Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

Xu, Haidi; Zhang, Zihao; Liu, Jixing; Do-Thanh, Chi-Linh; Chen, Hao; Xu, Shuhao; Lin, Qinjing; Jiao, Yi; Wang, Jianli; Wang, Yun; Chen, Yaoqiang; Dai, Sheng

doi:10.1038/s41467-020-17738-9

Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

Journal Article · Thu Aug 06 00:00:00 UTC 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-17738-9· OSTI ID:1805021

^[1]; Zhang, Zihao ^[2]; Liu, Jixing ^[3]; ^[3]; Chen, Hao ^[3]; Xu, Shuhao ^[4]; Lin, Qinjing ^[4]; Jiao, Yi ^[5]; Wang, Jianli ^[4]; ^[6]; ^[5]; ^[2]

Sichuan Univ., Chengdu (China). Institute of New Energy and Low-Carbon Technology; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States). Joint Institute for Advanced Materials
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States). Joint Institute for Advanced Materials
Univ. of Tennessee, Knoxville, TN (United States). Joint Institute for Advanced Materials
Sichuan Univ., Chengdu (China)
Sichuan Univ., Chengdu (China). Institute of New Energy and Low-Carbon Technology
Sinocat Environmental Technology Co. Ltd., Chengdu (China)

Single-atom catalysts (SACs) have attracted considerable attention in the catalysis community. However, fabricating intrinsically stable SACs on traditional supports (N-doped carbon, metal oxides, etc.) remains a formidable challenge, especially under high-temperature conditions. Here, we report a novel entropy-driven strategy to stabilize Pd single-atom on the high-entropy fluorite oxides (CeZrHfTiLa)O_x (HEFO) as the support by a combination of mechanical milling with calcination at 900 °C. Characterization results reveal that single Pd atoms are incorporated into HEFO (Pd1@HEFO) sublattice by forming stable Pd–O–M bonds (M = Ce/Zr/La). Compared to the traditional support stabilized catalysts such as Pd@CeO₂, Pd₁@HEFO affords the improved reducibility of lattice oxygen and the existence of stable Pd–O–M species, thus exhibiting not only higher low-temperature CO oxidation activity but also outstanding resistance to thermal and hydrothermal degradation. This work therefore exemplifies the superiority of high-entropy materials for the preparation of SACs.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1805021

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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