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Functional Photo-electrochemical Devices for Solar Cellsand Solar Fuels Based on Molecular Components
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis concerns the development and the study of molecular functional photo-electrochemical cells (PEC) for solar cells and solar fuels.

The first chapter gives a general introduction about photosynthesis, dye-sensitized solar cell and photo-electrochemical device for water splitting.

The second chapter describes a TiO2-Co-catalyst electrode manufactured by a direct photo-deposition method. The electrode showed activity for electrochemical water oxidation in an electrochemical device.

In the third chapter, a photo-electrochemical cell (PEC) with two-electrodes for visible light driven water splitting has been successfully demonstrated. One electrode was a photo-anode, which assembled a ruthenium water oxidation catalyst (complex 1) into a dye-sensitized porous nanostructured TiO2 electrode by employing a cation-exchange membrane (Nafion). The other electrode was platinum which was used as a passive cathode for proton reduction.

In the fourth chapter, an earth abundant metal complex with an anchoring group (cobalt complex 2) was synthesized and investigated as water oxidation catalyst. This complex was further applied into a photo-anode in a PEC. The photo-anode was assembled by co-sensitization of complex 2 to a dye-sensitized porous nanostructured TiO2 electrode. The PEC device gave ca. 250 υA/cm2 photo-current and 7.2 % IPCE without applying any bias voltage, which is much higher than the reported results in the sample type of PEC. Meanwhile, we have shown that the catalytic effect is not from free cobalt ions, CoOx film or nanoparticles formed in situ by using complex 2 in the device.

The last two chapters describe an optimization of the NiO films prepared in two steps rather than one step film and applied in p-type DSSCs. This optimized film could adsorb more dye (P1), leading to a significant light harvesting efficiency (LHE) and IPCE in DSSCs. We further combined this P1 sensitized photo-cathode with a hydrogen evolution catalyst (complex 3) and applied this photo-cathode into a PEC for visible light hydrogen evolution.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2012. , 71 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2012:51
Keyword [en]
artificial photosynthesis, dye sensitized solar cell, hydrogen generation catalyst, nickel oxide (NiO), titanium dioxide (TiO2), water oxidation catalyst, water splitting
National Category
Other Chemical Engineering
Identifiers
URN: urn:nbn:se:kth:diva-103623OAI: oai:DiVA.org:kth-103623DiVA: diva2:560993
Public defence
2012-11-09, F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20121017

Available from: 2012-10-17 Created: 2012-10-16 Last updated: 2012-10-17Bibliographically approved
List of papers
1. Double-Layered NiO Photocathodes for p-Type DSSCs with Record IPCE
Open this publication in new window or tab >>Double-Layered NiO Photocathodes for p-Type DSSCs with Record IPCE
Show others...
2010 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 22, no 15, 1759-1762 p.Article in journal (Refereed) Published
Abstract [en]

A way to achieve a high-efficiency dye-sensitized solar cell is to combine an n-type TiO2-based photoanode with a p-type photocathode in a tandem configuration. The development of an efficient photocathode is, at present, the key target. We have optimized the NiO, I-3(-)/I- p-DSSC system to obtain record photocurrent, giving 64% incident photon-to-current conversion efficiency (IPCE) and 5.48 mAcm(-2) J(SC).

National Category
Organic Chemistry
Identifiers
urn:nbn:se:kth:diva-24441 (URN)10.1002/adma.200903151 (DOI)000277369600011 ()2-s2.0-77951192634 (Scopus ID)
Note
QC 20100909Available from: 2010-09-09 Created: 2010-09-09 Last updated: 2017-12-12Bibliographically approved
2. A photoelectrochemical device for visible light driven water splitting by a molecular ruthenium catalyst assembled on dye-sensitized nanostructured TiO2
Open this publication in new window or tab >>A photoelectrochemical device for visible light driven water splitting by a molecular ruthenium catalyst assembled on dye-sensitized nanostructured TiO2
Show others...
2010 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 46, no 39, 7307-7309 p.Article in journal (Refereed) Published
Abstract [en]

A photoelectrochemical device with a molecular Ru catalyst assembled via pH-modified Nafion on a dye-sensitized nanostructured TiO2 film as anode and a Pt foil as cathode has been successfully demonstrated to split water into O-2 and H-2 driven by visible light.

