The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabric...The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabricate active electrocatalysts for the sluggish oxygen evolution process.However,there is generally an intrinsic gap between the as-prepared and real electrocatalysts due to structure evolution under the oxidative reaction conditions.Here,we combine in-situ anionic leaching and atomic deposition to realize single-atom catalysts with self-optimized structures.The introduced F ions facilitate structural transformation from Co(OH)xF into CoOOH(F),which generates an amorphous edge surface to provide more anchoring sites for Ir single atoms.Meanwhile,the in-situ anionic leaching of F ions elevates the Co valence state of Ir_(1)/CoOOH(F)more significantly than the counterpart without F ions(Ir_(1)/CoOOH),leading to stronger adsorption of oxygenated intermediates.As revealed by electrochemical measurements,the increased Ir loading together with the favored adsorption of*OH intermediates improve the catalytic activity of Ir_(1)/CoOOH(F).Specifically,Ir_(1)/CoOOH(F)delivered a current density of 10 mA cm-2at an overpotential of 238 mV,being lower than 314 mV for Ir_(1)/CoOOH.The results demonstrated the facility of the in-situ optimization process to optimize catalyst structure for improved performance.展开更多
Two-dimensional transition metal hydroxides with abundant reserves and low prices have played an indispensable role in energy catalytic applications.Recent reports indicated that the incorporation of Fe species into C...Two-dimensional transition metal hydroxides with abundant reserves and low prices have played an indispensable role in energy catalytic applications.Recent reports indicated that the incorporation of Fe species into Co-based catalysts can synergistically enhance oxygen evolution reaction(OER)activity.Constructing a heterointerface on the surface of Co-based catalysts can provide a platform to investigate the role of heterointerface in reaction kinetics.Herein,we constructed a Fe-O-Co heterointerface without electronic effect by depositing FeO_(x)clusters on the oxygen vacancies of CoOOH surface.FeO_(x)/CoOOH exhibited excellent OER intrinsic activity,which can deliver the turnover frequency(TOF)of 4.56 s^(-1)at the overpotentials of 300 mV and the Tafel slope of 33 mV·dec^(-1).In-situ electrochemical impedance spectroscopy(EIS)and density functional theory(DFT)calculations demonstrated that the synergistic effect between Fe sites and Co sites confined at the Fe-O-Co heterointerface accelerated the charge transfer during OER and optimized the adsorption of oxygen intermediates,consequently enhancing OER.展开更多
Group 3 innate lymphoid cells(ILC3s)play important roles in maintaining intestinal homeostasis by protecting the host from pathogen infections and tissue inflammation.The transcription factor PLZF(promyelocytic leukem...Group 3 innate lymphoid cells(ILC3s)play important roles in maintaining intestinal homeostasis by protecting the host from pathogen infections and tissue inflammation.The transcription factor PLZF(promyelocytic leukemia zinc finger),encoded by zinc finger BTB domain containing 16(Zbtb16),is highly and transiently expressed in ILC precursors(ILCPs).However,the role of PLZF in regulating ILC3 development and function remains unknown.Here,we show that PLZF was specifically expressed in mature intestinal ILC3s compared with other ILC subsets.PLZF was dispensable for ILC3 development.However,PLZF deficiency in ILC3s resulted in increased innate interleukin-22(IL-22)secretion and protection against gut infection and inflammation.Mechanistically,PLZF negatively regulated IL-22 expression by ILC3s in a cell-intrinsic manner by binding to the IL-22 promoter region for transcriptional repression.Together,our data suggest that PLZF restricts intestinal ILC3 function to regulate gut immune homeostasis.展开更多
基金supported by National Key Research and Development Program of China(2021YFA1500500,2019YFA0405600,2017YFA0204904,2019YFA0405602,and 2017YFA0403402)the National Science Fund for Distinguished Young Scholars(21925204)+8 种基金the National Natural Science Foundation of China(21972132,U1732149,U19A2015,U1732272,21673214,92045301,and 21902149)the Fundamental Research Funds for the Central Universities(20720220010)the Provincial Key Research and Development Program of Anhui(202004a05020074)the Anhui Natural Science Foundation for Young Scholars(2208085QB52)K.C.Wong Education(GJTD2020-15)the Hefei Municipal Natural Science Foundation(2021018)the DNL Cooperation Fund,CAS(DNL202003)Users with Excellence Program of Hefei Science Center CAS(2020HSCUE001)USTC Research Funds of the Double First-Class Initiative(YD2340002002)。
文摘The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabricate active electrocatalysts for the sluggish oxygen evolution process.However,there is generally an intrinsic gap between the as-prepared and real electrocatalysts due to structure evolution under the oxidative reaction conditions.Here,we combine in-situ anionic leaching and atomic deposition to realize single-atom catalysts with self-optimized structures.The introduced F ions facilitate structural transformation from Co(OH)xF into CoOOH(F),which generates an amorphous edge surface to provide more anchoring sites for Ir single atoms.Meanwhile,the in-situ anionic leaching of F ions elevates the Co valence state of Ir_(1)/CoOOH(F)more significantly than the counterpart without F ions(Ir_(1)/CoOOH),leading to stronger adsorption of oxygenated intermediates.As revealed by electrochemical measurements,the increased Ir loading together with the favored adsorption of*OH intermediates improve the catalytic activity of Ir_(1)/CoOOH(F).Specifically,Ir_(1)/CoOOH(F)delivered a current density of 10 mA cm-2at an overpotential of 238 mV,being lower than 314 mV for Ir_(1)/CoOOH.The results demonstrated the facility of the in-situ optimization process to optimize catalyst structure for improved performance.
