Investigation of effects of sulfur on dry reforming of biogas over nickel–iron based catalysts


Genc A., Arbağ H., Taşdemir H. M., Yaşyerli N., Yaşyerli S.

International Journal of Hydrogen Energy, cilt.48, sa.60, ss.23031-23043, 2023 (SCI-Expanded) identifier identifier

  • Yayın Türü: Makale / Tam Makale
  • Cilt numarası: 48 Sayı: 60
  • Basım Tarihi: 2023
  • Doi Numarası: 10.1016/j.ijhydene.2023.04.130
  • Dergi Adı: International Journal of Hydrogen Energy
  • Derginin Tarandığı İndeksler: Science Citation Index Expanded (SCI-EXPANDED), Scopus, Academic Search Premier, PASCAL, Artic & Antarctic Regions, Chemical Abstracts Core, Communication Abstracts, Environment Index, INSPEC
  • Sayfa Sayıları: ss.23031-23043
  • Anahtar Kelimeler: Dry reforming of methane, H2S, Iron, Nickel, Sulfur
  • Gazi Üniversitesi Adresli: Evet

Özet

The aim of this study is to maintain and increase the activity of the catalyst in the presence of H2S with the addition of iron to the Ni catalyst. Alumina-supported monometallic iron and bimetallic nickel-iron catalysts with different weight percentages (8% Fe, 3% Ni – 3% Fe and 8% Ni – 8% Fe) were synthesized using the wet impregnation method in this study. Alumina was prepared by the sol-gel method. The activities of these synthesized catalysts in the methane dry reforming reaction were investigated at different H2S concentrations (0 ppm, 2 ppm, and 50 ppm) with a total flow rate of 60 mL/min containing an equimolar ratio of CH4, CO2, and Ar at 750 °C and atmospheric pressure. To investigate the effect of sulfur compounds on the catalytic activity, the catalysts were also exposed to different gas compositions such as the mixture of H2S + He, H2S + CO2 + He, and H2S + CO2 + CH4 + He. In this case, FT-IR with a gas cell was used to determine the components in the gas stream at the reactor outlet. To explain catalytic performance, characterization studies were carried out using XRD, N2 adsorption/desorption, DRIFT, SEM, TGA, and XPS analysis. All-synthesized materials showed Type-IV isotherm with a hysteresis loop corresponding to an ordered mesoporous structure. The DRIFT analysis showed a decrease in the Lewis acid sites after the addition of iron into the Ni-catalysts. In the activity test carried out in the presence of 50 ppm H2S, it was observed that the iron-containing 8Ni–8Fe@SGA catalyst increased the sulfur resistance slightly, compared to the monometallic 8Ni@SGA catalyst. TGA analysis showed that Fe addition reduced coke deposition, as the Ni–Fe catalyst had a lower nickel crystal size than the Ni-based catalyst. FTIR analysis with a gas cell showed that sulfur in H2S transformed to other sulfur compounds such as COS and/or SO2 during dry reforming of biogas over alumina-supported Ni–Fe catalysts.