Polyethylene(PE)and polypropylene(PP)constitute approximately 57% of global polymer production.Their durability,light weight,and low cost have contributed to their wide adoption in various fields and a rapid increase ...Polyethylene(PE)and polypropylene(PP)constitute approximately 57% of global polymer production.Their durability,light weight,and low cost have contributed to their wide adoption in various fields and a rapid increase in their production.However,approximately 90% of these materials are discarded and contribute to global pollution(Fig.1(a)).展开更多
Diacylglycerol(DAG)is a functional oil that can reduce body fat accumulation and postprandial triglycerides.In this study,lipase-catalyzed esterification of oleic acid with glycerol was investigated to elucidate the k...Diacylglycerol(DAG)is a functional oil that can reduce body fat accumulation and postprandial triglycerides.In this study,lipase-catalyzed esterification of oleic acid with glycerol was investigated to elucidate the kinetics and selectivity of each reaction step.1H NMR monitoring revealed equilibrated positional isomerization among acylglycerols:sn-1 monoolein comprised 97.3%of total monoacylglycerols,and sn-1,3 diolein comprised 73.3%of total diacylglycerols.Acyl migration(isomer equilibration)occurred faster than overall esterification.The observed rate constants for successive esterification steps(glycerol→monoacylglycerol,monoacylglycerol→diacylglycerol,diacylglycerol→triacylglycerol)were 0.01068,0.00615,and 0.00304 min^(-1),respectively,indicating progressively slower reaction rates for larger acylglycerol species.Furthermore,molecular distillation at 200–220℃ purified the DAG without altering its fatty acid profile.These findings establish a kinetic model of the three-step esterification and highlight the importance of acyl migration in enzymatic DAG synthesis.展开更多
The agglomeration-prone properties of metal oxide catalysts limit their catalytic efficiency in the isomerization of glucose to fructose.Herein,the hierarchical structure and abundant coordination groups of collagen f...The agglomeration-prone properties of metal oxide catalysts limit their catalytic efficiency in the isomerization of glucose to fructose.Herein,the hierarchical structure and abundant coordination groups of collagen fibers were used to anchor Zr^(4+),and a highly dispersed ZrO_(2)-nitrogen-doped carbon(ZrO_(2)-NC)composite catalyst was subsequently fabricated by calcination.For the catalytic glucose-to-fructose isomerization over ZrO_(2)-NC,fructose was obtained in 41.3%yield and 85.3%selectivity in a water-acetone solvent at 120℃ for 10 min.The electron-deficient environment of ZrO_(2)surface during charge transfer from ZrO_(2)-to-NC layer facilitated the preferential adsorption of glucose,which accelerated glucose isomerization and fructose desorption.The amphoteric catalyst triggered both proton transfer on the Bronsted base sites and the intramolecular hydride shift of glucose on the Lewis acid sites of ZrO_(2)-NC in the mixed solvent.The latter isomerization mechanism depended on the presence of acetone,which lowered the energy barrier and increased fructose yield.展开更多
The study of nuclear isomers can deepen our understanding of nuclear structure and astrophysics.In this work,we have performed the ab initio calculations of isomers in the N=49 isotones.With a chiral two-plus three-nu...The study of nuclear isomers can deepen our understanding of nuclear structure and astrophysics.In this work,we have performed the ab initio calculations of isomers in the N=49 isotones.With a chiral two-plus three-nucleon force,the valence-space effective Hamiltonian was derived using the ab initio many-body perturbation theory named Q-box folded diagrams.The effective operators of electromagnetic operators andβ-decay were obtained using ■-box folded diagrams.With the effective Hamiltonian and operators,we studied the properties of the isomers,gaining a microscopic understanding of the single-particle behaviour of the isomers which we are interested in,showing the reliability of the ab initio calculations.展开更多
As Internet of Things(IoT)applications expand,Mobile Edge Computing(MEC)has emerged as a promising architecture to overcome the real-time processing limitations of mobile devices.Edge-side computation offloading plays...As Internet of Things(IoT)applications expand,Mobile Edge Computing(MEC)has emerged as a promising architecture to overcome the real-time processing limitations of mobile devices.Edge-side computation offloading plays a pivotal role in MEC performance but remains challenging due to complex task topologies,conflicting objectives,and limited resources.This paper addresses high-dimensional multi-objective offloading for serial heterogeneous tasks in MEC.We jointly consider task heterogeneity,high-dimensional objectives,and flexible resource scheduling,modeling the problem as a Many-objective optimization.To solve it,we propose a flexible framework integrating an improved cooperative co-evolutionary algorithm based on decomposition(MOCC/D)and a flexible scheduling strategy.Experimental results on benchmark functions and simulation scenarios show that the proposed method outperforms existing approaches in both convergence and solution quality.展开更多
Three-quasiparticle K-isomeric states in odd-mass N=106 isotones within the A~180 mass region were systematically investigated using configuration-constrained potential energy surface calculations.The calculations suc...Three-quasiparticle K-isomeric states in odd-mass N=106 isotones within the A~180 mass region were systematically investigated using configuration-constrained potential energy surface calculations.The calculations succes sfully reproduced the excitation energies and deformations of the known high-K isomers in nuclei from 175Tm to 181Re.For the nuclei closer to the Z=82 shell closure(^(183)Ir,^(185)Au,and^(187)Tl),predictions of the configurations of the observed and yet-to-be-observed isomers are provided.The results reveal strong shape polarization,where the three-quasiparticle states are driven to larger deformations compared to the often shape-soft or spherical ground states.A particularly rich spectrum of shape coexistence is predicted in^(187)Tl,where several high-K three-quasiparticle configurations with distinct prolate,oblate,and triaxial shapes are found to coexist at similar excitation energies.Notably,the oblate-deformed K^(π)=29/2^(+)configuration at E_(x)=1839 keV was proposed to be responsible for a long-lived isomer.This study provides a comprehensive picture of shape evolution and coexistence in high-K multi-quasiparticle states,offering valuable insights for future experimental studies.展开更多
