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Hydrogen Production and Utilization in a Membrane Reactor

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Modulation of Phosphorene for Optimal Hydrogen Evolution Reaction.

Jiang Lu¹, Xue Zhang¹, Danni Liu¹

¹Shenzhen Institutes of Advanced Technology , Chinese Academy of Sciences , Shenzhen 518055 , P. R. China.

ACS Applied Materials & Interfaces

|September 26, 2019

Summary

Few-layer black phosphorus (phosphorene) shows promise for hydrogen evolution reaction (HER) catalysis. Modifying phosphorene with edges, defects, and metal adatoms enhances its catalytic activity by optimizing hydrogen adsorption.

Keywords:

electronic structure first-principle calculation hydrogen evolution reaction phosphorene two-dimensional materials

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Area of Science:

Materials Science
Electrochemistry
Catalysis

Background:

Economical and effective catalysts are essential for the electrocatalytic hydrogen evolution reaction (HER).
Few-layer black phosphorus (phosphorene) is a promising HER catalyst due to its high carrier mobility, large surface area, and tunable properties.
The intrinsic HER activity of phosphorene is limited by weak hydrogen adsorption on its basal plane.

Purpose of the Study:

To create optimal active sites on phosphorene to enhance its electrocatalytic hydrogen evolution reaction (HER) activity.
To investigate the theoretical and experimental effectiveness of modified phosphorene as an HER catalyst.

Main Methods:

Density-functional theory (DFT) calculations were employed to investigate the electronic structure and HER activity.
Experimental verification was performed to validate theoretical predictions.
Analysis focused on the relationship between electronic properties (lowest unoccupied states, ε_LUS) and HER activity.

Main Results:

Edges and defects significantly influence the electronic density of states in phosphorene.
A linear relationship was established between HER activity and the lowest unoccupied states (ε_LUS), with medium ε_LUS values indicating optimal hydrogen adsorption.
Smaller phosphorene structures with more edges and defects exhibited enhanced HER activity.
Surface doping with metal adatoms further improved the catalytic performance.

Conclusions:

Modified phosphorene, particularly with engineered edges, defects, and metal adatom doping, demonstrates significant potential for efficient HER.
The study provides a convenient standard for exploring ideal electrocatalysts based on the relationship between electronic structure and catalytic activity.