Empirical in Operando Analysis of the Charge Carrier Dynamics in Hematite Photoanodes by PEIS, IMPS and IMVS

Overview

Journal Phys Chem Chem Phys

Publisher Royal Society of Chemistry

Specialties Biophysics
Chemistry

Date 2016 Aug 16

PMID 27524381

Citations 12

Authors

Dino Klotz

David Shai Ellis

Hen Dotan

Avner Rothschild

Affiliations

Soon will be listed here.

Abstract

In this Perspective, we introduce intensity modulated photocurrent/voltage spectroscopy (IMPS and IMVS) as powerful tools for the analysis of charge carrier dynamics in photoelectrochemical (PEC) cells for solar water splitting, taking hematite (α-Fe2O3) photoanodes as a case study. We complete the picture by including photoelectrochemical impedance spectroscopy (PEIS) and linking the trio of PEIS, IMPS and IMVS, introduced here as photoelectrochemical immittance triplets (PIT), both mathematically and phenomenologically, demonstrating what conclusions can be extracted from these measurements. A novel way of analyzing the results by an empirical approach with minimal presumptions is introduced, using the distribution of relaxation times (DRT) function. The DRT approach is compared to conventional analysis approaches that are based on physical models and therefore come with model presumptions. This work uses a thin film hematite photoanode as a model system, but the approach can be applied to other PEC systems as well.

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References

Klahr B, Gimenez S, Fabregat-Santiago F, Bisquert J, Hamann T . Photoelectrochemical and impedance spectroscopic investigation of water oxidation with "Co-Pi"-coated hematite electrodes. J Am Chem Soc. 2012; 134(40):16693-700. DOI: 10.1021/ja306427f. View

Iandolo B, Wickman B, Seger B, Chorkendorff I, Zoric I, Hellman A . Faradaic efficiency of O2 evolution on metal nanoparticle sensitized hematite photoanodes. Phys Chem Chem Phys. 2013; 16(3):1271-5. DOI: 10.1039/c3cp54288b. View

Le Formal F, Pastor E, Tilley S, Mesa C, Pendlebury S, Gratzel M . Rate law analysis of water oxidation on a hematite surface. J Am Chem Soc. 2015; 137(20):6629-37. PMC: 4448182. DOI: 10.1021/jacs.5b02576. View

Kirchartz T, Bisquert J, Mora-Sero I, Garcia-Belmonte G . Classification of solar cells according to mechanisms of charge separation and charge collection. Phys Chem Chem Phys. 2015; 17(6):4007-14. DOI: 10.1039/c4cp05174b. View

Ding C, Wang Z, Shi J, Yao T, Li A, Yan P . Substrate-Electrode Interface Engineering by an Electron-Transport Layer in Hematite Photoanode. ACS Appl Mater Interfaces. 2016; 8(11):7086-91. DOI: 10.1021/acsami.5b12818. View

Klahr B, Gimenez S, Fabregat-Santiago F, Hamann T, Bisquert J . Water oxidation at hematite photoelectrodes: the role of surface states. J Am Chem Soc. 2012; 134(9):4294-302. DOI: 10.1021/ja210755h. View

Zandi O, Hamann T . The potential versus current state of water splitting with hematite. Phys Chem Chem Phys. 2015; 17(35):22485-503. DOI: 10.1039/c5cp04267d. View

Dotan H, Mathews N, Hisatomi T, Gratzel M, Rothschild A . On the Solar to Hydrogen Conversion Efficiency of Photoelectrodes for Water Splitting. J Phys Chem Lett. 2015; 5(19):3330-4. DOI: 10.1021/jz501716g. View

Le Formal F, Pendlebury S, Cornuz M, Tilley S, Gratzel M, Durrant J . Back electron-hole recombination in hematite photoanodes for water splitting. J Am Chem Soc. 2014; 136(6):2564-74. DOI: 10.1021/ja412058x. View

10.

Cummings C, Marken F, Peter L, Tahir A, Upul Wijayantha K . Kinetics and mechanism of light-driven oxygen evolution at thin film α-Fe2O3 electrodes. Chem Commun (Camb). 2012; 48(14):2027-9. DOI: 10.1039/c2cc16382a. View

11.

Tilley S, Cornuz M, Sivula K, Gratzel M . Light-induced water splitting with hematite: improved nanostructure and iridium oxide catalysis. Angew Chem Int Ed Engl. 2010; 49(36):6405-8. DOI: 10.1002/anie.201003110. View

12.

Cummings C, Marken F, Peter L, Upul Wijayantha K, Tahir A . New insights into water splitting at mesoporous α-Fe2O3 films: a study by modulated transmittance and impedance spectroscopies. J Am Chem Soc. 2011; 134(2):1228-34. DOI: 10.1021/ja209530s. View

13.

Lopes T, Andrade L, Le Formal F, Gratzel M, Sivula K, Mendes A . Hematite photoelectrodes for water splitting: evaluation of the role of film thickness by impedance spectroscopy. Phys Chem Chem Phys. 2014; 16(31):16515-23. DOI: 10.1039/c3cp55473b. View

14.

Barroso M, Mesa C, Pendlebury S, Cowan A, Hisatomi T, Sivula K . Dynamics of photogenerated holes in surface modified α-Fe2O3 photoanodes for solar water splitting. Proc Natl Acad Sci U S A. 2012; 109(39):15640-5. PMC: 3465443. DOI: 10.1073/pnas.1118326109. View

15.

Chae Y, Kim S, Ellinger J, Markley J . Tracing Metabolite Footsteps of Along the Time Course of Recombinant Protein Expression by Two-Dimensional NMR Spectroscopy. Bull Korean Chem Soc. 2013; 33(12):4041-4046. PMC: 3686544. DOI: 10.5012/bkcs.2012.33.12.4041. View

16.

Warren S, Voitchovsky K, Dotan H, Leroy C, Cornuz M, Stellacci F . Identifying champion nanostructures for solar water-splitting. Nat Mater. 2013; 12(9):842-9. DOI: 10.1038/nmat3684. View

17.

Halme J . Linking optical and electrical small amplitude perturbation techniques for dynamic performance characterization of dye solar cells. Phys Chem Chem Phys. 2011; 13(27):12435-46. DOI: 10.1039/c1cp21134j. View

18.

Dunn H, Feckl J, Muller A, Fattakhova-Rohlfing D, Morehead S, Roos J . Tin doping speeds up hole transfer during light-driven water oxidation at hematite photoanodes. Phys Chem Chem Phys. 2014; 16(44):24610-20. DOI: 10.1039/c4cp03946g. View

19.

Peter L, Upul Wijayantha K, Tahir A . Kinetics of light-driven oxygen evolution at alpha-Fe2O3 electrodes. Faraday Discuss. 2012; 155:309-22. DOI: 10.1039/c1fd00079a. View

20.

Thorne J, Jang J, Liu E, Wang D . Understanding the origin of photoelectrode performance enhancement by probing surface kinetics. Chem Sci. 2018; 7(5):3347-3354. PMC: 6006950. DOI: 10.1039/c5sc04519c. View