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Pristine Ta3 N5 Nanotubes: Trap-Driven High External Biasing Perspective in Semiconductor/Electrolyte Interfaces
Sherdil Khan1,2, Marcos J L Santos3, Célia F Malfatti2
1Instituto de Fisica, Universidade Federal do Rio Grande do Sul, Av. Bento Gonçalves, 9500 PO Box - 15051, 91501-970, Porto Alegre, RS, Brazil.
Chemistry (Weinheim an Der Bergstrasse, Germany)
|November 19, 2016
Summary
Pristine tantalum nitride (Ta3N5) photoelectrodes show poor solar water oxidation performance due to interband trapping states. Using a sacrificial agent or co-catalyst improves photocurrent by mitigating hole accumulation.
Area of Science:
- Materials Science
- Electrochemistry
- Renewable Energy
Background:
- Tantalum nitride (Ta3N5) is a promising material for solar hydrogen production.
- Pristine Ta3N5 photoelectrodes exhibit limited photoelectrochemical (PEC) performance, requiring significant external bias for water oxidation.
Purpose of the Study:
- Investigate the origin of limited PEC performance in pristine Ta3N5 photoelectrodes.
- Identify the factors hindering efficient water oxidation and explore methods for improvement.
Main Methods:
- Fabrication of Ta3N5 nanotubes (NTs) via nitridation.
- Characterization using various techniques, including a novel PEC method and synchrotron-excited XPS.
- Evaluation of photocurrent and transient behavior under water oxidation conditions with and without sacrificial agents.
Main Results:
- Synchrotron-excited XPS revealed reduced tantalum species within the Ta3N5 surface.
- Lower photocurrent and transient spikes were observed during water oxidation, which were suppressed by sacrificial agents.
- Identified interband trapping states at the Ta3N5/electrolyte junction as the cause of poor PEC performance and high biasing requirements.
Conclusions:
- Interband trapping states, linked to structural defects in Ta3N5, significantly impair PEC performance.
- Employing sacrificial agents or co-catalysts is crucial to prevent hole accumulation and enhance photocurrent during water oxidation.
- Findings offer insights into optimizing PEC properties of semiconducting devices.
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