NiO/Poly(4-alkylthiazole) Hybrid Interface for Promoting Spatial Charge Separation in Photoelectrochemical Water Reduction

ACS Applied Materials & Interfaces, vol. 12, pp. 29173–29180

Abstract

Abstract Conjugated polymers are emerging as alternatives to inorganic semiconductors for the photoelectrochemical water splitting. Herein, semi-transparent poly(4-alkylthiazole) layers with different trialkylsilyloxymethyl (R3SiOCH2−) side chains (PTzTNB, R = n-butyl; PTzTHX, R = n-hexyl) are applied to functionalize NiO thin films to build hybrid photocathodes. The hybrid interface allows for the effective spatial separation of the photoexcited carriers. Specifically, the PTzTHX-deposited composite photocathode increases the photocurrent density 6- and 2-fold at 0 V versus the reversible hydrogen electrode in comparison to the pristine NiO and PTzTHX photocathodes, respectively. This is also reflected in the substantial anodic shift of onset potential under simulated Air Mass 1.5 Global illumination, owing to the prolonged lifetime, augmented density, and alleviated recombination of photogenerated electrons. Additionally, coupling the inorganic and organic components also enhances the photoabsorption and amends the stability of the photocathode-driven system. This work demonstrates the feasibility of poly(4-alkylthiazole)s as an effective alternative to known inorganic semiconductor materials. We highlight the interface alignment for polymer-based photoelectrodes.

Authors 9

1. Can Lu Aachen Institute of Inorganic Chemistry

   RWTH Aachen University

   Affiliation as printed

   RWTH Aachen University , , Landoltweg 1 , ,

   Institute of Inorganic Chemistry, RWTH Aachen University, Landoltweg 1, D-52056 Aachen, Germany

2. Zili Ma Aachen Institute of Inorganic Chemistry

   RWTH Aachen University

   Affiliation as printed

   RWTH Aachen University , , Landoltweg 1 , ,

   Institute of Inorganic Chemistry, RWTH Aachen University, Landoltweg 1, D-52056 Aachen, Germany

3. Jakob Jäger

   Carl Zeiss (Germany) · Universität Ulm

   Affiliation as printed

   University of Ulm , , Albert-Einstein-Allee 11 , ,

   Zeiss Group , , Carl-Zeiss-Straße 22 , ,

   Carl Zeiss Jena GmbH, Zeiss Group, Carl-Zeiss-Straße 22, D-73447 Oberkochen, Germany

   Institute of Organic Chemistry II and Advanced Materials, University of Ulm, Albert-Einstein-Allee 11, D-89081 Ulm, Germany

4. Tetyana M. Budnyak

   Stockholm University

   Affiliation as printed

   Stockholm University , , Svante Arrhenius väg 16C , ,

   Department of Materials and Environmental Chemistry, Stockholm University, Svante Arrhenius väg 16C, 10691 Stockholm, Sweden

5. Richard Dronskowski Aachen Institute of Inorganic Chemistry

   Shenzhen Polytechnic University · RWTH Aachen University

   Affiliation as printed

   RWTH Aachen University , , Landoltweg 1 , ,

   Shenzhen Polytechnic , , Liuxian Boulevard 7098 , , ,

   Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic, Liuxian Boulevard 7098, Shenzhen, Guangdong 518055, People's Republic of China

   Institute of Inorganic Chemistry, RWTH Aachen University, Landoltweg 1, D-52056 Aachen, Germany

6. Anna Rokicińska

   Jagiellonian University

   Affiliation as printed

   Jagiellonian University , , Gronostajowa 2 , ,

   Faculty of Chemistry, Jagiellonian University, Gronostajowa 2, 30-387 Krakow, Poland

7. Piotr Kuśtrowski

   Jagiellonian University

   Affiliation as printed

   Jagiellonian University , , Gronostajowa 2 , ,

   Faculty of Chemistry, Jagiellonian University, Gronostajowa 2, 30-387 Krakow, Poland

8. Frank Pammer

   Universität Ulm

   Affiliation as printed

   University of Ulm , , Albert-Einstein-Allee 11 , ,

   Institute of Organic Chemistry II and Advanced Materials, University of Ulm, Albert-Einstein-Allee 11, D-89081 Ulm, Germany

9. Adam Slabon corresponding

   Stockholm University

   Affiliation as printed

   Stockholm University , , Svante Arrhenius väg 16C , ,

   Department of Materials and Environmental Chemistry, Stockholm University, Svante Arrhenius väg 16C, 10691 Stockholm, Sweden