Imaging the kinetics of anisotropic dissolution of bimetallic core–shell nanocubes using graphene liquid cells

Chen, Lei; Leonardi, Alberto; Chen, Jun; Cao, Muhan; Li, Na; Su, Dong; Zhang, Qiao; Engel, Michael; Ye, Xingchen

doi:10.1038/s41467-020-16645-3

Imaging the kinetics of anisotropic dissolution of bimetallic core–shell nanocubes using graphene liquid cells

Journal Article · Tue Jun 16 00:00:00 EDT 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-16645-3· OSTI ID:1642411

Chen, Lei ^[1]; ^[2]; Chen, Jun ^[3]; Cao, Muhan ^[3]; Li, Na ^[4]; ^[5]; ^[6]; ^[2]; ^[3]

Soochow Univ., Suzhou (China). Inst. of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Lab. for Carbon-Based Functional Materials and Devices; Indiana Univ., Bloomington, IN (United States)
Friedrich-Alexander Univ., Erlangen (Germany). Inst. for Multiscale Simulation, IZFN
Indiana Univ., Bloomington, IN (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Xi'an Jiaotong Univ., Shaanxi (China). Frontier Inst. of Chemistry, Frontier Inst. of Science and Technology
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Soochow Univ., Suzhou (China). Inst. of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Lab. for Carbon-Based Functional Materials and Devices

Chemical design of multicomponent nanocrystals requires atomic-level understanding of reaction kinetics. Here, we apply single-particle imaging coupled with atomistic simulation to study reaction pathways and rates of Pd@Au and Cu@Au core-shell nanocubes undergoing oxidative dissolution. Quantitative analysis of etching kinetics using in situ transmission electron microscopy (TEM) imaging reveals that the dissolution mechanism changes from predominantly edge-selective to layer-by-layer removal of Au atoms as the reaction progresses. Dissolution of the Au shell slows down when both metals are exposed, which we attribute to galvanic corrosion protection. Morphological transformations are determined by intrinsic anisotropy due to coordination-number-dependent atom removal rates and extrinsic anisotropy induced by the graphene window. Our work demonstrates that bimetallic coreshell nanocrystals are excellent probes for the local physicochemical conditions inside TEM liquid cells. Furthermore, single-particle TEM imaging and atomistic simulation of reaction trajectories can inform future design strategies for compositionally and architecturally sophisticated nanocrystals.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1642411

Report Number(s):: BNL--216189-2020-JAAM

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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