Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated...Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated and poly(vinyl alcohol)‐protected reduction methods, respectively.The meso‐Mn2O3 had a high surface area, i.e., 106 m2/g, and a cubic crystal structure. Noble‐metalnanoparticles (NPs) of size 2.1?2.8 nm were uniformly dispersed on the meso‐Mn2O3 surfaces. AlloyingPd with Pt enhanced the catalytic activity in methane combustion; 1.41(Pd5.1Pt)/meso‐Mn2O3gave the best performance; T10%, T50%, and T90% (the temperatures required for achieving methaneconversions of 10%, 50%, and 90%) were 265, 345, and 425 °C, respectively, at a space velocity of20000 mL/(g?h). The effects of SO2, CO2, H2O, and NO on methane combustion over1.41(Pd5.1Pt)/meso‐Mn2O3 were also examined. We conclude that the good catalytic performance of1.41(Pd5.1Pt)/meso‐Mn2O3 is associated with its high‐quality porous structure, high adsorbed oxygen species concentration, good low‐temperature reducibility, and strong interactions between Pd‐Pt alloy NPs and the meso‐Mn2O3 support.展开更多
Patients with epidermal growth factor receptor(EGFR)wild-type non-small cell lung cancer(NSCLC)often show primary resistance to gefitinib therapy.It is thus necessary to study the metabolism of gefitinib in NSCLC cell...Patients with epidermal growth factor receptor(EGFR)wild-type non-small cell lung cancer(NSCLC)often show primary resistance to gefitinib therapy.It is thus necessary to study the metabolism of gefitinib in NSCLC cells to comprehensively reveal the reasons for the primary resistance of tumors.Herein,we develop a platform for studying drug metabolism heterogeneity based on single-cell mass spectrometry(sDMH-scMS)by integrating living-cell electrolaunching ionization MS(ILCEI-MS)and high-performance liquid chromatography-MS(HPLC-MS)analysis,and the primary resistance of NSCLC cells to gefitinib was studied using this platform.The ILCEI-MS analysis showed that approximately 11.9%of NSCLC single cells contained the gefitinib metabolite M11;HPLC-MS detection diluted the intensity of M11 in subpopulations and concealed the heterogeneity of drug metabolism in tumor single cells.The intensity of gefitinib in EGFR wild-type A549 cells was markedly lower than in mutant PC9 cells,and the intensity of gefitinib metabolites was significantly higher than in PC9 cells,suggesting that the primary resistance of NSCLC cells is related to gefitinib metabolism.Moreover,the combination of gefitinib and the drug-metabolizing enzyme inhibitorα-naphthoflavone was shown to overcome the primary resistance of the NSCLC cells.Overall,the results of this study are expected to be applicable for clinical drug resistance diagnosis and treatment at the single-cell level.展开更多
The ultrafine WC-Co composite powder was synthesized by a newly developed rapid route based on in situ reactions. By using the as-synthesized composite powder, the granulation processing was then carried out to prepar...The ultrafine WC-Co composite powder was synthesized by a newly developed rapid route based on in situ reactions. By using the as-synthesized composite powder, the granulation processing was then carried out to prepare the ultrafine-structured thermal spraying feedstock. The influences of the heat-treatment process on density of the feedstock powder, phase constitution and wear resistance of the resultant WC-Co coatings fabricated by high velocity oxy-fuel (HVOF) were investigated. The results showed that increasing the heating temperature and extending the holding time leaded to remarkable increase in the density and flowability of the feedstock powder. As a result, the decarburization of the in-flight particles could be decreased and the wear resistance of coating was significantly enhanced. The present study demonstrated that the developed techniques for the ultrafine powder and its thermal-sprayed coatings had very promising applications in scaling up to produce ultrafine-structured cermet coatings with excellent performance.展开更多
An anomalous enhancement of fluorescence of carbon dots (CDs) was observed via lanthanum (La) doping. La-doped CDs (La-CDs) were prepared through microwave pyrolysis within 4 min. With La^3+ doping, the emissio...An anomalous enhancement of fluorescence of carbon dots (CDs) was observed via lanthanum (La) doping. La-doped CDs (La-CDs) were prepared through microwave pyrolysis within 4 min. With La^3+ doping, the emission band shifted from blue to green although LaB+ is non-fluorescent. The quantum yield and fluorescence lifetime improved by about 20% and 35%, respectively. All experiment results indicate that La^3+ doping is an effective way to tune fluorescence and improve the performance of CDs. Another unique attribute of La-CDs is high sensitivity to Fe^3+. The La-CD-based fluorescence probe was established and used for sensitive and selective detection of Fe^3+ with a limit of detection of 91 nmol/L. The proposed fluorescence probe also was successfully employed to visualize intracellular Fe^3+ in live HeLa cells through cell imaging. It was also shown that yttrium exhibited the same fluorescence enhancement effect as La. The results may provide a new route for preparing CDs with special properties.展开更多
