Bae Sanghyun, Moehl Thomas, Service Erin, Kim Minjung, Adams Pardis, Wang Zhenbin, Choi Yuri, Ryu Jungki, Tilley S David
Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057, Zurich, Switzerland.
School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919, Republic of Korea.
Nat Commun. 2024 Nov 1;15(1):9439. doi: 10.1038/s41467-024-53754-9.
The use of conductive and corrosion-resistant protective layers represents a key strategy for improving the durability of light absorber materials in photoelectrochemical water splitting. For high performance photoanodes such as Si, GaAs, and GaP, amorphous TiO protective overlayers, deposited by atomic layer deposition, are conductive for holes via a defect band in the TiO. However, when coated on simply prepared, low-cost photoanodes such as metal oxides, no charge transfer is observed through amorphous TiO. Here, we report a hybrid polyethyleneimine/TiO layer that facilitates hole transfer from model oxides BiVO and FeO, enabling access to a broader scope of available materials for practical water oxidation. A thin polyethyleneimine layer between the light absorber and the hybrid polyethyleneimine/TiO acts as a hole-selective interface, improving the optoelectronic properties of the photoanode devices. These polyethyleneimine/TiO modified photoanodes exhibit high photostability for solar water oxidation over 400 h.
使用导电且耐腐蚀的保护层是提高光吸收材料在光电化学水分解中耐久性的关键策略。对于诸如硅、砷化镓和磷化镓等高性能光阳极，通过原子层沉积法沉积的非晶态二氧化钛保护覆盖层，通过二氧化钛中的缺陷带对空穴具有导电性。然而，当涂覆在简单制备的低成本光阳极（如金属氧化物）上时，未观察到通过非晶态二氧化钛的电荷转移。在此，我们报道了一种聚乙烯亚胺/二氧化钛混合层，它有助于空穴从模型氧化物钒酸铋和氧化铁中转移，从而能够使用更广泛的可用材料来进行实际的水氧化。光吸收体与聚乙烯亚胺/二氧化钛混合层之间的薄聚乙烯亚胺层充当空穴选择性界面，改善了光阳极器件的光电性能。这些聚乙烯亚胺/二氧化钛修饰的光阳极在超过400小时的太阳能水氧化过程中表现出高光稳定性。
