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Title: Iridium-Based Cubic Nanocages with 1.1-nm-Thick Walls: A Highly Efficient and Durable Electrocatalyst for Water Oxidation in an Acidic Medium

Abstract

We report a highly active and durable water oxidation electrocatalyst based on cubic nanocages with a composition of Ir44Pd10, together with well-defined {100} facets and porous walls of roughly 1.1 nm in thickness. Such nanocages substantially outperform all the water oxidation electrocatalysts reported in literature, with an overpotential of only 226 mV for reaching 10 mA·cm-2geo at a loading of Ir as low as 12.5 μgIr cm-2 on the electrode in acidic media. When benchmarked against a commercial Ir/C electrocatalyst at 250 mV of overpotential, such a nanocage-based catalyst not only shows enhancements (18.1- and 26.2-fold, respectively) in terms of mass (1.99 A·mg-1Ir) and specific (3.93 mA·cm-2Ir) activities, but also greatly enhanced durability. The enhancements can be attributed to a combination of multiple merits, including a high utilization efficiency of Ir atoms and an open structure beneficial to the electrochemical oxidation of Ir to the active form of IrOx.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5];  [6]; ORCiD logo [3]
  1. Georgia Inst. of Technology, Atlanta, GA (United States); Nanjing Tech Univ. (China)
  2. Georgia Inst. of Technology, Atlanta, GA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Georgia Inst. of Technology, Atlanta, GA (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Univ. of Wisconsin, Madison, WI (United States)
  6. Nanjing Tech Univ. (China)
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1571237
Grant/Contract Number:  
FG02-05ER15731
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 58; Journal Issue: 22; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; iridium; nanocages; ultrathin walls; water oxidation; acidic media

Citation Formats

Zhu, Jiawei, Chen, Zitao, Xie, Minghao, Lyu, Zhiheng, Chi, Miaofang, Mavrikakis, Manos, Jin, Wanqin, and Xia, Younan. Iridium-Based Cubic Nanocages with 1.1-nm-Thick Walls: A Highly Efficient and Durable Electrocatalyst for Water Oxidation in an Acidic Medium. United States: N. p., 2019. Web. doi:10.1002/anie.201901732.
Zhu, Jiawei, Chen, Zitao, Xie, Minghao, Lyu, Zhiheng, Chi, Miaofang, Mavrikakis, Manos, Jin, Wanqin, & Xia, Younan. Iridium-Based Cubic Nanocages with 1.1-nm-Thick Walls: A Highly Efficient and Durable Electrocatalyst for Water Oxidation in an Acidic Medium. United States. https://doi.org/10.1002/anie.201901732
Zhu, Jiawei, Chen, Zitao, Xie, Minghao, Lyu, Zhiheng, Chi, Miaofang, Mavrikakis, Manos, Jin, Wanqin, and Xia, Younan. Fri . "Iridium-Based Cubic Nanocages with 1.1-nm-Thick Walls: A Highly Efficient and Durable Electrocatalyst for Water Oxidation in an Acidic Medium". United States. https://doi.org/10.1002/anie.201901732. https://www.osti.gov/servlets/purl/1571237.
@article{osti_1571237,
title = {Iridium-Based Cubic Nanocages with 1.1-nm-Thick Walls: A Highly Efficient and Durable Electrocatalyst for Water Oxidation in an Acidic Medium},
author = {Zhu, Jiawei and Chen, Zitao and Xie, Minghao and Lyu, Zhiheng and Chi, Miaofang and Mavrikakis, Manos and Jin, Wanqin and Xia, Younan},
abstractNote = {We report a highly active and durable water oxidation electrocatalyst based on cubic nanocages with a composition of Ir44Pd10, together with well-defined {100} facets and porous walls of roughly 1.1 nm in thickness. Such nanocages substantially outperform all the water oxidation electrocatalysts reported in literature, with an overpotential of only 226 mV for reaching 10 mA·cm-2geo at a loading of Ir as low as 12.5 μgIr cm-2 on the electrode in acidic media. When benchmarked against a commercial Ir/C electrocatalyst at 250 mV of overpotential, such a nanocage-based catalyst not only shows enhancements (18.1- and 26.2-fold, respectively) in terms of mass (1.99 A·mg-1Ir) and specific (3.93 mA·cm-2Ir) activities, but also greatly enhanced durability. The enhancements can be attributed to a combination of multiple merits, including a high utilization efficiency of Ir atoms and an open structure beneficial to the electrochemical oxidation of Ir to the active form of IrOx.},
doi = {10.1002/anie.201901732},
journal = {Angewandte Chemie (International Edition)},
number = 22,
volume = 58,
place = {United States},
year = {Fri Mar 08 00:00:00 EST 2019},
month = {Fri Mar 08 00:00:00 EST 2019}
}

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Works referenced in this record:

Combining theory and experiment in electrocatalysis: Insights into materials design
journal, January 2017


Energy and fuels from electrochemical interfaces
journal, December 2016

  • Stamenkovic, Vojislav R.; Strmcnik, Dusan; Lopes, Pietro P.
  • Nature Materials, Vol. 16, Issue 1
  • DOI: 10.1038/nmat4738

A review on unitized regenerative fuel cell technologies, part-A: Unitized regenerative proton exchange membrane fuel cells
journal, November 2016


Li–O2 and Li–S batteries with high energy storage
journal, January 2012

  • Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J.
  • Nature Materials, Vol. 11, Issue 1, p. 19-29
  • DOI: 10.1038/nmat3191

Electrocatalytic Oxygen Evolution Reaction in Acidic Environments - Reaction Mechanisms and Catalysts
journal, October 2016

