Suppressing COx in oxidative dehydrogenation of propane with dual-atom catalysts - Details

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Oxidative　dehydrogenation　of　propane　(ODHP)　is　a　promising　route　for　propylene　production,　but　achieving　high　selectivity　towards　propylene　while　minimizing　COx　byproducts　remains　a　significant　challenge　for　conventional　metal　oxide　catalysts.　Here　we　propose　a　solution　to　this　challenge　by　employing　atomically　dispersed　dual-atom　catalysts　(M1M＇1-TiO2　DACs).　Ni1Fe1-TiO2　DACs　exhibit　an　ultralow　COx　selectivity　of　5.2%　at　a　high　propane　conversion　of　46.1%　and　520　°C,　with　stable　performance　for　over　1000　hours.　Mechanistic　investigations　reveal　that　these　catalysts　operate　via　a　cooperative　Langmuir-Hinshelwood　mechanism,　distinct　from　the　Mars-van　Krevelen　mechanism　typical　of　metal　oxides.　This　cooperative　pathway　facilitates　efficient　conversion　of　propane　and　oxygen　into　propylene　at　the　dual-atom　interface.　The　superior　selectivity　arises　from　facile　olefin　desorption　from　the　dual-atom　sites　and　suppressed　formation　of　electrophilic　oxygen　species,　which　are　preferentially　adsorbed　on　Fe1　sites　rather　than　oxygen　vacancies.　This　work　highlights　the　potential　of　dual-atom　catalysts　for　highly　selective　ODHP　and　provides　insights　into　their　unique　catalytic　mechanism.　©　The　Author(s)　2025.

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[ 1 ] [Yao Y.]Key Laboratory of Luminescence and Optical Information, Ministry of Education, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing, 100044, China
[ 2 ] [Yao Y.]Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031, China
[ 3 ] [Wang J.]Institute of Molecular Engineering Plus, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
[ 4 ] [Lu F.]College of Physical Science and Technology, Yangzhou University, Yangzhou, 225002, China
[ 5 ] [Li W.]College of Chemistry and Chemical Engineering, State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, 030024, China
[ 6 ] [Mei B.]Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, China
[ 7 ] [Zhang L.]Institute of Molecular Engineering Plus, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
[ 8 ] [Yan W.]National Synchrotron Radiation Laboratory, University of Science and Technology of China, Anhui, Hefei, 230026, China
[ 9 ] [Yuan F.]State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
[ 10 ] [Jiang G.]State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, 102249, China
[ 11 ] [Senanayake S.D.]Chemistry Division, Brookhaven National Laboratory, Upton, 11973, NY, United States
[ 12 ] [Wang X.]Key Laboratory of Luminescence and Optical Information, Ministry of Education, School of Physical Science and Engineering, Beijing Jiaotong University, Beijing, 100044, China
[ 13 ] [Wang X.]Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031, China

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Nature Communications

ISSN： 2041-1723

Year： 2025

Issue： 1

Volume： 16

1 4 . 7 0 0

JCR@2023

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ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 2

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