Binuclear iron phthalocyanine/reduced graphene oxide(bi-Fe Pc/RGO) nanocomposite with good electrocatalytic activity for ORR in alkaline medium was prepared in one step. High angle annular dark field image scanning tr...Binuclear iron phthalocyanine/reduced graphene oxide(bi-Fe Pc/RGO) nanocomposite with good electrocatalytic activity for ORR in alkaline medium was prepared in one step. High angle annular dark field image scanning transmission electron microscopy(HAADF-STEM) and energy dispersive X-ray spectroscopy element mapping results show bi-Fe Pc was uniformly distributed on RGO. An obvious cathodic peak located at about-0.23 V(vs. SCE) in CV and an onset potential of-0.004 V(vs. SCE) in LSV indicate the as-prepared bi-Fe Pc/RGO nanocomposite possesses high activity which is closed to Pt/C for ORR. The ORR on bi-Fe Pc/RGO nanocomposite follows four-electron transfer pathway in alkaline medium. Compared with Pt/C, there is only a slight decrease(about 0.02 V vs. SCE) for bi-Fe Pc/RGO nanocomposite when the methanol exists. The excellent activity and methanol tolerance in alkaline solutions proves that bi-Fe Pc/RGO nanocomposite could be considered as a promising cathode catalyst for alkaline fuel cells.展开更多
MicroRNAs are a class of important biomarkers,and the simultaneous detection of multiple miRNAs can provide valuable information about many diseases and biological processes.Amplification-free determination has been d...MicroRNAs are a class of important biomarkers,and the simultaneous detection of multiple miRNAs can provide valuable information about many diseases and biological processes.Amplification-free determination has been developed for the analysis of multiple miRNAs because of its characteristic low cost and high fidelity.Herein,a method for the amplification-free analysis and simultaneous detection of multiple miRNAs based on a so-called pico-HPLC-LIF system is described.In this process,a bare open capilla ry with an inner diameter of 680 nm is used as a sepa ration column for a sample volume of several hundreds of femtoliters(300 fL),followed by separation and detection.The technique has a zeptomolar limit of detection.The method was applied to detect cellular miRNA from adenocarcinomic human alveolar basal epithelial(A549)cell extracts,and the simultaneous detection of the mir-182,miR-155,and let-7 a was achieved.The results showed that the expression of mir-182 and miR-155 was up-regulated and that of let-7 a was down-regulated in A549 cells.This method for multiple miRNAs detection is expected to have broad applications in miRNA-based disease diagnosis,prognosis,treatment,and monitoring.展开更多
We have previously developed bare narrow-bore capillary chromatography. In this work, high-performance DNA separation was realized for a size range of 10–800 base pairs(bp) utilizing bare narrow-bore capillary chroma...We have previously developed bare narrow-bore capillary chromatography. In this work, high-performance DNA separation was realized for a size range of 10–800 base pairs(bp) utilizing bare narrow-bore capillary chromatography with 750 nm- radius capillaries. Separation behavior of double-stranded DNA(ds DNA) fragments was investigated over a range of eluent concentrations and elution pressures. DNA molecules were hydrodynamically separated in a size-dependent manner in free solution without any sieving matrices, with the longer fragments being eluted out from the capillary earlier. It was found that the eluent concentration variously influenced the transport behavior for different-sized DNA fragments depending upon the configuration of DNA molecules and the association of counterions. Ionic strength of the solutions strongly impacted DNA persistence length. Enhanced elution pressure could shorten analysis time with a slight loss in resolution. Excellent efficiency of two million theoretical plates per meter was achieved, which indicates the enormous potential of bare narrow-bore capillary chromatography for the analysis of DNA fragments. These findings would be useful in understanding the transport behavior of DNA fragments in confined dimensions for chromatography in free solution.展开更多
Single-cell imaging,a powerful analytical method to study single-cell behavior,such as gene expression and protein profiling,provides an essential basis for modern medical diagnosis.The coding and localization functio...Single-cell imaging,a powerful analytical method to study single-cell behavior,such as gene expression and protein profiling,provides an essential basis for modern medical diagnosis.The coding and localization function of microfluidic chips has been developed and applied in living single-cell imaging in recent years.Simultaneously,chip-based living single-cell imaging is also limited by complicated trapping steps,low cell utilization,and difficult high-resolution imaging.To solve these problems,an ultra-thin temperature-controllable microwell array chip(UTCMA chip)was designed to develop a living single-cell workstation in this