Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination
Abstract
Shifting electrochemical oxygen reduction towards 2e- pathway to hydrogen peroxide (H2O2), instead of the traditional 4e- to water, becomes increasingly important as a green method for H2O2 generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H2O2 catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm-2 H2O2 current, and a high H2O2 selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e-/4e- ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e-, are responsible for the H2O2 pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- National Science Foundation (NSF); Natural Sciences and Engineering Research Council of Canada (NSERC); National Research Council Canada; Canadian Institutes of Health Research; Province of Saskatchewan; Western Economic Diversification Canada; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1619658
- Alternate Identifier(s):
- OSTI ID: 1566880; OSTI ID: 1572051; OSTI ID: 1597946
- Report Number(s):
- BNL-212144-2019-JAAM
Journal ID: ISSN 2041-1723; 3997; PII: 11992
- Grant/Contract Number:
- SC0012704; AC02-05CH11231; AC02-76SF00515; ECS-0335765; SC0008685
- Resource Type:
- Published Article
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Name: Nature Communications Journal Volume: 10 Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Jiang, Kun, Back, Seoin, Akey, Austin J., Xia, Chuan, Hu, Yongfeng, Liang, Wentao, Schaak, Diane, Stavitski, Eli, Nørskov, Jens K., Siahrostami, Samira, and Wang, Haotian. Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination. United Kingdom: N. p., 2019.
Web. doi:10.1038/s41467-019-11992-2.
Jiang, Kun, Back, Seoin, Akey, Austin J., Xia, Chuan, Hu, Yongfeng, Liang, Wentao, Schaak, Diane, Stavitski, Eli, Nørskov, Jens K., Siahrostami, Samira, & Wang, Haotian. Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination. United Kingdom. https://doi.org/10.1038/s41467-019-11992-2
Jiang, Kun, Back, Seoin, Akey, Austin J., Xia, Chuan, Hu, Yongfeng, Liang, Wentao, Schaak, Diane, Stavitski, Eli, Nørskov, Jens K., Siahrostami, Samira, and Wang, Haotian. Thu .
"Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination". United Kingdom. https://doi.org/10.1038/s41467-019-11992-2.
@article{osti_1619658,
title = {Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination},
author = {Jiang, Kun and Back, Seoin and Akey, Austin J. and Xia, Chuan and Hu, Yongfeng and Liang, Wentao and Schaak, Diane and Stavitski, Eli and Nørskov, Jens K. and Siahrostami, Samira and Wang, Haotian},
abstractNote = {Shifting electrochemical oxygen reduction towards 2e- pathway to hydrogen peroxide (H2O2), instead of the traditional 4e- to water, becomes increasingly important as a green method for H2O2 generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H2O2 catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm-2 H2O2 current, and a high H2O2 selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e-/4e- ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e-, are responsible for the H2O2 pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.},
doi = {10.1038/s41467-019-11992-2},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United Kingdom},
year = {Thu Sep 05 00:00:00 EDT 2019},
month = {Thu Sep 05 00:00:00 EDT 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-019-11992-2
https://doi.org/10.1038/s41467-019-11992-2
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 351 works
Citation information provided by
Web of Science
Web of Science
Figures / Tables:
Fig. 1: TEM and XAS characterizations of M-CNT catalysts. High resolution TEM and aberration-corrected HAADF-STEM images of a, e Fe-, b, f Pd-, c, g Co-, d, h Mn-CNT are shown in upper and middle panels, respectively, in which multiple rolled graphene layers can be clearly distinguished with no metalmore »
All figures and tables
(5 total)
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
N-Doped Graphitized Carbon Nanohorns as a Forefront Electrocatalyst in Highly Selective O2 Reduction to H2O2
journal, January 2018
- Iglesias, Daniel; Giuliani, Angela; Melchionna, Michele
- Chem, Vol. 4, Issue 1
Atomic cobalt on nitrogen-doped graphene for hydrogen generation
journal, October 2015
- Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina
- Nature Communications, Vol. 6, Issue 1
Solar‐Driven Production of Hydrogen Peroxide from Water and Dioxygen
journal, February 2018
- Fukuzumi, Shunichi; Lee, Yong‐Min; Nam, Wonwoo
- Chemistry – A European Journal, Vol. 24, Issue 20
Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction
journal, February 2009
- Gong, K.; Du, F.; Xia, Z.
