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用于太阳能水分解的半透明氮化钽光阳极半导体特性的物理化学见解。

Physicochemical insights into semiconductor properties of a semitransparent tantalum nitride photoanode for solar water splitting.

作者信息

Higashi Tomohiro, Nishiyama Hiroshi, Pihosh Yuriy, Wakishima Kaisei, Kawase Yudai, Sasaki Yutaka, Nagaoka Akira, Yoshino Kenji, Takanabe Kazuhiro, Domen Kazunari

机构信息

Institute for Tenure Track Promotion, University of Miyazaki, 1-1 Gakuen-kibanadai-nishi, Miyazaki 889-2192, Japan.

Office of University Professors, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-8656, Japan.

出版信息

Phys Chem Chem Phys. 2023 Aug 2;25(30):20737-20748. doi: 10.1039/d3cp02563b.

Abstract

The self-conductivity of tantalum nitride (TaN) thin film-based semitransparent photoanodes was found to promote the current originating from the photoelectrochemical oxygen evolution reaction (PEC OER) without a conducting substrate. With surface modification by the NiFeO-electrocatalyst, an optimized TaN thin film fabricated directly on a transparent insulating quartz substrate generated a photocurrent density of ∼5.9 ± 0.1 mA cm at 1.23 V the reversible hydrogen electrode under simulated AM 1.5G solar illumination. The correlation between the PEC OER performance of NiFeO-modified TaN photoanodes and the electrical properties of TaN thin films was investigated based on the Hall effect measurements. By changing the nitridation conditions, these properties can be tuned so that the higher the Hall mobility (0.2 to 1.7 cm V s) and the lower the carrier concentration (10 to 10 cm). The surface chemical states of TaN thin films were investigated using X-ray photoelectron spectroscopy as a means of evaluating surface oxygen impurities and nitrogen vacancies, which may correlate with the PEC OER performance and the electrical properties of the material.

摘要

研究发现,基于氮化钽(TaN)薄膜的半透明光阳极的自导电性可在无导电基底的情况下促进源自光电化学析氧反应(PEC OER)的电流。通过用NiFeO电催化剂进行表面改性,直接在透明绝缘石英基底上制备的优化TaN薄膜在模拟AM 1.5G太阳光照下,于1.23 V(相对于可逆氢电极)时产生了约5.9±0.1 mA cm的光电流密度。基于霍尔效应测量,研究了NiFeO改性TaN光阳极的PEC OER性能与TaN薄膜电学性质之间的相关性。通过改变氮化条件,可以调节这些性质,使得霍尔迁移率越高(0.2至1.7 cm² V⁻¹ s⁻¹)且载流子浓度越低(10¹⁸至10²⁰ cm⁻³)。使用X射线光电子能谱研究了TaN薄膜的表面化学状态,以此作为评估表面氧杂质和氮空位的手段,这些可能与材料的PEC OER性能和电学性质相关。

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