TY - JOUR
T1 - The Design of Supramolecular Assemblies with Metal Salt as Precursors Enables The Growth of Stable Polymeric Carbon Nitride Photoanodes
AU - Garg, Devesh
AU - Shmila, Tirza
AU - Mark, Gabriel
AU - Mondal, Sanjit
AU - Battula, Venugopala Rao
AU - Volokh, Michael
AU - Shalom, Menny
N1 - Publisher Copyright:
© 2023 The Authors. Advanced Sustainable Systems published by Wiley-VCH GmbH.
PY - 2024/4/1
Y1 - 2024/4/1
N2 - Polymeric carbon nitrides (CN) have gained significant interest as photoanodes in photoelectrochemical cells (PEC). A widely researched approach for synthesizing CN films with controlled optical and photoelectrochemical properties relies on using supramolecular assemblies as the precursors for thermal polymerization over a transparent conductive substrate. However, the formation of supramolecular assemblies is highly dependent on the temperature and solubility in a given solvent, limiting the full potential of this method. Moreover, the intercalation of metal ions is challenging due to the use of polar solvents. Here, this study shows a new way of synthesizing supramolecular assemblies with metal ions using a solvothermal approach. The solvent, monomer composition, salt quantity, reaction temperature, and film thickness are varied in this study. As a result, well-attached, uniform CN films with good optoelectronic properties are achieved. The synthesized photoactive CN films exhibit very low onset potentials and reach ≈0.13, ≈0.15, and 0.30 ± 0.01 mA cm−2 photocurrents in 0.1 m phosphate buffer (neutral) solution, 0.1 m KOH(aq) (basic) solution, and 0.1 m KOH solution containing 10 vol.% triethanolamine as the hole scavenger, respectively.
AB - Polymeric carbon nitrides (CN) have gained significant interest as photoanodes in photoelectrochemical cells (PEC). A widely researched approach for synthesizing CN films with controlled optical and photoelectrochemical properties relies on using supramolecular assemblies as the precursors for thermal polymerization over a transparent conductive substrate. However, the formation of supramolecular assemblies is highly dependent on the temperature and solubility in a given solvent, limiting the full potential of this method. Moreover, the intercalation of metal ions is challenging due to the use of polar solvents. Here, this study shows a new way of synthesizing supramolecular assemblies with metal ions using a solvothermal approach. The solvent, monomer composition, salt quantity, reaction temperature, and film thickness are varied in this study. As a result, well-attached, uniform CN films with good optoelectronic properties are achieved. The synthesized photoactive CN films exhibit very low onset potentials and reach ≈0.13, ≈0.15, and 0.30 ± 0.01 mA cm−2 photocurrents in 0.1 m phosphate buffer (neutral) solution, 0.1 m KOH(aq) (basic) solution, and 0.1 m KOH solution containing 10 vol.% triethanolamine as the hole scavenger, respectively.
KW - carbon nitride
KW - photoelectrochemical cell
KW - supramolecular assemblies
KW - water-splitting
UR - http://www.scopus.com/inward/record.url?scp=85180714456&partnerID=8YFLogxK
U2 - 10.1002/adsu.202300447
DO - 10.1002/adsu.202300447
M3 - Article
AN - SCOPUS:85180714456
SN - 2366-7486
VL - 8
JO - Advanced Sustainable Systems
JF - Advanced Sustainable Systems
IS - 4
M1 - 2300447
ER -