Keyword
OXIDATION CATALYST, ARTIFICIAL PHOTOSYNTHESIS, POLYMER MEMBRANE, COMPLEX
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-26665 (URN)10.1039/c0cc01828g (DOI)000282218200003 ()2-s2.0-77957673474 (Scopus ID)
Note
QC 20101201Available from: 2010-12-01 Created: 2010-11-26 Last updated: 2017-12-12Bibliographically approved
3. Visible light driven hydrogen production from a photo-active cathode based on a molecular catalyst and organic dye-sensitized p-type nanostructured NiO
Open this publication in new window or tab >>Visible light driven hydrogen production from a photo-active cathode based on a molecular catalyst and organic dye-sensitized p-type nanostructured NiO
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2012 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 48, no 7, 988-990 p.Article in journal (Refereed) Published
Abstract [en]

A molecular device with a photocathode for hydrogen generation has been successfully demonstrated, based on an earth abundant and inexpensive p-type semiconductor NiO, an organic dye P1 and a cobalt catalyst Co1.

National Category
Organic Chemistry
Identifiers
urn:nbn:se:kth:diva-90643 (URN)10.1039/c2cc16101j (DOI)000299649900013 ()2-s2.0-84855394496 (Scopus ID)
Note
QC 20120315Available from: 2012-03-15 Created: 2012-02-27 Last updated: 2017-12-07Bibliographically approved
4. Electrochemical water oxidation by photo-deposited cobalt-based catalyst on a nano-structured TiO2 electrode
Open this publication in new window or tab >>Electrochemical water oxidation by photo-deposited cobalt-based catalyst on a nano-structured TiO2 electrode
2012 (English)In: Science China Chemistry, ISSN 1674-7291, Vol. 55, no 9, 1976-1981 p.Article in journal (Refereed) Published
Abstract [en]

A cobalt-based catalyst was directly photo-deposited on the surface of a widely used n-type nano-structured semiconductor (TiO2). Different thicknesses of the TiO2 films as well as different time of photo-deposition of the Co-based catalyst on TiO2 films have been optimized. It was found that the electrode with 3 layers of TiO2 film (in 8 mu m thickness) and 1 hour photo-deposition of the cobalt-based catalyst by light irradiation from a 500 W Xenon lamp gave the highest current density (similar to 5 mA/cm(2)). Using this cobalt-modified TiO2 film as a working electrode in an electrochemical device, highly efficient water oxidation has been demonstrated in a pH 7.0 aqueous solution with low overpotential.

Keyword
artificial photosynthesis, electrochemical water oxidation, cobalt-based catalyst, photo-deposition, water splitting
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-103149 (URN)10.1007/s11426-012-4551-8 (DOI)000308192400039 ()2-s2.0-84866136614 (Scopus ID)
Funder
Knut and Alice Wallenberg Foundation
Note

QC 20121017

Available from: 2012-10-09 Created: 2012-10-04 Last updated: 2012-10-17Bibliographically approved
5. Electrocatalytic water splitting: A bi-functional water-soluble molecular Co-based complex for both catalytic water oxidation and hydrogen generation
Open this publication in new window or tab >>Electrocatalytic water splitting: A bi-functional water-soluble molecular Co-based complex for both catalytic water oxidation and hydrogen generation
(English)Manuscript (preprint) (Other academic)
National Category
Organic Chemistry
Identifiers
urn:nbn:se:kth:diva-103681 (URN)
Note

QS 2012

Available from: 2012-10-17 Created: 2012-10-17 Last updated: 2012-10-17Bibliographically approved
6. A photoelectrochemical device for visible light driven water splitting with a molecular cobalt complex assembled on dye-sensitized porous nanocrystalline TiO2 electrode
Open this publication in new window or tab >>A photoelectrochemical device for visible light driven water splitting with a molecular cobalt complex assembled on dye-sensitized porous nanocrystalline TiO2 electrode
Show others...
(English)Manuscript (preprint) (Other academic)
National Category
Organic Chemistry
Identifiers
urn:nbn:se:kth:diva-103684 (URN)
Note

QS 2012

Available from: 2012-10-17 Created: 2012-10-17 Last updated: 2012-10-17Bibliographically approved

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