Shuttle effect of polysulfides overshadows the superiorities of lithium-sulfur batteries.Size-sieving effect could address this thorny trouble rely on size differ in polysulfides and lithium ions.However,clogged polys...Shuttle effect of polysulfides overshadows the superiorities of lithium-sulfur batteries.Size-sieving effect could address this thorny trouble rely on size differ in polysulfides and lithium ions.However,clogged polysulfides pose some challenges for cathode and are rarely recycled during charging/discharging.Herein,an amino functionalized titanium-organic framework is designed for modifying lithium-sulfur batteries separator to address the aforementioned challenges.Wherein,the introduction of amino narrows titanium-organic framework pore size,enabling functional separator to selectively modulate lithium ions and polysulfides migration using size-sieving effect,thereby completely suppressing polysulfides shuttle.Furthermore,the blocked polysulfides will be adsorbed on the separator surface by positively charged amino leveraging electrostatic adsorption,ensuring polysulfides to redistribute and reuse,and boosting active materials utilization.Significantly,the migration of lithium ions is not hindered since there are lithium ions transfer channels formed via Lewis acid-base interaction with the help of amino.Combined with these virtues,the lithium-sulfur batteries with amino functionalized titanium-organic framework modified separator enjoy an ultralow attenuation rate of 0.045%per cycle over 1000 cycles at 1.0C.Electrostatic adsorption and Lewis acid-base interaction cover deficiencies existing in the inhibition of polysulfides shuttle by size-sieving effect,providing fresh insight into the advancement of lithium-sulfur batteries.展开更多
The heavy biofouling on electrochemical sensor surface poses a formidable challenge for biosensing in human blood.Herein,we designed a multilayer filtering-sensing sandwich patch that served as a versatile platform to...The heavy biofouling on electrochemical sensor surface poses a formidable challenge for biosensing in human blood.Herein,we designed a multilayer filtering-sensing sandwich patch that served as a versatile platform to surmount the substantial fouling constraints for detection in human blood.The patch integrated two functional layers:(i) Inspired by dialysis phenomenon,a filtering-mass transfer hydrophilic membrane with heterogeneous nanostructure was used to filter large-size substances(like cells,bacteria and microorganisms,etc.) and continuously pass through the rest of the biological fluid(like proteins,metabolites and inorganic salts,etc.).(ii) the polypeptide composite hydrogel(r GO/PEPG) on the screenprinted electrode(SPE) surface,with the modulation of-COOH and-NH_2 groups,endowed a strong hydrophilic layer with electric neutrality to further facilitate the antifouling ability.Notably,the integration of the filtering porous membrane with the antifouling hydrogel ensures the strong antifouling ability of the electrochemical sensor in complex human blood.Furthermore,the self-healing property of the r GO/PEPG,relying on the physical π-π stacking forces,aligns the electrochemical sensor with practical needs.The constructed antifouling biosensor based on the filtering-sensing sandwich patch was successfully applied for the sensitive detection of cortisol in human blood,with an acceptable accuracy comparable to the enzyme-linked immunosorbent assay(ELISA) method.The strategy presented herein represent a promising advance along the road to construct effective antifouling biosensing devices with robust operation in diverse complex body fluids.展开更多
基金supported by the National Natural Science Foundation of China(52463013 and 52073133)Key Talent Project Foundation of Gansu Province+3 种基金Joint fund between Shenyang National Laboratory for Materials ScienceState Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals(18LHPY002)the Program for Hongliu Distinguished Young Scholars in Lanzhou University of Technologythe Incubation Program of Excellent Doctoral Dissertation–Lanzhou University of Technology
文摘Shuttle effect of polysulfides overshadows the superiorities of lithium-sulfur batteries.Size-sieving effect could address this thorny trouble rely on size differ in polysulfides and lithium ions.However,clogged polysulfides pose some challenges for cathode and are rarely recycled during charging/discharging.Herein,an amino functionalized titanium-organic framework is designed for modifying lithium-sulfur batteries separator to address the aforementioned challenges.Wherein,the introduction of amino narrows titanium-organic framework pore size,enabling functional separator to selectively modulate lithium ions and polysulfides migration using size-sieving effect,thereby completely suppressing polysulfides shuttle.Furthermore,the blocked polysulfides will be adsorbed on the separator surface by positively charged amino leveraging electrostatic adsorption,ensuring polysulfides to redistribute and reuse,and boosting active materials utilization.Significantly,the migration of lithium ions is not hindered since there are lithium ions transfer channels formed via Lewis acid-base interaction with the help of amino.Combined with these virtues,the lithium-sulfur batteries with amino functionalized titanium-organic framework modified separator enjoy an ultralow attenuation rate of 0.045%per cycle over 1000 cycles at 1.0C.Electrostatic adsorption and Lewis acid-base interaction cover deficiencies existing in the inhibition of polysulfides shuttle by size-sieving effect,providing fresh insight into the advancement of lithium-sulfur batteries.
基金supported by the National Natural Science Foundation of China (Nos.22174082,22374085)the Key Research and Development Program of Shandong Province (No.2021ZDSYS30)Natural Science Foundation of Shandong Province,China (No.ZR2024QB059)。
文摘The heavy biofouling on electrochemical sensor surface poses a formidable challenge for biosensing in human blood.Herein,we designed a multilayer filtering-sensing sandwich patch that served as a versatile platform to surmount the substantial fouling constraints for detection in human blood.The patch integrated two functional layers:(i) Inspired by dialysis phenomenon,a filtering-mass transfer hydrophilic membrane with heterogeneous nanostructure was used to filter large-size substances(like cells,bacteria and microorganisms,etc.) and continuously pass through the rest of the biological fluid(like proteins,metabolites and inorganic salts,etc.).(ii) the polypeptide composite hydrogel(r GO/PEPG) on the screenprinted electrode(SPE) surface,with the modulation of-COOH and-NH_2 groups,endowed a strong hydrophilic layer with electric neutrality to further facilitate the antifouling ability.Notably,the integration of the filtering porous membrane with the antifouling hydrogel ensures the strong antifouling ability of the electrochemical sensor in complex human blood.Furthermore,the self-healing property of the r GO/PEPG,relying on the physical π-π stacking forces,aligns the electrochemical sensor with practical needs.The constructed antifouling biosensor based on the filtering-sensing sandwich patch was successfully applied for the sensitive detection of cortisol in human blood,with an acceptable accuracy comparable to the enzyme-linked immunosorbent assay(ELISA) method.The strategy presented herein represent a promising advance along the road to construct effective antifouling biosensing devices with robust operation in diverse complex body fluids.
