The reduction of CO_(2)toward CO and CH_(4)over Ni-loaded MoS_(2)-like layered nanomaterials is investigated.The mild hydrothermal synthesis induced the formation of a molybdenum oxysulfide(MoO_(x)S_(y))phase,enriched...The reduction of CO_(2)toward CO and CH_(4)over Ni-loaded MoS_(2)-like layered nanomaterials is investigated.The mild hydrothermal synthesis induced the formation of a molybdenum oxysulfide(MoO_(x)S_(y))phase,enriched with sulfur defects and multiple Mo oxidation states that favor the insertion of Ni^(2+)cations via photo-assisted precipitation.The photocatalytic tests under LED irradiation at different wavelengths from 365 to 940 nm at 250℃rendered 1%CO_(2)conversion and continuous CO production up to 0.6 mmol/(gcat h).The incorporation of Ni into the MoO_(x)S_(y)structure boosted the continuous production of CO up to 5.1 mmol/(gcat h)with a CO_(2)conversion of 3.5%.In situ spectroscopic techniques and DFT simulations showed the O-incorporated MoS_(2)structure,in addition to Ni clusters as a supported metal catalyst.The mechanistic study of the CO_(2)reduction reaction over the catalysts revealed that the reverse water-gas shift reaction is favored due to the preferential formation of carboxylic species.展开更多
基金Financial support from the Spanish Ministry of Science and Universities through CEX2023-001286-S,PID2020-114926RB-I00,and CTQ2016-77144-Rthe MICINN Scholarship.
文摘The reduction of CO_(2)toward CO and CH_(4)over Ni-loaded MoS_(2)-like layered nanomaterials is investigated.The mild hydrothermal synthesis induced the formation of a molybdenum oxysulfide(MoO_(x)S_(y))phase,enriched with sulfur defects and multiple Mo oxidation states that favor the insertion of Ni^(2+)cations via photo-assisted precipitation.The photocatalytic tests under LED irradiation at different wavelengths from 365 to 940 nm at 250℃rendered 1%CO_(2)conversion and continuous CO production up to 0.6 mmol/(gcat h).The incorporation of Ni into the MoO_(x)S_(y)structure boosted the continuous production of CO up to 5.1 mmol/(gcat h)with a CO_(2)conversion of 3.5%.In situ spectroscopic techniques and DFT simulations showed the O-incorporated MoS_(2)structure,in addition to Ni clusters as a supported metal catalyst.The mechanistic study of the CO_(2)reduction reaction over the catalysts revealed that the reverse water-gas shift reaction is favored due to the preferential formation of carboxylic species.
