Grain‐Boundary‐Rich Noble Metal Nanoparticle Assemblies: Synthesis, Characterization, and Reactivity

Geng, Xin; Li, Shuwei; Heo, Jaeyoung; Peng, Yi; Hu, Wenhui; Liu, Yanchao; Huang, Jier; Ren, Yang; Li, Dongsheng; Zhang, Liang; Luo, Long

doi:10.1002/adfm.202204169

Title: Grain‐Boundary‐Rich Noble Metal Nanoparticle Assemblies: Synthesis, Characterization, and Reactivity

Journal Article · 14 June 2022 · Advanced Functional Materials

DOI: https://doi.org/10.1002/adfm.202204169 · OSTI ID:1872651

Geng, Xin ^[1]; Li, Shuwei ^[2]; Heo, Jaeyoung ^[3]; Peng, Yi ^[1]; Hu, Wenhui ^[4]; Liu, Yanchao ^[5]; Huang, Jier ^[4]; Ren, Yang ^[6]; Li, Dongsheng ^[3]; Zhang, Liang ^[2];

^[1]

Department of Chemistry Wayne State University Detroit MI 48202 USA
Center for Combustion Energy School of Vehicle and Mobility State Key Laboratory of Automotive Safety and Energy Tsinghua University Beijing 100084 China
Physical and Computational Sciences Directorate Pacific Northwest National Laboratory Richland WA 99352 USA
Department of Chemistry Marquette University Milwaukee WI 53201 United States
Department of Industrial and Systems Engineering Wayne State University Detroit MI 48202 USA
Department of Physics City University of Hong Kong Hong Kong SAR China

Abstract Here, a comprehensive study on the synthesis, characterization, and reactivity of grain‐boundary (GB)‐rich noble metal nanoparticle (NP) assemblies is presented. A facile and scalable synthesis of Pt, Pd, Au, Ag, and Rh NP assemblies is developed, in which NPs are predominantly connected via Σ3 (111) twin GBs, forming a network. Driven by water electrolysis, the random collisions and oriented attachment of colloidal NPs in solution lead to the formation of Σ3 (111) twin boundaries and some highly mismatched GBs. This synthetic method also provides convenient control over the GB density without altering the crystallite size or GB type by varying the NP collision frequency. The structural characterization reveals the presence of localized tensile strain at the GB sites. The ultrahigh activity of GB‐rich Pt NP assembly toward catalytic hydrogen oxidation in air is demonstrated, enabling room‐temperature catalytic hydrogen sensing for the first time. Finally, density functional theory calculations reveal that the strained Σ3(111) twin boundary facilitates oxygen dissociation, drastically enhancing the hydrogen oxidation rate via the dissociative pathway. This reported large‐scale synthesis of the Σ3 (111) twin GB‐rich structures enables the development of a broad range of high‐performance GB‐rich catalysts.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1872651

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 34 Vol. 32; ISSN 1616-301X

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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