Currently,it is of great significance to develop new proton-conduction materials with high proton conductivity,high stability,and good conducting durability to meet the demands of fuel cell and sensors.Herein,we prepa...Currently,it is of great significance to develop new proton-conduction materials with high proton conductivity,high stability,and good conducting durability to meet the demands of fuel cell and sensors.Herein,we prepared two composites DETA-HPW@MIL-101-SO_(3)H 1 and TETA-HPW@MIL-101-SO3H 2(DETA=diethylenetriamine,HPW=H_(3)PW_(12))_(4)0·xH_(2)O,MIL=Material Institut Lavoisier,TETA=triethylenetetramine)by encapsulating polyoxometalate(POM)and organic amine into a sulfonated MIL-101 through a step-by-step dipping method.Delightedly,1 and 2 have high proton conductivities of 6.4×10^(−2) and 2.9×10^(−2) S·cm^(−1) at 65℃ and 95%relative humidity(RH),respectively,which can be attributed to the fast proton transfer among acid–base pairs formed between HPW and organic amine as well between sulfonic acid and organic amine.Moreover,the time-dependent test in proton conductivity displays that their proton-conduction properties have good stability and durability,which benefit from that the electrostatic interactions among acid–base pairs and the limitation of opening size of MIL-101-SO3H make HPW and organic amine stably exist in the cages of MIL-101-SO_(3)H.The remarkable proton-conduction properties(high proton conductivity and high stability)of the two composites make them become promising proton-conduction materials.展开更多
Ethanol is a considerable platform molecule in biomass conversion,which could be acquired in quantity through acetone-butanol-ethanol(ABE)fermentation.People have been working on the upgrading of ethanol to value adde...Ethanol is a considerable platform molecule in biomass conversion,which could be acquired in quantity through acetone-butanol-ethanol(ABE)fermentation.People have been working on the upgrading of ethanol to value added chemicals for decades.In the meantime,1-butanol and a series of value added products have been selectively generated through C–C bond coupling.In this mini-review,we focus on the recent advances in selective C–C bond formation over balanced Lewis acid-base catalysts such as modified metal oxide,mixed metal oxide,hydroxyapatite and zeolite confined transition metal oxide catalysts.Among them,Pd-MgAlO_x and Sr-based hydroxyapatite exhibit>70%1-butanol selectivity,while Zn——xZr_yO_z and Ta-Si BEA zeolite achieve>80%of isobutene and butadiene selectivity respectively.The mechanism and reaction pathway of C–C bond formation in each reaction system are described in detail.The correlation between C–C bond coupling and the acidity/basicity of the Lewis acid-base pairs from the surface of the catalysts are also discussed.展开更多
基金financially supported by the National Natural Science Foundation of China (Grant Nos. 22071019 and 21872021)
文摘Currently,it is of great significance to develop new proton-conduction materials with high proton conductivity,high stability,and good conducting durability to meet the demands of fuel cell and sensors.Herein,we prepared two composites DETA-HPW@MIL-101-SO_(3)H 1 and TETA-HPW@MIL-101-SO3H 2(DETA=diethylenetriamine,HPW=H_(3)PW_(12))_(4)0·xH_(2)O,MIL=Material Institut Lavoisier,TETA=triethylenetetramine)by encapsulating polyoxometalate(POM)and organic amine into a sulfonated MIL-101 through a step-by-step dipping method.Delightedly,1 and 2 have high proton conductivities of 6.4×10^(−2) and 2.9×10^(−2) S·cm^(−1) at 65℃ and 95%relative humidity(RH),respectively,which can be attributed to the fast proton transfer among acid–base pairs formed between HPW and organic amine as well between sulfonic acid and organic amine.Moreover,the time-dependent test in proton conductivity displays that their proton-conduction properties have good stability and durability,which benefit from that the electrostatic interactions among acid–base pairs and the limitation of opening size of MIL-101-SO3H make HPW and organic amine stably exist in the cages of MIL-101-SO_(3)H.The remarkable proton-conduction properties(high proton conductivity and high stability)of the two composites make them become promising proton-conduction materials.
基金supported by the “111 Project” of China (B18030) and Nankai University
文摘Ethanol is a considerable platform molecule in biomass conversion,which could be acquired in quantity through acetone-butanol-ethanol(ABE)fermentation.People have been working on the upgrading of ethanol to value added chemicals for decades.In the meantime,1-butanol and a series of value added products have been selectively generated through C–C bond coupling.In this mini-review,we focus on the recent advances in selective C–C bond formation over balanced Lewis acid-base catalysts such as modified metal oxide,mixed metal oxide,hydroxyapatite and zeolite confined transition metal oxide catalysts.Among them,Pd-MgAlO_x and Sr-based hydroxyapatite exhibit>70%1-butanol selectivity,while Zn——xZr_yO_z and Ta-Si BEA zeolite achieve>80%of isobutene and butadiene selectivity respectively.The mechanism and reaction pathway of C–C bond formation in each reaction system are described in detail.The correlation between C–C bond coupling and the acidity/basicity of the Lewis acid-base pairs from the surface of the catalysts are also discussed.