High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst

Handle URI:
http://hdl.handle.net/10754/622635
Title:
High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst
Authors:
Zheng, Yao; Jiao, Yan; Zhu, Yihan; Li, Lu Hua; Han, Yu ( 0000-0003-1462-1118 ) ; Chen, Ying; Jaroniec, Mietek; Qiao, Shi Zhang
Abstract:
Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division
Citation:
Zheng Y, Jiao Y, Zhu Y, Li LH, Han Y, et al. (2016) High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst. Journal of the American Chemical Society 138: 16174–16181. Available: http://dx.doi.org/10.1021/jacs.6b11291.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
28-Nov-2016
DOI:
10.1021/jacs.6b11291
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
The authors gratefully acknowledge financial support by the Australian Research Council (ARC) through the Discovery Project programs (DP160104866, DP140104062, DP130104459, and DE160101163). NEXAFS measurements were performed on the soft X-ray beamline at Australian Synchrotron. DFT calculations were carried out using the NCI National Facility systems through the National Computational Merit Allocation Scheme.
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/jacs.6b11291
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorZheng, Yaoen
dc.contributor.authorJiao, Yanen
dc.contributor.authorZhu, Yihanen
dc.contributor.authorLi, Lu Huaen
dc.contributor.authorHan, Yuen
dc.contributor.authorChen, Yingen
dc.contributor.authorJaroniec, Mieteken
dc.contributor.authorQiao, Shi Zhangen
dc.date.accessioned2017-01-04T13:04:07Z-
dc.date.available2017-01-04T13:04:07Z-
dc.date.issued2016-11-28en
dc.identifier.citationZheng Y, Jiao Y, Zhu Y, Li LH, Han Y, et al. (2016) High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst. Journal of the American Chemical Society 138: 16174–16181. Available: http://dx.doi.org/10.1021/jacs.6b11291.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.doi10.1021/jacs.6b11291en
dc.identifier.urihttp://hdl.handle.net/10754/622635-
dc.description.abstractHydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.en
dc.description.sponsorshipThe authors gratefully acknowledge financial support by the Australian Research Council (ARC) through the Discovery Project programs (DP160104866, DP140104062, DP130104459, and DE160101163). NEXAFS measurements were performed on the soft X-ray beamline at Australian Synchrotron. DFT calculations were carried out using the NCI National Facility systems through the National Computational Merit Allocation Scheme.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/jacs.6b11291en
dc.rightsThis is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.en
dc.rights.urihttp://pubs.acs.org/page/policy/authorchoice_termsofuse.htmlen
dc.titleHigh Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalysten
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentImaging and Characterization Core Laben
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalJournal of the American Chemical Societyen
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.institutionSchool of Chemical Engineering, University of Adelaide, Adelaide, South Australia, 5005, Australiaen
dc.contributor.institutionInstitute for Frontier Materials, Deakin University, Waurn Ponds, Victoria, 3216, Australiaen
dc.contributor.institutionDepartment of Chemistry and Biochemistry, Kent State University, Kent, Ohio, 44242, United Statesen
kaust.authorZhu, Yihanen
kaust.authorHan, Yuen
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