Catalyst design by scanning probe block copolymer lithography

Scanning probe block copolymer lithography (SPBCL), in combination with density-functional theory (DFT), has been used to design and synthesize hydrogen evolution catalysts. DFT was used to calculate the hydrogen adsorption energy on a series of single-element, bimetallic, and trimetallic (Au, Pt, N...

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Published inProceedings of the National Academy of Sciences - PNAS Vol. 115; no. 15; pp. 3764 - 3769
Main Authors Huang, Liliang, Chen, Peng-Cheng, Liu, Mohan, Fu, Xianbiao, Gordiichuk, Pavlo, Yu, Yanan, Wolverton, Chris, Kang, Yijin, Mirkin, Chad A.
Format Journal Article
LanguageEnglish
Published United States National Academy of Sciences 10.04.2018
Subjects
Adsorption
Bimetals
Block copolymers
Catalysis
Catalysts
Chemical synthesis
Copolymers
Copper
Density functional theory
Gold
Hydrogen
Hydrogen evolution
hydrogen evolution reaction
Hydrogen-based energy
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Lithography
multimetallic nanocatalyst
Nickel
Physical Sciences
Platinum
Scanning
Stoichiometry
Substrates
catalysis
multimetallic nanocatalyst
lithography
hydrogen evolution reaction
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Summary:Scanning probe block copolymer lithography (SPBCL), in combination with density-functional theory (DFT), has been used to design and synthesize hydrogen evolution catalysts. DFT was used to calculate the hydrogen adsorption energy on a series of single-element, bimetallic, and trimetallic (Au, Pt, Ni, and Cu) substrates to provide leads that could be synthesized in the form of alloy or phase-separated particles via SPBCL. PtAuCu (18 nm, ∼1:1:1 stoichiometry) has been identified as a homogeneous alloy phase that behaves as an effective hydrogen evolution catalyst in acidic aqueous media, even when it is made in bulk form via solution phase methods. Significantly, the bulk-prepared PtAuCu/C nanocatalyst discovered via this process exhibits an activity seven times higher than that of the state-of-the-art commercial Pt/C catalyst (based upon Pt content). The advantage of using SPBCL in the discovery process is that one can uniformly make particles, each consisting of a uniform phase combination (e.g., all alloy or all phase-segregated species) at a fixed elemental ratio, an important consideration when working with polyelemental species where multiple phases may exist.
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Author contributions: L.H., P.-C.C., Y.K., and C.A.M. designed the experiments; M.L. and C.W. performed DFT studies; Y.K. and C.A.M. conceived and supervised the project; L.H., Y.K., and C.A.M. analyzed results; L.H. carried out the experiments (synthesis, characterization, and HER evaluation) on SPBCL; X.F. and Y.Y. synthesized nanoparticles in solution phase and evaluated their HER performance; L.H., P.-C.C., M.L., X.F., P.G., Y.Y., C.W., Y.K., and C.A.M. discussed the results; and L.H., P.-C.C., M.L., X.F., P.G., Y.Y., C.W., Y.K., and C.A.M. wrote the paper.
Contributed by Chad A. Mirkin, February 14, 2018 (sent for review January 18, 2018; reviewed by Thomas E. Mallouk and Younan Xia)
Reviewers: T.E.M., The Pennsylvania State University; and Y.X., Georgia Institute of Technology.
1L.H. and P.-C.C. contributed equally to this work.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.1800884115