Unique 3D heterojunction photoanode design to harness charge transfer for efficient and stable photoelectrochemical water splitting
Unique 3D heterojunction photoanode design to harness charge transfer for efficient and stable photoelectrochemical water splitting
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独特的 3D 异质结光阳极设计，利用电荷转移实现高效稳定的光电化学水分解
DOI：
10.1039/c4ee03707c
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发表时间：
2015-04
影响因子：
32.5
通讯作者：
Hongmin Zhu
中科院分区：
文献类型：
--
作者：
Jungang Hou;Huijie Cheng;Osamu Takeda;Hongmin Zhu
氮氧化物光电化学（PEC）太阳能分解水是一种很有前途的可再生制氢方法。然而，氮氧化物异质结光阳极具有高的电荷分离效率和稳定性，具有独特的尺寸依赖性的综合和协同效应，是有趣的，但仍不发达。本文设计并制备了具有高光电转换活性的一维/二维纳米棒/纳米片组装氮氧化钽（TaON）光阳极。特别是，首先制备了包括1D/2D钡掺杂的TaON（Ba-TaON）阵列和用CoOx纳米颗粒装饰的2D氮化碳（C3 N4）纳米片的集成3D异质结光阳极作为新的堆叠设计，并且3D CoOx/C3 N4/Ba-TaON纳米片被用于制备3D异质结光阳极。具有显著光稳定性的TaON光阳极在AM 1.5G模拟太阳光下在1.23 V vs. RHE下达到4.57 mA cm−2的显著光电流。更广泛地说，这种独特的3D异质结光电阳极的线束电荷转移过程的内在要求已被确定的定量分析结合电化学阻抗和光致发光分析。所有的结果突出了三维尺寸相关的异质结作为一个有前途的光电极模型在太阳能转换中的应用的重要意义。纳米工程的组合物调节，形态创新和异质结结构的协同放大效应为创造更具目的设计的高效性能（氧）氮化物光电极提供了有价值的见解。
Photoelectrochemical (PEC) solar water splitting over oxynitrides is a promising process for renewable hydrogen production. However, the oxynitride heterojunction photoanodes with high charge-separation efficiency and stability, which have unique dimensionality-dependent integrative and synergic effects, are intriguing but still underdeveloped. Here, we design and fabricate the 1D/2D nanorod/nanosheet-assembled tantalum oxynitride (TaON) photoanode with the high PEC activity. Especially, integrated 3D heterojunction photoanodes comprising the 1D/2D barium-doped TaON (Ba-TaON) array and 2D carbon nitride (C3N4) nanosheets decorated with CoOx nanoparticles as a novel stack design were firstly prepared and the 3D CoOx/C3N4/Ba-TaON photoanodes with the remarkable photostability reached the pronounced photocurrent of 4.57 mA cm−2 at 1.23 V vs. RHE under AM 1.5G simulated sunlight. More broadly, the harness charge transfer process of this unique 3D heterojunction photoanode with the intrinsic requirements has been identified by the quantitative analysis combined with the electrochemical impedance and photoluminescence analysis. All the results highlight the great significance of the 3D dimensionality-dependent heterojunction as a promising photoelectrode model for the application in solar conversion. The cooperating amplification effects of nanoengineering from composition regulation, morphology innovation and heterojunction construction provide a valuable insight for creating more purpose-designed (oxy)nitride photoelectrodes with highly efficient performance.
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