Unraveling the coordination structure-performance relationship in Pt1/Fe2O3 single-atom catalyst

Yujing Ren, Yan Tang, Leilei Zhang, Xiaoyan Liu, Lin Li, Shu Miao, Dang Sheng Su, Aiqin Wang (), Jun Li () and Tao Zhang ()
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Yujing Ren: Chinese Academy of Sciences
Yan Tang: Tsinghua University
Leilei Zhang: Chinese Academy of Sciences
Xiaoyan Liu: Chinese Academy of Sciences
Lin Li: Chinese Academy of Sciences
Shu Miao: Chinese Academy of Sciences
Dang Sheng Su: Chinese Academy of Sciences
Aiqin Wang: Chinese Academy of Sciences
Jun Li: Tsinghua University
Tao Zhang: Chinese Academy of Sciences

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: Abstract Heterogeneous single-atom catalyst (SAC) opens a unique entry to establishing structure–performance relationship at the molecular level similar to that in homogeneous catalysis. The challenge lies in manipulating the coordination chemistry of single atoms without changing single-atom dispersion. Here, we develop an efficient synthetic method for SACs by using ethanediamine to chelate Pt cations and then removing the ethanediamine by a rapid thermal treatment (RTT) in inert atmosphere. The coordination chemistry of Pt single atoms on a Fe2O3 support is finely tuned by merely adjusting the RTT temperature. With the decrease in Pt-O coordination number, the oxidation state of Pt decreases, and consequently the hydrogenation activity increases to a record level without loss of chemoselectivity. The tunability of the local coordination chemistry, oxidation states of the metal, and the catalytic performance of single atoms reveals the unique role of SACs as a bridge between heterogeneous and homogeneous catalysis.

Date: 2019
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DOI: 10.1038/s41467-019-12459-0

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