A new trick for an old support: Stabilizing gold single atoms on LaFeO3 perovskite

Chengcheng Tian, Haiyan Zhang, Xiang Zhu, Bo Lin, Xiaofei Liu, Hao Chen, Yafen Zhang, David R. Mullins, Carter W. Abney, Mohsen Shakouri, Roman Chernikov, Yongfeng Hu, Felipe Polo-Garzon, Zili Wu, Victor Fung, De en Jiang, Xiaoming Liu, Miaofang Chi, Jingyue Liu Jimmy, Sheng Dai

Research output: Contribution to journalArticlepeer-review

33 Scopus citations

Abstract

Single-atom catalysts (SACs) have shown great potential for achieving superior catalytic activity due to maximizing metal efficiency. The key obstacle in developing SACs lies in the availability of supports that can stabilize SACs. Here we report the first successful development of single gold (Au) atom catalysts supported on high-surface-area hierarchical perovskite oxides. The resulting Au single-atoms are extremely stable at calcination temperatures up to 700 °C in air and under reaction conditions. A high catalytic activity for CO oxidation and distinct self-activating property were also achieved. Furthermore, evidenced by theoretical calculations and experimental studies including X-ray absorption fine structures and in situ Fourier-transform infrared spectra, the surface Au active sites are confirmed to be predominately positively charged. This work provides a generalizable approach to fabricating highly stable Au single-atom catalysts with tunable catalytic performance, and we anticipate that this discovery will facilitate new possibilities for the development of single atom catalysts.

Original languageEnglish
Article number118178
JournalApplied Catalysis B: Environmental
Volume261
DOIs
StatePublished - Feb 2020

Funding

The research was supported financially by US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. J.L. acknowledges support of the National Science Foundation under CHE-1465057 and the use of facilities in the John M. Cowley Center for High Resolution Electron Microscopy at Arizona State University. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Use of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility, is supported by the Office of Science of US Department of Energy under Contract No. DE-AC02-05CH11231 . In situ FTIR studies and energy-dispersive X-ray spectroscopy (EDS) were conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. C.T. and H.Z. acknowledges support of Fundamental Research Funds for the Central Universities ( 50621021901007 ). X.Z. thanks the financial support from the Open Project of State Key Laboratory of Chemical Engineering (SKL-ChE-19C02) and the Young Thousand Talents Program. Appendix A The research was supported financially by US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. J.L. acknowledges support of the National Science Foundationunder CHE-1465057 and the use of facilities in the John M. Cowley Center for High Resolution Electron Microscopy at Arizona State University. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Use of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility, is supported by the Office of Science of US Department of Energy under Contract No. DE-AC02-05CH11231. In situ FTIR studies and energy-dispersive X-ray spectroscopy (EDS) were conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. C.T. and H.Z. acknowledges support of Fundamental Research Fundsfor the Central Universities (50621021901007). X.Z. thanks the financial support from the Open Project of State Key Laboratory of Chemical Engineering (SKL-ChE-19C02) and the Young Thousand Talents Program.

Keywords

  • CO oxidation
  • Gold single atoms
  • Perovskite
  • Self-activating
  • Sintering-resistance

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