Heterostructure engineering holds exceptional promise for the development of high-performance electrocatalysts for overall water splitting.However,production of inexpensive and high-efficiency bifunctional electrocata...Heterostructure engineering holds exceptional promise for the development of high-performance electrocatalysts for overall water splitting.However,production of inexpensive and high-efficiency bifunctional electrocatalysts remains a challenge.Herein,we demonstrate a simple method to synthesize a paper-mulberry(Broussonetia papyrifera)-inspired Co_(9)S_(8)@CoNi_(2)S_(4)/nickel foam(Co_(9)S_(8)@CoNi_(2)S_(4)/NF)heterojunction with high catalytic activity and stability.The process involves in situ growth of NiCo layered double hydroxide and in situ derivatization of ZIF-67,followed by the S heteroatom doping.The Co_(9)S_(8)@CoNi_(2)S_(4)/NF benefits from the heterostructure and functional advantages of multidimensional building blocks including one-dimensional(1D)nanowires,2D nanosheets and nanoparticles.The optimized Co_(9)S_(8)@CoNi_(2)S_(4)/NF heterojunction with 10% sulphur content reveals excellent electrocatalytic activity with the lower overpotentials of 68 mV for hydrogen evolution reaction(HER)and 170 mV for oxygen evolution reaction(OER)at 10 mA cm^(-2) in the 1.0 mol L^(-1) KOH solution,which is superior to the recently reported transition metal based electrocatalysts.The outstanding performance is attributed to the strong interface coupling between CoNi_(2)S_(4) and Co_(9)S_(8),the advantage of multidimensional structure and the customized electronic structure.The density functional theory suggests that the interface between Co_(9)S_(8) and CoNi_(2)S_(4) optimizes the adsorption of the multiple intermediates and further facilitates water splitting kinetics.This work offers a generic approach for heterostructure engineering design of highperformance catalytic system applications.展开更多
基金supported by the National Natural Science Foundation of China(21776129,21706121,and U22B6011)the Natural Science Foundation of Jiangsu Province(BK20170995 and BK20201120)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
基金supported by the National Natural Science Foundation of China(22005273,21825106,and 21671175)the Program for Science&Technology Innovative Research Team in the University of Henan Province(20IRTSTHN007)the Australian Research Council and QUT Centre for Materials Science for partial support。
文摘Heterostructure engineering holds exceptional promise for the development of high-performance electrocatalysts for overall water splitting.However,production of inexpensive and high-efficiency bifunctional electrocatalysts remains a challenge.Herein,we demonstrate a simple method to synthesize a paper-mulberry(Broussonetia papyrifera)-inspired Co_(9)S_(8)@CoNi_(2)S_(4)/nickel foam(Co_(9)S_(8)@CoNi_(2)S_(4)/NF)heterojunction with high catalytic activity and stability.The process involves in situ growth of NiCo layered double hydroxide and in situ derivatization of ZIF-67,followed by the S heteroatom doping.The Co_(9)S_(8)@CoNi_(2)S_(4)/NF benefits from the heterostructure and functional advantages of multidimensional building blocks including one-dimensional(1D)nanowires,2D nanosheets and nanoparticles.The optimized Co_(9)S_(8)@CoNi_(2)S_(4)/NF heterojunction with 10% sulphur content reveals excellent electrocatalytic activity with the lower overpotentials of 68 mV for hydrogen evolution reaction(HER)and 170 mV for oxygen evolution reaction(OER)at 10 mA cm^(-2) in the 1.0 mol L^(-1) KOH solution,which is superior to the recently reported transition metal based electrocatalysts.The outstanding performance is attributed to the strong interface coupling between CoNi_(2)S_(4) and Co_(9)S_(8),the advantage of multidimensional structure and the customized electronic structure.The density functional theory suggests that the interface between Co_(9)S_(8) and CoNi_(2)S_(4) optimizes the adsorption of the multiple intermediates and further facilitates water splitting kinetics.This work offers a generic approach for heterostructure engineering design of highperformance catalytic system applications.