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Sol−Gel Processing of Water‐Soluble Carbon Nitride Enables High‐Performance Photoanodes **
Author(s) -
Adler Christiane,
Krivtsov Igor,
Mitoraj Dariusz,
SantosGómez Lucía,
GarcíaGranda Santiago,
Neumann Christof,
Kund Julian,
Kranz Christine,
Mizaikoff Boris,
Turchanin Andrey,
Beranek Radim
Publication year - 2021
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.202100313
Subject(s) - carbon nitride , sol gel , nitride , materials science , carbon fibers , water splitting , nanotechnology , chemical engineering , water soluble , chemistry , photocatalysis , catalysis , organic chemistry , layer (electronics) , engineering , composite material , composite number
In spite of the enormous promise that polymeric carbon nitride (PCN) materials hold for various applications, the fabrication of high‐quality, binder‐free PCN films and electrodes has been a largely elusive goal to date. Here, we tackle this challenge by devising, for the first time, a water‐based sol−gel approach that enables facile preparation of thin films based on poly(heptazine imide) (PHI), a polymer belonging to the PCN family. The sol−gel process capitalizes on the use of a water‐soluble PHI precursor that allows formation of a non‐covalent hydrogel. The hydrogel can be deposited on conductive substrates, resulting in formation of mechanically stable polymeric thin layers. The resulting photoanodes exhibit unprecedented photoelectrochemical (PEC) performance in alcohol reforming and highly selective (∼100 %) conversions with very high photocurrents (>0.25 mA cm −2 under 2 sun) down to <0 V vs. RHE. This enables even effective PEC operation under zero‐bias conditions and represents the very first example of a ‘soft matter’‐based PEC system capable of bias‐free photoreforming. The robust binder‐free films derived from sol−gel processing of water‐soluble PCN thus constitute a new paradigm for high‐performance ‘soft matter’ photoelectrocatalytic systems and pave the way for further applications in which high‐quality PCN films are required.