State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, The Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Adv Mater. 2019 Apr;31(15):e1808185. doi: 10.1002/adma.201808185. Epub 2019 Feb 20.
Heterostructures are widely fabricated for promotion of photogenerated charge separation and solar cell/fuel production. (Oxy)nitrides are extremely promising for solar energy conversion, but the fabrication of heterostructures based on nitrogen-containing semiconductors is still challenging. Here, a simple ammonia thermal synthesis of a heterostructure (denoted as Ta N /BTON) composed of 1D Ta N nanorods and BaTaO N (BTON) nanoparticles (0D), which is demonstrated to result in a remarkable increase in photogenerated charge separation and solar hydrogen production from water, is introduced. As analyzed and discussed, the Ta N /BTON heterostructure is type II and tends to create intimate interfaces between the 1D nanorods and 0D nanoparticles. The 1D Ta N nanorods are demonstrated to transfer electrons along the rod orientation direction. Furthermore, the intimate interfaces of the heterostructure are believed to originate from the similar Ta-based octahedron units of Ta N and BTON. All of the above features are expected to integrally endow increased photoinduced charge separation and one order of magnitude higher solar overall water splitting activity with respect to counterpart systems. These results may open a new avenue to fabricate heterostructures on the basis of nitrogen-containing semiconductors that is extremely promising for solar energy conversion.
异质结构被广泛制备以促进光生电荷分离和太阳能电池/燃料生产。(氧)氮化物在太阳能转换方面极具前景,但基于含氮半导体的异质结构的制备仍然具有挑战性。本文介绍了一种通过氨热合成的由一维 TaN 纳米棒和 BaTaO3N(BTON)纳米颗粒(0D)组成的异质结构(记为 TaN/BTON)的简单方法,该异质结构显著提高了光生电荷分离和太阳能制氢效率。通过分析和讨论,发现 TaN/BTON 异质结构为 II 型,倾向于在一维纳米棒和 0D 纳米颗粒之间形成紧密的界面。一维 TaN 纳米棒被证明可以沿着棒的取向方向转移电子。此外,异质结构的紧密界面被认为源于 TaN 和 BTON 中类似的基于 Ta 的八面体单元。所有这些特征有望整体赋予光诱导电荷分离的增加,以及相对于对照体系一个数量级更高的太阳能整体水分解活性。这些结果可能为基于含氮半导体的异质结构的制备开辟一条新途径,这种异质结构在太阳能转换方面极具前景。