Issue 22, 2023

Iron phthalocyanine derived Fe1/h-BN single atom catalysts for CO2 hydrogenation

Abstract

Iron phthalocyanine-coated hexagonal boron nitride (FePc/h-BN) nanoparticles, obtained by FePcCl adsorption on the h-BN surface from a dimethylformamide solution, were subjected to heat treatment in order to form single atom Fe1/h-BN catalysts. Samples were characterized by means of X-ray diffraction, Raman spectroscopy, Fourier transform infrared spectroscopy, scanning and transmission electron microscopy, and temperature-programmed oxidation/reduction/desorption. The FePc deposition process was optimized to avoid the formation of nanoparticles. FePc exhibits high thermal stability in a hydrogen atmosphere and decomposes into a single iron atom when oxidizing in an O2 flow at 350 °C (sample Fe1-ox/h-BN). Subsequent reductive heat treatment in hydrogen (sample Fe1-red/h-BN) results in the formation of Fe-based nanoparticles due to Fe1 diffusion and association, resulting in a decrease in catalytic activity. Hydrogenation proceeds according to the Eley–Rideal mechanism with CO2 chemisorption on the Fe1 surface species (Fe1-ox/h-BN) and is changed to the Langmuir–Hinshelwood mechanism (Fe1-red/h-BN). Selectivity for hydrocarbons increases after reduction of the Fe1-ox/h-BN sample. Our results open up new possibilities for using metal phthalocyanine as a precursor for cheap, reproducible, and efficient single atom catalysts for CO2 hydrogenation.

Graphical abstract: Iron phthalocyanine derived Fe1/h-BN single atom catalysts for CO2 hydrogenation

Supplementary files

Article information

Article type
Paper
Submitted
19 Jan 2023
Accepted
09 May 2023
First published
23 May 2023

J. Mater. Chem. A, 2023,11, 11874-11888

Iron phthalocyanine derived Fe1/h-BN single atom catalysts for CO2 hydrogenation

D. V. Leybo, A. A. Ryzhova, A. T. Matveev, K. L. Firestein, P. A. Tarakanov, A. S. Konopatsky, A. L. Trigub, E. V. Sukhanova, Z. I. Popov, D. V. Golberg and D. V. Shtansky, J. Mater. Chem. A, 2023, 11, 11874 DOI: 10.1039/D3TA00356F

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