Reduced mixed Ni-Co-Al metal oxide catalysts with rich oxygen vacancy derived from layered double hydrotalcite for selective hydrogenation of furfuryl alcohol to 1,5-Pentanediol - Details

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Abstract：

The　C2-O　cleavage　of　furanic　ring　is　the　crucial　step　in　selective　hydrogenation　of　furfuryl　alcohol　(FOL)　to　1,5-pentanediol　(1,5-PDO).　In　this　study,　reduced　mixed　Ni-Co-Al　metal　oxide　catalysts　with　rich　oxygen　vacancy　(Ov)　and　different　Co/Ni　molar　ratios　were　prepared　through　intercalation　modification　of　Co-based　hydrotalcite　by　ammonium　citrate　(CA),　followed　by　calcination　and　reduction.　The　catalytic　performance　exhibited　that　a　quantitative　conversion　of　FOL　with　44.4　%　yield　and　8.2　mmol1,5-PDO·gcat-1·h−1　productivity　of　1,5-PDO　were　achieved　by　using　Co2Ni1Al1Ox-CA(0.1)　(molar　ratio　of　Co:Ni　=　2:1;　molar　concentration　ratio　of　CA:Na2CO3　=　0.1)　under　optimal　conditions.　The　stability　test　showed　that　Co2Ni1Al1Ox-CA(0.1)　consistently　rendered　above　40　%　yield　of　1,5-PDO　in　seven　consecutive　cycles.　Catalyst　characterizations　were　carried　out　using　a　series　of　techniques　including　XPS,　EPR,　O2-TPD,　etc.　The　results　demonstrate　that　the　addition　of　CA　effectively　altered　the　surface　molar　ratios　of　Co2+/(Co2++Co3+),　thereby　regulating　the　Ov　content　of　the　obtained　catalysts.　The　CoO-Ov　sites　in　the　catalyst　might　enhance　the　adsorption　of　FOL　by　η1-(O)-alcoholic　model,　which　weakened　C2-O　bond　on　the　furanic　ring　of　FOL.　Besides,　the　H2-TPD　anslysis　confirmed　that　the　enhanced　spillover　of　hydrogen　from　Ni0　onto　CoO-Ov　site,　thereby　promoting　the　cleavage　of　the　C2-O　bond　in　FOL　and　subsequent　hydrogenation　of　enol　intermediates.　In　addition,　the　DFT　calculations　imply　that　FOL　adsorption　on　CoO-Ov　site　by　η1-(O)-alcoholic　model　was　significantly　favorable　than　that　on　pristine　CoO　sites　(−1.68　eV　versus　−1.55　eV).　Consequently,　this　study　has　substantiated　the　crucial　role　played　by　CoO-Ov　in　the　reaction　pathway　leading　to　1,5-PDO　formation　via　FOL,　proposing　a　viable　scheme　for　designing　catalysts　based　on　transition　metals　and　elucidating　their　underlying　reaction　mechanism.　©　2025　Elsevier　B.V.

Keyword：

1,5-pentanediol Furfuryl alcohol Oxygen vacancy Reduced mixed metal oxide catalysts Selective hydrogenation

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[ 1 ] [Xi N.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 2 ] [Li Q.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 3 ] [Chen Y.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 4 ] [Bao R.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 5 ] [Wang Q.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 6 ] [Wang Q.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 7 ] [Lin Y.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 8 ] [Lin Y.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 9 ] [Yue J.]Department of Chemical Engineering, Engineering and Technology Institute Groningen, University of Groningen, Nijenborgh 3, Groningen, 9747 AG, Netherlands
[ 10 ] [Wang R.]School of Chemistry and Chemical Engineering, Environmental Testing Center, Key Laboratory of Poyang Lake Environment and Resource Utilization, Ministry of Education, Nanchang University, Jiangxi, Nanchang, 330031, China
[ 11 ] [Yang C.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 12 ] [Yang C.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 13 ] [Yin W.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 14 ] [Yin W.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 15 ] [Qiu T.]Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass, Fujian Universities Engineering Research Center of Reactive Distillation Technology, College of Chemical Engineering, Fuzhou University, Fujian, Fuzhou, 350108, China
[ 16 ] [Qiu T.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China

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