Abstract
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.
Original language | English (US) |
---|---|
Pages (from-to) | 3764-3769 |
Number of pages | 6 |
Journal | Proceedings of the National Academy of Sciences of the United States of America |
Volume | 115 |
Issue number | 15 |
DOIs | |
State | Published - 2018 |
Funding
Office of Scientific Research Award FA9550-16-1-0150, and the National Science Foundation Award DBI-1353682. P.G. gratefully acknowledges The Netherlands Organization for Scientific Research for the Rubicon Grant. M.L. gratefully acknowledges the support from the National Science Foundation (CBET-1264963). Y.K., X.F., and Y.Y. acknowledge the support from International Institute for Nanotechnology (IIN), Institute for Sustainability and Energy at Northwestern, National Natural Science Foundation of China, under Award 51601030, 21773023, and award of 1000-Talents Program (to Y.K.). This work made use of the Electron Probe Instrumentation Center (EPIC) facility of Northwestern University’s Atomic and Nanoscale Characterization Experimental Center (NUANCE), which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the Materials Research Science and Engineering Centers (MRSEC) program (NSF DMR-1121262) at the Materials Research Center; the IIN; the Keck Foundation; and the State of Illinois, through the IIN. This work made use of the J.B. Cohen X-Ray Diffraction Facility supported by MRSEC and SHyNE. This work made use of resources in National Energy Research Scientific Computing Center and Northwestern University’s Quest high-performance computing system. ACKNOWLEDGMENTS. This material is based, in part, upon work supported by GlaxoSmithKline LLC, Sherman Fairchild Foundation Inc., the Air Force This material is based, in part, upon work supported by GlaxoSmithKline LLC, Sherman Fairchild Foundation Inc., the Air Force Office of Scientific Research Award FA9550-16-1-0150, and the National Science Foundation Award DBI-1353682. P.G. gratefully acknowledges The Netherlands Organization for Scientific Research for the Rubicon Grant. M.L. gratefully acknowledges the support from the National Science Foundation (CBET-1264963). Y.K., X.F., and Y.Y. acknowledge the support from International Institute for Nanotechnology (IIN), Institute for Sustainability and Energy at Northwestern, National Natural Science Foundation of China, under Award 51601030, 21773023, and award of 1000-Talents Program (to Y.K.). This work made use of the Electron Probe Instrumentation Center (EPIC) facility of Northwestern University's Atomic and Nanoscale Characterization Experimental Center (NUANCE), which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the Materials Research Science and Engineering Centers (MRSEC) program (NSF DMR-1121262) at the Materials Research Center; the IIN; the Keck Foundation; and the State of Illinois, through the IIN. This work made use of the J.B. Cohen X-Ray Diffraction Facility supported by MRSEC and SHyNE. This work made use of resources in National Energy Research Scientific Computing Center and Northwestern University's Quest high-performance computing system.
Keywords
- Catalysis
- Hydrogen evolution reaction
- Lithography
- Multimetallic nanocatalyst
ASJC Scopus subject areas
- General