Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeol...Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.展开更多
Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneo...Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneous catalysts(isolated active sites)and heterogeneous catalysts(stable and easy to separate),and are thus predicted to be able to bridge the homo-and heterogeneous catalysis.This prediction was first experimentally demonstrated in 2016.In this mini-review,we summarize the few homogeneous catalysis progresses reported recently where SACs have exhibited promising application:a)Rh/ZnO and Rh/CoO SAC have been used successfully in hydroformylation of olefin of which the activity are comparable to the homogeneous Wilkinson’s catalyst;b)a Pt/Al2O3 SAC has shown excellent performance in hydrosilylation reaction;and c)M-N-C SACs(M=Fe,Co etc.)have been applied in the activation of C–H bonds.All of these examples suggest that fabrication of suitable SACs could provide a new avenue for the heterogenization of homogeneous catalysts.These pioneering works shed new light on the recognition of single-atom catalysis in bridging the homo-and heterogeneous catalysis.展开更多
Alcohol-based disinfectants have protected people in the coronavirus disease 2019(COVID-19)pandemic,but olfactory stimuli of ethanol may evoke unpleasant memories associated with stressful situations in the devastatin...Alcohol-based disinfectants have protected people in the coronavirus disease 2019(COVID-19)pandemic,but olfactory stimuli of ethanol may evoke unpleasant memories associated with stressful situations in the devastating infectious disease.The smell of ethanol in household cleaning and disinfectant products can be covered up by the fragrance additives,and 3-hexenol is especially appreciated for the characteristic,strong odor of green plants.Industrial production of 3-hexenol relies on the selective hydrogenation of 3-hexyn-1-ol,where Lindlar catalyst is normally used for the superior selectivity.Although achieving such catalytic transformation in ethanol solution seems as a direct way to produce a disinfectant with green aroma,a popular consumer product in the post-COVID era,severe leaching of toxic Pb hinders Lindlar catalyst as a promising candidate.We find that the Fe_(2)O_(3) supported Pd single-atom catalyst is highly selective to fulfill semi-hydrogenation of 3-hexyn-1-ol in 75%ethanol,and the aforementioned household product is readily generated after filtrating the stable,solid catalyst out of reaction solution.Single-atom catalysts have been frequently utilized for fine-chemical synthesis,while in this work they make stunning debut in practical manufacture of daily used products.展开更多
Oxidative dehydrogenation of propane has been an ever-growing field for propylene production due to its exothermic properties,of which overoxidation is the major drawback,with CO and even CO_(2) as undesired by-produc...Oxidative dehydrogenation of propane has been an ever-growing field for propylene production due to its exothermic properties,of which overoxidation is the major drawback,with CO and even CO_(2) as undesired by-products.For the purpose of getting higher propylene selectivity as well as yield,herein,we report Ni single atoms supported on calcium aluminate as an efficient catalyst candidate for propane oxidative dehydrogenation.Beneficial from higher valence states of Ni1 species,it shows 2—3 times as much propylene selectivity as that of Ni nanoparticles.About 14.2%C_(3)H_(6) yield with 47.3%propylene selectivity has been achieved on Ni single atom catalyst and a good stability during 20 h test can be obtained as well.展开更多
基金supported financially by the National Natural Science Foundation of China(51776206)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N092)+4 种基金the National Key R&D Program of China(2018YFB1501504)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_0095)the Fundamental Research Funds for the Central Universities(3203002104D)the Research Foundation-Flanders(FWO,grant 12E8617N)for funding and KU Leuven grant C14/20/086visiting scholar(2017-20202)at the Guangzhou Institute of Energy Conversion,Chinese Academy of Sciences。
文摘Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence.Here,a unique structured hybrid catalyst composed of Fe_(3)O_(4) nanoparticles intimately dispersed inside an acidic zeolite is developed.1 to 4 nm sized Fe_(3)O_(4) nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe_(3)O_(4) restructuring during co-hydro thermal synthesis using organosilane modification.A very high aromatic productivity of 214 mmolaromatics h^(-1) gFe^(-1) can be obtained with a remarkable 62%aromatic selectivity in hydrocarbons.This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h.The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform,well-dispersed oxide nanoparticles in close intimacy with-and partially confined in-a zeolite matrix.
