摘With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.
基金financially supported by the HAAFS Science and Technology Innovation Special Project China(2022KJCXZX-LYS-9)the Natural Science Foundation of Hebei Province China(C2021301004)the Key Research and Dvelopment Program of Hebei Province China(20326401D)。
文摘Adjusting agronomic measures to alleviate the kernel position effect in maize is important for ensuring high yields.In order to clarify whether the combined application of organic fertilizer and chemical fertilizer(CAOFCF)can alleviate the kernel position effect of summer maize,field experiments were conducted during the 2019 and 2020 growing seasons,and five treatments were assessed:CF,100%chemical fertilizer;OFCF1,15%organic fertilizer+85%chemical fertilizer;OFCF2,30%organic fertilizer+70%chemical fertilizer;OFCF3,45%organic fertilizer+55%chemical fertilizer;and OFCF4,60%organic fertilizer+40%chemical fertilizer.Compared with the CF treatment,the OFCF1 and OFCF2 treatments significantly alleviated the kernel position effect by increasing the weight ratio of inferior kernels to superior kernels and reducing the weight gap between the superior and inferior kernels.These effects were largely due to the improved filling and starch accumulation of inferior kernels.However,there were no obvious differences in the kernel position effect among plants treated with CF,OFCF3,or OFCF4 in most cases.Leaf area indexes,post-silking photosynthetic rates,and net assimilation rates were higher in plants treated with OFCF1 or OFCF2 than in those treated with CF,reflecting an enhanced photosynthetic capacity and improved postsilking dry matter accumulation(DMA)in the plants treated with OFCF1 or OFCF2.Compared with the CF treatment,the OFCF1 and OFCF2 treatments increased post-silking N uptake by 66.3 and 75.5%,respectively,which was the major factor driving post-silking photosynthetic capacity and DMA.Moreover,the increases in root DMA and zeatin riboside content observed following the OFCF1 and OFCF2 treatments resulted in reduced root senescence,which is associated with an increased post-silking N uptake.Analyses showed that post-silking N uptake,DMA,and grain yield in summer maize were negatively correlated with the kernel position effect.In conclusion,the combined application of 15-30%organic fertilizer and 70-85%chemical fertilizer alleviated the kernel position effect in summer maize by improving post-silking N uptake and DMA.These results provide new insights into how CAOFCF can be used to improve maize productivity.
基金funded by the National Natural Science Foundation of China(Grant nos.42276255 and 41976227)project“Impact and Response of Antarctic Seas to Climate Change,IRASCC 2020-2022”(Grant nos.01-01-02A and 02-02-05).
文摘The Southern Ocean is an important carbon sink pool and plays a critical role in the global carbon cycling.The Amundsen Sea was reported to be highly productive in inshore area in the Southern Ocean.In order to investigate the influence of transparent exopolymer particles(TEP)on the behavior of dissolved organic carbon(DOC)in this region,a comprehensive study was conducted,encompassing both open water areas and highly productive polynyas.It was found that microbial heterotrophic metabolism is the primary process responsible for the production of humic-like fluorescent components in the open ocean.The relationship between apparent oxygen utilization and the two humic-like components can be accurately described by a power-law function,with a conversion rate consistent with that observed globally.The presence of TEP was found to have little impact on this process.Additionally,the study revealed the accumulation of DOC at the sea surface in the Amundsen Sea Polynya,suggesting that TEP may play a critical role in this phenomenon.These findings contribute to a deeper understanding of the dynamics and surface accumulation of DOC in the Amundsen Sea Polynya,and provide valuable insights into the carbon cycle in this region.
基金funded by the National Key Research and Development Program of China(2018YFA0900702).
文摘Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.
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.
