Developing low-cost,efficient,and stable non-precious-metal electrocatalysts with controlled crystal structure,morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions.Herein,a seri...Developing low-cost,efficient,and stable non-precious-metal electrocatalysts with controlled crystal structure,morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions.Herein,a series of phosphorus-doped Fe_(7)S_(8)nanowires integrated within carbon(P-Fe_(7)S_(8)@C)are rationally synthesized via a one-step phosphorization of one-dimensional(1D)Fe-based organicinorganic nanowires.The as-obtained P-Fe_(7)S_(8)@C catalysts with modified electronic configurations present typical porous structure,providing plentiful active sites for rapid reaction kinetics.Density functional calculations demonstrate that the doping Fe_(7)S_(8)with P can effectively enhance the electron density of Fe_(7)S_(8)around the Fermi level and weaken the Fe-H bonding,leading to the decrease of adsorption free energy barrier on active sites.As a result,the optimal catalyst of P-Fe_(7)S_(8)-600@C exhibits a relatively low overpotential of 136 mV for hydrogen evolution reaction(HER)to reach the current density of 10 mA/cm^(2),and a significantly low overpotential of 210 mV for oxygen evolution reaction(OER)at 20 mA/cm^(2)in alkaline media.The work presented here may pave the way to design and synthesis of other prominent Fe-based catalysts for water splitting via electronic regulation.展开更多
A key requirement for well performing devices based onorganic semiconductors is to ensure ohmic contacts, where anefficient hole and electron injection and extraction can beachieved at the electrode/semiconductor inte...A key requirement for well performing devices based onorganic semiconductors is to ensure ohmic contacts, where anefficient hole and electron injection and extraction can beachieved at the electrode/semiconductor interfaces. The usualway to obtain ohmic contacts involves fine tuning of the energet-ics at the interfaces by using dopants (p- type and n-type) to con-trol the Fermi level of the semiconductor [1,2], or using suitablemetals or metal oxides as electrodes [3].展开更多
Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis.Herein,the n...Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis.Herein,the nitrogen-doped carbon-decorated tricomponent metal phosphides of FeP4 nanotube@Ni-Co-P nanocage(NC-FNCP)with unique nested hollow architectures are fabricated by a self-sacrifice template strategy.Benefiting from the multi-component synergy,the modification of nitrogen-doped carbon,and the modulation of nested porous hollow morphology,NC-FNCP facilitates rapid electron/mass transport in water and urea electrolysis.NC-FNCP-based anode shows low potentials of 248 mV and 1.37 V(vs.reversible hydrogen electrode)to attain 10 mA/cm^(2) for oxygen evolution reaction(OER)and urea oxidation reaction(UOR),respectively.In addition,the overall urea electrolysis drives 10 mA/cm^(2) at a comparatively low voltage of 1.52 V(vs.RHE)that is 110 mV lower than that of overall water electrolysis,as well as exhibits excellent stability over 20 h.This work strategizes a multi-shell-structured electrocatalyst with multi-compositions and explores its applications in a sustainable combination of hydrogen production and sewage remediation.展开更多
Mitophagy has a critical role in maintaining cellular homeostasis through acidic lysosomes engulfing excess or impaired mitochondria,thereby pH fluctuation is one of the most significant indicators for tracking mitoph...Mitophagy has a critical role in maintaining cellular homeostasis through acidic lysosomes engulfing excess or impaired mitochondria,thereby pH fluctuation is one of the most significant indicators for tracking mitophagy.Then such precise pH tracking demands the fluorogenic probe that has tailored contemporaneous features,including mitochondrial-specificity,excellent biocompatibility,wide pH-sensitive range of 8.0–4.0,and especially quantitative ability.However,available molecular probes cannot simultaneously meet all the requirements since it is extremely difficult to integrate multiple functionalities into a single molecule.To fully address this issue,we herein integrate two fluorogenic pH sensitive units,a mitochondria-specific block,cellpenetrating facilitator,and biocompatible segments into an elegant silica nano scaffold,which greatly ensures the applicability for real-time tracking of pH fluctuations in mitophagy.Most significantly,at a single wavelength excitation,the integrated pHsensitive units have spectra-distinguishable fluorescence towards alkaline and acidic pH in a broad range that covers mitochondrial and lysosomal pH,thus enabling a ratiometric analysis of pH variations during the whole mitophagy.This work also provides constructive insights into the fabrication of advanced fluorescent nanoprobes for diverse biomedical applications.展开更多