基金supported by National Natural Science Foundation of China(21606222,21776270)Postdoctoral Science Foundation(2017M621170,2016M601350)~~
文摘Single-atom catalysis,the catalysis by single-atom catalysts(SACs),has attracted considerable attention in recent years as a new frontier in the heterogeneous catalysis field.SACs have the advantages of both homogeneous catalysts(isolated active sites)and heterogeneous catalysts(stable and easy to separate),and are thus predicted to be able to bridge the homo-and heterogeneous catalysis.This prediction was first experimentally demonstrated in 2016.In this mini-review,we summarize the few homogeneous catalysis progresses reported recently where SACs have exhibited promising application:a)Rh/ZnO and Rh/CoO SAC have been used successfully in hydroformylation of olefin of which the activity are comparable to the homogeneous Wilkinson’s catalyst;b)a Pt/Al2O3 SAC has shown excellent performance in hydrosilylation reaction;and c)M-N-C SACs(M=Fe,Co etc.)have been applied in the activation of C–H bonds.All of these examples suggest that fabrication of suitable SACs could provide a new avenue for the heterogenization of homogeneous catalysts.These pioneering works shed new light on the recognition of single-atom catalysis in bridging the homo-and heterogeneous catalysis.
基金supported by the National Natural Science Foundation of China(Nos.22378079,22102210)Guangzhou Projects for Fundamental Research(No.202102020202)+1 种基金the Guangdong Provincial Key Laboratory of Plant Resources Biorefinery(No.2021GDKLPRB10)the start-up funding of Guangdong University of Technology.
文摘Alcohol-based disinfectants have protected people in the coronavirus disease 2019(COVID-19)pandemic,but olfactory stimuli of ethanol may evoke unpleasant memories associated with stressful situations in the devastating infectious disease.The smell of ethanol in household cleaning and disinfectant products can be covered up by the fragrance additives,and 3-hexenol is especially appreciated for the characteristic,strong odor of green plants.Industrial production of 3-hexenol relies on the selective hydrogenation of 3-hexyn-1-ol,where Lindlar catalyst is normally used for the superior selectivity.Although achieving such catalytic transformation in ethanol solution seems as a direct way to produce a disinfectant with green aroma,a popular consumer product in the post-COVID era,severe leaching of toxic Pb hinders Lindlar catalyst as a promising candidate.We find that the Fe_(2)O_(3) supported Pd single-atom catalyst is highly selective to fulfill semi-hydrogenation of 3-hexyn-1-ol in 75%ethanol,and the aforementioned household product is readily generated after filtrating the stable,solid catalyst out of reaction solution.Single-atom catalysts have been frequently utilized for fine-chemical synthesis,while in this work they make stunning debut in practical manufacture of daily used products.
基金supported by the National Key Research and Development program of China(2021YFA1500503)the National Natural Science Foundation of China(21961142006,21972135)CAS Project for Young Scientists in Basic Research(YSBR-022).
文摘Oxidative dehydrogenation of propane has been an ever-growing field for propylene production due to its exothermic properties,of which overoxidation is the major drawback,with CO and even CO_(2) as undesired by-products.For the purpose of getting higher propylene selectivity as well as yield,herein,we report Ni single atoms supported on calcium aluminate as an efficient catalyst candidate for propane oxidative dehydrogenation.Beneficial from higher valence states of Ni1 species,it shows 2—3 times as much propylene selectivity as that of Ni nanoparticles.About 14.2%C_(3)H_(6) yield with 47.3%propylene selectivity has been achieved on Ni single atom catalyst and a good stability during 20 h test can be obtained as well.
