Highly dispersed Pd clusters/nanoparticles encapsulated in MOFs via in situ auto-reduction method for aqueous phenol hydrogenation  

作　　者：Xiubing Huang Xiaoyu Li Wei Xia Bin Hu Martin Muhler Baoxiang Peng 

机构地区：[1]Beijing Advanced Innovation Center for Materials Genome Engineering,Beijing Key Laboratory of Function Materials for Molecule&Structure Construction,School of Materials Science and Engineering,University of Science and Technology Beijing,Beijing 10083,China [2]Laboratory of Industrial Chemistry,Faculty of Chemistry and Biochemistry,Ruhr University Bochum,Bochum 44780,Germany [3]Max Planck Institute for Chemical Energy Conversion,Mülheim a.d.Ruhr 45470,Germany

出　　处：《Journal of Materials Science & Technology》2022年第14期167-175,共9页材料科学技术（英文版）

基　　金：financial support from the National Natural Science Foundation of China(Grant No.51802015);the Research Department Closed Carbon Cycle Economy(CCCE)at the Ruhr-University Bochum,Fundamental Research Funds for the Central Universities(No.FRF-TP-20-005A3);the Fundamental Research Funds for the Central Universities and the Youth Teacher International Exchange&Growth Program(Grant No.QNXM20210016)。

摘　　要：In this work,a novel in situ auto-reduction strategy was developed to encapsulate uniformly dispersed Pd clusters/nanoparticles in MIL-125-NH_(2).It is demonstrated that the amino groups in MIL-125-NH_(2)can react with formaldehyde to form novel reducing groups(-NH-CH_(2)OH),which can in situ auto-reduce the encapsulated Pd^(2+)ions to metallic Pd clusters/nanoparticles.As no additional reductants are required,the strategy limits the aggregation and migration of Pd clusters and the formation of large Pd nanoparticles via controlling the amount of Pd^(2+)precursor.When applied as catalysts in the hydrogenation of phenol in the aqueous phase,the obtained Pd(1.5)/MIL-125-NH-CH_(2)OH catalyst with highly dispersed Pd clusters/nanoparticles with the size of around 2 nm exhibited 100%of phenol conversion and 100%of cyclohexanone selectivity at 70℃ after 5 h,as well as remarkable reusability for at least five cycles due to the large MOF surface area,the highly dispersed Pd clusters/nanoparticles and their excellent stability within the MIL-125-NH-CH_(2)OH framework.

关 键 词：Pd clusters Pd nanoparticles MIL-125-NH_(2) In situ auto-reduction Double solvent method Hydrogenation of phenol 

分 类 号：TB383.1[一般工业技术—材料科学与工程] O643.36[理学—物理化学]