Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways
Abstract
Despite progress in small scale electrocatalytic production of hydrogen peroxide (H2O2) using a rotating ring-disk electrode, further work is needed to develop a non-toxic, selective, and stable O2-to-H2O2 electrocatalyst for realizing continuous on-site production of neutral hydrogen peroxide. We report ultrasmall and monodisperse colloidal PtP2 nanocrystals that achieve H2O2 production at near zero-overpotential with near unity H2O2 selectivity at 0.27 V vs. RHE. Density functional theory calculations indicate that P promotes hydrogenation of OOH* to H2O2 by weakening the Pt-OOH* bond and suppressing the dissociative OOH* to O* pathway. Atomic layer deposition of Al2O3 prevents NC aggregation and enables application in a polymer electrolyte membrane fuel cell (PEMFC) with a maximum r(H2O2) of 2.26 mmol h-1 cm-2 and a current efficiency of 78.8% even at a high current density of 150 mA cm-2. Catalyst stability enables an accumulated neutral H2O2 concentration in 600 mL of 3.0 wt% (pH = 6.6).
- Authors:
-
[4];
[1];
[1];
[5];
[1]
- Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Chemistry
- Harbin Inst. of Technology, Shenzhen (China). School of Materials Science and Engineering, Shenzhen Engineering Lab of Flexible Transparent Conductive Film
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
- Wake Forest Univ., Winston-Salem, NC (United States). Center for Nanotechnology and Molecular Materials and Dept. of Physics
- Soochow Univ., Suzhou, Jiangsu (China). Inst. of Functional Nano and Soft Materials (FUNSOM)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation of Guangdong Province; Shenzhen Bureau of Science, Technology and Innovation Commission
- OSTI Identifier:
- 1815618
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalyst synthesis; Electrocatalysis; Energy
Citation Formats
Li, Hui, Wen, Peng, Itanze, Dominique S., Hood, Zachary D., Adhikari, Shiba, Lu, Chang, Ma, Xiao, Dun, Chaochao, Jiang, Lin, Carroll, David L., Qiu, Yejun, and Geyer, Scott M. Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways. United States: N. p., 2020.
Web. doi:10.1038/s41467-020-17584-9.
Li, Hui, Wen, Peng, Itanze, Dominique S., Hood, Zachary D., Adhikari, Shiba, Lu, Chang, Ma, Xiao, Dun, Chaochao, Jiang, Lin, Carroll, David L., Qiu, Yejun, & Geyer, Scott M. Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways. United States. https://doi.org/10.1038/s41467-020-17584-9
Li, Hui, Wen, Peng, Itanze, Dominique S., Hood, Zachary D., Adhikari, Shiba, Lu, Chang, Ma, Xiao, Dun, Chaochao, Jiang, Lin, Carroll, David L., Qiu, Yejun, and Geyer, Scott M. Thu .
"Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways". United States. https://doi.org/10.1038/s41467-020-17584-9. https://www.osti.gov/servlets/purl/1815618.
@article{osti_1815618,
title = {Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways},
author = {Li, Hui and Wen, Peng and Itanze, Dominique S. and Hood, Zachary D. and Adhikari, Shiba and Lu, Chang and Ma, Xiao and Dun, Chaochao and Jiang, Lin and Carroll, David L. and Qiu, Yejun and Geyer, Scott M.},
abstractNote = {Despite progress in small scale electrocatalytic production of hydrogen peroxide (H2O2) using a rotating ring-disk electrode, further work is needed to develop a non-toxic, selective, and stable O2-to-H2O2 electrocatalyst for realizing continuous on-site production of neutral hydrogen peroxide. We report ultrasmall and monodisperse colloidal PtP2 nanocrystals that achieve H2O2 production at near zero-overpotential with near unity H2O2 selectivity at 0.27 V vs. RHE. Density functional theory calculations indicate that P promotes hydrogenation of OOH* to H2O2 by weakening the Pt-OOH* bond and suppressing the dissociative OOH* to O* pathway. Atomic layer deposition of Al2O3 prevents NC aggregation and enables application in a polymer electrolyte membrane fuel cell (PEMFC) with a maximum r(H2O2) of 2.26 mmol h-1 cm-2 and a current efficiency of 78.8% even at a high current density of 150 mA cm-2. Catalyst stability enables an accumulated neutral H2O2 concentration in 600 mL of 3.0 wt% (pH = 6.6).},
doi = {10.1038/s41467-020-17584-9},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Thu Aug 06 00:00:00 EDT 2020},
month = {Thu Aug 06 00:00:00 EDT 2020}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
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:
Colloidal Cobalt Phosphide Nanocrystals as Trifunctional Electrocatalysts for Overall Water Splitting Powered by a Zinc-Air Battery
journal, January 2018
- Li, Hui; Li, Qi; Wen, Peng
- Advanced Materials, Vol. 30, Issue 9
Electrocatalytic Production of H 2 O 2 by Selective Oxygen Reduction Using Earth-Abundant Cobalt Pyrite (CoS 2 )
journal, August 2019
- Sheng, Hongyuan; Hermes, Eric D.; Yang, Xiaohua
- ACS Catalysis, Vol. 9, Issue 9
Enabling direct H2O2 production through rational electrocatalyst design
journal, November 2013
- Siahrostami, Samira; Verdaguer-Casadevall, Arnau; Karamad, Mohammadreza
- Nature Materials, Vol. 12, Issue 12
Surface Restructuring of Nickel Sulfide Generates Optimally Coordinated Active Sites for Oxygen Reduction Catalysis
journal, November 2017
- Yan, Bing; Krishnamurthy, Dilip; Hendon, Christopher H.
