物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2015年
4期
729-737
,共9页
韩优%何志远%管永川%李韡%张金利
韓優%何誌遠%管永川%李韡%張金利
한우%하지원%관영천%리위%장금리
负载顺序%PdAu双金属%蒽醌加氢%降解产物
負載順序%PdAu雙金屬%蒽醌加氫%降解產物
부재순서%PdAu쌍금속%은곤가경%강해산물
Loading sequence%Bimetal ic PdAu%Anthraquinone hydrogenation%Degradation product
通过改变Pd和Au的负载顺序合成了一系列具有不同结构和电子性质的PdAu双金属催化剂,并用于蒽醌加氢反应.其中通过先负载Au后负载Pd的顺序制得的Pd/Au/Al2O3催化剂,其加氢效率可高达14.27 g?L-1. X射线衍射、透射电子显微镜、H2程序升温还原和X射线光电子能谱等分析表征结果显示, Pd/Au/Al2O3催化剂中分散在Au颗粒表面的Pd纳米颗粒具有独特的爆米花结构,其表面零价态的单质Pd含量最多,而这种表面零价态的单质Pd是蒽醌加氢反应中的关键活性组分.此外, Au的加入可有效抑制副反应的发生,减少降解产物的生成,从而大大提高了催化选择性.
通過改變Pd和Au的負載順序閤成瞭一繫列具有不同結構和電子性質的PdAu雙金屬催化劑,併用于蒽醌加氫反應.其中通過先負載Au後負載Pd的順序製得的Pd/Au/Al2O3催化劑,其加氫效率可高達14.27 g?L-1. X射線衍射、透射電子顯微鏡、H2程序升溫還原和X射線光電子能譜等分析錶徵結果顯示, Pd/Au/Al2O3催化劑中分散在Au顆粒錶麵的Pd納米顆粒具有獨特的爆米花結構,其錶麵零價態的單質Pd含量最多,而這種錶麵零價態的單質Pd是蒽醌加氫反應中的關鍵活性組分.此外, Au的加入可有效抑製副反應的髮生,減少降解產物的生成,從而大大提高瞭催化選擇性.
통과개변Pd화Au적부재순서합성료일계렬구유불동결구화전자성질적PdAu쌍금속최화제,병용우은곤가경반응.기중통과선부재Au후부재Pd적순서제득적Pd/Au/Al2O3최화제,기가경효솔가고체14.27 g?L-1. X사선연사、투사전자현미경、H2정서승온환원화X사선광전자능보등분석표정결과현시, Pd/Au/Al2O3최화제중분산재Au과립표면적Pd납미과립구유독특적폭미화결구,기표면령개태적단질Pd함량최다,이저충표면령개태적단질Pd시은곤가경반응중적관건활성조분.차외, Au적가입가유효억제부반응적발생,감소강해산물적생성,종이대대제고료최화선택성.
A series of bimetal ic PdAu catalysts with different structures were prepared by changing the loading sequence of Pd and Au for the hydrogenation of 2-ethylanthraquinone. Pd/Au/Al2O3 was obtained by loading Pd onto Au particles deposited onto an Al2O3 support with a hydrogenation efficiency up to 14.27 g?L-1. According to X-ray diffraction, transmission electron microscopy, hydrogen temperature program reduction, and X-ray photoelectron spectroscopy measurements, the popcorn structure and unique electronic properties of the Pd species in the Pd/Au/Al2O3 catalyst resulted in the highest content of surface metal ic Pd, which was the most active component for the reaction. What is more, the addition of Au can effectively reduce the amount of degradation products by suppressing side reactions.