Exploring earth-abundant,highly active bifunctional electrocatalysts for efficient hydrogen and oxygen evolution is crucial for water splitting.However,due to their distinct free energies and conducting behaviors(elec...Exploring earth-abundant,highly active bifunctional electrocatalysts for efficient hydrogen and oxygen evolution is crucial for water splitting.However,due to their distinct free energies and conducting behaviors(electron/hole),balancing the catalytic efficiency between hydrogen and oxygen evolution remains challenging for achieving bifunctional electrocatalysts.Here,we report a locally-doped MoS_(2)monolayer with an in-plane heterostructure acting as a bifunctional electrocatalyst and apply it to the overall water splitting.In this heterostructure,the core region contains Mo/S vacancies,while the ring region was doped by Fe atoms(in two substitution configurations:1FeMo and 3FeMo-VS clusters)with a p-type conductive characteristic.Our micro-cell measurements,combined with density functional theory(DFT)calculations,reveal that the vacancies-rich core region presents remarkable hydrogen evolution reaction(HER)activity while the Fe-doped ring gives an excellent oxygen evolution reaction(OER)activity,thus forming an in-plane bifunctional electrocatalyst.Finally,as a proof-of-concept for overall water splitting,we constructed a full-cell configuration based on a locally-doped MoS_(2)monolayer,which achieved a cell voltage of 1.87 V at 10 mA·cm^(-2),demonstrating outstanding performance in strong acid electrolytes.Our work provides insight into the hetero-integration of bifunctional electrocatalysts at the atomic level,paving the way for designing transition metal dichalcogenide catalysts with activity-manipulated regions capable of multiple reactions.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22175060 and 22376062)JSPS Grant-in-Aid for Scientific Research(Nos.JP21H05235,JP22H05478 and JP22F22358)+1 种基金China Postdoctoral Science Foundation(No.2022M722867)the Key Research Project of Higher Education Institutions in Henan Province(No.23A530001).
文摘Exploring earth-abundant,highly active bifunctional electrocatalysts for efficient hydrogen and oxygen evolution is crucial for water splitting.However,due to their distinct free energies and conducting behaviors(electron/hole),balancing the catalytic efficiency between hydrogen and oxygen evolution remains challenging for achieving bifunctional electrocatalysts.Here,we report a locally-doped MoS_(2)monolayer with an in-plane heterostructure acting as a bifunctional electrocatalyst and apply it to the overall water splitting.In this heterostructure,the core region contains Mo/S vacancies,while the ring region was doped by Fe atoms(in two substitution configurations:1FeMo and 3FeMo-VS clusters)with a p-type conductive characteristic.Our micro-cell measurements,combined with density functional theory(DFT)calculations,reveal that the vacancies-rich core region presents remarkable hydrogen evolution reaction(HER)activity while the Fe-doped ring gives an excellent oxygen evolution reaction(OER)activity,thus forming an in-plane bifunctional electrocatalyst.Finally,as a proof-of-concept for overall water splitting,we constructed a full-cell configuration based on a locally-doped MoS_(2)monolayer,which achieved a cell voltage of 1.87 V at 10 mA·cm^(-2),demonstrating outstanding performance in strong acid electrolytes.Our work provides insight into the hetero-integration of bifunctional electrocatalysts at the atomic level,paving the way for designing transition metal dichalcogenide catalysts with activity-manipulated regions capable of multiple reactions.
