TY - JOUR
T1 - Self-regeneration of supported transition metals by a high entropy-driven principle
AU - Hou, Shengtai
AU - Ma, Xuefeng
AU - Shu, Yuan
AU - Bao, Jiafeng
AU - Zhang, Qiuyue
AU - Chen, Mingshu
AU - Zhang, Pengfei
AU - Dai, Sheng
N1 - Publisher Copyright:
© 2021, The Author(s).
PY - 2021/12/1
Y1 - 2021/12/1
N2 - The sintering of Supported Transition Metal Catalysts (STMCs) is a core issue during high temperature catalysis. Perovskite oxides as host matrix for STMCs are proven to be sintering-resistance, leading to a family of self-regenerative materials. However, none other design principles for self-regenerative catalysts were put forward since 2002, which cannot satisfy diverse catalytic processes. Herein, inspired by the principle of high entropy-stabilized structure, a concept whether entropy driving force could promote the self-regeneration process is proposed. To verify it, a high entropy cubic Zr0.5(NiFeCuMnCo)0.5Ox is constructed as a host model, and interestingly in situ reversible exsolution-dissolution of supported metallic species are observed in multi redox cycles. Notably, in situ exsolved transition metals from high entropy Zr0.5(NiFeCuMnCo)0.5Ox support, whose entropic contribution (TΔSconfig = T⋆12.7 J mol−1 K−1) is predominant in ∆G, affording ultrahigh thermal stability in long-term CO2 hydrogenation (400 °C, >500 h). Current theory may inspire more STWCs with excellent sintering-resistance performance.
AB - The sintering of Supported Transition Metal Catalysts (STMCs) is a core issue during high temperature catalysis. Perovskite oxides as host matrix for STMCs are proven to be sintering-resistance, leading to a family of self-regenerative materials. However, none other design principles for self-regenerative catalysts were put forward since 2002, which cannot satisfy diverse catalytic processes. Herein, inspired by the principle of high entropy-stabilized structure, a concept whether entropy driving force could promote the self-regeneration process is proposed. To verify it, a high entropy cubic Zr0.5(NiFeCuMnCo)0.5Ox is constructed as a host model, and interestingly in situ reversible exsolution-dissolution of supported metallic species are observed in multi redox cycles. Notably, in situ exsolved transition metals from high entropy Zr0.5(NiFeCuMnCo)0.5Ox support, whose entropic contribution (TΔSconfig = T⋆12.7 J mol−1 K−1) is predominant in ∆G, affording ultrahigh thermal stability in long-term CO2 hydrogenation (400 °C, >500 h). Current theory may inspire more STWCs with excellent sintering-resistance performance.
UR - http://www.scopus.com/inward/record.url?scp=85116839263&partnerID=8YFLogxK
U2 - 10.1038/s41467-021-26160-8
DO - 10.1038/s41467-021-26160-8
M3 - Article
C2 - 34635659
AN - SCOPUS:85116839263
SN - 2041-1723
VL - 12
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 5917
ER -
