A stable and highly active core‐shell heterostructure electrocatalyst is essential for catalyzing oxygen evolution reaction(OER).Here,a dual‐trimetallic core‐shell heterostructure OER electrocatalyst that consists ...A stable and highly active core‐shell heterostructure electrocatalyst is essential for catalyzing oxygen evolution reaction(OER).Here,a dual‐trimetallic core‐shell heterostructure OER electrocatalyst that consists of a NiFeWS_(2)inner core and an amorphous NiFeW(OH)_(z)outer shell is designed and synthesized using in situ electrochemical tuning.The electrochemical measurements of different as‐synthesized catalysts with a similar mass loading suggest that the core‐shell Ni_(0.66)Fe_(0.17)W_(0.17)S_(2)@amorphous NiFeW(OH)_(z)nanosheets exhibit the highest overall performance compared with that of other bimetallic reference catalysts for the OER.Additionally,the nanosheet arrays were in situ grown on hydrophilic‐treated carbon paper to fabricate an integrated three‐dimensional electrode that affords a current density of 10 mA cm^(−2)at a small overpotential of 182 mV and a low Tafel slope of 35 mV decade^(−1)in basic media.The Faradaic efficiency of core‐shell Ni_(0.66)Fe_(0.17)W_(0.17)S_(2)@amorphous NiFeW(OH)_(z)is as high as 99.5%for OER.The scanning electron microscope,transmission electron microscope,and X‐ray photoelectron spectroscopy analyses confirm that this electrode has excellent stability in morphology and elementary composition after long‐term electrochemical measurements.Importantly,density functional theory calculations further indicate that the core‐shell heterojunction increased the conductivity of the catalyst,optimized the adsorption energy of the OER intermediates,and improved the OER activity.This study provides a universal strategy for designing more active core‐shell structure electrocatalysts based on the rule of coordinated regulation between electronic transport and active sites.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:21978160,52003300,52373087Shaanxi Province Natural Science Foundation,Grant/Award Number:2024JC‐YBMS‐131。
文摘A stable and highly active core‐shell heterostructure electrocatalyst is essential for catalyzing oxygen evolution reaction(OER).Here,a dual‐trimetallic core‐shell heterostructure OER electrocatalyst that consists of a NiFeWS_(2)inner core and an amorphous NiFeW(OH)_(z)outer shell is designed and synthesized using in situ electrochemical tuning.The electrochemical measurements of different as‐synthesized catalysts with a similar mass loading suggest that the core‐shell Ni_(0.66)Fe_(0.17)W_(0.17)S_(2)@amorphous NiFeW(OH)_(z)nanosheets exhibit the highest overall performance compared with that of other bimetallic reference catalysts for the OER.Additionally,the nanosheet arrays were in situ grown on hydrophilic‐treated carbon paper to fabricate an integrated three‐dimensional electrode that affords a current density of 10 mA cm^(−2)at a small overpotential of 182 mV and a low Tafel slope of 35 mV decade^(−1)in basic media.The Faradaic efficiency of core‐shell Ni_(0.66)Fe_(0.17)W_(0.17)S_(2)@amorphous NiFeW(OH)_(z)is as high as 99.5%for OER.The scanning electron microscope,transmission electron microscope,and X‐ray photoelectron spectroscopy analyses confirm that this electrode has excellent stability in morphology and elementary composition after long‐term electrochemical measurements.Importantly,density functional theory calculations further indicate that the core‐shell heterojunction increased the conductivity of the catalyst,optimized the adsorption energy of the OER intermediates,and improved the OER activity.This study provides a universal strategy for designing more active core‐shell structure electrocatalysts based on the rule of coordinated regulation between electronic transport and active sites.