study for continuous on-chip culture and real-time high-resolution imaging of living single cells.The chip-based on ultra-thin ITO glass is highly matched with an inverted microscope(or confocal microscope)with a high magnification objective(100×oil lens),and the temperature of the chip can be controlled by combining it with a home-made temperature control device.High-throughput single-cell patterning is realized in one step when the microwell array on the chip uses hydrophilic glass as the substrate and hydrophobic SU-8 photoresist as the wall.The cell utilization rate,single-cell capture rate,and microwell occupancy rate are all close to 100%in the microwell array.This method will be useful in rare single-cell research,extending its application in the biological and medical-related fields,such as early diagnosis of disease,personalized therapy,and research-based on single-cell analysis.展开更多
Chromatography theory shows that when the inner diameter of the chromatography column is very narrow(e.g.,1—2μm),the maximum efficiency will be produced in liquid chromatography.In addition,the increasing demand for...Chromatography theory shows that when the inner diameter of the chromatography column is very narrow(e.g.,1—2μm),the maximum efficiency will be produced in liquid chromatography.In addition,the increasing demand for ultrasmall volume sample analysis has produced the trend of narrowing the diameter of the liquid chromatography column.Experiments have verified that ultranarrow-bore open tubular liquid chromatography(i.d.≤2μm)has the advantages of small sample requirement and high separation efficiency.However,there also exist huge challenges along with such obvious advantages.This review summarizes the efforts made by our research group and other research groups to develop this field.We hope that in the near future,ultranarrow bore open-tube liquid chromatography can be successfully and maturely applied to the application of analytes with ultrasmall size and volume such as single-cell and even subcellular organelles omics research.展开更多
基金supported by the Ph.D.Program Foundation of Ministry of Education of China(20131103110002)the NNSF of China(21377008)+2 种基金National High Technology Research and Development Program(863 Program,2015AA034603)Foundation on the Creative Research Team Con-struction Promotion Project of Beijing Municipal InstitutionsScientific Research Base Construction-Science and Technology Creation Plat-form-National Materials Research Base Construction~~
文摘Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated and poly(vinyl alcohol)‐protected reduction methods, respectively.The meso‐Mn2O3 had a high surface area, i.e., 106 m2/g, and a cubic crystal structure. Noble‐metalnanoparticles (NPs) of size 2.1?2.8 nm were uniformly dispersed on the meso‐Mn2O3 surfaces. AlloyingPd with Pt enhanced the catalytic activity in methane combustion; 1.41(Pd5.1Pt)/meso‐Mn2O3gave the best performance; T10%, T50%, and T90% (the temperatures required for achieving methaneconversions of 10%, 50%, and 90%) were 265, 345, and 425 °C, respectively, at a space velocity of20000 mL/(g?h). The effects of SO2, CO2, H2O, and NO on methane combustion over1.41(Pd5.1Pt)/meso‐Mn2O3 were also examined. We conclude that the good catalytic performance of1.41(Pd5.1Pt)/meso‐Mn2O3 is associated with its high‐quality porous structure, high adsorbed oxygen species concentration, good low‐temperature reducibility, and strong interactions between Pd‐Pt alloy NPs and the meso‐Mn2O3 support.
基金supported by the Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910005017)the National Natural Science Foundation of China(Nos.22127805 and 22206008).
文摘Patients with epidermal growth factor receptor(EGFR)wild-type non-small cell lung cancer(NSCLC)often show primary resistance to gefitinib therapy.It is thus necessary to study the metabolism of gefitinib in NSCLC cells to comprehensively reveal the reasons for the primary resistance of tumors.Herein,we develop a platform for studying drug metabolism heterogeneity based on single-cell mass spectrometry(sDMH-scMS)by integrating living-cell electrolaunching ionization MS(ILCEI-MS)and high-performance liquid chromatography-MS(HPLC-MS)analysis,and the primary resistance of NSCLC cells to gefitinib was studied using this platform.The ILCEI-MS analysis showed that approximately 11.9%of NSCLC single cells contained the gefitinib metabolite M11;HPLC-MS detection diluted the intensity of M11 in subpopulations and concealed the heterogeneity of drug metabolism in tumor single cells.The intensity of gefitinib in EGFR wild-type A549 cells was markedly lower than in mutant PC9 cells,and the intensity of gefitinib metabolites was significantly higher than in PC9 cells,suggesting that the primary resistance of NSCLC cells is related to gefitinib metabolism.Moreover,the combination of gefitinib and the drug-metabolizing enzyme inhibitorα-naphthoflavone was shown to overcome the primary resistance of the NSCLC cells.Overall,the results of this study are expected to be applicable for clinical drug resistance diagnosis and treatment at the single-cell level.