To establish practical,evidence-based strategies for noninvasive assessment and referral of patients with metabolic dysfunction-associated steatotic liver disease(MASLD)in Japan,we must address the urgent clinical nee...To establish practical,evidence-based strategies for noninvasive assessment and referral of patients with metabolic dysfunction-associated steatotic liver disease(MASLD)in Japan,we must address the urgent clinical need for accurate risk stratification and timely specialist intervention.A panel of 11 Japanese hepatology experts conducted a modified Delphi process to evaluate consensus recommendations regarding the use of noninvasive tests(NITs),including the fibrosis-4 index,enhanced liver fibrosis test,Mac-2-binding protein glycosylation isomer,type IV collagen 7S,cytokeratin-18 fragments,and imaging modalities such as ultrasound elastography and magnetic resonance elastography,for MASLD assessment and clinical referral.Practical algorithms were developed based on current Japanese data and panel consensus.The expert panel validated the utility of NITs as reliable tools for identifying patients with MASLD at risk for advanced fibrosis.Sequential use of NITs improved diagnostic accuracy and referral appropriateness while minimizing unnecessary specialist consultations.The proposed algorithms offer stepwise guidance for primary care physicians,supporting efficient,evidence-based decisionmaking.However,prospective longitudinal studies remain necessary for full prognostic validation of NITs in MASLD management.Noninvasive testing algorithms enable effective risk stratification and referral for MASLD in real-world Japanese practice with anticipated benefit for patient outcomes and healthcare systems.Broader adoption and further validation are warranted.展开更多
1 Introduction Recently,the increasing demand for advanced telecommunication systems has spurred extensive research into bandpass filters(BPFs),with particular emphasis on miniaturization,reduction of insertion loss(I...1 Introduction Recently,the increasing demand for advanced telecommunication systems has spurred extensive research into bandpass filters(BPFs),with particular emphasis on miniaturization,reduction of insertion loss(IL),and enhancement of upper stopband rejection(Huang et al.,2021;Snyder et al.,2021;Lin et al.,2023;Zeng et al.,2023).展开更多
Binuclear complexes have attracted extensive attention in fields such as catalysis because of their likely bimetallic synergistic effect;however,the mechanism and factors influencing this synergism remain unclear.In t...Binuclear complexes have attracted extensive attention in fields such as catalysis because of their likely bimetallic synergistic effect;however,the mechanism and factors influencing this synergism remain unclear.In this work,six bis-β-ketoimine binuclear titanium complexes4a-4f containing different alkylthio sidearms and configurations were synthesized and characterized by nuclear magnetic resonance hydrogen spectrum(~1H-NMR),nuclear magnetic resonance carbon spectrum(^(13)C-NMR),Fourier transform infrared spectrum(FTIR),and elemental analysis.The intermetallic distances of isomeric complexes 4a,4d,4e and 4f determined through density functional theory(DFT)optimization were in the order 4a<4d<4e<4f and were found to significantly influence the catalytic performance for ethylene(co)polymerization.These complexes could efficiently catalyze ethylene polymerization and ethylene/1-hexene or ethylene/1-octene copolymerization with high activity to produce highmolecular-weight ethylene homo-and co-polymers.Among the three binuclear titanium complexes 4a-4c with similar structures but different lengths of alkylthio sidearms,complex 4a,which contained the shortest methylthio sidearm,exhibited the highest activity for ethylene polymerization and copolymerization with 1-hexene or 1-octene.Additionally,for ethylene/1-hexene or ethylene/1-octene copolymerization,it showed the highest comonomer incorporation compared with propylthio(4b)and octylthio(4c)derivatives because of the smaller steric hindrance of the methyl group in 4a and the more open coordination space for vinyl monomers.Furthermore,among the isomeric complexes 4a,4d,4e and4f,complex 4a with the shortest bimetallic distance also exhibited the highest activity towards ethylene(co)polymerization,and the highest 1-hexene or 1-octene incorporation in comparison with its regioisomeric counterparts 4d,4e and p-phenyl-bridged analog 4f,owing to a more appropriate bimetallic distance that is conducive to a synergistic effect.展开更多
The synthesis of Ta-substituted polyoxometalates has always been an attractive but challenging goal.Three novel tantalum-containing 12-tungsto-2-phosphates were successfully prepared using the water bath method.The mo...The synthesis of Ta-substituted polyoxometalates has always been an attractive but challenging goal.Three novel tantalum-containing 12-tungsto-2-phosphates were successfully prepared using the water bath method.The monomer,K_(11)Li[P_(2)W_(12)(TaO_(2))_(6)O_(56)]·19H_(2)O(1),is composed of{P_(2)W_(12)}and 6{Ta(O_(2))}building blocks,similar to[P_(2)W_(12)(NbO_(2))_(6)O_(56)]^(12-).Monomer 1 polymerized to form two cis-trans dimers,K1_(3)Li_(6)H-cis-[P_(2)W_(12)Ta_(4)(TaO_(2))_(2)O_(59)]_(2)·61H_(2)O(2)and KNa_(3)Li_(4)H_(12)-trans-[P_(2)W_(12)Ta_(4)(TaO_(2))_(2)O_(59)]_(2)·37H_(2)O(3).Compounds 1-3 can serve as a structural motif to manufacture additional fascinating molecular clusters,promoting the advancement of POM chemistry.In contrast to[P_(2)W_(12)(NbO_(2))_(6)O_(56)]^(12-),compound 1 exhibits exceptional stability,evidenced by ESI-MS,IR,and NMR spectroscopy.In addition,2 and 3 exhibit high proton conductivity and superior water adsorption properties.展开更多
Six coordination polymers based on 9,10-di(pyridine-4-yl)-anthracene(DPA)and 1,6-di(1H-imidazol-1-yl)pyrene(DIP)were obtained by solvothermal reactions.{[Zn(DPA)Cl_(2)]·DMF·2H_(2)O}n(1)and{[Zn_(1.5)(DPA)_(1....Six coordination polymers based on 9,10-di(pyridine-4-yl)-anthracene(DPA)and 1,6-di(1H-imidazol-1-yl)pyrene(DIP)were obtained by solvothermal reactions.{[Zn(DPA)Cl_(2)]·DMF·2H_(2)O}n(1)and{[Zn_(1.5)(DPA)_(1.5)Cl_(3)]·5H_(2)O}n(2)are framework isomers,which both contain zigzag chains formed by DPA,Zn^(2+),and Cl-.The zigzag chains in 1 are further assembled by C—H…Cl interactions into layers,and these layers exhibit two different orientations,displaying a rare 2D to 3D interpenetration mode.The zigzag chains in 2 are parallelly arranged.{[Zn_(3)(DPA)_(3)Br_(6)]·2DMF·_(1.5)H_(2)O}n(3)is isostructural to 2.3 was obtained using ZnBr_(2)instead of ZnCl_(2).[M(DPA)(formate)_(2)(H_(2)O)_(2)]n[M=Co(4),Cu(5)]are isostructural,contain chain structures formed by DPA,Cu^(2+)/Co^(2+),and for-mate ions,which were formed in situ in the solvothermal reaction.{[Zn(DIP)_(2)Cl]ClO_(4)}n(6)contains a layer structure formed by DIP and Zn^(2+).Free DPA and DIP ligands exhibited high fluorescence at room temperature,and coordina-tion polymers 3 and 6 displayed enhanced fluorescent emissions.展开更多