基金This work was supported by the National Key Research and Development Program of China(Nos.2017YFA0403402,2019YFA0405600,2019YFA0405602,and 2021YFA1500500)National Natural Science Foundation of China(NSFC,Nos.21972132,21673214,22202192,U19A2015,92045301,U1732149,and U1732272)+8 种基金National Science Fund for Distinguished Young Scholars(No.21925204)Fundamental Research Funds for the Central Universities(No.20720220010)Provincial Key Research and Development Program of Anhui(No.202004a05020074)K.C.Wong Education(No.GJTD-2020-15)the DNL Cooperation Fund,Chinese Academy of Sciences(CAS,No.DNL202003)Users with Excellence Program of Hefei Science Center CAS(No.2020HSC-UE001)USTC Research Funds of the Double First-Class Initiative(No.YD2340002002)Anhui Natural Science Foundation for Young Scholars(Nos.2208085QB52 and 2208085QB41)CAS Project for Young Scientists in Basic Research(No.YSBR-051).
文摘Two-dimensional transition metal hydroxides with abundant reserves and low prices have played an indispensable role in energy catalytic applications.Recent reports indicated that the incorporation of Fe species into Co-based catalysts can synergistically enhance oxygen evolution reaction(OER)activity.Constructing a heterointerface on the surface of Co-based catalysts can provide a platform to investigate the role of heterointerface in reaction kinetics.Herein,we constructed a Fe-O-Co heterointerface without electronic effect by depositing FeO_(x)clusters on the oxygen vacancies of CoOOH surface.FeO_(x)/CoOOH exhibited excellent OER intrinsic activity,which can deliver the turnover frequency(TOF)of 4.56 s^(-1)at the overpotentials of 300 mV and the Tafel slope of 33 mV·dec^(-1).In-situ electrochemical impedance spectroscopy(EIS)and density functional theory(DFT)calculations demonstrated that the synergistic effect between Fe sites and Co sites confined at the Fe-O-Co heterointerface accelerated the charge transfer during OER and optimized the adsorption of oxygen intermediates,consequently enhancing OER.
基金grant 2020YFA0509200(to LS)from the Ministry of Science and Technology of Chinagrant 81971487(to LS)from the National Natural Science Foundation of China+1 种基金grants 20ZR1430200 and 20142202300(to LS)from the Science and Technology Commission of Shanghai Municipalitygrant 20194Y0275(to JS)from the Shanghai Municipal Health Commission,and the Shanghai Frontiers Science Center of Cellular Homeostasis and Human Diseases.
文摘Group 3 innate lymphoid cells(ILC3s)play important roles in maintaining intestinal homeostasis by protecting the host from pathogen infections and tissue inflammation.The transcription factor PLZF(promyelocytic leukemia zinc finger),encoded by zinc finger BTB domain containing 16(Zbtb16),is highly and transiently expressed in ILC precursors(ILCPs).However,the role of PLZF in regulating ILC3 development and function remains unknown.Here,we show that PLZF was specifically expressed in mature intestinal ILC3s compared with other ILC subsets.PLZF was dispensable for ILC3 development.However,PLZF deficiency in ILC3s resulted in increased innate interleukin-22(IL-22)secretion and protection against gut infection and inflammation.Mechanistically,PLZF negatively regulated IL-22 expression by ILC3s in a cell-intrinsic manner by binding to the IL-22 promoter region for transcriptional repression.Together,our data suggest that PLZF restricts intestinal ILC3 function to regulate gut immune homeostasis.
