4.8 Article

A Hydrothermally Stable Single-Atom Catalyst of Pt Supported on High-Entropy Oxide/Al2O3: Structural Optimization and Enhanced Catalytic Activity

期刊

ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 41, 页码 48764-48773

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c14456

关键词

high-entropy oxides; single-atom Pt; interface design; hydrothermally stable; heterogeneous catalyst

资金

  1. National Key Research and Development Program of China [2018YFA0209600]
  2. Science and Technology Key Project of Guangdong Province, China [2020B010188002]
  3. Guangdong Innovative and Entrepreneurial Research Team Program [2019ZT08L075]
  4. Foshan Innovative and Entrepreneurial Research Team Program [2018IT100031]
  5. Guangdong Pearl River Talent Program [2 0 19QN01L0 5 4]
  6. Shenzhen Peacock Plan [KQTD2016053015544057]
  7. Nanshan Pilot Plan [LHTD20170001]
  8. Science and Technology Program of Guangzhou, China [202002030153]
  9. Guangdong Science and Technology Program [2017B030314002]
  10. National Natural Science Foundation of China [22176063, 52000076, 22106048]
  11. Natural Science Foundation of Guangdong Province [2021A1515010091]
  12. Innovation and Entrepreneurship Talent Program of Shaoguan City, China Postdoctoral Science Foundation [2020 M682714]
  13. Fundamental Research Funds for the Central Universities [2020ZYGXZR061]

向作者/读者索取更多资源

The study presents a single-atom Pt-HEO/Al2O3 catalyst achieved through a sol-gel-assisted mechanical milling strategy, where the strong interaction between HEO and Al2O3 effectively inhibits the growth of HEO microparticles, while another strong interaction between Pt and HEO stabilizes single-atom Pt on HEO. This catalyst shows superior stability against hydrothermal aging and long-term reaction stability for CO catalytic oxidation, exceeding 540 hours, opening up new possibilities for practical applications.
A catalyst with high-entropy oxide (HEO)-stabilized single-atom Pt can afford low-temperature activity for catalytic oxidation and remarkable durability even under harsh conditions. However, HEO is easy to harden during sintering, which results in a few defective sites for anchoring single-atom metals. Herein, we present a sol-gel-assisted mechanical milling strategy to achieve a single-atom catalyst of Pt-HEO/Al2O3. The strong interaction between HEO and Al2O3 effectively inhibits the growth of HEO microparticles, which leads to generation of more surface defects because of the nanoscale effect. Meanwhile, another strong interaction between Pt and HEO stabilizes single-atom Pt on HEO. Temperature-programmed techniques further verify that the reactivity of surface lattice oxygen species is enhanced because of the Pt-O-M bonds on the surface of HEO. Unlike conventional single-atom Pt catalysts, Pt-HEO/Al2O3 as a heterogeneous catalyst not only exhibits superior stability against hydrothermal aging but also presents long-term reaction stability for CO catalytic oxidation, which exceeds 540 h. The present work opens a new door for rational design of hydrothermally stable single-atom Pt catalysts, which are highly promising in practical applications.

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