Fully utilizing renewable biomass energy is important for saving energy,reducing carbon emissions,and mitigating climate change.As the main hydrolysate of cellulose,a primary component of lignocellulose,glucose could ...Fully utilizing renewable biomass energy is important for saving energy,reducing carbon emissions,and mitigating climate change.As the main hydrolysate of cellulose,a primary component of lignocellulose,glucose could be employed as a starting material to prepare some other functional derivatives for improving the value of biomass resources.The isomerization of glucose to produce fructose is an important intermediate process during numerous high-value-added chemical preparations.Therefore,the development of efficient and selective catalysts for glucose isomerization is of great significance.Currently,glucose isomerase catalysts are limited by the harsh conditions required for microbial activity,which restricts further improvements in fructose yield.Additionally,heterogeneous Bronsted-base and Lewis-acid catalysts commonly employed in chemical isomerization methods often lead to the formation of undesirable by-products,resulting in reduced selectivity toward fructose.This study has demonstrated that lithium-loaded heterogeneous catalysts possess excellent isomerization capabilities under mild conditions.A highly efficient Li-C_(3)N_(4) catalyst was developed,achieving a fructose selectivity of 99.9% and a yield of 42.6% at 60℃ within 1.0 h-comparable to the performance of the enzymatic method.Characterization using X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD),proton nuclear magnetic resonance(^(1)H NMR),and inductively coupled plasma(ICP)analyses confirmed that lithium was stably incorporated into the g-C_(3)N_(4) framework through the formation of Li-N bonds.Further investigations using CO_(2) temperature-programmed desorption(CO_(2)-TPD),in situ Fourier-transform infrared spectroscopy(FT-IR)and 7Li magic angle spinning nuclear magnetic resonance(^(7)Li MAS NMR)indicated that the isomerization proceeded via a base-catalyzed mechanism.The Li species were found to interact with hydroxyl groups generated through hydrolysis and simultaneously coordinated with nitrogen atoms in the C_(3)N_(4) matrix,resulting in the formation of Li-N_(6)-H_(2)O active sites.These active sites facilitated the deprotonation of glucose to form an enolate intermediate,followed by a proton transfer step that generated fructose.This mechanism not only improved the efficiency of fructose production but also provided valuable insight into the catalytic role of lithium within the isomerization process.展开更多
Nuclear excitation by electron capture(NEEC)is a fundamental process in nuclear physics.Despite its theoretical framework established nearly half a century ago,the experimental confirmation of NEEC remains elusive bec...Nuclear excitation by electron capture(NEEC)is a fundamental process in nuclear physics.Despite its theoretical framework established nearly half a century ago,the experimental confirmation of NEEC remains elusive because of significant technical challenges.A notable effort to validate NEEC experimentally involved the enhanced ^(93m)Mo isomer-depletion experiment,which was ultimately hindered by substantial noise interference.This mini-review provides a brief historical overview of NEEC studies and explores the role of NEEC processes in astrophysical environments and laser-induced plasmas.Several platforms have been proposed to facilitate the observation of NEEC,including traditional cooling-storage rings,ion accelerators,and electron beam ion traps.These approaches aim to enhance the nuclear excitation rate,thereby improving the signal-to-noise ratio.In addition,the employment of exotic vortex beams is discussed as a potential methodological approach to address these challenges.展开更多
In this study,a pair of dicarboxylic acids as cis-trans isomerism—citraconic acid(CA)and mesaconic acid(MA),was incorporated into polymeric networks of poly(N-isopropylacrylamide)(PNIPAM)-based core-shell microgels v...In this study,a pair of dicarboxylic acids as cis-trans isomerism—citraconic acid(CA)and mesaconic acid(MA),was incorporated into polymeric networks of poly(N-isopropylacrylamide)(PNIPAM)-based core-shell microgels via semi-batch precipitation polymerization.We demonstrated that the pH-temperature dual responsiveness of the core-shell microgels is highly correlated with the structure and position of the acid isomers.Both the cis-trans molecular structure and the crosslinking position of the dicarboxylic acids significantly influenced the hydration capacity and surface charge density of the core-shell microgels.These diverse properties first influenced the swelling behavior,further affecting the interfacial behavior of the microgels,including the oil-water dynamic interfacial tension and air-water compression isotherms.Furthermore,the rheological behavior of the microgel suspensions also displayed distinct dependences on the frequency and temperature,illustrating that the cis-trans molecular structure and crosslinked position of the dicarboxylic acids also significantly influenced the interparticle clustering in the bulk solution.Our results suggest that the pH sensitivity of the cis-trans dicarboxylic acid isomer affects the ionization and surface charge distribution of the core or shell layers of individual microgels,which further determines the interparticle interaction and cooperative rearrangement at interfaces and in the bulk.展开更多
Double bonds of internal olefins can be efficiently migrated to the terminal carbons and regioselectively hydroesterified with formates in the presence of Pd(OAc)_(2) and 1,2-DTBPMB under mild reaction conditions,prov...Double bonds of internal olefins can be efficiently migrated to the terminal carbons and regioselectively hydroesterified with formates in the presence of Pd(OAc)_(2) and 1,2-DTBPMB under mild reaction conditions,providing a wide variety of corresponding linear carboxylic esters bearing various functional groups in good yields and>20:1 linear/branch ratios.The reaction is optionally simple and does not need to use CO gas and acid co-catalysts.展开更多
