The recent emergence of tetragonal phases zirconium dioxide(ZrO_(2))with vacancies has generated significant interest as a highly efficient and stable electrocatalyst with potential applications in trapping polysulfid...The recent emergence of tetragonal phases zirconium dioxide(ZrO_(2))with vacancies has generated significant interest as a highly efficient and stable electrocatalyst with potential applications in trapping polysulfides and facilitating rapid conversion in lithium-sulfur batteries(LSBs).However,the reduction of ZrO_(2)is challenging,even under strong reducing atmospheres at high temperatures and pressures.Consequently,the limited presence of oxygen vacancies results in insufficient active sites and reaction interfaces,thereby hindering practical implementation.Herein,we successfully introduced abundant oxygen vacancies into ZrO_(2)at the nanoscale with the help of carbon nanotubes(CNTs-OH)through hydrogen-etching at lower temperatures and pressures.The introduced oxygen vacancies on ZrO_(2-x)/CNTs-OH can effectively rearrange charge distribution,enhance sulfiphilicity and increase active sites,contributing to high ionic and electronic transfer kinetics,strong binding energy and low redox barriers between polysulfides and ZrO_(2-x).These findings have been experimentally validated and supported by theory calculations.As a result,LSBs assembled with the ZrO_(2-x)/CNTs-OH modified separators demonstrate excellent rate performance,superior cycling stability,and ultra-high sulfur utilization.Especially,at high sulfur loading of 6 mg cm^(-2),the area capacity is still up to 6.3 mA h cm^(-2).This work provides valuable insights into the structural and functional optimization of electrocatalysts for batteries.展开更多
Familial hypercholesterolemia(FH)is a lipoprotein disorder characterized by elevated plasma levels of low-density lipoprotein cholesterol(LDL-C)and an increased risk of premature atherosclerotic cardiovascular disease...Familial hypercholesterolemia(FH)is a lipoprotein disorder characterized by elevated plasma levels of low-density lipoprotein cholesterol(LDL-C)and an increased risk of premature atherosclerotic cardiovascular disease.Recent evidences have shown that several glycerophospholipid species were markedly altered in experimental FH animals and exhibited diverse bioactivities.Nevertheless,the glycerophospholipid profiles and their associated biological implications in human FH remain largely unknown.In this study,we sought to comprehensively delineate the glycerophospholipid phenotypes in human FH and to investigate the functional roles of key FH-altered glycerophospholipid molecules on cholesterol metabolism.Targeted analysis of 328 glycerophospholipid metabolites was used to profile the differentiated alterations in patients with homozygous FH(HoFH;n=181),heterozygous FH(HeFH;n=452),and non-FH hypercholesterolemia(n=382).Our findings revealed that the glycerophospholipid phenotypes of FH and non-FH hypercholesterolemia were dominated by a spectrum of metabolites involved in the lysophosphatidic acid(LPA)metabolism.Among the LPA features,palmitoyl-LPA(16:0)showed significant association with the clinical levels of LDL-C and total cholesterol in HoFH and HeFH populations.Using functional metabolomic strategy and murine FH model,we demonstrated that supplementation with LPA 16:0 elevated the plasma levels of LDL and free/esterified cholesterol and exacerbated the atherosclerotic lesions.Conversely,inhibition of autotaxin-mediated LPA 16:0 production significantly ameliorated dyslipidemia.Mechanistically,we uncovered that LPA 16:0 could disrupt hepatic cholesterol homeostasis by impairing cholesterol excretion and inhibiting primary bile acid synthesis.In summary,our study offers novel insights into lipid metabolism in human FH and posits that targeting LPA metabolism may represent a promising therapeutic strategy for reducing cholesterol levels in the FH population.展开更多
基金the Natural Science Foundation of Shandong Province (ZR2021MB101,ZR2021ME113,ZR2021ME177,and ZR2021QE096)。
文摘The recent emergence of tetragonal phases zirconium dioxide(ZrO_(2))with vacancies has generated significant interest as a highly efficient and stable electrocatalyst with potential applications in trapping polysulfides and facilitating rapid conversion in lithium-sulfur batteries(LSBs).However,the reduction of ZrO_(2)is challenging,even under strong reducing atmospheres at high temperatures and pressures.Consequently,the limited presence of oxygen vacancies results in insufficient active sites and reaction interfaces,thereby hindering practical implementation.Herein,we successfully introduced abundant oxygen vacancies into ZrO_(2)at the nanoscale with the help of carbon nanotubes(CNTs-OH)through hydrogen-etching at lower temperatures and pressures.The introduced oxygen vacancies on ZrO_(2-x)/CNTs-OH can effectively rearrange charge distribution,enhance sulfiphilicity and increase active sites,contributing to high ionic and electronic transfer kinetics,strong binding energy and low redox barriers between polysulfides and ZrO_(2-x).These findings have been experimentally validated and supported by theory calculations.As a result,LSBs assembled with the ZrO_(2-x)/CNTs-OH modified separators demonstrate excellent rate performance,superior cycling stability,and ultra-high sulfur utilization.Especially,at high sulfur loading of 6 mg cm^(-2),the area capacity is still up to 6.3 mA h cm^(-2).This work provides valuable insights into the structural and functional optimization of electrocatalysts for batteries.
基金supported by the Noncommunicable Chronic Diseases-National Science and Technology Major Project(nos.2023ZD0503400 and 2023ZD0503403)the National Key Research and Development Program of China(grant no.2021YFC2500603)+1 种基金the Beijing Natural Science Foundation(grant no.7252215)the National Natural Science Foundation of China(grant no.82100295).
文摘Familial hypercholesterolemia(FH)is a lipoprotein disorder characterized by elevated plasma levels of low-density lipoprotein cholesterol(LDL-C)and an increased risk of premature atherosclerotic cardiovascular disease.Recent evidences have shown that several glycerophospholipid species were markedly altered in experimental FH animals and exhibited diverse bioactivities.Nevertheless,the glycerophospholipid profiles and their associated biological implications in human FH remain largely unknown.In this study,we sought to comprehensively delineate the glycerophospholipid phenotypes in human FH and to investigate the functional roles of key FH-altered glycerophospholipid molecules on cholesterol metabolism.Targeted analysis of 328 glycerophospholipid metabolites was used to profile the differentiated alterations in patients with homozygous FH(HoFH;n=181),heterozygous FH(HeFH;n=452),and non-FH hypercholesterolemia(n=382).Our findings revealed that the glycerophospholipid phenotypes of FH and non-FH hypercholesterolemia were dominated by a spectrum of metabolites involved in the lysophosphatidic acid(LPA)metabolism.Among the LPA features,palmitoyl-LPA(16:0)showed significant association with the clinical levels of LDL-C and total cholesterol in HoFH and HeFH populations.Using functional metabolomic strategy and murine FH model,we demonstrated that supplementation with LPA 16:0 elevated the plasma levels of LDL and free/esterified cholesterol and exacerbated the atherosclerotic lesions.Conversely,inhibition of autotaxin-mediated LPA 16:0 production significantly ameliorated dyslipidemia.Mechanistically,we uncovered that LPA 16:0 could disrupt hepatic cholesterol homeostasis by impairing cholesterol excretion and inhibiting primary bile acid synthesis.In summary,our study offers novel insights into lipid metabolism in human FH and posits that targeting LPA metabolism may represent a promising therapeutic strategy for reducing cholesterol levels in the FH population.