- Science, Vol. 323, Issue 5915, p. 760-764
Catalysis by Supported Single Metal Atoms
journal, November 2016
- Liu, Jingyue
- ACS Catalysis, Vol. 7, Issue 1
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Rapid water disinfection using vertically aligned MoS2 nanofilms and visible light
journal, August 2016
- Liu, Chong; Kong, Desheng; Hsu, Po-Chun
- Nature Nanotechnology, Vol. 11, Issue 12
The Rise of Hydrogen Peroxide as the Main Product by Metal‐Free Catalysis in Oxygen Reductions
journal, August 2018
- Melchionna, Michele; Fornasiero, Paolo; Prato, Maurizio
- Advanced Materials, Vol. 31, Issue 13
Heterogeneous single-atom catalysis
journal, May 2018
- Wang, Aiqin; Li, Jun; Zhang, Tao
- Nature Reviews Chemistry, Vol. 2, Issue 6
High-Activity, Single-Site Mesoporous Pd/Al2O3 Catalysts for Selective Aerobic Oxidation of Allylic Alcohols
journal, November 2007
- Hackett, Simon F. J.; Brydson, Rik M.; Gass, Mhairi H.
- Angewandte Chemie, Vol. 119, Issue 45
Impact of Loading in RRDE Experiments on Fe–N–C Catalysts: Two- or Four-Electron Oxygen Reduction?
journal, January 2008
- Bonakdarpour, Arman; Lefevre, Michel; Yang, Ruizhi
- Electrochemical and Solid-State Letters, Vol. 11, Issue 6, p. B105-B108
Development of a reactor with carbon catalysts for modular-scale, low-cost electrochemical generation of H 2 O 2
journal, January 2017
- Chen, Zhihua; Chen, Shucheng; Siahrostami, Samira
- Reaction Chemistry & Engineering, Vol. 2, Issue 2
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
journal, April 2011
- Wu, G.; More, K. L.; Johnston, C. M.
- Science, Vol. 332, Issue 6028, p. 443-447
Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide
journal, May 2018
- Chen, Shucheng; Chen, Zhihua; Siahrostami, Samira
- Journal of the American Chemical Society, Vol. 140, Issue 25
Electrocatalyst approaches and challenges for automotive fuel cells
journal, June 2012
- Debe, Mark K.
- Nature, Vol. 486, Issue 7401
Hydrogen Peroxide Synthesis via Enhanced Two-Electron Oxygen Reduction Pathway on Carbon-Coated Pt Surface
journal, December 2014
- Choi, Chang Hyuck; Kwon, Han Chang; Yook, Sunwoo
- The Journal of Physical Chemistry C, Vol. 118, Issue 51
Single-atom catalysts for CO 2 electroreduction with significant activity and selectivity improvements
journal, January 2017
- Back, Seoin; Lim, Juhyung; Kim, Na-Young
- Chemical Science, Vol. 8, Issue 2
On an Easy Way To Prepare Metal–Nitrogen Doped Carbon with Exclusive Presence of MeN 4 -type Sites Active for the ORR
journal, January 2016
- Kramm, Ulrike I.; Herrmann-Geppert, Iris; Behrends, Jan
- Journal of the American Chemical Society, Vol. 138, Issue 2
Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation
journal, June 2012
- Wellendorff, Jess; Lundgaard, Keld T.; Møgelhøj, Andreas
- Physical Review B, Vol. 85, Issue 23
Novel synthesis of N-doped porous carbons from collagen for electrocatalytic production of H2O2
journal, September 2012
- Lee, Ying-Hui; Li, Feng; Chang, Kuo-Hsin
- Applied Catalysis B: Environmental, Vol. 126
Activity origin and catalyst design principles for electrocatalytic hydrogen evolution on heteroatom-doped graphene
journal, September 2016
- Jiao, Yan; Zheng, Yao; Davey, Kenneth
- Nature Energy, Vol. 1, Issue 10
Elucidation of the Mechanism of Dioxygen Reduction on Metal-Free Carbon Electrodes
journal, January 2000
- Yang, Hsueh-Hui; McCreery, Richard L.
- Journal of The Electrochemical Society, Vol. 147, Issue 9
Emerging opportunities for nanotechnology to enhance water security
journal, August 2018
- Alvarez, Pedro J. J.; Chan, Candace K.; Elimelech, Menachem
- Nature Nanotechnology, Vol. 13, Issue 8
An object-oriented scripting interface to a legacy electronic structure code
journal, January 2002
- Bahn, S. R.; Jacobsen, K. W.
- Computing in Science & Engineering, Vol. 4, Issue 3
Metal-Free Catalysts for Oxygen Reduction Reaction
journal, May 2015
- Dai, Liming; Xue, Yuhua; Qu, Liangti
- Chemical Reviews, Vol. 115, Issue 11
Lattice-strain control of the activity in dealloyed core–shell fuel cell catalysts
journal, April 2010
- Strasser, Peter; Koh, Shirlaine; Anniyev, Toyli
- Nature Chemistry, Vol. 2, Issue 6
Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst
journal, March 2016
- Choi, Chang Hyuck; Kim, Minho; Kwon, Han Chang
- Nature Communications, Vol. 7, Issue 1
Improved Oxygen Reduction Activity on Pt3Ni(111) via Increased Surface Site Availability
journal, January 2007
- Stamenkovic, V. R.; Fowler, B.; Mun, B. S.