Organic additives with multiple functional groups have shown great promise in improving the performance and stability of perovskite solar cells.The functional groups can passivate undercoordinated ions to reduce nonra...Organic additives with multiple functional groups have shown great promise in improving the performance and stability of perovskite solar cells.The functional groups can passivate undercoordinated ions to reduce nonradiative recombination losses.However,how these groups synergistically affect the enhancement beyond passivation is still unclear.Specifically,isomeric molecules with different substitution patterns or molecular shapes remain elusive in designing new organic additives.Here,we report two isomeric carbazolyl bisphosphonate additives,2,7-Cz BP and 3,6-Cz BP.The isomerism effect on passivation and charge transport process was studied.The two molecules have similar passivation effects through multiple interactions,e.g.,P=O···Pb,P=O···H–N and N–H···I.2,7-CzBP can further bridge the perovskite crystallites to facilitates charge transport.Power conversion efficiencies(PCEs)of 25.88%and 21.04%were achieved for 0.09 cm^(2)devices and 14 cm^(2)modules after 2,7-Cz BP treatment,respectively.The devices exhibited enhanced operational stability maintaining 95%of initial PCE after 1000 h of continuous maximum power point tracking.This study of isomerism effect hints at the importance of tuning substitution positions and molecular shapes for organic additives,which paves the way for innovation of next-generation multifunctional aromatic additives.展开更多
In recent years,the ternary strategy of adding a vip molecule to the active layer has been proven to be effective for improving the performance of organic solar cells(OSCs).Isomerization engineering of the vip mol...In recent years,the ternary strategy of adding a vip molecule to the active layer has been proven to be effective for improving the performance of organic solar cells(OSCs).Isomerization engineering of the vip molecule is a simple method to increase the amount of promising material,but there are only limited reports,and the structure-property relationships are still unclear.In this work,we synthesized three isomers named BTA5-F-o,BTA5-F-m,and BTA5-F-p,with different fluorine substitution positions,to study the influence of isomerization on the photovoltaic performance.After introducing them as the third components to the classic host system PM6:Y6,all three ternary devices showed improved power conversion efficiency(PCEs)compared to the binary system(PCE of 17.46%).The ternary OSCs based on BTA5-F-o achieved a champion PCE of 19.11%,while BTA5-F-m and BTA5-F-p realized PCEs of 18.65%and 18.45%,respectively.Mechanism studies have shown that the dipole moment of the BTA5-F-o end group is closer to that of the Y6 end group,despite the three isomers with almost identical energy levels and optical properties.It is indicated that the electron attraction ability of BTA5-F-o best matches that of Y6,which leads to the higher charge mobility,less charge recombination,and stronger exciton dissociation and extraction ability in the ternary blend system.This study suggests that rationally adjusting the position of substituents in the terminal group can be an effective way to construct nonfullerene vip acceptors to achieve highly efficient ternary OSCs.展开更多
Aqueous zinc-ion batteries(AZIBs) have garnered significant attention as promising candidates for gridscale energy storage.However,the interfacial instability of zinc anodes caused by the hydrogen evolution reaction(H...Aqueous zinc-ion batteries(AZIBs) have garnered significant attention as promising candidates for gridscale energy storage.However,the interfacial instability of zinc anodes caused by the hydrogen evolution reaction(HER) and aqueous electrolyte corrosion severely restricts their practical implementation.This study introduces 2-mercaptothiazoline(MT) as a dynamic electrolyte additive,leveraging its thiolthione tautomerism for interfacial stabilization.Theoretical calculations and experimental investigations reveal that MT can adsorb onto the zinc surface to form a protective layer to suppress corrosion.Simultaneously,the spatial effect of the thiazoline ring prevents excessive molecular aggregation while enabling homogeneous Zn^(2+) electrodeposition.The electronegativity difference between sulfur and nitrogen atoms induces localized polarization,strengthening electronic interactions with the metal surface to accelerate Zn^(2+) reduction kinetics and inhibit side reactions.Consequently,smooth and low-porosity Zn deposits with enhanced interfacial stability are achieved.The optimized Zn//Zn symmetric cells exhibit extraordinary cycling stability exceeding 1800 h at 0.5 mA cm^(-2),0.5 mAh cm^(-2),while sustaining400 h of operation at 28.5 % depth of discharge(DOD).Zn//MnO_(2) full cells incorporating MT additive maintain 122.6 mAh g^(-1) capacity retention after 500 cycles(1 A g^(-1)).This work provides a facile yet effective strategy for stabilizing Zn metal-based batteries through synergistic interface engineering.展开更多
BACKGROUND Cirrhosis is a progressive condition characterized by fibrosis that can lead to severe complications and increased mortality.The mac-2 binding protein glyco-sylation isomer(M2BPGi)is a prominent biomarker f...BACKGROUND Cirrhosis is a progressive condition characterized by fibrosis that can lead to severe complications and increased mortality.The mac-2 binding protein glyco-sylation isomer(M2BPGi)is a prominent biomarker for predicting hepatocellular carcinoma(HCC)and cirrhosis-induced esophageal varices(EV).AIM To investigate thresholds of M2BPGi associated with HCC,EV,and decomp-ensation in patients with cirrhosis.METHODS This was a prospective study.A total of 153 patients with cirrhosis who met the inclusion criteria were enrolled.The patients were diagnosed with HCC and EV according to the Baveno VII and European Association for the Study of the Liver guidelines.Baseline serum M2BPGi levels were assessed along with other routine tests.The data analysis aimed to determine the cutoff values of M2BPGi for pre-dicting EV and HCC.RESULTS In the study 85.6%of patients were Child-Pugh B and C.M2BPGi mean cutoff index was 7.1±3.7,showing no significant etiological differences.However,M2BPGi levels varied significantly among Child-Pugh classes,EV classifications,and between patients with and without HCC(P<0.01).M2BPGi cutoff values for predicting HCC,EV,and decompensated cirrhosis were 6.50,6.64,and 5.25,respectively.Mul-tivariate analysis confirmed M2BPGi as an independent risk factor for EV[adjusted odds ratio(aOR):1.3,95%CI:1.08-1.64]and liver decompensation(aOR:2.11,95%CI:1.37-3.83).Area under the curve of M2BPGi for HCC differ-entiation was 0.71.An algorithm combining alpha-fetoprotein(AFP)and M2BPGi detected 26 of 28 HCC cases with 98.04%accuracy vs 10 cases by AFP alone.CONCLUSION Serum M2BPGi predicted cirrhosis complications,including decompensation and varices,especially in HCC.Combined with AFP,it enhanced HCC detection.Future liver biopsy studies are needed for tissue confirmation.展开更多
基金financially supported by the National Key R&D Program of China(2021YFA1501700)National Science Foundation of China(22272114)+1 种基金Funding for the Hundred Talent Program from Sichuan University(20822041E4079)Fundamental Research Funds from Sichuan University(2022SCUNL103).
