The synergistic effect between Ru single-atomic sites and nanoclusters during catalytic hydrotreatment of fast pyrolysis liquids from lignocellulosic biomass - Details

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Abstract：

Catalytic　hydrotreatment　is　a　promising　technique　to　upgrade　pyrolysis　liquids　(PLs)　with　undesired　properties　into　intermediate　that　can　be　co-processed　with　vacuum　gas　oil　in　FCC　refinery.　Highly　active　catalysts　are　key　in　such　a　process.　In　this　study,　a　ruthenium-based　catalyst　possessing　both　single-atomic　and　nanocluster　sites　supported　on　hierarchically　porous　nitrogen-doped　carbon　(Ru1+NPs/HPNC)　was　prepared　by　a　two-step　alcohol　reduction　method.　Catalytic　performance　was　evaluated　for　both　model　compound　vanillin　(VL)　and　PLs　in　a　batch　autoclave.　The　model　compound　study　showed　that　Ru1+NPs/HPNC　exhibited　excellent　intrinsic　activity　in　VL　hydrogenation,　with　a　TOF　of　26.9　s−1,　which　is　approximately　3　times　higher　than　that　of　Ru1/HPNC　(8.4　s−1)　and　RuNPs/HPNC　(8.8　s−1),　and　6　times　that　of　Ru/AC　(4.2　s−1).　Catalytic　hydrotreatment　of　PLs　indicated　that　Ru1+NPs/HPNC　possessed　the　best　activity　regarding　to　the　highest　H/C　ratio　(mild　hydrotreatment:　1.33;　deep　hydrotreatment:　1.29)　and　the　lowest　TG　residue　(mild　hydrotreatment:　14.4　wt%;　deep　hydrotreatment:　6.5　wt%)　of　the　product　oils.　To　obtain　understanding　of　the　synergistic　effect　between　single-atoms　and　nanoclusters,　the　adsorption　of　VL　and　H2　on　the　catalyst　was　examined　by　ATR-FTIR　and　DFT　calculations.　The　results　revealed　that　VL　is　preferentially　adsorbed　and　activated　on　the　single-atomic　sites,　while　the　H2　is　preferentially　dissociated　on　the　nanocluster　sites.　Based　on　these　findings,　a　plausible　mechanism　is　proposed.　This　study　offers　new　ideas　for　developing　better-performing　catalysts　for　catalytic　hydrotreatment　of　PLs.　©　2025　Elsevier　Ltd

Keyword：

Nanocatalysts Nanoclusters Pyrolysis

Community：

[ 1 ] [Zhu, Xingchao]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 ] [Gan, Zhiwei]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 ] [Wang, Yueqi]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 ] [Xi, Nan]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, Qinglian]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, Qinglian]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 7 ] [Lin, Yixiong]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, Yixiong]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 9 ] [Yang, Chen]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
[ 10 ] [Yang, Chen]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 11 ] [Xia, Shuqian]Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering and Technology, Tianjin University, Tianjin; 300350, China
[ 12 ] [Yin, Wang]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
[ 13 ] [Yin, Wang]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China
[ 14 ] [Qiu, Ting]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
[ 15 ] [Qiu, Ting]Qingyuan Innovation Laboratory, Fujian, Quanzhou; 362801, China

Reprint 's Address：

[yin, wang]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;;[yin, wang]qingyuan innovation laboratory, fujian, quanzhou; 362801, china

Email：

wangyin@fzu.edu.cn

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