The rational design and construction of inexpensive and highly active electrocatalysts for hydrogen evolution reaction(HER)is of great importance for water splitting.Herein,we develop a facile approach for preparation...The rational design and construction of inexpensive and highly active electrocatalysts for hydrogen evolution reaction(HER)is of great importance for water splitting.Herein,we develop a facile approach for preparation of porous carbon-confined Ru-doped Cu nanoparticles(denoted as Ru-Cu@C)by direct pyrolysis of the Ru-exchanged Cu-BTC metal–organic framework.When served as the electrocatalyst for HER,strikingly,the obtained Ru-Cu@C catalyst exhibits an ultralow overpotential(only 20 mV at 10 mA cm^(-2))with a small Tafel slope of 37 m V dec^(-1)in alkaline electrolyte.The excellent performance is comparable or even superior to that of commercial Pt/C catalyst.Density functional theory(DFT)calculations confirm that introducing Ru atoms into Cu nanocrystals can significantly alter the desorption of H_(2) to achieve a close-to-zero hydrogen adsorption energy and thereby boost the HER process.This strategy gives a fresh impetus to explore low-cost and high-performance catalysts for HER in alkaline media.展开更多
Supramolecular assemblies are introduced here as new-concept hard templates for the synthesis of hollow nanostructures(exemplified with Ti O2 hollow nanostructures in this work). Supramolecular templates with tunable ...Supramolecular assemblies are introduced here as new-concept hard templates for the synthesis of hollow nanostructures(exemplified with Ti O2 hollow nanostructures in this work). Supramolecular templates with tunable morphology and rich surface functional groups facilitate the tight coating of other materials for the formation of hollow nanostructures. The weak interaction between the supramolecules or micromolecules benefits the facile removal of the templates for large-scale synthesis of hollow nanostructures and also affords excellent template reusability. This method allows for the incorporation of various metal dopants into the Ti O2 lattice, as a typical example of nanocatalyst, by introducing the corresponding metal salt as a dopant source. High-resolution transmission electron microscopy(HRTEM), X-ray diffraction(XRD) and UV-vis absorption spectroscopy investigations suggested substitution of Ti4+ sites by Co2+, which increased the activity of the catalytic sites in the doped materials, reducing the overpotential of Ti O2 for the oxygen evolution reaction.展开更多
基金the National Key R&D Program of China(2018YFB0605700)the National Natural Science Foundation of China(51778570,51879230,21725101,21871244,21521001,and 21703145)+1 种基金China Postdoctoral Science Foundation(2019TQ0298,2019M660151)Fujian Institute of Innovation(CAS)。
文摘The rational design and construction of inexpensive and highly active electrocatalysts for hydrogen evolution reaction(HER)is of great importance for water splitting.Herein,we develop a facile approach for preparation of porous carbon-confined Ru-doped Cu nanoparticles(denoted as Ru-Cu@C)by direct pyrolysis of the Ru-exchanged Cu-BTC metal–organic framework.When served as the electrocatalyst for HER,strikingly,the obtained Ru-Cu@C catalyst exhibits an ultralow overpotential(only 20 mV at 10 mA cm^(-2))with a small Tafel slope of 37 m V dec^(-1)in alkaline electrolyte.The excellent performance is comparable or even superior to that of commercial Pt/C catalyst.Density functional theory(DFT)calculations confirm that introducing Ru atoms into Cu nanocrystals can significantly alter the desorption of H_(2) to achieve a close-to-zero hydrogen adsorption energy and thereby boost the HER process.This strategy gives a fresh impetus to explore low-cost and high-performance catalysts for HER in alkaline media.
基金financially supported by the National Basic Research Program of China (2013CB934102 and 2011CB808703)the National Natural Science Foundation of China (21331004 and 21301116)
文摘Supramolecular assemblies are introduced here as new-concept hard templates for the synthesis of hollow nanostructures(exemplified with Ti O2 hollow nanostructures in this work). Supramolecular templates with tunable morphology and rich surface functional groups facilitate the tight coating of other materials for the formation of hollow nanostructures. The weak interaction between the supramolecules or micromolecules benefits the facile removal of the templates for large-scale synthesis of hollow nanostructures and also affords excellent template reusability. This method allows for the incorporation of various metal dopants into the Ti O2 lattice, as a typical example of nanocatalyst, by introducing the corresponding metal salt as a dopant source. High-resolution transmission electron microscopy(HRTEM), X-ray diffraction(XRD) and UV-vis absorption spectroscopy investigations suggested substitution of Ti4+ sites by Co2+, which increased the activity of the catalytic sites in the doped materials, reducing the overpotential of Ti O2 for the oxygen evolution reaction.