As one of the major causes of antimicrobial resistance,β‐lactamase develops rapidly among bacteria.Detection of β‐lactamase in an efficient and low‐cost point‐of‐care testing(POCT)way is urgently needed.However...As one of the major causes of antimicrobial resistance,β‐lactamase develops rapidly among bacteria.Detection of β‐lactamase in an efficient and low‐cost point‐of‐care testing(POCT)way is urgently needed.However,due to the volatile environmental factors,the quantitative measurement of current POCT is often inaccurate.Herein,we demonstrate an artificial intelligence(AI)‐assisted mobile health system that consists of a paper‐basedβ‐lactamase fluorogenic probe analytical device and a smartphone‐based AI cloud.An ultrafast broad‐spectrum fluorogenic probe(B1)that could respond toβ‐lactamase within 20 s was first synthesized,and the detection limit was determined to be 0.13 nmol/L.Meanwhile,a three‐dimensional microfluidic paper‐based analytical device was fabricated for integration of B1.Also,a smartphone‐based AI cloud was developed to correct errors automatically and output results intelligently.This smart system could calibrate the temperature and pH in theβ‐lactamase level detection in complex samples and mice infected with various bacteria,which shows the problem‐solving ability in interdisciplinary research,and demonstrates potential clinical benefits.展开更多
基金the National Natural Science Foundation of China(Nos.21601120 and 21805181)the Science and Technology Commission of Shanghai Municipality(Nos.17ZR1410500 and 19ZR1418100)+1 种基金the High Performance Computing Center of Shanghai UniversityShanghai Engineering Research Center of Intelligent Computing System(No.19DZ2252600)for providing the computing resources and technical support。
文摘Developing low-cost,efficient,and stable non-precious-metal electrocatalysts with controlled crystal structure,morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions.Herein,a series of phosphorus-doped Fe_(7)S_(8)nanowires integrated within carbon(P-Fe_(7)S_(8)@C)are rationally synthesized via a one-step phosphorization of one-dimensional(1D)Fe-based organicinorganic nanowires.The as-obtained P-Fe_(7)S_(8)@C catalysts with modified electronic configurations present typical porous structure,providing plentiful active sites for rapid reaction kinetics.Density functional calculations demonstrate that the doping Fe_(7)S_(8)with P can effectively enhance the electron density of Fe_(7)S_(8)around the Fermi level and weaken the Fe-H bonding,leading to the decrease of adsorption free energy barrier on active sites.As a result,the optimal catalyst of P-Fe_(7)S_(8)-600@C exhibits a relatively low overpotential of 136 mV for hydrogen evolution reaction(HER)to reach the current density of 10 mA/cm^(2),and a significantly low overpotential of 210 mV for oxygen evolution reaction(OER)at 20 mA/cm^(2)in alkaline media.The work presented here may pave the way to design and synthesis of other prominent Fe-based catalysts for water splitting via electronic regulation.
基金supported by the Knut and Alice Wallenberg Foundation(KAW)through a Wallenberg Scholar grant to Olle Ingans。
文摘A key requirement for well performing devices based onorganic semiconductors is to ensure ohmic contacts, where anefficient hole and electron injection and extraction can beachieved at the electrode/semiconductor interfaces. The usualway to obtain ohmic contacts involves fine tuning of the energet-ics at the interfaces by using dopants (p- type and n-type) to con-trol the Fermi level of the semiconductor [1,2], or using suitablemetals or metal oxides as electrodes [3].
基金the National Natural Science Foundation of China(No.21601120)the Science and Technology Commission of Shanghai Municipality(Nos.17ZR1410500 and 19ZR1418100)+3 种基金Science and Technology Program of Shanghai(No.21010500300)STINT Joint China-Sweden Mobility Project(No.CH2017-7243)Swedish Government strategic faculty grant in material science(SFO,MATLIU)in Advanced Functional Materials(AFM)(VR Dnr.5.1-2015-5959)We also appreciate the High-Performance Computing Center of Shanghai University,and Shanghai Engineering Research Center of Intelligent Computing System(No.19DZ2252600)for providing the computing resources and technical support.
