Synthesizing active and durable cubic ceria catalysts(＜6 nm)for fast dehydrogenation of bio-polyols to carboxylic acids coproducing green H2

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外文摘要：Dehydrogenation is considered as one of the most important industrial applications for renewable energy.Cubic ceria-based catalysts are known to display promising dehydrogenation performances in this area.Large particle size(＞20 nm)and less surface defects,however,hinder further application of ceria materials.Herein,an alternative strategy involving lactic acid(LA)assisted hydrothermal method was developed to synthesize active,selective and durable cubic ceria of＜6 nm for dehydrogenation reactions.Detailed studies of growth mechanism revealed that,the carboxyl and hydroxyl groups in LA molecule synergistically manipulate the morphological evolution of ceria precursors.Carboxyl groups determine the cubic shape and particle size,while hydroxyl groups promote compositional transformation of ceria precursors into CeO2 phases.Moreover,enhanced oxygen vacancies(Vö)on the surface of CeO2 were obtained owing to continuous removal of O species under reductive atmosphere.Cubic CeO2 catalysts synthesized by the LA-assisted method,immobilized with bimetallic PtCo clusters,exhibit a record high activity(TOF:29,241 h-1)and Vö-dependent synergism for dehydrogenation of bio-derived polyols at 200 ℃.We also found that quenching Vö defects at air atmosphere causes activity loss of PtCo/CeO2 catalysts.To regenerate Vö defects,a simple strategy was developed by irra-diating deactivated catalysts using hernia lamp.The outcome of this work will provide new insights into manufacturing durable catalyst ma-terials for aqueous phase dehydrogenation applications.

外文关键词：

Cubic ceriaOxygen vacancyDehydrogenationC-H bond activation

作者：

Mengyuan Liu、Puhua Sun、Guangyu Zhang、Xin Jin、Chaohe Yang、Honghong Shan

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作者单位：

State Key Laboratory of Heavy Oil Processing,College of Chemical Engineering,China University of Petroleum,No.66 Changjiang West Road,Qingdao,Shandong,266580,China

SINOPEC Research Institute of Safety Engineering Co.,Ltd.,No.339 Songling Road,Qingdao,Shandong,266000,China

基金：

国家自然科学基金国家自然科学基金山东省自然科学基金Innovative Research Funding from Qingdao City,Shandong Province中央高校基本科研业务费专项Development Fund of State Key Laboratory of Heavy Oil ProcessingDevelopment Fund of State Key Laboratory of Heavy Oil ProcessingPostgraduate Innovation Project from China University of Petroleum

项目编号：

2207836521706290ZR2017MB00417-1-1-80-jch17CX02017A20CX02204AYCX2021057

出版年：

2024

DOI：

10.1016/j.gee.2022.08.008

绿色能源与环境(英文)

CSTPCD

ISSN：

年,卷(期)：2024.9(3)

参考文献量60