Cu-incorporated NH2-MIL-125(Ti): a versatile visible-light-driven platform for enhanced photocatalytic H2 generation and CO2 photoconversion

Anna Pancielejko; Mateusz A Baluk; Hanna Zagórska; Magdalena Miodyńska-Melzer; Anna Gołąbiewska; Tomasz Klimczuk; Mirosław Krawczyk; Mirosława Pawlyta; Krzysztof Matus; Alicja Mikolajczyk; Henry P Pinto; Aleksandra Pieczyńska; Joanna Dołżonek; Adriana Zaleska-Medynska

doi:10.1039/d4mh01116c

Cu-incorporated NH₂-MIL-125(Ti): a versatile visible-light-driven platform for enhanced photocatalytic H₂ generation and CO₂ photoconversion

Mater Horiz. 2024 Nov 15. doi: 10.1039/d4mh01116c. Online ahead of print.

Authors

Affiliations

¹ Department of Environmental Technology, Faculty of Chemistry, University of Gdansk, 80-308 Gdansk, Poland. anna.pancielejko@ug.edu.pl.
² Faculty of Applied Physics and Mathematics and Advanced Materials Centre, Gdansk University of Technology, 80-233 Gdansk, Poland.
³ Institute of Physical Chemistry, Polish Academy of Sciences, 01-224 Warsaw, Poland.
⁴ Faculty of Mechanical Engineering, Silesian University of Technology, 44-100 Gliwice, Poland.
⁵ Laboratory of Environmental Chemoinformatics, Faculty of Chemistry, University of Gdansk, 80-308 Gdansk, Poland.
⁶ QSAR LAB, 80-172 Gdansk, Poland.
⁷ CompNano Group, School of Physical Sciences and Nanotechnology, Yachay Tech University, Urcuqui 100119, Ecuador.
⁸ Department of Environmental Analysis, Faculty of Chemistry, University of Gdańsk, 80-309 Gdansk, Poland.

PMID: 39545857
DOI: 10.1039/d4mh01116c

Abstract

Here, we present for the first time an efficient platform for simultaneous H₂ generation and CO₂ conversion into HCOOH, utilizing a Cu-incorporated NH₂-MIL-125(Ti) material with triethanolamine as the sacrificial agent. When subjected to light, Cu-NH₂-MIL-125(Ti) exhibits a remarkable enhancement in H₂ generation, with a 30-fold increase under UV-Vis light and an 8-fold increase under visible irradiation compared to the pristine MOF. The study on the CO₂ photoreduction ability of Cu-NH₂-MIL-125(Ti) indicated successful conversion into formic acid yielding 62.4 μmol g_cat^-1 under visible irradiation. This notable improvement in photocatalytic activity can be attributed to the heightened light absorption capacity and efficient charge transportation and separation mechanisms inherent in Cu-NH₂-MIL-125(Ti). Furthermore, the stability of the Cu-NH₂-MIL-125(Ti) photocatalyst remains steady even after 24 hours of continuous irradiation. The theoretical simulations suggest that Cu introduction effectively reduces the bandgap while leaving the position and composition of the valence band unaffected.