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@ARTICLE{Zhang:1006569,
      author       = {Zhang, Kun and Guo, Qiang and Wang, Yehong and Cao, Pengfei
                      and Zhang, Bojian and Heggen, Marc and Mayer, Joachim and
                      Dunin-Borkowski, Rafal E. and Wang, Feng},
      title        = {{E}thylene {C}arbonylation to 3-{P}entanone with {I}n
                      {S}itu {H}ydrogen via a {W}ater–{G}as {S}hift {R}eaction
                      on {R}h/{C}e{O} 2},
      journal      = {ACS catalysis},
      volume       = {13},
      number       = {5},
      issn         = {2155-5435},
      address      = {Washington, DC},
      publisher    = {ACS},
      reportid     = {FZJ-2023-01717},
      pages        = {3164 - 3169},
      year         = {2023},
      abstract     = {Alkene carbonylation, in which hydrogenation plays pivotal
                      roles, is one of the most efficient method for the
                      production of oxygenated chemicals like aldehydes, amides,
                      and esters, among others. In this work, using in situ
                      produced hydrogen via a water–gas shift (WGS) reaction,
                      selective ethylene carbonylation to 3-pentanone was achieved
                      instead of hydroformylation to propionaldehyde with gaseous
                      H2 on a defective ceria-supported Rh catalyst. The interface
                      of Rh/CeO2, which consists of oxygen vacancies and
                      positively charged Rh, activates water, CO, and ethylene and
                      the subsequent reactions, including the WGS reaction and
                      ethylene carbonylation. The lean hydrogen circumstance
                      created by the WGS reaction suppresses the hydrogenation of
                      the propionyl group and promotes its ethylation to
                      3-pentanone. A redox pathway was proposed for the WGS
                      reaction based on the in situ FTIR results, and the origin
                      of hydrogen for ethylene carbonylation is water, as
                      confirmed by a mass spectrometry (MS) study using d2-water
                      as one of the reactants. This work provides a promising
                      method for heavier ketone synthesis.},
      cin          = {ER-C-1},
      ddc          = {540},
      cid          = {I:(DE-Juel1)ER-C-1-20170209},
      pnm          = {5351 - Platform for Correlative, In Situ and Operando
                      Characterization (POF4-535)},
      pid          = {G:(DE-HGF)POF4-5351},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000944488200001},
      doi          = {10.1021/acscatal.2c06123},
      url          = {https://juser.fz-juelich.de/record/1006569},
}