Harnessing strong metal-support interactions via a reverse route

Peiwen Wu; Shuai Tan; Jisue Moon; Zihao Yan; Victor Fung; Na Li; Shi-Ze Yang; Yongqiang Cheng; Carter W Abney; Zili Wu; Aditya Savara; Ayyoub M Momen; De-En Jiang; Dong Su; Huaming Li; Wenshuai Zhu; Sheng Dai; Huiyuan Zhu

doi:10.1038/s41467-020-16674-y

Harnessing strong metal-support interactions via a reverse route

Nat Commun. 2020 Jun 16;11(1):3042. doi: 10.1038/s41467-020-16674-y.

Authors

Peiwen Wu^#^{1

2}, Shuai Tan^#¹, Jisue Moon¹, Zihao Yan³, Victor Fung⁴, Na Li^{5

6}, Shi-Ze Yang¹, Yongqiang Cheng⁷, Carter W Abney¹, Zili Wu¹, Aditya Savara¹, Ayyoub M Momen⁸, De-En Jiang⁴, Dong Su⁵, Huaming Li², Wenshuai Zhu⁹, Sheng Dai^{10

11}, Huiyuan Zhu^{12

13}

Affiliations

¹ Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
² School of Chemistry & Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China.
³ Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, VA, 24061, USA.
⁴ Department of Chemistry, University of California, Riverside, CA, 92521, USA.
⁵ Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA.
⁶ Frontier Institute of Science and Technology, Xi'an Jiaotong University, Xi'an, 710054, China.
⁷ Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
⁸ Energy and Transportation Science Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
⁹ School of Chemistry & Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China. zhuws@ujs.edu.cn.
¹⁰ Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA. dais@ornl.gov.
¹¹ Joint Institute for Advanced Materials, University of Tennessee, Knoxville, TN, 37996, USA. dais@ornl.gov.
¹² Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA. huiyuanz@vt.edu.
¹³ Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, VA, 24061, USA. huiyuanz@vt.edu.

^# Contributed equally.

Abstract

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-Fe₃O₄-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.