Engineering g-C3N4 with CuAl-layered double hydroxide in 2D/2D heterostructures for visible-light water splitting

Hanane Boumeriame; Alexey Cherevan; Dominik Eder; Dogukan H Apaydin; Tarik Chafik; Eliana S Da Silva; Joaquim L Faria

doi:10.1016/j.jcis.2023.08.159

Engineering g-C₃N₄ with CuAl-layered double hydroxide in 2D/2D heterostructures for visible-light water splitting

J Colloid Interface Sci. 2023 Dec 15;652(Pt B):2147-2158. doi: 10.1016/j.jcis.2023.08.159. Epub 2023 Aug 26.

Authors

Hanane Boumeriame¹, Alexey Cherevan², Dominik Eder³, Dogukan H Apaydin³, Tarik Chafik⁴, Eliana S Da Silva⁵, Joaquim L Faria⁶

Affiliations

¹ LSRE-LCM - Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias s/n, 4200-465 Porto, Portugal; ALiCE - Associate Laboratory in Chemical Engineering, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias, 4200-465 Porto, Portugal; Laboratory of Chemical Engineering and Valorization of Resources (LGCVR-UAE/L01FST), Faculty of Sciences and Techniques, University Abdelmalek Essaadi, Tangier, Morocco; Institute of Materials Chemistry, Technische Universität Wien (TU Wien), Getreidemarkt 9, Vienna 1060, Austria.
² Institute of Materials Chemistry, Technische Universität Wien (TU Wien), Getreidemarkt 9, Vienna 1060, Austria. Electronic address: alexey.cherevan@tuwien.ac.at.
³ Institute of Materials Chemistry, Technische Universität Wien (TU Wien), Getreidemarkt 9, Vienna 1060, Austria.
⁴ Laboratory of Chemical Engineering and Valorization of Resources (LGCVR-UAE/L01FST), Faculty of Sciences and Techniques, University Abdelmalek Essaadi, Tangier, Morocco.
⁵ LSRE-LCM - Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias s/n, 4200-465 Porto, Portugal; ALiCE - Associate Laboratory in Chemical Engineering, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias, 4200-465 Porto, Portugal.
⁶ LSRE-LCM - Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias s/n, 4200-465 Porto, Portugal; ALiCE - Associate Laboratory in Chemical Engineering, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias, 4200-465 Porto, Portugal. Electronic address: jlfaria@fe.up.pt.

PMID: 37703684
DOI: 10.1016/j.jcis.2023.08.159

Abstract

CuAl layered double hydroxide (LDH) and polymeric carbon nitride (g-C₃N₄, GCNN) were assembled to construct a set of novel 2D/2D CuAl-LDH/GCNN heterostructures. These materials were tested towards H₂ and O₂ generation from water splitting using visible-light irradiation. Compared to pristine materials, the heterostructures displayed strongly enhanced visible-light H₂ evolution, dependent on the LDH content, which acts as a cocatalyst, replacing the benchmark Pt. The optimal LDH loading was achieved for 0.2CuAl-LDH/GCNN that exhibited an increased number of active sites and showed a trade-off between charge separation efficiency and light shading, resulting in a 32-fold increase in the amount of evolved H₂ compared with GCNN. In addition, the 0.2CuAl-LDH/GCNN heterostructure generated 1.5 times more O₂ than GCNN. The higher photocatalytic performance was due to efficient charge carriers' separation at the heterojunction interface via an S-scheme (corroborated by work function, steady-state and time-resolved photoluminescence studies), enhanced utilisation of longer-wavelength photons (>460 nm) and higher surface area available for the catalytic reactions.

Keywords: 2D/2D heterostructure; CuAl layered double hydroxide; Graphitic carbon nitride; Photocatalytic water splitting; S-scheme heterojunction.