文摘Polyethylene(PE)and polypropylene(PP)constitute approximately 57% of global polymer production.Their durability,light weight,and low cost have contributed to their wide adoption in various fields and a rapid increase in their production.However,approximately 90% of these materials are discarded and contribute to global pollution(Fig.1(a)).
基金Bureau of Science and Information of Guangzhou under grant 2024A04J3254the National Key Research and Development Program of China under grant 2024YFE0214900+2 种基金the National Natural Science Foundation of China under grant 32272341,he National Key Research and Development Program of China under grant 2023YFD2100401the Opening Project of Hubei Key Laboratory of Lipid Chemistry and Nutrition under grant 202401,are gratefully acknowledged.
文摘Diacylglycerol(DAG)is a functional oil that can reduce body fat accumulation and postprandial triglycerides.In this study,lipase-catalyzed esterification of oleic acid with glycerol was investigated to elucidate the kinetics and selectivity of each reaction step.1H NMR monitoring revealed equilibrated positional isomerization among acylglycerols:sn-1 monoolein comprised 97.3%of total monoacylglycerols,and sn-1,3 diolein comprised 73.3%of total diacylglycerols.Acyl migration(isomer equilibration)occurred faster than overall esterification.The observed rate constants for successive esterification steps(glycerol→monoacylglycerol,monoacylglycerol→diacylglycerol,diacylglycerol→triacylglycerol)were 0.01068,0.00615,and 0.00304 min^(-1),respectively,indicating progressively slower reaction rates for larger acylglycerol species.Furthermore,molecular distillation at 200–220℃ purified the DAG without altering its fatty acid profile.These findings establish a kinetic model of the three-step esterification and highlight the importance of acyl migration in enzymatic DAG synthesis.
基金supported by National Natural Science Foundation of China(22478265)Sichuan Science and Technology Program(2024NSFSC0222)the Fundamental Research Funds for the Central Universities.We are thankful to Hui Wang at the Analytical&Testing Center,Sichuan University,for assisting with SEM characterization.We appreciate Dr.Xiu He and Dr.Ying Song from the College of Biomass Science and Engineering of Sichuan University for helping with experimental.
文摘The agglomeration-prone properties of metal oxide catalysts limit their catalytic efficiency in the isomerization of glucose to fructose.Herein,the hierarchical structure and abundant coordination groups of collagen fibers were used to anchor Zr^(4+),and a highly dispersed ZrO_(2)-nitrogen-doped carbon(ZrO_(2)-NC)composite catalyst was subsequently fabricated by calcination.For the catalytic glucose-to-fructose isomerization over ZrO_(2)-NC,fructose was obtained in 41.3%yield and 85.3%selectivity in a water-acetone solvent at 120℃ for 10 min.The electron-deficient environment of ZrO_(2)surface during charge transfer from ZrO_(2)-to-NC layer facilitated the preferential adsorption of glucose,which accelerated glucose isomerization and fructose desorption.The amphoteric catalyst triggered both proton transfer on the Bronsted base sites and the intramolecular hydride shift of glucose on the Lewis acid sites of ZrO_(2)-NC in the mixed solvent.The latter isomerization mechanism depended on the presence of acetone,which lowered the energy barrier and increased fructose yield.
基金supported by the National Key R&D Program of China under Grant Nos.2024YFA1610900 and 2023YFA1606401the National Natural Science Foundation of China under Grant Nos.12335007 and 12035001。
文摘The study of nuclear isomers can deepen our understanding of nuclear structure and astrophysics.In this work,we have performed the ab initio calculations of isomers in the N=49 isotones.With a chiral two-plus three-nucleon force,the valence-space effective Hamiltonian was derived using the ab initio many-body perturbation theory named Q-box folded diagrams.The effective operators of electromagnetic operators andβ-decay were obtained using ■-box folded diagrams.With the effective Hamiltonian and operators,we studied the properties of the isomers,gaining a microscopic understanding of the single-particle behaviour of the isomers which we are interested in,showing the reliability of the ab initio calculations.
基金supported by Youth Talent Project of Scientific Research Program of Hubei Provincial Department of Education under Grant Q20241809Doctoral Scientific Research Foundation of Hubei University of Automotive Technology under Grant 202404.
文摘As Internet of Things(IoT)applications expand,Mobile Edge Computing(MEC)has emerged as a promising architecture to overcome the real-time processing limitations of mobile devices.Edge-side computation offloading plays a pivotal role in MEC performance but remains challenging due to complex task topologies,conflicting objectives,and limited resources.This paper addresses high-dimensional multi-objective offloading for serial heterogeneous tasks in MEC.We jointly consider task heterogeneity,high-dimensional objectives,and flexible resource scheduling,modeling the problem as a Many-objective optimization.To solve it,we propose a flexible framework integrating an improved cooperative co-evolutionary algorithm based on decomposition(MOCC/D)and a flexible scheduling strategy.Experimental results on benchmark functions and simulation scenarios show that the proposed method outperforms existing approaches in both convergence and solution quality.
基金supported by the National Natural Science Foundation of China(No.12275369)。
文摘Three-quasiparticle K-isomeric states in odd-mass N=106 isotones within the A~180 mass region were systematically investigated using configuration-constrained potential energy surface calculations.The calculations succes sfully reproduced the excitation energies and deformations of the known high-K isomers in nuclei from 175Tm to 181Re.For the nuclei closer to the Z=82 shell closure(^(183)Ir,^(185)Au,and^(187)Tl),predictions of the configurations of the observed and yet-to-be-observed isomers are provided.The results reveal strong shape polarization,where the three-quasiparticle states are driven to larger deformations compared to the often shape-soft or spherical ground states.A particularly rich spectrum of shape coexistence is predicted in^(187)Tl,where several high-K three-quasiparticle configurations with distinct prolate,oblate,and triaxial shapes are found to coexist at similar excitation energies.Notably,the oblate-deformed K^(π)=29/2^(+)configuration at E_(x)=1839 keV was proposed to be responsible for a long-lived isomer.This study provides a comprehensive picture of shape evolution and coexistence in high-K multi-quasiparticle states,offering valuable insights for future experimental studies.
