Intrinsic kinetics of plasmon-enhanced reverse water gas shift on Au and Au–Mo interfacial sites supported on silica

Abstract

Well characterized AuMo x catalysts were synthesized by controlled surface reactions (CSR) and studied in reverse water gas shift (RWGS) reaction with and without visible light addition. The numbers of Au and Au-Mo interfacial sites on these catalysts were quantified using low temperature (173 K) CO adsorption with Fourier transform infrared spectroscopy (FT-IR) and electron microscopy. Due to the localized surface plasmon resonance (LSPR) effect, visible light irradiation of the catalyst caused a decrease in the apparent activation energy from 80.2 ± 3.9 kJ/mol to 55.5 ± 3.1 kJ/mol and 67.5 ± 1.3 kJ/mol to 38.7 ± 1.9 kJ/mol with visible light irradiation over Au/SiO 2 and Au 1 Mo 0.1 /SiO 2 , respectively. The catalytic activity went through a maximum upon addition of Mo, with Au 1 Mo 0.1 /SiO 2 being the most active catalyst. The Au 1 Mo 0.1 catalyst with LSPR was 30 times more active than the reference Au catalyst under dark conditions. Visible light irradiation increased the reaction rate 4.7-4.8 times at 573 K for all catalysts. The turnover rates (CO mole produced per mole of Au or AuMo x site per min) on the Au and AuMo x interfacial sites were measured to be 0.98 min-1 and 14 min-1 in the dark conditions and 4.4 min-1 and 63 min-1 under the light conditions at 573 K. The rate per AuMo x interfacial site is 14 times greater than the rate per Au site under both dark and light conditions. These results indicate that the LSPR has the same enhancement effect on both Au and AuMo x catalytic sites.

Noble-metal-free and Pt nanoparticles-loaded, mesoporous oxides as efficient catalysts for CO2 hydrogenation and dry reforming with methane

“…CO + H 2 O    kJ mol  However, CO 2 hydrogenation is an endothermic reaction and requires high operation temperature [10]. Various metals such as Pt [11][12][13][14], Pd [15][16][17][18], Rh [19][20][21][22][23][24] and Au [25,26],…”

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C1‐Solarchemie

“…[130] Ferner konnte Lichtbestrahlung die Grenzflächenwechselwirkung von Pt-MoO x [131] und Au-MoO x [132] wirkungsvoll modulieren, um die RWGS-Aktivitätz uerhçhen. [130] Ferner konnte Lichtbestrahlung die Grenzflächenwechselwirkung von Pt-MoO x [131] und Au-MoO x [132] wirkungsvoll modulieren, um die RWGS-Aktivitätz uerhçhen.…”

“…Aufsätze CeO 2 erhçht die katalytische Leistungsfähigkeit infolge einer stark verringerten effektiven Aktivierungsenergie weiter. [130] Ferner konnte Lichtbestrahlung die Grenzflächenwechselwirkung von Pt-MoO x [131] und Au-MoO x [132] wirkungsvoll modulieren, um die RWGS-Aktivitätz uerhçhen.…”

A theoretical study of the reverse water‐gas shift reaction on Ni(111) and Ni(311) surfaces

“…The endothermic RWGS reaction requires a catalyst that can be operated at a relatively high temperature. Noble metal catalysts such as Pt, Rh, and Au usually have high activity and stability for the RWGS reaction; however, their high cost limits their industrial application. Ni is a commonly used low‐cost transition metal catalyst for the RWGS reaction …”