Understanding the catalytic performance and deactivation behaviour of second-promoter doped Pt/WO_(χ)/γ-Al_(2)O_(3) catalysts in the glycerol hydrogenolysis for selective and cleaner production of 1,3-propanediol  

作　　者：Rafik Rajjak Shaikh Sittichai Damruang Rais Ahmad Khan Supareak Praserthdam Piyasan Praserthdam 

机构地区：[1]Center of Excellence on Catalysis and Catalytic Reaction Engineering(CECC),Department of Chemical Engineering,Faculty of Engineering,Chulalongkorn University,Bangkok 10330,Thailand [2]Department of Chemistry,College of Science,King Saud University,P.O.Box 2455,Riyadh 11451,Saudi Arabia [3]High-Performance Computing Unit(CECC-HCU),Centre of Excellence on Catalysis and Catalytic Reaction Engineering(CECC),Department of Chemical Engineering,Faculty of Engineering,Chulalongkorn University,Bangkok 10330,Thailand

出　　处：《Journal of Energy Chemistry》2024年第7期486-507,共22页能源化学（英文版）

基　　金：funded by the National Research Council of Thailand (NRCT);the Second Century Foundation (C2F),Chulalongkorn University,Thailand;Researcher Supporting Project RSP2024RR400,King Saud University,Saudi Arabia

摘　　要：The selective aqueous-phase glycerol hydrogenolysis is a promising reaction to produce commercially useful 1,3-propanediol(1,3-PDO).The Pt-WOx bifunctional catalyst can catalyse the glycerol hydrogenol-ysis but the catalyst deactivation via sintering,metal leaching,and coking can predominantly occur in the aqueous phase reaction.In this work,the effect of reaction temperature,pressure and second promoter(Cu,Fe,Rh,Mn,Re,Ru,Ir,Sn,B,and P)on catalytic performance and deactivation behaviour of Pt/WOx/-Al2O3 was investigated.When doped with Rh,Mn,Re,Ru,Ir,B,and P,the second promoter boosts catalytic activity by promoting great dispersion of Pt on support and increasing Pt surface area.The increased Bronsted acid sites lead to selective synthesis of 1,3-PDO than 1,2-propanediol(1,2-PDO).The characterization studies of fresh and spent catalysts reveal that the main cause of catalyst deactivation is the Pt sintering,as interpreted based on XRD,CO chemisorption,and TEM analyses.The Pt sintering is affected depending on the second promoter that can either or reduce the interaction between Pt,WO_(χ)/γ and Al_(2)O_(3).As an electron acceptor of Pt in Pt/WO_(χ)/γ-Al_(2)O_(3),Re and Mn as second promoters resulted in increased Pt^(2+) on the catalytic surface,which strengthens the contact between Pt andγ-Al_(2)O_(3) and WO_(χ),resulting in a decrease in Pt sintering.The metal leaching and coking are not affected by the presence of second promoter.The catalyst modified with a second promoter possesses improved catalytic activity and 1,3-PDO production,however the stability continues to remain a challenge.The present work unrav-elled the determining parameters of catalytic activity and deactivation,thus providing a promising pro-tocol toward effective catalysts for glycerol hydrogenolysis.

关 键 词：Glycerol hydrogenolysis 1 3-PROPANEDIOL Metal-support interaction Second promoter Liquid phase Catalyst deactivation 

分 类 号：TQ223.162[化学工程—有机化工] TQ426