基金Supported by Japan Society for the Promotion of Science KAKENHI,No.25K11274.
文摘To establish practical,evidence-based strategies for noninvasive assessment and referral of patients with metabolic dysfunction-associated steatotic liver disease(MASLD)in Japan,we must address the urgent clinical need for accurate risk stratification and timely specialist intervention.A panel of 11 Japanese hepatology experts conducted a modified Delphi process to evaluate consensus recommendations regarding the use of noninvasive tests(NITs),including the fibrosis-4 index,enhanced liver fibrosis test,Mac-2-binding protein glycosylation isomer,type IV collagen 7S,cytokeratin-18 fragments,and imaging modalities such as ultrasound elastography and magnetic resonance elastography,for MASLD assessment and clinical referral.Practical algorithms were developed based on current Japanese data and panel consensus.The expert panel validated the utility of NITs as reliable tools for identifying patients with MASLD at risk for advanced fibrosis.Sequential use of NITs improved diagnostic accuracy and referral appropriateness while minimizing unnecessary specialist consultations.The proposed algorithms offer stepwise guidance for primary care physicians,supporting efficient,evidence-based decisionmaking.However,prospective longitudinal studies remain necessary for full prognostic validation of NITs in MASLD management.Noninvasive testing algorithms enable effective risk stratification and referral for MASLD in real-world Japanese practice with anticipated benefit for patient outcomes and healthcare systems.Broader adoption and further validation are warranted.
基金supported by the National Natural Science Foundation of China(No.62371263)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.SJCK25_1995).
文摘1 Introduction Recently,the increasing demand for advanced telecommunication systems has spurred extensive research into bandpass filters(BPFs),with particular emphasis on miniaturization,reduction of insertion loss(IL),and enhancement of upper stopband rejection(Huang et al.,2021;Snyder et al.,2021;Lin et al.,2023;Zeng et al.,2023).
基金financially supported by the National Natural Science Foundation of China(No.21172269)the Fundamental Research Funds for the Central Universities,SouthCentral Minzu University(No.CZH24005)。
文摘Binuclear complexes have attracted extensive attention in fields such as catalysis because of their likely bimetallic synergistic effect;however,the mechanism and factors influencing this synergism remain unclear.In this work,six bis-β-ketoimine binuclear titanium complexes4a-4f containing different alkylthio sidearms and configurations were synthesized and characterized by nuclear magnetic resonance hydrogen spectrum(~1H-NMR),nuclear magnetic resonance carbon spectrum(^(13)C-NMR),Fourier transform infrared spectrum(FTIR),and elemental analysis.The intermetallic distances of isomeric complexes 4a,4d,4e and 4f determined through density functional theory(DFT)optimization were in the order 4a<4d<4e<4f and were found to significantly influence the catalytic performance for ethylene(co)polymerization.These complexes could efficiently catalyze ethylene polymerization and ethylene/1-hexene or ethylene/1-octene copolymerization with high activity to produce highmolecular-weight ethylene homo-and co-polymers.Among the three binuclear titanium complexes 4a-4c with similar structures but different lengths of alkylthio sidearms,complex 4a,which contained the shortest methylthio sidearm,exhibited the highest activity for ethylene polymerization and copolymerization with 1-hexene or 1-octene.Additionally,for ethylene/1-hexene or ethylene/1-octene copolymerization,it showed the highest comonomer incorporation compared with propylthio(4b)and octylthio(4c)derivatives because of the smaller steric hindrance of the methyl group in 4a and the more open coordination space for vinyl monomers.Furthermore,among the isomeric complexes 4a,4d,4e and4f,complex 4a with the shortest bimetallic distance also exhibited the highest activity towards ethylene(co)polymerization,and the highest 1-hexene or 1-octene incorporation in comparison with its regioisomeric counterparts 4d,4e and p-phenyl-bridged analog 4f,owing to a more appropriate bimetallic distance that is conducive to a synergistic effect.
基金supported by the National Natural Science Foundation of China(Nos.22071044,21771054 and 22171071)。
文摘The synthesis of Ta-substituted polyoxometalates has always been an attractive but challenging goal.Three novel tantalum-containing 12-tungsto-2-phosphates were successfully prepared using the water bath method.The monomer,K_(11)Li[P_(2)W_(12)(TaO_(2))_(6)O_(56)]·19H_(2)O(1),is composed of{P_(2)W_(12)}and 6{Ta(O_(2))}building blocks,similar to[P_(2)W_(12)(NbO_(2))_(6)O_(56)]^(12-).Monomer 1 polymerized to form two cis-trans dimers,K1_(3)Li_(6)H-cis-[P_(2)W_(12)Ta_(4)(TaO_(2))_(2)O_(59)]_(2)·61H_(2)O(2)and KNa_(3)Li_(4)H_(12)-trans-[P_(2)W_(12)Ta_(4)(TaO_(2))_(2)O_(59)]_(2)·37H_(2)O(3).Compounds 1-3 can serve as a structural motif to manufacture additional fascinating molecular clusters,promoting the advancement of POM chemistry.In contrast to[P_(2)W_(12)(NbO_(2))_(6)O_(56)]^(12-),compound 1 exhibits exceptional stability,evidenced by ESI-MS,IR,and NMR spectroscopy.In addition,2 and 3 exhibit high proton conductivity and superior water adsorption properties.
