Harnessing strong metal-support interactions via a reverse route

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dc.contributor.authorWu, Peiwenen
dc.contributor.authorTan, Shuaien
dc.contributor.authorMoon, Jisueen
dc.contributor.authorYan, Zihaoen
dc.contributor.authorFung, Victoren
dc.contributor.authorLi, Naen
dc.contributor.authorYang, Shi-Zeen
dc.contributor.authorCheng, Yongqiangen
dc.contributor.authorAbney, Carter W.en
dc.contributor.authorWu, Zilien
dc.contributor.authorSavara, Adityaen
dc.contributor.authorMomen, Ayyoub M.en
dc.contributor.authorJiang, De-enen
dc.contributor.authorSu, Dongen
dc.contributor.authorLi, Huamingen
dc.contributor.authorZhu, Wenshuaien
dc.contributor.authorDai, Shengen
dc.contributor.authorZhu, Huiyuanen
dc.contributor.departmentChemical Engineeringen
dc.date.accessioned2020-08-04T17:38:24Zen
dc.date.available2020-08-04T17:38:24Zen
dc.date.issued2020-06-16en
dc.description.abstractEngineering 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-FeOx 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-Fe3O4-H, exhibits excellent catalytic performance in semi-hydrogenation of acetylene with 100% conversion and 85.1% selectivity to ethylene at 80 degrees 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.en
dc.description.notesThis research is sponsored by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program. The computational calculations used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility. XAFS data were collected at the Advanced Photon Source at Argonne National Laboratory on Beamline 10ID-B, supported by the Materials Research Collaborative Access Team (MRCAT). MRCAT operations are supported by the DOE and the MRCAT member institutions. This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. The neutron studies used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. Part of the work including the chemisorption was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. The Spallation Neutron Source at Oak Ridge National Laboratory is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE, under contract no. DE-AC0500OR22725 with UT Battelle, LLC. Part of the TEM work was performed at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. DOE, Office of Basic Energy Science, under contract no. DE-SC0012704. P.W.W., W.S.Z., and H.M.L. were financially supported by the National Natural Science Foundation of China (21722604), Natural Science Foundation of Jiangsu Province (BK20190852). P.W.W. is thankful to the scholarship from China Scholarship Council (CSC).en
dc.description.sponsorshipU.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science ProgramUnited States Department of Energy (DOE); Materials Research Collaborative Access Team (MRCAT); DOEUnited States Department of Energy (DOE); MRCAT; DOE Office of ScienceUnited States Department of Energy (DOE) [DE-AC02-06CH11357]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOEUnited States Department of Energy (DOE) [DE-AC0500OR22725]; UT Battelle, LLC; U.S. DOE, Office of Basic Energy ScienceUnited States Department of Energy (DOE) [DE-SC0012704]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China [21722604]; Natural Science Foundation of Jiangsu ProvinceJiangsu Planned Projects for Postdoctoral Research FundsNatural Science Foundation of Jiangsu Province [BK20190852]; China Scholarship Council (CSC)China Scholarship Councilen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1038/s41467-020-16674-yen
dc.identifier.issn2041-1723en
dc.identifier.issue1en
dc.identifier.other3042en
dc.identifier.pmid32546680en
dc.identifier.urihttp://hdl.handle.net/10919/99477en
dc.identifier.volume11en
dc.language.isoenen
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.titleHarnessing strong metal-support interactions via a reverse routeen
dc.title.serialNature Communicationsen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.dcmitypeStillImageen

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