Bottom-up fabrication of BN-doped graphene electrodes from thiol-terminated borazine molecules working in solar cells

Ibarra-Barreno, Carolina M., Chowdhury, Sanchari, Crosta, Martina, Zehra, Tashfeen, Fasano, Francesco, Kundu, Paromita, Verstraelen, Jenthe, Bals, Sara, Subrati, Mohammed, Bonifazi, Davide ORCID: https://orcid.org/0000-0001-5717-0121, Costa, Rubén D. and Rudolf, Petra 2025. Bottom-up fabrication of BN-doped graphene electrodes from thiol-terminated borazine molecules working in solar cells. ACS Applied Materials & Interfaces 10.1021/acsami.4c23116

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Abstract

Graphene exhibits exceptional properties, including high tensile strength, mechanical stiffness, and electron mobility. Chemical functionalization of graphene with boron and nitrogen is a powerful strategy for tuning these properties for specific applications. Molecular self-assembly provides an efficient pathway for the tailored synthesis of doped graphene, depending on the molecular precursor used. This study presents a scalable approach to synthesizing large-area boron- and nitrogen-doped graphene using two borazine precursors bearing thiol functionalities. After self-assembly on electropolished polycrystalline copper foil, the precursors undergo photopolymerization under UV irradiation, and subsequent annealing in vacuum transforms the cross-linked BN-doped layer into a graphenoid structure. X-ray photoelectron spectroscopy confirms the integration of the borazine rings into the BNC architecture, while Raman spectroscopy reveals a red shift in the characteristic G bands along with intense and broad D bands, highlighting boron–nitrogen contributions. Transmission electron microscopy provides insight into the morphology and structural quality of the BNC films. The BNC films were successfully integrated as counter electrodes in dye-sensitized solar cells, achieving a power conversion efficiency of up to 6% under 1 sun illumination and 11.8% under low-intensity indoor ambient light. Hence, this work not only establishes a straightforward, controllable route for heteroatom doping but also introduces a novel concept of Pt-free counter electrodes for efficient indoor energy harvesting applications.

Item Type:	Article
Date Type:	Published Online
Status:	Published
Schools:	Schools > Chemistry
Additional Information:	License information from Publisher: LICENSE 1: URL: https://creativecommons.org/licenses/by/4.0/, Start Date: 2025-04-02
Publisher:	American Chemical Society
ISSN:	1944-8244
Date of First Compliant Deposit:	15 April 2025
Date of Acceptance:	17 March 2025
Last Modified:	15 Apr 2025 09:45
URI:	https://orca.cardiff.ac.uk/id/eprint/177689

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