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Atomically synergistic Zn-Cr catalyst for iso-stoichiometric co-conversion of ethane and CO2 to ethylene and CO.
Yang, Ji; Wang, Lu; Wan, Jiawei; El Gabaly, Farid; Fernandes Cauduro, Andre L; Mills, Bernice E; Chen, Jeng-Lung; Hsu, Liang-Ching; Lee, Daewon; Zhao, Xiao; Zheng, Haimei; Salmeron, Miquel; Wang, Caiqi; Dong, Zhun; Lin, Hongfei; Somorjai, Gabor A; Rosner, Fabian; Breunig, Hanna; Prendergast, David; Jiang, De-En; Singh, Seema; Su, Ji.
Affiliation
  • Yang J; Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Wang L; The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Wan J; Department of Chemistry, University of California, Riverside, CA, USA.
  • El Gabaly F; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Fernandes Cauduro AL; Sandia National Laboratories, Livermore, CA, US.
  • Mills BE; Sandia National Laboratories, Livermore, CA, US.
  • Chen JL; Sandia National Laboratories, Livermore, CA, US.
  • Hsu LC; National Synchrotron Radiation Research Center, Science-Based Industrial Park, Hsinchu, Taiwan.
  • Lee D; Department of Soil and Environmental Sciences, National Chung Hsing University, Taichung, Taiwan.
  • Zhao X; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Zheng H; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Salmeron M; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Wang C; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Dong Z; Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, USA.
  • Lin H; Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, USA.
  • Somorjai GA; Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, WA, USA.
  • Rosner F; Department of Chemistry, University of California, Berkeley, CA, USA.
  • Breunig H; Energy Analysis and Environmental Impacts Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Prendergast D; Energy Analysis and Environmental Impacts Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Jiang DE; The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
  • Singh S; Department of Chemistry, University of California, Riverside, CA, USA. de-en.jiang@vanderbilt.edu.
  • Su J; Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN, USA. de-en.jiang@vanderbilt.edu.
Nat Commun ; 15(1): 911, 2024 Jan 30.
Article in En | MEDLINE | ID: mdl-38291043
ABSTRACT
Developing atomically synergistic bifunctional catalysts relies on the creation of colocalized active atoms to facilitate distinct elementary steps in catalytic cycles. Herein, we show that the atomically-synergistic binuclear-site catalyst (ABC) consisting of [Formula see text]-O-Cr6+ on zeolite SSZ-13 displays unique catalytic properties for iso-stoichiometric co-conversion of ethane and CO2. Ethylene selectivity and utilization of converted CO2 can reach 100 % and 99.0% under 500 °C at ethane conversion of 9.6%, respectively. In-situ/ex-situ spectroscopic studies and DFT calculations reveal atomic synergies between acidic Zn and redox Cr sites. [Formula see text] ([Formula see text]) sites facilitate ß-C-H bond cleavage in ethane and the formation of Zn-Hδ- hydride, thereby the enhanced basicity promotes CO2 adsorption/activation and prevents ethane C-C bond scission. The redox Cr site accelerates CO2 dissociation by replenishing lattice oxygen and facilitates H2O formation/desorption. This study presents the advantages of the ABC concept, paving the way for the rational design of novel advanced catalysts.
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Nat Commun Journal subject: BIOLOGIA / CIENCIA Year: 2024 Type: Article Affiliation country: United States
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Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: Nat Commun Journal subject: BIOLOGIA / CIENCIA Year: 2024 Type: Article Affiliation country: United States