针对在室温环境下探测瓦斯浓度,提出一种基于钯掺杂单壁碳纳米管(Pd-SWCNTs)的超宽带射频识别(UWB-RFID)传感器。传感器为薄型标签,由传感探头和电磁界面组成,其中传感探头为一PdSWCNTs加载的交叉指型电极(IDE);电磁界面由天线、微带线...针对在室温环境下探测瓦斯浓度,提出一种基于钯掺杂单壁碳纳米管(Pd-SWCNTs)的超宽带射频识别(UWB-RFID)传感器。传感器为薄型标签,由传感探头和电磁界面组成,其中传感探头为一PdSWCNTs加载的交叉指型电极(IDE);电磁界面由天线、微带线和终端负载组成。Pd-SWCNTs感知瓦斯浓度,引起IDE电流的变化,形成带隙幅度调制和带隙频率调制两种识别模式。当瓦斯浓度从0×10-6增加到100×10-6,基于带隙调幅调制的识别灵敏度为-9.32 d B;而基于带隙调频调制的识别灵敏度为-11.30 d B。展开更多
Cu‐alloyed Pd single‐atom catalysts exhibit excellent catalytic performance for the semi‐hydrogenation of acetylene;however,the limit of the Cu/Pd atomic ratio for forming the alloyed Pd single‐atom catalyst is am...Cu‐alloyed Pd single‐atom catalysts exhibit excellent catalytic performance for the semi‐hydrogenation of acetylene;however,the limit of the Cu/Pd atomic ratio for forming the alloyed Pd single‐atom catalyst is ambiguous.Herein,silica‐supported Cu-Pd bimetallic catalysts with fixed Pd content and varied Cu loadings were synthesized using an incipient wetness co‐impregnation method.The X‐ray absorption spectroscopy results indicated that Pd formed an alloy with Cu after reduction at250°C and that the Pd atoms were completely isolated by Cu for Cu/Pd atomic ratios≥40/1.Notably,increasing the reduction temperature from250to400°C hardly affected the catalytic performances of the Cu-Pd/SiO2catalysts.This finding can be attributed to the similar chemical environments of Pd demonstrated by the X‐ray absorption spectroscopy results.展开更多
Palladium(Pd)‐based catalysts are essential to drive high‐performance Suzuki coupling reactions,which are powerful tools for the synthesis of functional organic compounds.Herein,we developed a solution‐rapid‐annea...Palladium(Pd)‐based catalysts are essential to drive high‐performance Suzuki coupling reactions,which are powerful tools for the synthesis of functional organic compounds.Herein,we developed a solution‐rapid‐annealing process to stabilize nitrogen‐mesoporous carbon supported Pd single‐atom/cluster(Pd/NMC)material,which provided a catalyst with superior performance for Suzuki coupling reactions.In comparison with commercial palladium/carbon(Pd/C)catalysts,the Pd/NMC catalyst exhibited significantly boosted activity(100%selectivity and 95%yield)and excellent stability(almost no decay in activity after 10 reuse cycles)for the Suzuki coupling reactions of chlorobenzenes,together with superior yield and excellent selectivity in the fields of the board scope of the reactants.Moreover,our newly developed rapid annealing process of precursor solutions is applied as a generalized method to stabilize metal clusters(e.g.Pd,Pt,Ru),opening new possibilities in the construction of efficient highly dispersed metal atom and sub‐nanometer cluster catalysts with high performance.展开更多
An account of recent work on supported single‐atom catalyst design is given here for reactions as diverse as the low‐temperature water‐gas shift,methanol steam reforming,selective ethanol dehydrogenation,and select...An account of recent work on supported single‐atom catalyst design is given here for reactions as diverse as the low‐temperature water‐gas shift,methanol steam reforming,selective ethanol dehydrogenation,and selective hydrogenation of alkynes and dienes.It is of fundamental interest to investigate the intrinsic activity and selectivity of the active metal atom site and compare them to the properties of the corresponding metal nanoparticles and sub‐nm clusters.It is also important to understand what constitutes a stable active metal atom site in the various reaction environments,and maximize their loadings to allow us to design robust catalysts for industrial applications.Combined activity and stability studies,ideally following the evolution of the active site as a function of catalyst treatment in real time are recommended.Advanced characterization methods with atomic resolution will play a key role here and will be used to guide the design of new catalysts.展开更多
Selective aerobic oxidation of alcohols under mild conditions is of great importance yet challenging,with the activation of molecular oxygen(O2)as a crucial capability of the catalysts.Herein,we demonstrate that an Al...Selective aerobic oxidation of alcohols under mild conditions is of great importance yet challenging,with the activation of molecular oxygen(O2)as a crucial capability of the catalysts.Herein,we demonstrate that an Al2O3-supported Pd single-atom catalyst leads to higher activity and selectivity compared to Pd nanoparticles for the oxidation of cinnamyl alcohol.The Al2O3 support used in this study is rich in coordinately unsaturated Al3+sites,which are apt for binding to Pd atoms through oxygen bridges and present a distinct metal-support interaction(MSI).The suitable MSI then leads to a unique electronic characteristic of the Pd single atoms,which can be confirmed via X-ray photoelectron spectroscopy,normalized X-ray absorption near-edge structure,and diffuse reflectance Fourier transform infrared spectroscopy.Moreover,this unique electronic state is proposed to be responsible for its high catalytic activity.With the help of in-situ UV-vis spectra and electron spin resonance spectra,a specific alcohol oxidation route with O2 activation mechanism is then identified.Active oxygen species behaving chemically like singlet-O2 are generated from the interaction of O2 with Pd1/Al2O3,and then oxidize the partially dehydrogenated intermediates produced by the adsorbed allylic alcohols and Pd atoms to the desired alkenyl aldehyde.This work provides a promising path for the design and development of high-activity catalysts for aerobic oxidation reactions.展开更多
