Regulating chemical bonds to balance the adsorption and disassociation of water molecules on catalyst surfaces is crucial for overall water splitting in alkaline solution.Here we report a facile strategy for designing...Regulating chemical bonds to balance the adsorption and disassociation of water molecules on catalyst surfaces is crucial for overall water splitting in alkaline solution.Here we report a facile strategy for designing Ni2W4C-W3C Janus structures with abundant Ni-W metallic bonds on surfaces through interfacial engineering.Inserting Ni atoms into the W3C crystals in reaction progress generates a new Ni2 W4C phase,making the inert W atoms in W3C be active sites in Ni2W4C for overall water splitting.The Ni2W4CW3C/carbon nanofibers(Ni2 W4-W3C/CNFs)require overpotentials of 63 mV to reach 10 mA cm^-2 for hydrogen evolution reaction(HER)and 270 mV to reach 30 mA cm^-2 for oxygen evolution reaction(OER)in alkaline electrolyte,respectively.When utilized as both cathode and anode in alkaline solution for overall water splitting,cell voltages of 1.55 and 1.87 V are needed to reach 10 and 100 mA cm^-2,respectively.Density functional theory(DFT)results indicate that the strong interactions between Ni and W increase the local electronic states of W atoms.The Ni2W4C provides active sites for cleaving H-OH bonds,and the W3C facilitates the combination of Hads intermediates into H2 molecules.The in situ electrochemical-Raman results demonstrate that the strong absorption ability for hydroxyl and water molecules and further demonstrate that W atoms are the real active sites.展开更多
基金supported by the National Natural Science Foundation of China(51803077,51872204)the National Key Research and Development Program of China(2017YFA0204600)+4 种基金the Natural Science Foundation of Jiangsu Province(BK20180627)Postdoctoral Science Foundation of China(2018M630517,2019T120389)the Ministry of Education(MOE)and the State Administration for Foreign Expert Affairs(SAFEA),111 Project(B13025)the National First-Class Discipline Program of Light Industry Technology and Engineering(LITE2018-19)the Fundamental Research Funds for the Central Universities。
文摘Regulating chemical bonds to balance the adsorption and disassociation of water molecules on catalyst surfaces is crucial for overall water splitting in alkaline solution.Here we report a facile strategy for designing Ni2W4C-W3C Janus structures with abundant Ni-W metallic bonds on surfaces through interfacial engineering.Inserting Ni atoms into the W3C crystals in reaction progress generates a new Ni2 W4C phase,making the inert W atoms in W3C be active sites in Ni2W4C for overall water splitting.The Ni2W4CW3C/carbon nanofibers(Ni2 W4-W3C/CNFs)require overpotentials of 63 mV to reach 10 mA cm^-2 for hydrogen evolution reaction(HER)and 270 mV to reach 30 mA cm^-2 for oxygen evolution reaction(OER)in alkaline electrolyte,respectively.When utilized as both cathode and anode in alkaline solution for overall water splitting,cell voltages of 1.55 and 1.87 V are needed to reach 10 and 100 mA cm^-2,respectively.Density functional theory(DFT)results indicate that the strong interactions between Ni and W increase the local electronic states of W atoms.The Ni2W4C provides active sites for cleaving H-OH bonds,and the W3C facilitates the combination of Hads intermediates into H2 molecules.The in situ electrochemical-Raman results demonstrate that the strong absorption ability for hydroxyl and water molecules and further demonstrate that W atoms are the real active sites.