文摘Six coordination polymers based on 9,10-di(pyridine-4-yl)-anthracene(DPA)and 1,6-di(1H-imidazol-1-yl)pyrene(DIP)were obtained by solvothermal reactions.{[Zn(DPA)Cl_(2)]·DMF·2H_(2)O}n(1)and{[Zn_(1.5)(DPA)_(1.5)Cl_(3)]·5H_(2)O}n(2)are framework isomers,which both contain zigzag chains formed by DPA,Zn^(2+),and Cl-.The zigzag chains in 1 are further assembled by C—H…Cl interactions into layers,and these layers exhibit two different orientations,displaying a rare 2D to 3D interpenetration mode.The zigzag chains in 2 are parallelly arranged.{[Zn_(3)(DPA)_(3)Br_(6)]·2DMF·_(1.5)H_(2)O}n(3)is isostructural to 2.3 was obtained using ZnBr_(2)instead of ZnCl_(2).[M(DPA)(formate)_(2)(H_(2)O)_(2)]n[M=Co(4),Cu(5)]are isostructural,contain chain structures formed by DPA,Cu^(2+)/Co^(2+),and for-mate ions,which were formed in situ in the solvothermal reaction.{[Zn(DIP)_(2)Cl]ClO_(4)}n(6)contains a layer structure formed by DIP and Zn^(2+).Free DPA and DIP ligands exhibited high fluorescence at room temperature,and coordina-tion polymers 3 and 6 displayed enhanced fluorescent emissions.
基金supported by the National Natural Science Foundation of China(22278419)the Key Core Technology Research(Social Development)Foundation of Suzhou(2023ss06)the Suzhou National Joint Laboratory for Green and Low-carbon Wastewater Treatment and Resource Utilization Technology,Suzhou University of Science and Technology(SZLSDT202404).
文摘Fully utilizing renewable biomass energy is important for saving energy,reducing carbon emissions,and mitigating climate change.As the main hydrolysate of cellulose,a primary component of lignocellulose,glucose could be employed as a starting material to prepare some other functional derivatives for improving the value of biomass resources.The isomerization of glucose to produce fructose is an important intermediate process during numerous high-value-added chemical preparations.Therefore,the development of efficient and selective catalysts for glucose isomerization is of great significance.Currently,glucose isomerase catalysts are limited by the harsh conditions required for microbial activity,which restricts further improvements in fructose yield.Additionally,heterogeneous Bronsted-base and Lewis-acid catalysts commonly employed in chemical isomerization methods often lead to the formation of undesirable by-products,resulting in reduced selectivity toward fructose.This study has demonstrated that lithium-loaded heterogeneous catalysts possess excellent isomerization capabilities under mild conditions.A highly efficient Li-C_(3)N_(4) catalyst was developed,achieving a fructose selectivity of 99.9% and a yield of 42.6% at 60℃ within 1.0 h-comparable to the performance of the enzymatic method.Characterization using X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD),proton nuclear magnetic resonance(^(1)H NMR),and inductively coupled plasma(ICP)analyses confirmed that lithium was stably incorporated into the g-C_(3)N_(4) framework through the formation of Li-N bonds.Further investigations using CO_(2) temperature-programmed desorption(CO_(2)-TPD),in situ Fourier-transform infrared spectroscopy(FT-IR)and 7Li magic angle spinning nuclear magnetic resonance(^(7)Li MAS NMR)indicated that the isomerization proceeded via a base-catalyzed mechanism.The Li species were found to interact with hydroxyl groups generated through hydrolysis and simultaneously coordinated with nitrogen atoms in the C_(3)N_(4) matrix,resulting in the formation of Li-N_(6)-H_(2)O active sites.These active sites facilitated the deprotonation of glucose to form an enolate intermediate,followed by a proton transfer step that generated fructose.This mechanism not only improved the efficiency of fructose production but also provided valuable insight into the catalytic role of lithium within the isomerization process.
基金supported by the National Key R&D Program of China(No.2023YFA1606900)the National Natural Science Foundation of China(NSFC)(No.12235003&12447106).
文摘Nuclear excitation by electron capture(NEEC)is a fundamental process in nuclear physics.Despite its theoretical framework established nearly half a century ago,the experimental confirmation of NEEC remains elusive because of significant technical challenges.A notable effort to validate NEEC experimentally involved the enhanced ^(93m)Mo isomer-depletion experiment,which was ultimately hindered by substantial noise interference.This mini-review provides a brief historical overview of NEEC studies and explores the role of NEEC processes in astrophysical environments and laser-induced plasmas.Several platforms have been proposed to facilitate the observation of NEEC,including traditional cooling-storage rings,ion accelerators,and electron beam ion traps.These approaches aim to enhance the nuclear excitation rate,thereby improving the signal-to-noise ratio.In addition,the employment of exotic vortex beams is discussed as a potential methodological approach to address these challenges.
基金financially supported by the National Natural Science Foundation of China(No.22303033)the Fundamental Research Funds for the Central Universities,China(No.JUSRP123017)+1 种基金Wuxi“Taihu Light”Science and Technology Project-Basic Research(No.K20231063)the Research Matching Grant Scheme at CUHK(No.8601309)。
文摘In this study,a pair of dicarboxylic acids as cis-trans isomerism—citraconic acid(CA)and mesaconic acid(MA),was incorporated into polymeric networks of poly(N-isopropylacrylamide)(PNIPAM)-based core-shell microgels via semi-batch precipitation polymerization.We demonstrated that the pH-temperature dual responsiveness of the core-shell microgels is highly correlated with the structure and position of the acid isomers.Both the cis-trans molecular structure and the crosslinking position of the dicarboxylic acids significantly influenced the hydration capacity and surface charge density of the core-shell microgels.These diverse properties first influenced the swelling behavior,further affecting the interfacial behavior of the microgels,including the oil-water dynamic interfacial tension and air-water compression isotherms.Furthermore,the rheological behavior of the microgel suspensions also displayed distinct dependences on the frequency and temperature,illustrating that the cis-trans molecular structure and crosslinked position of the dicarboxylic acids also significantly influenced the interparticle clustering in the bulk solution.Our results suggest that the pH sensitivity of the cis-trans dicarboxylic acid isomer affects the ionization and surface charge distribution of the core or shell layers of individual microgels,which further determines the interparticle interaction and cooperative rearrangement at interfaces and in the bulk.
基金financial support from the National Natural Science Foundation of China(Nos.22271024,21632005)Changzhou University.
文摘Double bonds of internal olefins can be efficiently migrated to the terminal carbons and regioselectively hydroesterified with formates in the presence of Pd(OAc)_(2) and 1,2-DTBPMB under mild reaction conditions,providing a wide variety of corresponding linear carboxylic esters bearing various functional groups in good yields and>20:1 linear/branch ratios.The reaction is optionally simple and does not need to use CO gas and acid co-catalysts.