- Science, Vol. 315, Issue 5811, p. 493-497
Recent Advances in Electrocatalysts for Oxygen Reduction Reaction
journal, February 2016
- Shao, Minhua; Chang, Qiaowan; Dodelet, Jean-Pol
- Chemical Reviews, Vol. 116, Issue 6
Long-Chain Terminal Alcohols through Catalytic CO Hydrogenation
journal, May 2013
- Xiang, Yizhi; Chitry, Véronique; Liddicoat, Peter
- Journal of the American Chemical Society, Vol. 135, Issue 19
Enabling direct H2O2 production through rational electrocatalyst design
journal, November 2013
- Siahrostami, Samira; Verdaguer-Casadevall, Arnau; Karamad, Mohammadreza
- Nature Materials, Vol. 12, Issue 12
Defect Chemistry of Nonprecious-Metal Electrocatalysts for Oxygen Reactions
journal, May 2017
- Yan, Dafeng; Li, Yunxiao; Huo, Jia
- Advanced Materials, Vol. 29, Issue 48
Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials
journal, August 2015
- Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa
- Nature Materials, Vol. 14, Issue 9
Direct observation of noble metal nanoparticles transforming to thermally stable single atoms
journal, July 2018
- Wei, Shengjie; Li, Ang; Liu, Jin-Cheng
- Nature Nanotechnology, Vol. 13, Issue 9
Epitaxial Growth of Au-Pt-Ni Nanorods for Direct High Selectivity H 2 O 2 Production
journal, October 2016
- Zheng, Zhaoke; Ng, Yun Hau; Wang, Da-Wei
- Advanced Materials, Vol. 28, Issue 45
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications
journal, July 2018
- Chen, Yuanjun; Ji, Shufang; Chen, Chen
- Joule, Vol. 2, Issue 7
Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction
journal, December 2017
- Kulkarni, Ambarish; Siahrostami, Samira; Patel, Anjli
- Chemical Reviews, Vol. 118, Issue 5
Trends in Adsorption Energies of the Oxygenated Species on Single Platinum Atom Embedded in Carbon Nanotubes
journal, September 2017
- Siahrostami, Samira; Li, Guo-Ling; Nørskov, Jens K.
- Catalysis Letters, Vol. 147, Issue 11
Design of N-Coordinated Dual-Metal Sites: A Stable and Active Pt-Free Catalyst for Acidic Oxygen Reduction Reaction
journal, November 2017
- Wang, Jing; Huang, Zhengqing; Liu, Wei
- Journal of the American Chemical Society, Vol. 139, Issue 48
Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide
journal, November 2017
- Chen, Shucheng; Chen, Zhihua; Siahrostami, Samira
- ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 1
Structural and mechanistic basis for the high activity of Fe–N–C catalysts toward oxygen reduction
journal, January 2016
- Li, Jingkun; Ghoshal, Shraboni; Liang, Wentao
- Energy & Environmental Science, Vol. 9, Issue 7
High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials
journal, January 2018
- Lu, Zhiyi; Chen, Guangxu; Siahrostami, Samira
- Nature Catalysis, Vol. 1, Issue 2
Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in Fe-N-C Catalysts
journal, June 2017
- Choi, Chang Hyuck; Choi, Won Seok; Kasian, Olga
- Angewandte Chemie International Edition, Vol. 56, Issue 30
Co3O4 nanocrystals on graphene as a synergistic catalyst for oxygen reduction reaction
journal, August 2011
- Liang, Yongye; Li, Yanguang; Wang, Hailiang
- Nature Materials, Vol. 10, Issue 10, p. 780-786
A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
journal, December 2015
- Deng, Dehui; Chen, Xiaoqi; Yu, Liang
- Science Advances, Vol. 1, Issue 11
Single Atom Hot-Spots at Au–Pd Nanoalloys for Electrocatalytic H 2 O 2 Production
journal, December 2011
- Jirkovský, Jakub S.; Panas, Itai; Ahlberg, Elisabet
- Journal of the American Chemical Society, Vol. 133, Issue 48
Mesoporous Nitrogen-Doped Carbon for the Electrocatalytic Synthesis of Hydrogen Peroxide
journal, February 2012
- Fellinger, Tim-Patrick; Hasché, Frédéric; Strasser, Peter
- Journal of the American Chemical Society, Vol. 134, Issue 9
Single-Site Heterogeneous Catalysts
journal, October 2005
- Thomas, John Meurig; Raja, Robert; Lewis, Dewi W.
