Oriented attachment growth of hundred-nanometer-size LaTaON2 single crystals in molten salts for enhanced photoelectrochemical water splitting

Oriented attachment growth of hundred-nanometer-size LaTaON2 single crystals in molten salts for enhanced photoelectrochemical water splitting
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熔盐中百纳米级LaTaON2单晶的定向附着生长增强光电化学水分解

DOI:
10.1039/c8ta02233j
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发表时间:
2018-05
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:
Zhou Junkang;Zhou Chenguang;Shi Zhan;Xu Zhe;Yan Shicheng;Zou Zhigang

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定向附着(OA)已被广泛用作描述通过晶体学对准进行的基于溶液的颗粒(通常,尺寸<10 nm)生长的术语。通过OA结晶过程进行大尺寸晶体生长的一个大挑战是去除导致OA组装过程发生的添加剂。在这里,我们发现,熔盐环境是一个理想的介质,为OA生长的大尺寸无机颗粒,而不需要任何添加剂。例如,在Li离子基熔融盐中,没有特定形态的100纳米尺寸的LaTaON 2单晶可以自发地组装成微米尺寸的规则晶体。理论和实验证据表明,大尺寸晶体中的OA生长过程是静电排斥和货车范德华吸引之间的平衡,这种平衡可以通过正负离子在晶体表面的吸附差异来调节。最后,由于晶界处电荷复合的显著减少,大单晶电极在1.23VRHE下表现出5.1 mA cm-2的增强光电化学性能,这是先前报道的LaTaON 2光电阳极中的最高性能。我们的研究结果提供了一种新的方法来组装先进的纳米器件的大尺寸单晶。
Oriented attachment (OA) has been widely used as a term to describe solution-based particle (generally, <10 nm in size) growth proceeding by crystallographic alignment. A big challenge in large-sized crystal growth by the OA crystallization process is the removal of the additives that cause the OA assembling process to occur. Here, we find that the molten salt environment is an ideal medium for OA growth of large-sized inorganic particles without the requirement of any additives. As an example, in Li ion-based molten salts, hundred-nanometer-size LaTaON2 single crystals with no specific morphology can spontaneously assemble into micrometer-size regular crystals. Theoretical and experimental evidence indicated that this OA growth process among the large-sized crystals is governed by a trade-off between electrostatic repulsion and van der Waals attraction, which can be adjusted by the adsorption difference of positive and negative ions on the crystal surface. Finally, due to the significant decrease in charge recombination at grain boundaries, the large single crystal electrode exhibited an enhanced photoelectrochemical performance of 5.1 mA cm−2 at 1.23VRHE, the highest performance among the previously reported LaTaON2 photoanodes. Our findings offer a new approach to assemble large-size single crystals for advanced nanodevices.
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