Silicalite-1 zeolite encapsulated Cu–ZnO nanoparticles for selective CO_(2)hydrogenation to oxygenatesOA
Selective conversion of CO_(2)into value-added oxygenates,particularly methanol and dimethyl ether(DME),presents a promising route for CO_(2)utilization.However,achieving both high selectivity and catalyst stability remained significant challenges.To address this,we report the fabrication of a core–shell-structured catalyst prepared by a steam-assisted crystallization(SAC)approach,in which highly dispersed Cu–ZnO nanoparticles(2.0–3.5 nm)are encapsulated within nanocrystalline silicalite-1 zeolite.The spatial confinement effects from silicalite-1 frameworks induce strong metal–zeolite interactions,effectively suppressing Cu–ZnO nanoparticle aggregation and sintering phenomena.This structural feature helps to preserve dominant populations of active Cu^(+)species on thermally stabilized Cu–ZnO nanoparticles.As a result,the optimized catalyst enables efficient tandem conversion of CO_(2)to oxygenates,achieving a CO_(2)conversion of 21.5%with an oxygenate selectivity of 83.0%toward dimethyl ether(DME,72.5%)and methanol(10.5%),where an optimized catalyst exhibits exceptional catalytic performance for the tandem CO_(2)-to-DME reaction.Comprehensive characterization reveals that the spatial confinement within the protective silicalite-1 matrix not only stabilizes highly dispersed Cu–ZnO nanoparticles and Cu^(+)sites but also facilitates the formation and stabilization of key reaction intermediates.These synergistic effects are directly responsible for an enhanced catalytic activity,high DME selectivity,and prolonged operational durability observed during 300 h of continuous CO_(2)hydrogenation.
Xu Wang;Dongming Shen;Hui Kang;Kangzhou Wang;Chundong Zhang;Xinhua Gao;Jianli Zhang;Eunjoo Jang;Jong Wook Bae
Institute for Advanced Study,Chengdu University,Chengdu 610106,China School of Chemical Engineering,Sungkyunkwan University(SKKU),2066 Seoburo,Jangan-gu,Suwon,Gyeonggi-do 16419,Republic of KoreaSchool of Chemical Engineering,Sungkyunkwan University(SKKU),2066 Seoburo,Jangan-gu,Suwon,Gyeonggi-do 16419,Republic of KoreaInstitute for Advanced Study,Chengdu University,Chengdu 610106,ChinaSchool of Materials and New Energy,Ningxia University,Yinchuan 750021,Ningxia,ChinaState Key Laboratory of Materials-Oriented Chemical Engineering,College of Chemical Engineering,Nanjing Tech University,Nanjing 211816,ChinaState Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering,College of Chemistry&Chemical Engineering,Ningxia University,Yinchuan 750021,ChinaState Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering,College of Chemistry&Chemical Engineering,Ningxia University,Yinchuan 750021,ChinaSKKU Advanced Institute of Nanotechnology(SAINT),Sungkyunkwan University(SKKU),2066 Seobu-ro,Jangan-gu,Suwon,Gyeonggi-do 16419,Republic of KoreaSchool of Chemical Engineering,Sungkyunkwan University(SKKU),2066 Seoburo,Jangan-gu,Suwon,Gyeonggi-do 16419,Republic of Korea
化学化工
core shell structured catalystsilicalitedimethyl etheroxygenatesdimethyl ether dme presentsCO hydrogenationmethanolcu zno nanoparticles
《Industrial Chemistry & Materials》 2026 (3)
P.342-354,13
supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(RS-2024-00405818)by the startup grant for talent introduction of Chengdu University(2081925056)the financial support of“Cooperative Research Program for Agriculture Science and Technology Development(Project No.PJ016259032021)”Rural Development Administration,Republic of Korea。
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