TY - JOUR

T1 - Mn-promoted MoS2 catalysts for CO2 hydrogenation

T2 - enhanced methanol selectivity due to MoS2/MnOx interfaces

AU - Alves, Gustavo A.S.

AU - Pacholik, Gernot

AU - Pollitt, Stephan

AU - Wagner, Tobias

AU - Rameshan, Raffael

AU - Rameshan, Christoph

AU - Föttinger, Karin

N1 - Publisher Copyright: © 2024 The Royal Society of Chemistry.

PY - 2024/2/2

Y1 - 2024/2/2

N2 - Considering the alarming scenario of climate change, CO2 hydrogenation to methanol is considered a key process for phasing out fossil fuels by means of CO2 utilization. In this context, MoS2 catalysts have recently shown to be promising catalysts for this reaction, especially in the presence of abundant basal-plane sulfur vacancies and due to synergistic mechanisms with other phases. In this work, Mn-promoted MoS2 prepared by a hydrothermal method presents considerable selectivity for CO2 hydrogenation to methanol in comparison with pure MoS2 and other promoters such as K and Co. Interestingly, if CO is used as a carbon source for the reaction, methanol production is remarkably lower, which suggests the absence of a CO intermediate during CO2 hydrogenation to methanol. After optimization of synthesis parameters, a methanol selectivity of 64% is achieved at a CO2 conversion of 2.8% under 180 °C. According to material characterization by X-ray Diffraction and X-ray Absorption, the Mn promoter is present mainly in the form of MnO and MnCO3 phases, with the latter undergoing convertion to MnO upon H2 pretreatment. However, following exposure to reaction conditions, X-ray photoelectron spectroscopy suggests that higher oxidation states of Mn may be present at the surface, suggesting that the improved catalytic activity for CO2 hydrogenation to methanol arises from a synergy between MoS2 and MnOx at the catalyst surface.

AB - Considering the alarming scenario of climate change, CO2 hydrogenation to methanol is considered a key process for phasing out fossil fuels by means of CO2 utilization. In this context, MoS2 catalysts have recently shown to be promising catalysts for this reaction, especially in the presence of abundant basal-plane sulfur vacancies and due to synergistic mechanisms with other phases. In this work, Mn-promoted MoS2 prepared by a hydrothermal method presents considerable selectivity for CO2 hydrogenation to methanol in comparison with pure MoS2 and other promoters such as K and Co. Interestingly, if CO is used as a carbon source for the reaction, methanol production is remarkably lower, which suggests the absence of a CO intermediate during CO2 hydrogenation to methanol. After optimization of synthesis parameters, a methanol selectivity of 64% is achieved at a CO2 conversion of 2.8% under 180 °C. According to material characterization by X-ray Diffraction and X-ray Absorption, the Mn promoter is present mainly in the form of MnO and MnCO3 phases, with the latter undergoing convertion to MnO upon H2 pretreatment. However, following exposure to reaction conditions, X-ray photoelectron spectroscopy suggests that higher oxidation states of Mn may be present at the surface, suggesting that the improved catalytic activity for CO2 hydrogenation to methanol arises from a synergy between MoS2 and MnOx at the catalyst surface.

UR - http://www.scopus.com/inward/record.url?scp=85184902688&partnerID=8YFLogxK

U2 - 10.1039/d3cy01711g

DO - 10.1039/d3cy01711g

M3 - Article

AN - SCOPUS:85184902688

VL - 14.2024

SP - 1138

EP - 1147

JO - Catalysis science & technology

JF - Catalysis science & technology

SN - 2044-4753

IS - 5

ER -