Microwave-Assisted Synthesis of Classically Immiscible Ag–Ir Alloy Nanoparticle Catalysts

Guo, Hongyu; Li, Hao; Jarvis, Karalee; Wan, Haiqin; Kunal, Pranaw; Dunning, Samuel G.; Liu, Yulu; Henkelman, Graeme; Humphrey, Simon M.

doi:10.1021/acscatal.8b02103

Title: Microwave-Assisted Synthesis of Classically Immiscible Ag–Ir Alloy Nanoparticle Catalysts

Journal Article · 03 October 2018 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.8b02103 · OSTI ID:1543703

Guo, Hongyu ^[1]; Li, Hao ^[1];

^[2];

^[3]; Kunal, Pranaw ^[1]; Dunning, Samuel G. ^[1]; Liu, Yulu ^[1];

^[1];

^[1]

Univ. of Texas, Austin, TX (United States). Dept. of Chemistry
Univ. of Texas, Austin, TX (United States). Texas Materials Inst.
Univ. of Texas, Austin, TX (United States). Dept. of Chemistry; Nanjing Univ., Nanjing, Jiangsu (China). School of Environment

In this work, we present the synthesis of Ag–Ir alloys in the form of solid-solution nanoparticles (NPs). Ag and Ir are classically immiscible in the bulk and therefore the physical properties of Ag–Ir alloys are unknown. A convenient microwave-assisted, solution-phase method that employs readily available Ag(NO₃) and IrCl₃ precursors enables the preparation of small (2.5–5.5 nm) Ag–IrNPs with alloyed structures. Ag_$$x$$Ir_{(100–$$x$$)}NPs can be obtained by this method between $$x$$ = 6–31. The Ag–IrNPs resist dealloying upon heating up to 300 °C. Ir-rich Ag–IrNPs dispersed on amorphous silica are significantly more active gas-phase alkene hydrogenation catalysts than pure IrNPs. Density functional theory (DFT) and theoretical modeling studies reveal that the Ag–IrNPs—which are consistently larger than monometallic IrNPs prepared under the same conditions—have comparatively fewer strong H-binding edge sites. This promotes faster H atom transfer to coadsorbed alkenes. Ag–IrNPs supported on amorphous Co₃O₄ show a linear composition dependence in the selective hydrogenation of C$$=$$O versus C$$=$$C bonds: more Ag-rich Ag–IrNPs are more selective toward C$$=$$O hydrogenation of the α,β-unsaturated aldehyde crotonaldehyde, yielding the industrially desirable crotyl alcohol. Furthermore, deposition of Ag–IrNPs inside Co₃O₄ mesopores results in an additional ~56% selectivity enhancement.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE

OSTI ID:: 1543703

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 12 Vol. 8; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Microwave-Assisted Synthesis of Classically Immiscible Ag–Ir Alloy Nanoparticle Catalysts

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