Mg-doped Ta3N5 nanorods coated with a conformal CoOOH layer for water oxidation: bulk and surface dual modification of photoanodes

Mg-doped Ta3N5 nanorods coated with a conformal CoOOH layer for water oxidation: bulk and surface dual modification of photoanodes
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涂覆有共形 CoOOH 层的掺镁 Ta3N5 纳米棒用于水氧化:光电阳极的本体和表面双重改性

DOI:
10.1039/c7ta06227c
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发表时间:
2017-10
影响因子:
11.9
通讯作者:
Zou Zhigang
Zou Zhigang
中科院分区:
材料科学2区
文献类型:
--
作者:
Pei Lang;Xu Zhe;Shi Zhan;Zhu Heng;Yan Shicheng;Zou Zhigang

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电荷分离/转移和光腐蚀是限制Ta 3 N5光催化剂光电化学(PEC)应用的两个主要因素。本文采用助熔剂辅助晶体生长法制备了Mg掺杂的Ta 3 N5单晶纳米棒,旨在缩短电荷传输距离,提高电导率。优化的Mg掺杂Ta 3 N5光阳极表现出前所未有的PEC水分解活性,在1.23 VRHE下AM 1.5G光电流为1.5 mA cm−2。高性能归因于这样一个事实,即体改性,Mg掺杂,可以诱导氧杂质的表面态作为有效的电子陷阱中心,从而提高Ta 3 N5的导电性和电荷分离效率。在通过简单的电沉积方法用CoOOH作为水氧化电催化剂进行保形表面改性以改善空穴提取和反应动力学之后,Mg掺杂的Ta 3 N5光阳极提供超过4倍的光电流增加(约1.5倍)。6.5 mA cm-2,在1.23 VRHE下),并且在1.0 VRHE下照射70分钟后初始光电流保持约70%。研究结果表明,本体和表面共改性是开发高性能PEC水裂解装置的有效途径。
Charge separation/transfer and photocorrosion are two major factors limiting the photoelectrochemical (PEC) applications of the Ta3N5 photocatalyst. Herein, we have fabricated Ta3N5 single-crystal nanorods with Mg doping by flux-assisted crystal growth, aiming to shorten the charge transport distance and increase the electrical conductivity. The optimized Mg-doped Ta3N5 photoanodes exhibit an unprecedented PEC water splitting activity with an AM 1.5G photocurrent of 1.5 mA cm−2 at 1.23 VRHE. The high performance is attributed to the fact that the bulk modification, Mg doping, can induce oxygen-impurity surface states as effective electron trap centers, thus increasing the electrical conductivity of Ta3N5 and charge separation efficiency. After a conformal surface modification with CoOOH by a simple electrodeposition method as a water oxidation electrocatalyst to improve the hole extraction and reaction kinetics, the Mg-doped Ta3N5 photoanodes afford an over 4-fold increase in photocurrent (ca. 6.5 mA cm−2 at 1.23 VRHE) and about 70% retention of the initial photocurrent after 70 min irradiation at 1.0 VRHE. Our results testify that the bulk and surface co-modification is an effective route to develop high-performance PEC water splitting devices.
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