- Angewandte Chemie International Edition, Vol. 44, Issue 40, p. 6456-6482
Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis
journal, December 2017
- Jiang, Kun; Siahrostami, Samira; Akey, Austin J.
- Chem, Vol. 3, Issue 6
Efficient hydrogen peroxide generation using reduced graphene oxide-based oxygen reduction electrocatalysts
journal, March 2018
- Kim, Hyo Won; Ross, Michael B.; Kornienko, Nikolay
- Nature Catalysis, Vol. 1, Issue 4
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction
journal, February 2018
- Yang, Hong Bin; Hung, Sung-Fu; Liu, Song
- Nature Energy, Vol. 3, Issue 2
Nonprecious Metal Catalysts for Oxygen Reduction in Heterogeneous Aqueous Systems
journal, December 2017
- Gewirth, Andrew A.; Varnell, Jason A.; DiAscro, Angela M.
- Chemical Reviews, Vol. 118, Issue 5
Efficient Electrochemical Hydrogen Peroxide Production from Molecular Oxygen on Nitrogen-Doped Mesoporous Carbon Catalysts
journal, February 2018
- Sun, Yanyan; Sinev, Ilya; Ju, Wen
- ACS Catalysis, Vol. 8, Issue 4
Oxygen reduction on a high-surface area Pt/Vulcan carbon catalyst: a thin-film rotating ring-disk electrode study
journal, January 2001
- Paulus, U. A.; Schmidt, T. J.; Gasteiger, H. A.
- Journal of Electroanalytical Chemistry, Vol. 495, Issue 2
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004
- Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
- The Journal of Physical Chemistry B, Vol. 108, Issue 46
Atomic Imaging of Carbon-Supported Pt, Pt/Co, and Ir@Pt Nanocatalysts by Atom-Probe Tomography
journal, December 2013
- Li, Tong; Bagot, Paul A. J.; Christian, Elvis
- ACS Catalysis, Vol. 4, Issue 2
Hydrogen production from formic acid decomposition at room temperature using a Ag–Pd core–shell nanocatalyst
journal, April 2011
- Tedsree, Karaked; Li, Tong; Jones, Simon
- Nature Nanotechnology, Vol. 6, Issue 5
Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells
journal, April 2009
- Lefèvre, Michel; Proietti, Eric; Jaouen, Frédéric
- Science, Vol. 324, Issue 5923, p. 71-74
Electrochemical water splitting by layered and 3D cross-linked manganese oxides: correlating structural motifs and catalytic activity
journal, January 2013
- Bergmann, Arno; Zaharieva, Ivelina; Dau, Holger
- Energy & Environmental Science, Vol. 6, Issue 9
Trends in the Electrochemical Synthesis of H 2 O 2 : Enhancing Activity and Selectivity by Electrocatalytic Site Engineering
journal, February 2014
- Verdaguer-Casadevall, Arnau; Deiana, Davide; Karamad, Mohammadreza
- Nano Letters, Vol. 14, Issue 3
Isolated Ni single atoms in graphene nanosheets for high-performance CO 2 reduction
journal, January 2018
- Jiang, Kun; Siahrostami, Samira; Zheng, Tingting
- Energy & Environmental Science, Vol. 11, Issue 4
Toward the Decentralized Electrochemical Production of H 2 O 2 : A Focus on the Catalysis
journal, March 2018
- Yang, Sungeun; Verdaguer-Casadevall, Arnau; Arnarson, Logi
- ACS Catalysis, Vol. 8, Issue 5
Hydrogen Peroxide: A Key Chemical for Today's Sustainable Development
journal, November 2016
- Ciriminna, Rosaria; Albanese, Lorenzo; Meneguzzo, Francesco
- ChemSusChem, Vol. 9, Issue 24
Experimental Observation of Redox-Induced Fe–N Switching Behavior as a Determinant Role for Oxygen Reduction Activity
journal, October 2015
- Jia, Qingying; Ramaswamy, Nagappan; Hafiz, Hasnain
- ACS Nano, Vol. 9, Issue 12
Conducting Nanosponge Electroporation for Affordable and High-Efficiency Disinfection of Bacteria and Viruses in Water
journal, August 2013
- Liu, Chong; Xie, Xing; Zhao, Wenting
- Nano Letters, Vol. 13, Issue 9
Nanoscale tomography reveals the deactivation of automotive copper-exchanged zeolite catalysts
journal, November 2017
- Schmidt, Joel E.; Oord, Ramon; Guo, Wei
- Nature Communications, Vol. 8, Issue 1
Figures / Tables found in this record:
Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.