Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 15, Pages 3764-3769Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1800884115
Keywords
lithography; hydrogen evolution reaction; multimetallic nanocatalyst; catalysis
Categories
Funding
- GlaxoSmithKline LLC
- Sherman Fairchild Foundation Inc.
- Air Force Office of Scientific Research Award [FA9550-16-1-0150]
- National Science Foundation Award [DBI-1353682]
- Netherlands Organization for Scientific Research for the Rubicon Grant
- National Science Foundation [CBET-1264963]
- International Institute for Nanotechnology (IIN)
- Institute for Sustainability and Energy at Northwestern
- National Natural Science Foundation of China [51601030, 21773023]
- 1000-Talents Program
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-1542205]
- Materials Research Science and Engineering Centers (MRSEC) program at the Materials Research Center [NSF DMR-1121262]
- IIN
- Keck Foundation
- State of Illinois, through the IIN
- MRSEC
- SHyNE
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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, similar to 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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