基金supported by the National Natural Science Foundation of China(No.51174009)the Beijing Key Program of Natural Science Foundation(No.2131001)+1 种基金the National Key Program for Fundamental Research and Development(No.2011CB612207)the National High-tech R&D Program of China(No.SS2013AA031401)
文摘The ultrafine WC-Co composite powder was synthesized by a newly developed rapid route based on in situ reactions. By using the as-synthesized composite powder, the granulation processing was then carried out to prepare the ultrafine-structured thermal spraying feedstock. The influences of the heat-treatment process on density of the feedstock powder, phase constitution and wear resistance of the resultant WC-Co coatings fabricated by high velocity oxy-fuel (HVOF) were investigated. The results showed that increasing the heating temperature and extending the holding time leaded to remarkable increase in the density and flowability of the feedstock powder. As a result, the decarburization of the in-flight particles could be decreased and the wear resistance of coating was significantly enhanced. The present study demonstrated that the developed techniques for the ultrafine powder and its thermal-sprayed coatings had very promising applications in scaling up to produce ultrafine-structured cermet coatings with excellent performance.
基金The authors gratefully acknowledge the financial support from the National Natural Science Foundation of China (Nos. 21375005, 21575054 and 21527808).
文摘An anomalous enhancement of fluorescence of carbon dots (CDs) was observed via lanthanum (La) doping. La-doped CDs (La-CDs) were prepared through microwave pyrolysis within 4 min. With La^3+ doping, the emission band shifted from blue to green although LaB+ is non-fluorescent. The quantum yield and fluorescence lifetime improved by about 20% and 35%, respectively. All experiment results indicate that La^3+ doping is an effective way to tune fluorescence and improve the performance of CDs. Another unique attribute of La-CDs is high sensitivity to Fe^3+. The La-CD-based fluorescence probe was established and used for sensitive and selective detection of Fe^3+ with a limit of detection of 91 nmol/L. The proposed fluorescence probe also was successfully employed to visualize intracellular Fe^3+ in live HeLa cells through cell imaging. It was also shown that yttrium exhibited the same fluorescence enhancement effect as La. The results may provide a new route for preparing CDs with special properties.
基金supported by the National Natural Science Foundation of China (21275014, 21375005)the Excellent Young Scientists Fund of NSFC (21322501)+2 种基金the Importation and Development of High-Caliber Talents Project of Beijing Municipal Institutions (CIT& TCD20140309)the Program for New Century Excellent Talents in University (NCET-12-0603)the Beijing Natural Science Foundation Program and Scientific Research Key Program of the Beijing Municipal Commission of Education (KZ201310005001)
文摘Binuclear iron phthalocyanine/reduced graphene oxide(bi-Fe Pc/RGO) nanocomposite with good electrocatalytic activity for ORR in alkaline medium was prepared in one step. High angle annular dark field image scanning transmission electron microscopy(HAADF-STEM) and energy dispersive X-ray spectroscopy element mapping results show bi-Fe Pc was uniformly distributed on RGO. An obvious cathodic peak located at about-0.23 V(vs. SCE) in CV and an onset potential of-0.004 V(vs. SCE) in LSV indicate the as-prepared bi-Fe Pc/RGO nanocomposite possesses high activity which is closed to Pt/C for ORR. The ORR on bi-Fe Pc/RGO nanocomposite follows four-electron transfer pathway in alkaline medium. Compared with Pt/C, there is only a slight decrease(about 0.02 V vs. SCE) for bi-Fe Pc/RGO nanocomposite when the methanol exists. The excellent activity and methanol tolerance in alkaline solutions proves that bi-Fe Pc/RGO nanocomposite could be considered as a promising cathode catalyst for alkaline fuel cells.
