Harnessing strong metal-support interactions via a reverse route.

Autor: Wu P; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.; School of Chemistry & Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China., Tan S; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Moon J; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Yan Z; Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, VA, 24061, USA., Fung V; Department of Chemistry, University of California, Riverside, CA, 92521, USA., Li N; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA.; Frontier Institute of Science and Technology, Xi'an Jiaotong University, Xi'an, 710054, China., Yang SZ; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Cheng Y; Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Abney CW; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Wu Z; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Savara A; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Momen AM; Energy and Transportation Science Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA., Jiang DE; Department of Chemistry, University of California, Riverside, CA, 92521, USA., Su D; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA., Li H; School of Chemistry & Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China., Zhu W; School of Chemistry & Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China. zhuws@ujs.edu.cn., Dai S; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA. dais@ornl.gov.; Joint Institute for Advanced Materials, University of Tennessee, Knoxville, TN, 37996, USA. dais@ornl.gov., Zhu H; Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA. huiyuanz@vt.edu.; Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, VA, 24061, USA. huiyuanz@vt.edu.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2020 Jun 16; Vol. 11 (1), pp. 3042. Date of Electronic Publication: 2020 Jun 16.
DOI: 10.1038/s41467-020-16674-y
Abstrakt: Engineering strong metal-support interactions (SMSI) is an effective strategy for tuning structures and performances of supported metal catalysts but induces poor exposure of active sites. Here, we demonstrate a strong metal-support interaction via a reverse route (SMSIR) by starting from the final morphology of SMSI (fully-encapsulated core-shell structure) to obtain the intermediate state with desirable exposure of metal sites. Using core-shell nanoparticles (NPs) as a building block, the Pd-FeO x NPs are transformed into a porous yolk-shell structure along with the formation of SMSIR upon treatment under a reductive atmosphere. The final structure, denoted as Pd-Fe 3 O 4 -H, exhibits excellent catalytic performance in semi-hydrogenation of acetylene with 100% conversion and 85.1% selectivity to ethylene at 80 °C. Detailed electron microscopic and spectroscopic experiments coupled with computational modeling demonstrate that the compelling performance stems from the SMSIR, favoring the formation of surface hydrogen on Pd instead of hydride.
Databáze: MEDLINE