基金financially supported by the National Science Foundation of China(62474142)Natural Science Foundation of Shandong Province(No.ZR2024YQ070)。
文摘Organic additives with multiple functional groups have shown great promise in improving the performance and stability of perovskite solar cells.The functional groups can passivate undercoordinated ions to reduce nonradiative recombination losses.However,how these groups synergistically affect the enhancement beyond passivation is still unclear.Specifically,isomeric molecules with different substitution patterns or molecular shapes remain elusive in designing new organic additives.Here,we report two isomeric carbazolyl bisphosphonate additives,2,7-Cz BP and 3,6-Cz BP.The isomerism effect on passivation and charge transport process was studied.The two molecules have similar passivation effects through multiple interactions,e.g.,P=O···Pb,P=O···H–N and N–H···I.2,7-CzBP can further bridge the perovskite crystallites to facilitates charge transport.Power conversion efficiencies(PCEs)of 25.88%and 21.04%were achieved for 0.09 cm^(2)devices and 14 cm^(2)modules after 2,7-Cz BP treatment,respectively.The devices exhibited enhanced operational stability maintaining 95%of initial PCE after 1000 h of continuous maximum power point tracking.This study of isomerism effect hints at the importance of tuning substitution positions and molecular shapes for organic additives,which paves the way for innovation of next-generation multifunctional aromatic additives.
基金support from the National Natural Science Foundation of China(62204146,52303259)the Start-up Grant of Henan University of Technology(2023BS035)。
文摘In recent years,the ternary strategy of adding a vip molecule to the active layer has been proven to be effective for improving the performance of organic solar cells(OSCs).Isomerization engineering of the vip molecule is a simple method to increase the amount of promising material,but there are only limited reports,and the structure-property relationships are still unclear.In this work,we synthesized three isomers named BTA5-F-o,BTA5-F-m,and BTA5-F-p,with different fluorine substitution positions,to study the influence of isomerization on the photovoltaic performance.After introducing them as the third components to the classic host system PM6:Y6,all three ternary devices showed improved power conversion efficiency(PCEs)compared to the binary system(PCE of 17.46%).The ternary OSCs based on BTA5-F-o achieved a champion PCE of 19.11%,while BTA5-F-m and BTA5-F-p realized PCEs of 18.65%and 18.45%,respectively.Mechanism studies have shown that the dipole moment of the BTA5-F-o end group is closer to that of the Y6 end group,despite the three isomers with almost identical energy levels and optical properties.It is indicated that the electron attraction ability of BTA5-F-o best matches that of Y6,which leads to the higher charge mobility,less charge recombination,and stronger exciton dissociation and extraction ability in the ternary blend system.This study suggests that rationally adjusting the position of substituents in the terminal group can be an effective way to construct nonfullerene vip acceptors to achieve highly efficient ternary OSCs.
基金supported by the Natural Science Foundation of Hunan Province (No.2020JJ4734)supported in part by the High Performance Computing Center of Central South University。
文摘Aqueous zinc-ion batteries(AZIBs) have garnered significant attention as promising candidates for gridscale energy storage.However,the interfacial instability of zinc anodes caused by the hydrogen evolution reaction(HER) and aqueous electrolyte corrosion severely restricts their practical implementation.This study introduces 2-mercaptothiazoline(MT) as a dynamic electrolyte additive,leveraging its thiolthione tautomerism for interfacial stabilization.Theoretical calculations and experimental investigations reveal that MT can adsorb onto the zinc surface to form a protective layer to suppress corrosion.Simultaneously,the spatial effect of the thiazoline ring prevents excessive molecular aggregation while enabling homogeneous Zn^(2+) electrodeposition.The electronegativity difference between sulfur and nitrogen atoms induces localized polarization,strengthening electronic interactions with the metal surface to accelerate Zn^(2+) reduction kinetics and inhibit side reactions.Consequently,smooth and low-porosity Zn deposits with enhanced interfacial stability are achieved.The optimized Zn//Zn symmetric cells exhibit extraordinary cycling stability exceeding 1800 h at 0.5 mA cm^(-2),0.5 mAh cm^(-2),while sustaining400 h of operation at 28.5 % depth of discharge(DOD).Zn//MnO_(2) full cells incorporating MT additive maintain 122.6 mAh g^(-1) capacity retention after 500 cycles(1 A g^(-1)).This work provides a facile yet effective strategy for stabilizing Zn metal-based batteries through synergistic interface engineering.
文摘BACKGROUND Cirrhosis is a progressive condition characterized by fibrosis that can lead to severe complications and increased mortality.The mac-2 binding protein glyco-sylation isomer(M2BPGi)is a prominent biomarker for predicting hepatocellular carcinoma(HCC)and cirrhosis-induced esophageal varices(EV).AIM To investigate thresholds of M2BPGi associated with HCC,EV,and decomp-ensation in patients with cirrhosis.METHODS This was a prospective study.A total of 153 patients with cirrhosis who met the inclusion criteria were enrolled.The patients were diagnosed with HCC and EV according to the Baveno VII and European Association for the Study of the Liver guidelines.Baseline serum M2BPGi levels were assessed along with other routine tests.The data analysis aimed to determine the cutoff values of M2BPGi for pre-dicting EV and HCC.RESULTS In the study 85.6%of patients were Child-Pugh B and C.M2BPGi mean cutoff index was 7.1±3.7,showing no significant etiological differences.However,M2BPGi levels varied significantly among Child-Pugh classes,EV classifications,and between patients with and without HCC(P<0.01).M2BPGi cutoff values for predicting HCC,EV,and decompensated cirrhosis were 6.50,6.64,and 5.25,respectively.Mul-tivariate analysis confirmed M2BPGi as an independent risk factor for EV[adjusted odds ratio(aOR):1.3,95%CI:1.08-1.64]and liver decompensation(aOR:2.11,95%CI:1.37-3.83).Area under the curve of M2BPGi for HCC differ-entiation was 0.71.An algorithm combining alpha-fetoprotein(AFP)and M2BPGi detected 26 of 28 HCC cases with 98.04%accuracy vs 10 cases by AFP alone.CONCLUSION Serum M2BPGi predicted cirrhosis complications,including decompensation and varices,especially in HCC.Combined with AFP,it enhanced HCC detection.Future liver biopsy studies are needed for tissue confirmation.
