Simultaneous enhancements in photon absorption and charge transport of bismuth vanadate photoanodes for solar water splitting

Nature Communications - Tập 6 Số 1
Tae Woo Kim1, Yuan Ping2, Giulia Galli3, Kyoung‐Shin Choi1
1Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706 USA
2Department of Chemistry University of California Davis California 95616 USA
3Institute for Molecular Engineering, University of Chicago, Chicago, Illinois 60637, USA

Tóm tắt

Abstractn-Type bismuth vanadate has been identified as one of the most promising photoanodes for use in a water-splitting photoelectrochemical cell. The major limitation of BiVO4 is its relatively wide bandgap (∼2.5 eV), which fundamentally limits its solar-to-hydrogen conversion efficiency. Here we show that annealing nanoporous bismuth vanadate electrodes at 350 °C under nitrogen flow can result in nitrogen doping and generation of oxygen vacancies. This gentle nitrogen treatment not only effectively reduces the bandgap by ∼0.2 eV but also increases the majority carrier density and mobility, enhancing electron–hole separation. The effect of nitrogen incorporation and oxygen vacancies on the electronic band structure and charge transport of bismuth vanadate are systematically elucidated by ab initio calculations. Owing to simultaneous enhancements in photon absorption and charge transport, the applied bias photon-to-current efficiency of nitrogen-treated BiVO4 for solar water splitting exceeds 2%, a record for a single oxide photon absorber, to the best of our knowledge.

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