Tin doping speeds up hole transfer during light-driven water oxidation at hematite photoanodes.

نویسندگان

  • Halina K Dunn
  • Johann M Feckl
  • Alexander Müller
  • Dina Fattakhova-Rohlfing
  • Samuel G Morehead
  • Julian Roos
  • Laurence M Peter
  • Christina Scheu
  • Thomas Bein
چکیده

Numerous studies have shown that the performance of hematite photoanodes for light-driven water splitting is improved substantially by doping with various metals, including tin. Although the enhanced performance has commonly been attributed to bulk effects such as increased conductivity, recent studies have noted an impact of doping on the efficiency of the interfacial transfer of holes involved in the oxygen evolution reaction. However, the methods used were not able to elucidate the origin of this improved efficiency, which could originate from passivation of surface electron-hole recombination or catalysis of the oxygen evolution reaction. The present study used intensity-modulated photocurrent spectroscopy (IMPS), which is a powerful small amplitude perturbation technique that can de-convolute the rate constants for charge transfer and recombination at illuminated semiconductor electrodes. The method was applied to examine the kinetics of water oxidation on thin solution-processed hematite model photoanodes, which can be Sn-doped without morphological change. We observed a significant increase in photocurrent upon Sn-doping, which is attributed to a higher transfer efficiency. The kinetic data obtained using IMPS show that Sn-doping brings about a more than tenfold increase in the rate constant for water oxidation by photogenerated holes. This result provides the first demonstration that Sn-doping speeds up water oxidation on hematite by increasing the rate constant for hole transfer.

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

منابع مشابه

Onset potential behavior in α-Fe2O3 photoanodes: the influence of surface and diffusion Sn doping on the surface states.

The onset potential is an important parameter that affects the water oxidation performance of photoanodes. Herein, we investigated the behavior of the photocurrent onset potential of hematite (α-Fe2O3) photoanodes by incorporating Sn(4+) cations via external (surface overlayer) or self (underlying FTO substrate) doping. The α-Fe2O3/FTO photoanodes fabricated at both low (550 °C) and high (800 °...

متن کامل

Doping-Promoted Solar Water Oxidation on Hematite Photoanodes.

As one of the most promising materials for solar water oxidation, hematite has attracted intense research interest for four decades. Despite their desirable optical band gap, stability and other attractive features, there are great challenges for the implementation of hematite-based photoelectrochemical cells. In particular, the extremely low electron mobility leads to severe energy loss by ele...

متن کامل

Solution growth of Ta-doped hematite nanorods for efficient photoelectrochemical water splitting: a tradeoff between electronic structure and nanostructure evolution.

Ta-doped hematite (α-Fe2O3) nanorod array films were successfully prepared on fluorine-doped tin dioxide (FTO) coated glass substrates via a facile solution growth process with TaCl5 as a Ta doping precursor. Under 1 sun illumination and at an applied potential of 1.0 V vs. Ag/AgCl, the Ta-doped α-Fe2O3 photoanode with optimized dopant concentration showed a photocurrent density as high as 0.53...

متن کامل

Surface Engineered Doping of Hematite Nanorod Arrays for Improved Photoelectrochemical Water Splitting

Given the narrow band gap enabling excellent optical absorption, increased charge carrier density and accelerated surface oxidation reaction kinetics become the key points for improved photoelectrochemical performances for water splitting over hematite (α-Fe2O3) photoanodes. In this study, a facile and inexpensive method was demonstrated to develop core/shell structured α-Fe2O3 nanorod arrays. ...

متن کامل

ذخیره در منابع من


  با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

عنوان ژورنال:
  • Physical chemistry chemical physics : PCCP

دوره 16 44  شماره 

صفحات  -

تاریخ انتشار 2014