Thermoresponsive luminescent organic materials have great potential for intelligent optical devices,but their applicability remains limited due to formidable challenges in achieving tunable response temperature and di...Thermoresponsive luminescent organic materials have great potential for intelligent optical devices,but their applicability remains limited due to formidable challenges in achieving tunable response temperature and different colors.In this study,we developed a thermoresponsive polymer/lanthanide ion(Ln^(3+))complex system,enabling precise regulation of luminescence color and response temperature.The polymer was synthesized via copolymerization of acrylamide(Am)with 6-(3-(2-(methacryloyloxy)ethyl)ureido)picolinate(MAUP).The MAUP unit incorporates ligands capable of coordinating with Ln^(3+)and functions as an“antenna”,absorbing incident light and efficiently transferring energy to Ln^(3+),leading to diverse luminescent emissions.The thermoresponsive property of the poly(Am-co-MAUP)/Ln^(3+)complexes,based on the synergy of ionic coordination and hydrogen bonding,imparts the precise regulation of luminescence with temperature.The response temperature of the poly(Amco-MAUP)/Ln^(3+)complexes can be finely tuned by various factors synergistically,including polymer composition and Ln^(3+)concentrations.Moreover,these thermoresponsive luminescent complexes enable potential applications in multi-level information encryption and visual temperature sensing.展开更多
Alkaline hydrogen evolution reaction(HER)for scalable hydrogen production largely hinges on addressing the sluggish bubble-involved kinetics on the traditional Ni-based electrode,especially for ampere-level current de...Alkaline hydrogen evolution reaction(HER)for scalable hydrogen production largely hinges on addressing the sluggish bubble-involved kinetics on the traditional Ni-based electrode,especially for ampere-level current densities and beyond.Herein,3D-printed Ni-based sulfide(3DPNS)electrodes with varying scaffolds are designed and fabricated.In situ observations at microscopic levels demonstrate that the bubble escape velocity increases with the number of hole sides(HS)in the scaffolds.Subsequently,we conduct multiphysics field simulations to illustrate that as the hole shapes transition from square,pentagon,and hexagon to circle,where a noticeable reduction in the bubble-attached HS length and the pressure balance time around the bubbles results in a decrease in bubble size and an acceleration in the rate of bubble escape.Ultimately,the 3DPNS electrode with circular hole configura-tions exhibits the most favorable HER performance with an overpotential of 297 mV at the current density of up to 1000 mA cm^(-2) for 120 h.The present study highlights a scalable and effective electrode scaffold design that promotes low-cost and low-energy green hydrogen production through the ampere-level alkaline HER.展开更多
The site-specific N-glycosylation changes of human plasma immunoglobulin gamma molecules(IgGs)have been shown to modulate the immune response and could serve as potential biomarkers for the accurate diagnosis of vario...The site-specific N-glycosylation changes of human plasma immunoglobulin gamma molecules(IgGs)have been shown to modulate the immune response and could serve as potential biomarkers for the accurate diagnosis of various diseases.However,quantifying intact N-glycopeptides accurately in large-scale clinical samples remains a challenge,and the quantitative N-glycosylation of plasma IgGs in patients with chronic kidney diseases(CKDs)has not yet been studied.In this study,we present a novel integrated intact N-glycopeptide quantitative pipeline(termed GlycoQuant),which combines our recently developed mass spectrometry fragmentation method(EThcD-sceHCD)and an intact N-glycopeptide batch quantification software tool(the upgraded PANDA v.1.2.5).We purified and digested human plasma IgGs from 58 healthy controls(HCs),48 patients with membranous nephropathy(MN),and 35 patients with IgA nephropathy(IgAN)within an hour.Then,we analyzed the digested peptides without enrichment using EThcD-sceHCD-MS/MS,which provided higher spectral quality and greater identified depth.Using upgraded PANDA,we performed site-specific N-glycosylation quantification of IgGs.Several quantified intact N-glycopeptides not only distinguished CKDs from HCs,but also different types of CKD(MN and IgAN)and may serve as accurate diagnostic tools for renal tubular function.In addition,we proved the applicability of this pipeline to complex samples by reanalyzing the intact N-glycopeptides from cell,urine,plasma,and tissue samples that we had previously identified.We believe that this pipeline can be applied to large-scale clinical N-glycoproteomic studies,facilitating the discovery of novel glycosylated biomarkers.展开更多
基金supported by the Ningbo Youth Leading Talent Project(2024QL020)the National Natural Science Foundation of China(52373118 and 22075154)+1 种基金the“Mechanics+”Interdisciplinary Top Innovative Youth Fund Project of Ningbo University(LJ2024006)the Ningbo Major Science and Technology Project(2024Z205)。
文摘Thermoresponsive luminescent organic materials have great potential for intelligent optical devices,but their applicability remains limited due to formidable challenges in achieving tunable response temperature and different colors.In this study,we developed a thermoresponsive polymer/lanthanide ion(Ln^(3+))complex system,enabling precise regulation of luminescence color and response temperature.The polymer was synthesized via copolymerization of acrylamide(Am)with 6-(3-(2-(methacryloyloxy)ethyl)ureido)picolinate(MAUP).The MAUP unit incorporates ligands capable of coordinating with Ln^(3+)and functions as an“antenna”,absorbing incident light and efficiently transferring energy to Ln^(3+),leading to diverse luminescent emissions.The thermoresponsive property of the poly(Am-co-MAUP)/Ln^(3+)complexes,based on the synergy of ionic coordination and hydrogen bonding,imparts the precise regulation of luminescence with temperature.The response temperature of the poly(Amco-MAUP)/Ln^(3+)complexes can be finely tuned by various factors synergistically,including polymer composition and Ln^(3+)concentrations.Moreover,these thermoresponsive luminescent complexes enable potential applications in multi-level information encryption and visual temperature sensing.
