he catalytic activities of [H_nRu_3(CO)_9(CCO)]￣(-(2-n)) (n=0, 1 , 2 , 3) support-ed on oxides have been estimated using INDO calculations and correlation betweencatalytic activity and electronic structure for these ...he catalytic activities of [H_nRu_3(CO)_9(CCO)]￣(-(2-n)) (n=0, 1 , 2 , 3) support-ed on oxides have been estimated using INDO calculations and correlation betweencatalytic activity and electronic structure for these clusters have been established.The activity in ￣(13)CO isotopic exchange strongly relates to the bond orders of Ru-CO and C-CO, and the activity in alkylation with nucleophile or electrophile de-pends mainly on the net charges at Ca atoms. In addition, the possible species of[H_3Ru_3(CO)_9(CCO)]￣+ has been proposed although it has not been synthesized upto now.展开更多
Photothermal hydrogenation of carbon monoxide(CO)holds the potential to generate valuable C_(2+)chemicals using renewable solar energy.However,its activity and selectivity towards C_(2)—C_(3) alkanes are limited comp...Photothermal hydrogenation of carbon monoxide(CO)holds the potential to generate valuable C_(2+)chemicals using renewable solar energy.However,its activity and selectivity towards C_(2)—C_(3) alkanes are limited compared to conventional thermal catalysis.In this study,we developed a robust catalyst consisting of Cu/Fe_(3)O_(4) nanoparticles on Mo_(2)CT_(x) MXene,showing enhanced photothermal C_(2)—C_(3) production.The Cu component plays a crucial role in H_(2) dissociation and subsequent H spillover,facilitating the in situ generation of Fe^(0) in Fe_(5)C_(2) active sites and thus efficiently promoting photothermal CO hydrogenation.As a result,we achieved a 51.3%C_(2+)selectivity and 78.5%CO conversion at a high gas hourly space velocity(GHSV)of 12000 mL·gcat^(-1)·h^(-1) and 2.5 MPa in a flow reactor at 320℃.The overall C_(2)—C_(3) yield reached 23.6% with Cu/Fe_(3)O_(4)/Mo_(2)CT_(x) catalysts,marking a 2.8-fold increase compared to the performance of the bare Fe_(3)O_(4)/Mo_(2)CT_(x) catalyst.展开更多
文摘he catalytic activities of [H_nRu_3(CO)_9(CCO)]￣(-(2-n)) (n=0, 1 , 2 , 3) support-ed on oxides have been estimated using INDO calculations and correlation betweencatalytic activity and electronic structure for these clusters have been established.The activity in ￣(13)CO isotopic exchange strongly relates to the bond orders of Ru-CO and C-CO, and the activity in alkylation with nucleophile or electrophile de-pends mainly on the net charges at Ca atoms. In addition, the possible species of[H_3Ru_3(CO)_9(CCO)]￣+ has been proposed although it has not been synthesized upto now.
基金supported by the National Natural Science Foundation of China(Grant Nos.22272078,2240090130)the National Key Research and Development Program of the Ministry of Science and Technology of China(No.2020YFA0406102)the Frontiers Science Center for Critical Earth Material Cycling of Nanjing University,and the“Innovation and Entrepreneurship of Talentsplan"of Jiangsu Province。
文摘Photothermal hydrogenation of carbon monoxide(CO)holds the potential to generate valuable C_(2+)chemicals using renewable solar energy.However,its activity and selectivity towards C_(2)—C_(3) alkanes are limited compared to conventional thermal catalysis.In this study,we developed a robust catalyst consisting of Cu/Fe_(3)O_(4) nanoparticles on Mo_(2)CT_(x) MXene,showing enhanced photothermal C_(2)—C_(3) production.The Cu component plays a crucial role in H_(2) dissociation and subsequent H spillover,facilitating the in situ generation of Fe^(0) in Fe_(5)C_(2) active sites and thus efficiently promoting photothermal CO hydrogenation.As a result,we achieved a 51.3%C_(2+)selectivity and 78.5%CO conversion at a high gas hourly space velocity(GHSV)of 12000 mL·gcat^(-1)·h^(-1) and 2.5 MPa in a flow reactor at 320℃.The overall C_(2)—C_(3) yield reached 23.6% with Cu/Fe_(3)O_(4)/Mo_(2)CT_(x) catalysts,marking a 2.8-fold increase compared to the performance of the bare Fe_(3)O_(4)/Mo_(2)CT_(x) catalyst.