基金financially supported by the National Natural Science Foundation of China(Nos.21625501,21527808)the Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910005017)。
文摘MicroRNAs are a class of important biomarkers,and the simultaneous detection of multiple miRNAs can provide valuable information about many diseases and biological processes.Amplification-free determination has been developed for the analysis of multiple miRNAs because of its characteristic low cost and high fidelity.Herein,a method for the amplification-free analysis and simultaneous detection of multiple miRNAs based on a so-called pico-HPLC-LIF system is described.In this process,a bare open capilla ry with an inner diameter of 680 nm is used as a sepa ration column for a sample volume of several hundreds of femtoliters(300 fL),followed by separation and detection.The technique has a zeptomolar limit of detection.The method was applied to detect cellular miRNA from adenocarcinomic human alveolar basal epithelial(A549)cell extracts,and the simultaneous detection of the mir-182,miR-155,and let-7 a was achieved.The results showed that the expression of mir-182 and miR-155 was up-regulated and that of let-7 a was down-regulated in A549 cells.This method for multiple miRNAs detection is expected to have broad applications in miRNA-based disease diagnosis,prognosis,treatment,and monitoring.
基金supported by the National Natural Science Foundation of China(21275014)the Excellent Young Scientists Fund of NSFC(21322501)+3 种基金the Importation and Development of High-Caliber Talents Project of Beijing Municipal Institutions(CIT&TCD20140309)the Program for New Century Excellent Talents in University(NCET-12-0603)the Beijing Natural Science Foundation ProgramScientific Research Key Program of Beijing Municipal Commission of Education(KZ201310005001)
文摘We have previously developed bare narrow-bore capillary chromatography. In this work, high-performance DNA separation was realized for a size range of 10–800 base pairs(bp) utilizing bare narrow-bore capillary chromatography with 750 nm- radius capillaries. Separation behavior of double-stranded DNA(ds DNA) fragments was investigated over a range of eluent concentrations and elution pressures. DNA molecules were hydrodynamically separated in a size-dependent manner in free solution without any sieving matrices, with the longer fragments being eluted out from the capillary earlier. It was found that the eluent concentration variously influenced the transport behavior for different-sized DNA fragments depending upon the configuration of DNA molecules and the association of counterions. Ionic strength of the solutions strongly impacted DNA persistence length. Enhanced elution pressure could shorten analysis time with a slight loss in resolution. Excellent efficiency of two million theoretical plates per meter was achieved, which indicates the enormous potential of bare narrow-bore capillary chromatography for the analysis of DNA fragments. These findings would be useful in understanding the transport behavior of DNA fragments in confined dimensions for chromatography in free solution.
基金supported by the National Natural Science Foundation of China(Nos.21625501,21936001)the Beijing Outstanding Young Scientist Program(No.BJJWZYJH01201910005017).
文摘Single-cell imaging,a powerful analytical method to study single-cell behavior,such as gene expression and protein profiling,provides an essential basis for modern medical diagnosis.The coding and localization function of microfluidic chips has been developed and applied in living single-cell imaging in recent years.Simultaneously,chip-based living single-cell imaging is also limited by complicated trapping steps,low cell utilization,and difficult high-resolution imaging.To solve these problems,an ultra-thin temperature-controllable microwell array chip(UTCMA chip)was designed to develop a living single-cell workstation in this study for continuous on-chip culture and real-time high-resolution imaging of living single cells.The chip-based on ultra-thin ITO glass is highly matched with an inverted microscope(or confocal microscope)with a high magnification objective(100×oil lens),and the temperature of the chip can be controlled by combining it with a home-made temperature control device.High-throughput single-cell patterning is realized in one step when the microwell array on the chip uses hydrophilic glass as the substrate and hydrophobic SU-8 photoresist as the wall.The cell utilization rate,single-cell capture rate,and microwell occupancy rate are all close to 100%in the microwell array.This method will be useful in rare single-cell research,extending its application in the biological and medical-related fields,such as early diagnosis of disease,personalized therapy,and research-based on single-cell analysis.
基金financial support from the National Natural Science Foundation of China(Nos.21625501,21936001)the Beijing Outsta nding Young Scie ntist Program(No.BJJWZYJH01201910005017).
文摘Chromatography theory shows that when the inner diameter of the chromatography column is very narrow(e.g.,1—2μm),the maximum efficiency will be produced in liquid chromatography.In addition,the increasing demand for ultrasmall volume sample analysis has produced the trend of narrowing the diameter of the liquid chromatography column.Experiments have verified that ultranarrow-bore open tubular liquid chromatography(i.d.≤2μm)has the advantages of small sample requirement and high separation efficiency.However,there also exist huge challenges along with such obvious advantages.This review summarizes the efforts made by our research group and other research groups to develop this field.We hope that in the near future,ultranarrow bore open-tube liquid chromatography can be successfully and maturely applied to the application of analytes with ultrasmall size and volume such as single-cell and even subcellular organelles omics research.