The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N‐heterocycles is a challenge.In this study,Ru_(2)P/AC effectively promoted reversible transformations bet...The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N‐heterocycles is a challenge.In this study,Ru_(2)P/AC effectively promoted reversible transformations between unsaturated and saturated N‐heterocycles affording yields of 98%and 99%,respectively.Moreover,a remarkable enhancement in the reusability of Ru_(2)P/AC was observed compared with other Ru‐based catalysts.According to density functional theory calculations,the superior performance of Ru_(2)P/AC was ascribed to specific synergistic factors,namely geometric and electronic effects induced by P.P greatly reduced the large Ru‐Ru ensembles and finely modified the electronic structures,leading to a low reaction barrier and high desorption ability of the catalyst,further boosting the hydrogenation and acceptorless dehydrogenation processes.展开更多
A series of ammonium-bifunctionalized ionic liquid extractants (ammonium-Bif-ILEs) combined with a number of anions, in- cluding carboxylic acids and 1,3-diketonates, have been prepared and studied in this report. T...A series of ammonium-bifunctionalized ionic liquid extractants (ammonium-Bif-ILEs) combined with a number of anions, in- cluding carboxylic acids and 1,3-diketonates, have been prepared and studied in this report. Their extraction behavior and properties toward rare earth ions (REs(III)) are systematically investigated in chloride media as a function of important param- eters such as aqueous phase pH, salting-out agent concentrations, and extraction temperature. The separation performance of ammonium-Bif-ILEs toward REs(III) are systematically discussed. The results demonstrate that ammonium-Bif-ILEs have a synergistic effect between the cation and anions in separation of REs(III). The influences of different anions on separation fac- tor (β) values are further studied. By comparison, ammonium-Bif-ILEs containing 1,3-diketonates have more potential appli- cations in La(III)/RE(III) separation than those containing carboxylic acids.展开更多
文摘The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N‐heterocycles is a challenge.In this study,Ru_(2)P/AC effectively promoted reversible transformations between unsaturated and saturated N‐heterocycles affording yields of 98%and 99%,respectively.Moreover,a remarkable enhancement in the reusability of Ru_(2)P/AC was observed compared with other Ru‐based catalysts.According to density functional theory calculations,the superior performance of Ru_(2)P/AC was ascribed to specific synergistic factors,namely geometric and electronic effects induced by P.P greatly reduced the large Ru‐Ru ensembles and finely modified the electronic structures,leading to a low reaction barrier and high desorption ability of the catalyst,further boosting the hydrogenation and acceptorless dehydrogenation processes.
基金supported by the National Basic Research Program of China (2012CBA01202)the National Natural Science Foundation of China (51174184, 21401110)+1 种基金the Key Research Program of the Chinese Academy of Sciences (KGZD-EW-201-1)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China (14KJB150019)
文摘A series of ammonium-bifunctionalized ionic liquid extractants (ammonium-Bif-ILEs) combined with a number of anions, in- cluding carboxylic acids and 1,3-diketonates, have been prepared and studied in this report. Their extraction behavior and properties toward rare earth ions (REs(III)) are systematically investigated in chloride media as a function of important param- eters such as aqueous phase pH, salting-out agent concentrations, and extraction temperature. The separation performance of ammonium-Bif-ILEs toward REs(III) are systematically discussed. The results demonstrate that ammonium-Bif-ILEs have a synergistic effect between the cation and anions in separation of REs(III). The influences of different anions on separation fac- tor (β) values are further studied. By comparison, ammonium-Bif-ILEs containing 1,3-diketonates have more potential appli- cations in La(III)/RE(III) separation than those containing carboxylic acids.