Spontaneously polarized ceramic-carbon-supported Ni-Co for reinforcing water-assisted proton hopping to facilitate catalytic hydrogenation of levulinic acid  

作　　者：Hongguang Zhang Ying Zhu Furui Hu Wuxiang Zhang Fuzheng Fu Tao Gan Zuqiang Huang Huayu Hu Yanjuan Zhang 

机构地区：[1]School of Chemistry and Chemical Engineering,Guangxi University,Nanning 530004,China [2]Key Laboratory of New Low-carbon Green Chemical Technology,Education Department of Guangxi Zhuang Autonomous Region,Nanning 530004,China

出　　处：《Journal of Materials Science & Technology》2024年第36期255-268,共14页材料科学技术(英文版)

基　　金：supported by the National Natural Science Foundation of China(No.22008041);the Natural Science Foun-dation of Guangxi Province,China(Nos.2019GXNSFDA245020 and 2020GXNSFGA297001).

摘　　要：Water-assisted proton hopping(WAPH)plays an important role in the aqueous-phase hydrogenation of levulinic acid(LA)toγ-valerolactone(GVL).In this study,based on a strategy of spontaneously polarized ceramic(SPCE)-reinforced WAPH,a Ni-Co/SPCE-C catalyst was constructed by high-temperature calci-nation of a dual mechanical activation-treated precursor.Ni-Co/SPCE-C with favorable structural char-acteristics,intimate interfacial compatibility,and unique spontaneous polarization effect enhanced the migration efficiency of active hydrogen and activated water to form small water clusters,contributing to outstanding catalytic activity for aqueous-phase hydrogenation of LA to produce GVL at relatively low re-action temperature and H2 pressure.A LA conversion of 99.9%and a GVL yield of 92.3%were achieved at 160℃ and 1.5 MPa H2 over the Ni-Co/SPCE-C catalyst,which were significantly higher than those catalyzed by contrastive catalysts.A variety of tests and theoretical calculations reveal that SPCE with far-infrared emission and surface electric field was conducive to the reduction in the hydrogen spillover energy barrier,the stabilization of the transition state,and the facile exchange of H2 and water for ac-celerating WAPH.Moreover,a reasonable SPCE-reinforced WAPH mechanism was proposed to explain the enhanced aqueous hydrogenation of LA.This research can provide valuable insights into the design and development of high-performance non-noble metal catalysts for aqueous hydrogenation applications.

关 键 词：Non-noble metal catalyst Spontaneous polarization Aqueous-phase hydrogenation Proton hopping Smaller water clusters 

分 类 号：O64[理学—物理化学]