材料科学
光电流
兴奋剂
半导体
接受者
带隙
载流子
光电子学
分解水
离子键合
化学物理
离子
光电导性
俘获
纳米技术
凝聚态物理
光催化
生态学
生物化学
化学
物理
量子力学
生物
催化作用
作者
Laura I. Wagner,Elise Sirotti,Oliver Brune,Gabriel Grötzner,Johanna Eichhorn,Saswati Santra,F. Munnik,Luca Olivi,Simone Pollastri,Verena Streibel,Ian D. Sharp
标识
DOI:10.1002/adfm.202306539
摘要
Abstract While Ta 3 N 5 shows excellent potential as a semiconductor photoanode for solar water splitting, its performance is hindered by poor charge carrier transport and trapping due to native defects that introduce electronic states deep within its bandgap. Here, it is demonstrated that controlled Ti doping of Ta 3 N 5 can dramatically reduce the concentration of deep‐level defects and enhance its photoelectrochemical performance, yielding a sevenfold increase in photocurrent density and a 300 mV cathodic shift in photocurrent onset potential compared to undoped material. Comprehensive characterization reveals that Ti 4+ ions substitute Ta 5+ lattice sites, thereby introducing compensating acceptor states, reducing the concentrations of deleterious nitrogen vacancies and reducing Ta 3+ states, and thereby suppressing trapping and recombination. Owing to the similar ionic radii of Ti 4+ and Ta 5+ , substitutional doping does not introduce lattice strain or significantly affect the underlying electronic structure of the host semiconductor. Furthermore, Ti can be incorporated without increasing the oxygen donor content, thereby enabling the electrical conductivity to be tuned by over seven orders of magnitude. Thus, Ti doping of Ta 3 N 5 provides a powerful basis for precisely engineering its optoelectronic characteristics and to substantially improve its functional characteristics as an advanced photoelectrode for solar fuels applications.
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