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Balancing Catalytic Activity and Interface Energetics of Electrocatalyst-Coated Photoanodes for Photoelectrochemical Water Splitting
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-01-19 00:00:00 , DOI: 10.1021/acsami.7b17348
Zhe Xu , Haoyu Wang , Yunzhou Wen 1 , Wenchao Li , Chuyu Sun , Yuting He , Zhan Shi , Lang Pei , Yongda Chen , Shicheng Yan , Zhigang Zou
Affiliation  

For photoelectrochemical (PEC) water splitting, the interface interactions among semiconductors, electrocatalysts, and electrolytes affect the charge separation and catalysis in turn. Here, through the changing of the bath temperature, Co-based oxygen evolution catalysts (OEC) with different crystallinities were electrochemically deposited on Ti-doped Fe2O3 (Ti–Fe2O3) photoanodes. We found: (1) the OEC with low crystallinity is highly ion-permeable, decreasing the interactions between OEC and photoanode due to the intimate interaction between semiconductor and electrolyte; (2) the OEC with high crystallinity is nearly ion-impermeable, is beneficial to form a constant buried junction with semiconductor, and exhibits the low OEC catalytic activity; and (3) the OEC with moderate crystallinity is partially electrolyte-screened, thus contributing to the formation of ideal band bending underneath surface of semiconductor for charge separation and the highly electrocatalytic activity of OEC for lowering over-potentials of water oxidation. Our results demonstrate that to balance the water oxidation activity of OEC and OEC–semiconductor interface energetics is crucial for highly efficient solar energy conversion; in particular, the energy transducer is a semiconductor with a shallow or moderate valence-band level.

中文翻译:

用于光电化学水分解的电催化剂涂覆光阳极的平衡催化活性和界面能

对于光电化学(PEC)水分解,半导体,电催化剂和电解质之间的界面相互作用依次影响电荷分离和催化作用。在这里,通过改变浴温,将具有不同结晶度的钴基氧析出催化剂(OEC)电化学沉积在掺Ti的Fe 2 O 3(Ti–Fe 2 O 3)上。)光阳极。我们发现:(1)低结晶度的OEC具有很高的离子渗透性,由于半导体与电解质之间的紧密相互作用,降低了OEC与光电阳极之间的相互作用;(2)高结晶度的OEC几乎不渗透离子,有利于与半导体形成恒定的掩埋结,并具有较低的OEC催化活性;(3)具有中等结晶度的OEC进行了部分电解质筛选,从而有助于在半导体表面下形成理想的能带弯曲以进行电荷分离以及OEC的高电催化活性,从而降低了水氧化的超电势。我们的结果表明,平衡OEC和OEC-半导体界面高能能的水氧化活性对于高效转换太阳能至关重要。
更新日期:2018-01-19
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