Abstract
Rational design and controlled synthesis of hybrid structures comprising multiple components with distinctive functionalities are an intriguing and challenging approach to materials development for important energy applications like electrocatalytic hydrogen production, where there is a great need for cost effective, active and durable catalyst materials to replace the precious platinum. Here we report a structure design and sequential synthesis of a highly active and stable hydrogen evolution electrocatalyst material based on pyrite-structured cobalt phosphosulfide nanoparticles grown on carbon nanotubes. The three synthetic steps in turn render electrical conductivity, catalytic activity and stability to the material. The hybrid material exhibits superior activity for hydrogen evolution, achieving current densities of 10 mA cm−2 and 100 mA cm−2 at overpotentials of 48 mV and 109 mV, respectively. Phosphorus substitution is crucial for the chemical stability and catalytic durability of the material, the molecular origins of which are uncovered by X-ray absorption spectroscopy and computational simulation.
Highlights
Rational design and controlled synthesis of hybrid structures comprising multiple components with distinctive functionalities are an intriguing and challenging approach to materials development for important energy applications like electrocatalytic hydrogen production, where there is a great need for cost effective, active and durable catalyst materials to replace the precious platinum
We report a design and synthesis of a highly active and stable hydrogen evolution reaction (HER) electrocatalyst material consisting of pyrite-structured cobalt phosphosulfide (CoS|P) nanoparticles anchored on carbon nanotubes (CNTs)
The material architecture is built by a three-step chemical synthesis: Strong interactions with CNTs and particle size control are first established by the selective growth of cobalt(II,III) oxide (Co3O4) nanoparticles on CNTs; High catalytic activity for HER is rendered by conversion of Co3O4 to CoS2 nanoparticles; Good chemical stability and catalytic durability are lastly obtained from substituting some of the sulfur with phosphorus
Summary
Rational design and controlled synthesis of hybrid structures comprising multiple components with distinctive functionalities are an intriguing and challenging approach to materials development for important energy applications like electrocatalytic hydrogen production, where there is a great need for cost effective, active and durable catalyst materials to replace the precious platinum. We report a structure design and sequential synthesis of a highly active and stable hydrogen evolution electrocatalyst material based on pyrite-structured cobalt phosphosulfide nanoparticles grown on carbon nanotubes. We report a design and synthesis of a highly active and stable HER electrocatalyst material consisting of pyrite-structured cobalt phosphosulfide (CoS|P) nanoparticles anchored on carbon nanotubes (CNTs). Phosphorus substitution in the pyrite structure is a critical step that renders chemical stability and catalytic durability to the CoS|P/CNT hybrid material. Density functional theory (DFT) calculations confirm the structural stability of pyrite CoS|P and suggest stronger metal–ligand bonding as a contributor to the improved stability, which is supported by X-ray absorption spectroscopy data
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