High-entropy(HE)design provides ample opportunities for accessing catalysts with unique physiochemical properties for advanced energy and environmental applications.Although a variety of multi-cationic high-entropy ma...High-entropy(HE)design provides ample opportunities for accessing catalysts with unique physiochemical properties for advanced energy and environmental applications.Although a variety of multi-cationic high-entropy materials(HEMs)have been identified,HEMs consisted of multiple cationic and anionic elements are still limited.Herein,we present the design and synthesis of a series of rutile-structured high-entropy oxy fluorides(HEOFs),including[RuO_(2)]_(x)[MgMnZnCoF_(2)]_(y),[MnO_(2)]_(x)[MgMnZnCoF_(2)]_(y),[MoO_(2)]_(x)[MgMnZnCoF_(2)]_(y),[SnO_(2)]_(x)[MgMnZnCoF_(2)]_(y)and[TiO_(2)]_(x)[MgMnZnCoF_(2)]_(y)(x:y=3:1,2:1,1:1).All the HEOFs are obtained through mechanochemical alloying rutile-structured oxide and fluoride precursors and the HEOFs inherit the crystal structures of the skeleton oxides.Moreover,the HEOFs exhibit enhanced electrocatalytic oxygen evolution reaction(OER)activity than the corresponding oneelement precursors.Typically,the best-performed HEOF[RuO_(2)]_(3)[MgMnZnCoF_(2)]_(1)catalyst requires an overpotential of 240 mV to achieve a current density of 10 mA cm^(-2),which is lower than RuO_(2)(291 mV),More impressively,the specific mass activity of[RuO_(2)]_(3)[MgMnZnCoF_(2)]_(1)is 537.1 A g_(Ru)^(-1)at1.55 V(vs RHE),which is ca.7.6 times that of RuO_(2)(70.5 A g_(Ru)^(-1)).The enhanced electrocata lytic OER performance obtained on[RuO_(2)]_(3)[MgMnZnCoF_(2)]_(1)is ascribed to the contribution of the different cationic and anionic elements that modulates the electronic structures of the pristine RuO_(2),which facilitates efficient OER kinetics.This work demonstrates the efficacy of high-entropy design towards approaching excellent catalysts for enhanced electrocatalysis.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant No.22179015,21872142,22302026)the Liao Ning Revitalization Talents Program(XLYC1807196)+1 种基金the fund of the State Key Laboratory of Catalysis in DICP(N-22-06)the open fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP,CAS(SKLMRD-K202414)。
文摘High-entropy(HE)design provides ample opportunities for accessing catalysts with unique physiochemical properties for advanced energy and environmental applications.Although a variety of multi-cationic high-entropy materials(HEMs)have been identified,HEMs consisted of multiple cationic and anionic elements are still limited.Herein,we present the design and synthesis of a series of rutile-structured high-entropy oxy fluorides(HEOFs),including[RuO_(2)]_(x)[MgMnZnCoF_(2)]_(y),[MnO_(2)]_(x)[MgMnZnCoF_(2)]_(y),[MoO_(2)]_(x)[MgMnZnCoF_(2)]_(y),[SnO_(2)]_(x)[MgMnZnCoF_(2)]_(y)and[TiO_(2)]_(x)[MgMnZnCoF_(2)]_(y)(x:y=3:1,2:1,1:1).All the HEOFs are obtained through mechanochemical alloying rutile-structured oxide and fluoride precursors and the HEOFs inherit the crystal structures of the skeleton oxides.Moreover,the HEOFs exhibit enhanced electrocatalytic oxygen evolution reaction(OER)activity than the corresponding oneelement precursors.Typically,the best-performed HEOF[RuO_(2)]_(3)[MgMnZnCoF_(2)]_(1)catalyst requires an overpotential of 240 mV to achieve a current density of 10 mA cm^(-2),which is lower than RuO_(2)(291 mV),More impressively,the specific mass activity of[RuO_(2)]_(3)[MgMnZnCoF_(2)]_(1)is 537.1 A g_(Ru)^(-1)at1.55 V(vs RHE),which is ca.7.6 times that of RuO_(2)(70.5 A g_(Ru)^(-1)).The enhanced electrocata lytic OER performance obtained on[RuO_(2)]_(3)[MgMnZnCoF_(2)]_(1)is ascribed to the contribution of the different cationic and anionic elements that modulates the electronic structures of the pristine RuO_(2),which facilitates efficient OER kinetics.This work demonstrates the efficacy of high-entropy design towards approaching excellent catalysts for enhanced electrocatalysis.