- Joule, Vol. 1, Issue 3
Surface-Protected Etching of Mesoporous Oxide Shells for the Stabilization of Metal Nanocatalysts
journal, June 2010
- Zhang, Qiao; Lee, Ilkeun; Ge, Jianping
- Advanced Functional Materials, Vol. 20, Issue 14
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
Degradation of Carbon-Supported Pt Bimetallic Nanoparticles by Surface Segregation
journal, November 2009
- Mayrhofer, Karl J. J.; Hartl, Katrin; Juhart, Viktorija
- Journal of the American Chemical Society, Vol. 131, Issue 45
Carbon Dioxide Electroreduction into Syngas Boosted by a Partially Delocalized Charge in Molybdenum Sulfide Selenide Alloy Monolayers
journal, June 2017
- Xu, Jiaqi; Li, Xiaodong; Liu, Wei
- Angewandte Chemie International Edition, Vol. 56, Issue 31
Roles of Mo Surface Dopants in Enhancing the ORR Performance of Octahedral PtNi Nanoparticles
journal, January 2018
- Jia, Qingying; Zhao, Zipeng; Cao, Liang
- Nano Letters, Vol. 18, Issue 2
A review on research progress in the direct synthesis of hydrogen peroxide from hydrogen and oxygen: noble-metal catalytic method, fuel-cell method and plasma method
journal, January 2016
- Yi, Yanhui; Wang, Li; Li, Gang
- Catalysis Science & Technology, Vol. 6, Issue 6
Rh-MnO Interface Sites Formed by Atomic Layer Deposition Promote Syngas Conversion to Higher Oxygenates
journal, August 2017
- Yang, Nuoya; Yoo, Jong Suk; Schumann, Julia
- ACS Catalysis, Vol. 7, Issue 9
Area-Selective Atomic Layer Deposition of Metal Oxides on Noble Metals through Catalytic Oxygen Activation
journal, January 2018
- Singh, Joseph A.; Thissen, Nick F. W.; Kim, Woo-Hee
- Chemistry of Materials, Vol. 30, Issue 3
Drinking Water Purification by Electrosynthesis of Hydrogen Peroxide in a Power-Producing PEM Fuel Cell
journal, September 2013
- Li, Winton; Bonakdarpour, Arman; Gyenge, Előd
- ChemSusChem, Vol. 6, Issue 11
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
Oxygen Electroreduction through a Superoxide Intermediate on Bi-Modified Au Surfaces
journal, April 2005
- Li, Xiao; Gewirth, Andrew A.
- Journal of the American Chemical Society, Vol. 127, Issue 14
Development of a hydrophobic coating for the porous gas diffusion layer in a PEM-based electrochemical hydrogen pump to mitigate anode flooding
journal, March 2019
- Lee, Myoungseok; Huang, Xinyu
- Electrochemistry Communications, Vol. 100
Electrocatalytic performance of fuel cell reactions at low catalyst loading and high mass transport
journal, January 2013
- Zalitis, Christopher M.; Kramer, Denis; Kucernak, Anthony R.
- Physical Chemistry Chemical Physics, Vol. 15, Issue 12
Coking- and Sintering-Resistant Palladium Catalysts Achieved Through Atomic Layer Deposition
journal, March 2012
- Lu, Junling; Fu, Baosong; Kung, Mayfair C.
- Science, Vol. 335, Issue 6073
Recent Advances in the Stabilization of Platinum Electrocatalysts for Fuel-Cell Reactions
journal, October 2013
- Cao, Minna; Wu, Dongshuang; Cao, Rong
- ChemCatChem, Vol. 6, Issue 1
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
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
Catalytic Synthesis of Neutral H 2 O 2 Solutions from O 2 and H 2 by a Fuel Cell Reaction
journal, December 2008
- Yamanaka, Ichiro; Tazawa, Satoshi; Murayama, Toru
- ChemSusChem, Vol. 1, Issue 12
Selective Electrochemical H 2 O 2 Production through Two-Electron Oxygen Electrochemistry
journal, September 2018
- Jiang, Yuanyuan; Ni, Pengjuan; Chen, Chuanxia
- Advanced Energy Materials, Vol. 8, Issue 31
In Vitro Studies Evaluating Leaching of Mercury from Mine Waste Calcine Using Simulated Human Body Fluids
journal, May 2010
- Gray, John E.; Plumlee, Geoffrey S.; Morman, Suzette A.