基金supported by the National High Technology Research and Development Program of China (863 Program 2011AA03A406)Zhejiang Leading Team of Science and Technology Innovation (2009R50020)~~
文摘针对在室温环境下探测瓦斯浓度,提出一种基于钯掺杂单壁碳纳米管(Pd-SWCNTs)的超宽带射频识别(UWB-RFID)传感器。传感器为薄型标签,由传感探头和电磁界面组成,其中传感探头为一PdSWCNTs加载的交叉指型电极(IDE);电磁界面由天线、微带线和终端负载组成。Pd-SWCNTs感知瓦斯浓度,引起IDE电流的变化,形成带隙幅度调制和带隙频率调制两种识别模式。当瓦斯浓度从0×10-6增加到100×10-6,基于带隙调幅调制的识别灵敏度为-9.32 d B;而基于带隙调频调制的识别灵敏度为-11.30 d B。
基金supported by the National Natural Science Foundation of China(21303194,21476227,21522608 and 21690084)Youth Innovation Promotion Association of the Chinese Academy of Sciences(2014163)+2 种基金the National Key Projects for Fundamental Research and Development of China(2016YFA0202801)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020100)the department of science and technology of Liaoning province under contract of 2015020086-101~~
文摘Cu‐alloyed Pd single‐atom catalysts exhibit excellent catalytic performance for the semi‐hydrogenation of acetylene;however,the limit of the Cu/Pd atomic ratio for forming the alloyed Pd single‐atom catalyst is ambiguous.Herein,silica‐supported Cu-Pd bimetallic catalysts with fixed Pd content and varied Cu loadings were synthesized using an incipient wetness co‐impregnation method.The X‐ray absorption spectroscopy results indicated that Pd formed an alloy with Cu after reduction at250°C and that the Pd atoms were completely isolated by Cu for Cu/Pd atomic ratios≥40/1.Notably,increasing the reduction temperature from250to400°C hardly affected the catalytic performances of the Cu-Pd/SiO2catalysts.This finding can be attributed to the similar chemical environments of Pd demonstrated by the X‐ray absorption spectroscopy results.
文摘Palladium(Pd)‐based catalysts are essential to drive high‐performance Suzuki coupling reactions,which are powerful tools for the synthesis of functional organic compounds.Herein,we developed a solution‐rapid‐annealing process to stabilize nitrogen‐mesoporous carbon supported Pd single‐atom/cluster(Pd/NMC)material,which provided a catalyst with superior performance for Suzuki coupling reactions.In comparison with commercial palladium/carbon(Pd/C)catalysts,the Pd/NMC catalyst exhibited significantly boosted activity(100%selectivity and 95%yield)and excellent stability(almost no decay in activity after 10 reuse cycles)for the Suzuki coupling reactions of chlorobenzenes,together with superior yield and excellent selectivity in the fields of the board scope of the reactants.Moreover,our newly developed rapid annealing process of precursor solutions is applied as a generalized method to stabilize metal clusters(e.g.Pd,Pt,Ru),opening new possibilities in the construction of efficient highly dispersed metal atom and sub‐nanometer cluster catalysts with high performance.
基金financial support of the work by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), under Awards Grant Number DE-FG02-05ER15730
文摘An account of recent work on supported single‐atom catalyst design is given here for reactions as diverse as the low‐temperature water‐gas shift,methanol steam reforming,selective ethanol dehydrogenation,and selective hydrogenation of alkynes and dienes.It is of fundamental interest to investigate the intrinsic activity and selectivity of the active metal atom site and compare them to the properties of the corresponding metal nanoparticles and sub‐nm clusters.It is also important to understand what constitutes a stable active metal atom site in the various reaction environments,and maximize their loadings to allow us to design robust catalysts for industrial applications.Combined activity and stability studies,ideally following the evolution of the active site as a function of catalyst treatment in real time are recommended.Advanced characterization methods with atomic resolution will play a key role here and will be used to guide the design of new catalysts.
文摘Selective aerobic oxidation of alcohols under mild conditions is of great importance yet challenging,with the activation of molecular oxygen(O2)as a crucial capability of the catalysts.Herein,we demonstrate that an Al2O3-supported Pd single-atom catalyst leads to higher activity and selectivity compared to Pd nanoparticles for the oxidation of cinnamyl alcohol.The Al2O3 support used in this study is rich in coordinately unsaturated Al3+sites,which are apt for binding to Pd atoms through oxygen bridges and present a distinct metal-support interaction(MSI).The suitable MSI then leads to a unique electronic characteristic of the Pd single atoms,which can be confirmed via X-ray photoelectron spectroscopy,normalized X-ray absorption near-edge structure,and diffuse reflectance Fourier transform infrared spectroscopy.Moreover,this unique electronic state is proposed to be responsible for its high catalytic activity.With the help of in-situ UV-vis spectra and electron spin resonance spectra,a specific alcohol oxidation route with O2 activation mechanism is then identified.Active oxygen species behaving chemically like singlet-O2 are generated from the interaction of O2 with Pd1/Al2O3,and then oxidize the partially dehydrogenated intermediates produced by the adsorbed allylic alcohols and Pd atoms to the desired alkenyl aldehyde.This work provides a promising path for the design and development of high-activity catalysts for aerobic oxidation reactions.