文摘Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis.Herein,the nitrogen-doped carbon-decorated tricomponent metal phosphides of FeP4 nanotube@Ni-Co-P nanocage(NC-FNCP)with unique nested hollow architectures are fabricated by a self-sacrifice template strategy.Benefiting from the multi-component synergy,the modification of nitrogen-doped carbon,and the modulation of nested porous hollow morphology,NC-FNCP facilitates rapid electron/mass transport in water and urea electrolysis.NC-FNCP-based anode shows low potentials of 248 mV and 1.37 V(vs.reversible hydrogen electrode)to attain 10 mA/cm^(2) for oxygen evolution reaction(OER)and urea oxidation reaction(UOR),respectively.In addition,the overall urea electrolysis drives 10 mA/cm^(2) at a comparatively low voltage of 1.52 V(vs.RHE)that is 110 mV lower than that of overall water electrolysis,as well as exhibits excellent stability over 20 h.This work strategizes a multi-shell-structured electrocatalyst with multi-compositions and explores its applications in a sustainable combination of hydrogen production and sewage remediation.
基金supported by STINT Joint China-Sweden Mobility Project(No.CH2017-7243)the Swedish Research Council(VR)(Nos.2019-02409 and 2020-05437)+2 种基金the China Scholarship Council(CSC),Carl Tryggers Stiftelse(No.CTS 19:379)Swedish Government strategic faculty grant in material science(SFO,MATLIU)in Advanced Functional Materials(AFM)(VR No.5.1-2015-5959)the Centre in Nano Science and technology at LiTH(CeNano),and LiU Cancer network at Linköping University.
文摘Mitophagy has a critical role in maintaining cellular homeostasis through acidic lysosomes engulfing excess or impaired mitochondria,thereby pH fluctuation is one of the most significant indicators for tracking mitophagy.Then such precise pH tracking demands the fluorogenic probe that has tailored contemporaneous features,including mitochondrial-specificity,excellent biocompatibility,wide pH-sensitive range of 8.0–4.0,and especially quantitative ability.However,available molecular probes cannot simultaneously meet all the requirements since it is extremely difficult to integrate multiple functionalities into a single molecule.To fully address this issue,we herein integrate two fluorogenic pH sensitive units,a mitochondria-specific block,cellpenetrating facilitator,and biocompatible segments into an elegant silica nano scaffold,which greatly ensures the applicability for real-time tracking of pH fluctuations in mitophagy.Most significantly,at a single wavelength excitation,the integrated pHsensitive units have spectra-distinguishable fluorescence towards alkaline and acidic pH in a broad range that covers mitochondrial and lysosomal pH,thus enabling a ratiometric analysis of pH variations during the whole mitophagy.This work also provides constructive insights into the fabrication of advanced fluorescent nanoprobes for diverse biomedical applications.
基金supported by the National Key R&D Program of China(No.2020YFA0709900)the National Natural Science Foundation of China(Nos.62288102,22077101,and 52073230)+3 种基金the Joint Research Funds of Department of Science&Technology of Shaanxi Province and Northwestern Polytechnical University(Nos.2020GXLH‐Z‐008 and 2020GXLH‐Z‐013)the Key Research and Development Program of Shaanxi(No.2022ZDLGY13‐04)Shanxi Provincial Science Fund for Distinguished Young Scholars(No.2023‐JC‐JQ‐32)Fundamental Research Funds for the Central Universities,and the Innovation Foundation for Doctorate Dissertation of Northwestern Polytechnical University(No.CX2021121).
文摘As one of the major causes of antimicrobial resistance,β‐lactamase develops rapidly among bacteria.Detection of β‐lactamase in an efficient and low‐cost point‐of‐care testing(POCT)way is urgently needed.However,due to the volatile environmental factors,the quantitative measurement of current POCT is often inaccurate.Herein,we demonstrate an artificial intelligence(AI)‐assisted mobile health system that consists of a paper‐basedβ‐lactamase fluorogenic probe analytical device and a smartphone‐based AI cloud.An ultrafast broad‐spectrum fluorogenic probe(B1)that could respond toβ‐lactamase within 20 s was first synthesized,and the detection limit was determined to be 0.13 nmol/L.Meanwhile,a three‐dimensional microfluidic paper‐based analytical device was fabricated for integration of B1.Also,a smartphone‐based AI cloud was developed to correct errors automatically and output results intelligently.This smart system could calibrate the temperature and pH in theβ‐lactamase level detection in complex samples and mice infected with various bacteria,which shows the problem‐solving ability in interdisciplinary research,and demonstrates potential clinical benefits.