- Environmental Science & Technology, Vol. 44, Issue 12
Synthesis and Stabilization of Supported Metal Catalysts by Atomic Layer Deposition
journal, March 2013
- Lu, Junling; Elam, Jeffrey W.; Stair, Peter C.
- Accounts of Chemical Research, Vol. 46, Issue 8
H2O2 Determination by the I3- Method and by KMnO4 Titration
journal, September 1994
- Klassen, Normal V.; Marchington, David.; McGowan, Heather C. E.
- Analytical Chemistry, Vol. 66, Issue 18
Understanding Structure–Property Relationships of MoO 3 -Promoted Rh Catalysts for Syngas Conversion to Alcohols
journal, November 2019
- Asundi, Arun S.; Hoffman, Adam S.; Bothra, Pallavi
- Journal of the American Chemical Society, Vol. 141, Issue 50
Origin of synergistic effects in bicomponent cobalt oxide-platinum catalysts for selective hydrogenation reaction
journal, September 2019
- Zhang, Jiankang; Gao, Zhe; Wang, Sen
- Nature Communications, Vol. 10, Issue 1
Electrochemical water splitting by gold: evidence for an oxide decomposition mechanism
journal, January 2013
- Diaz-Morales, Oscar; Calle-Vallejo, Federico; de Munck, Casper
- Chemical Science, Vol. 4, Issue 6
Neutral H2O2 Synthesis by Electrolysis of Water and O2
journal, February 2008
- Yamanaka, Ichiro; Murayama, Toru
- Angewandte Chemie International Edition, Vol. 47, Issue 10
Electrocatalysis on Platinum Nanoparticles: Particle Size Effect on Oxygen Reduction Reaction Activity
journal, September 2011
- Shao, Minhua; Peles, Amra; Shoemaker, Krista
- Nano Letters, Vol. 11, Issue 9
Review Article: Catalysts design and synthesis via selective atomic layer deposition
journal, January 2018
- Cao, Kun; Cai, Jiaming; Liu, Xiao
- Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 36, Issue 1
Earth-Abundant Iron Diboride (FeB 2 ) Nanoparticles as Highly Active Bifunctional Electrocatalysts for Overall Water Splitting
journal, May 2017
- Li, Hui; Wen, Peng; Li, Qi
- Advanced Energy Materials, Vol. 7, Issue 17
Reduction of Oxygen on Dispersed Nanocrystalline CoS 2
journal, November 2012
- Jirkovský, Jakub S.; Björling, Alexander; Ahlberg, Elisabet
- The Journal of Physical Chemistry C, Vol. 116, Issue 46
Surface functionalization on nanoparticles via atomic layer deposition
journal, April 2020
- Cao, Kun; Cai, Jiaming; Shan, Bin
- Science Bulletin, Vol. 65, Issue 8
A mechanistic study of the electrochemical oxygen reduction on the model semiconductor n-Ge(100) by ATR-IR and DFT
journal, January 2013
- Nayak, Simantini; Biedermann, P. Ulrich; Stratmann, Martin
- Phys. Chem. Chem. Phys., Vol. 15, Issue 16
Direct and Continuous Production of Hydrogen Peroxide with 93 % Selectivity Using a Fuel-Cell System
journal, August 2003
- Yamanaka, Ichiro; Onizawa, Takeshi; Takenaka, Sakae
- Angewandte Chemie International Edition, Vol. 42, Issue 31
Atomic Structure of Pt 3 Ni Nanoframe Electrocatalysts by in Situ X-ray Absorption Spectroscopy
journal, December 2015
- Becknell, Nigel; Kang, Yijin; Chen, Chen
- Journal of the American Chemical Society, Vol. 137, Issue 50
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
Adsorbed Intermediates in Oxygen Reduction on Platinum Nanoparticles Observed by In Situ IR Spectroscopy
journal, August 2018
- Nayak, Simantini; McPherson, Ian J.; Vincent, Kylie A.
- Angewandte Chemie International Edition, Vol. 57, Issue 39
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
journal, September 2009
- Greeley, J.; Stephens, I. E. L.; Bondarenko, A. S.
- Nature Chemistry, Vol. 1, Issue 7, p. 552-556
A Review of Phosphide-Based Materials for Electrocatalytic Hydrogen Evolution
journal, October 2015
- Xiao, Peng; Chen, Wei; Wang, Xin
- Advanced Energy Materials, Vol. 5, Issue 24
Interface Tailoring of Heterogeneous Catalysts by Atomic Layer Deposition
journal, September 2018
- Zhang, Bin; Qin, Yong
- ACS Catalysis, Vol. 8, Issue 11