基金Natural Science Foundation of Hainan Province,Grant/Award Number:623MS068Fundamental Research Funds for the Central Universities,Grant/Award Number:40120631+2 种基金Natural Science Foundation of Hubei Province,Grant/Award Number:2022CFB388National Natural Science Foundation of China,Grant/Award Number:52202291Singapore MOE,Grant/Award Number:Tier 1,A-8000186-01-00。
文摘Alkaline hydrogen evolution reaction(HER)for scalable hydrogen production largely hinges on addressing the sluggish bubble-involved kinetics on the traditional Ni-based electrode,especially for ampere-level current densities and beyond.Herein,3D-printed Ni-based sulfide(3DPNS)electrodes with varying scaffolds are designed and fabricated.In situ observations at microscopic levels demonstrate that the bubble escape velocity increases with the number of hole sides(HS)in the scaffolds.Subsequently,we conduct multiphysics field simulations to illustrate that as the hole shapes transition from square,pentagon,and hexagon to circle,where a noticeable reduction in the bubble-attached HS length and the pressure balance time around the bubbles results in a decrease in bubble size and an acceleration in the rate of bubble escape.Ultimately,the 3DPNS electrode with circular hole configura-tions exhibits the most favorable HER performance with an overpotential of 297 mV at the current density of up to 1000 mA cm^(-2) for 120 h.The present study highlights a scalable and effective electrode scaffold design that promotes low-cost and low-energy green hydrogen production through the ampere-level alkaline HER.
基金funded by Grants from the National Key Research and Development Program of China(2022YFF0608401,2022YFF0608404)National Natural Science Foundation of China(Grant number 31901038)+2 种基金Department of Science and Technology of Sichuan Province(2021YJ0479)CAMS Innovation Fund for Medical Sciences(2019-I2M-5-063)Research Project of the National Institute of Metrology(AKYZD2111).
文摘The site-specific N-glycosylation changes of human plasma immunoglobulin gamma molecules(IgGs)have been shown to modulate the immune response and could serve as potential biomarkers for the accurate diagnosis of various diseases.However,quantifying intact N-glycopeptides accurately in large-scale clinical samples remains a challenge,and the quantitative N-glycosylation of plasma IgGs in patients with chronic kidney diseases(CKDs)has not yet been studied.In this study,we present a novel integrated intact N-glycopeptide quantitative pipeline(termed GlycoQuant),which combines our recently developed mass spectrometry fragmentation method(EThcD-sceHCD)and an intact N-glycopeptide batch quantification software tool(the upgraded PANDA v.1.2.5).We purified and digested human plasma IgGs from 58 healthy controls(HCs),48 patients with membranous nephropathy(MN),and 35 patients with IgA nephropathy(IgAN)within an hour.Then,we analyzed the digested peptides without enrichment using EThcD-sceHCD-MS/MS,which provided higher spectral quality and greater identified depth.Using upgraded PANDA,we performed site-specific N-glycosylation quantification of IgGs.Several quantified intact N-glycopeptides not only distinguished CKDs from HCs,but also different types of CKD(MN and IgAN)and may serve as accurate diagnostic tools for renal tubular function.In addition,we proved the applicability of this pipeline to complex samples by reanalyzing the intact N-glycopeptides from cell,urine,plasma,and tissue samples that we had previously identified.We believe that this pipeline can be applied to large-scale clinical N-glycoproteomic studies,facilitating the discovery of novel glycosylated biomarkers.