  • Reier, Tobias; Nong, Hong Nhan; Teschner, Detre
  • Advanced Energy Materials, Vol. 7, Issue 1
  • DOI: 10.1002/aenm.201601275

Electrocatalysis for the oxygen evolution reaction: recent development and future perspectives
journal, January 2017

  • Suen, Nian-Tzu; Hung, Sung-Fu; Quan, Quan
  • Chemical Society Reviews, Vol. 46, Issue 2
  • DOI: 10.1039/C6CS00328A

Electrocatalytic Oxygen Evolution Reaction (OER) on Ru, Ir, and Pt Catalysts: A Comparative Study of Nanoparticles and Bulk Materials
journal, July 2012

  • Reier, Tobias; Oezaslan, Mehtap; Strasser, Peter
  • ACS Catalysis, Vol. 2, Issue 8
  • DOI: 10.1021/cs3003098

Oxygen electrocatalysts for water electrolyzers and reversible fuel cells: status and perspective
journal, January 2012

  • Park, Sehkyu; Shao, Yuyan; Liu, Jun
  • Energy & Environmental Science, Vol. 5, Issue 11
  • DOI: 10.1039/c2ee22554a

Activity–Stability Trends for the Oxygen Evolution Reaction on Monometallic Oxides in Acidic Environments
journal, July 2014

  • Danilovic, Nemanja; Subbaraman, Ramachandran; Chang, Kee-Chul
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 14
  • DOI: 10.1021/jz501061n

The Common Intermediates of Oxygen Evolution and Dissolution Reactions during Water Electrolysis on Iridium
journal, February 2018

  • Kasian, Olga; Grote, Jan-Philipp; Geiger, Simon
  • Angewandte Chemie International Edition, Vol. 57, Issue 9
  • DOI: 10.1002/anie.201709652

Die gemeinsamen Zwischenprodukte von Sauerstoffentwicklung und Auflösung während der Wasserelektrolyse an Iridium
journal, February 2018

  • Kasian, Olga; Grote, Jan-Philipp; Geiger, Simon
  • Angewandte Chemie, Vol. 130, Issue 9
  • DOI: 10.1002/ange.201709652

Oxide-supported Ir nanodendrites with high activity and durability for the oxygen evolution reaction in acid PEM water electrolyzers
journal, January 2015

  • Oh, Hyung-Suk; Nong, Hong Nhan; Reier, Tobias
  • Chemical Science, Vol. 6, Issue 6
  • DOI: 10.1039/C5SC00518C

Synthesis and Activities of Rutile IrO 2 and RuO 2 Nanoparticles for Oxygen Evolution in Acid and Alkaline Solutions
journal, January 2012

  • Lee, Youngmin; Suntivich, Jin; May, Kevin J.
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 3
  • DOI: 10.1021/jz2016507

Nanosized IrO x -Ir Catalyst with Relevant Activity for Anodes of Proton Exchange Membrane Electrolysis Produced by a Cost-Effective Procedure
journal, November 2015

  • Lettenmeier, Philipp; Wang, Li; Golla-Schindler, Ute
  • Angewandte Chemie International Edition, Vol. 55, Issue 2
  • DOI: 10.1002/anie.201507626

Nanosized IrO x -Ir Catalyst with Relevant Activity for Anodes of Proton Exchange Membrane Electrolysis Produced by a Cost-Effective Procedure
journal, November 2015

  • Lettenmeier, Philipp; Wang, Li; Golla-Schindler, Ute
  • Angewandte Chemie, Vol. 128, Issue 2
  • DOI: 10.1002/ange.201507626

IrO 2 -TiO 2 : A High-Surface-Area, Active, and Stable Electrocatalyst for the Oxygen Evolution Reaction
journal, February 2017


Colloidal synthesis of monodisperse trimetallic IrNiFe nanoparticles as highly active bifunctional electrocatalysts for acidic overall water splitting
journal, January 2017

  • Fu, Luhong; Cheng, Gongzhen; Luo, Wei
  • Journal of Materials Chemistry A, Vol. 5, Issue 47
  • DOI: 10.1039/C7TA08982A

General Formation of Monodisperse IrM (M = Ni, Co, Fe) Bimetallic Nanoclusters as Bifunctional Electrocatalysts for Acidic Overall Water Splitting
journal, May 2017

  • Pi, Yecan; Shao, Qi; Wang, Pengtang
  • Advanced Functional Materials, Vol. 27, Issue 27
  • DOI: 10.1002/adfm.201700886

Synthesis and Demonstration of Subnanometric Iridium Oxide as Highly Efficient and Robust Water Oxidation Catalyst
journal, August 2017


Toward Cost-Effective and Sustainable Use of Precious Metals in Heterogeneous Catalysts
journal, March 2017


Synthesis of Ni–Ir Nanocages with Improved Electrocatalytic Performance for the Oxygen Evolution Reaction
journal, October 2017


Synthesis of Cu–Ir nanocages with enhanced electrocatalytic activity for the oxygen evolution reaction
journal, January 2015

  • Wang, Chao; Sui, Yongming; Xiao, Guanjun
  • Journal of Materials Chemistry A, Vol. 3, Issue 39
  • DOI: 10.1039/C5TA05384F

Iridium-Based Multimetallic Porous Hollow Nanocrystals for Efficient Overall-Water-Splitting Catalysis
journal, October 2017


Cobalt Assisted Synthesis of IrCu Hollow Octahedral Nanocages as Highly Active Electrocatalysts toward Oxygen Evolution Reaction
journal, January 2017

  • Kwon, Taehyun; Hwang, Hyeyoun; Sa, Young Jin
  • Advanced Functional Materials, Vol. 27, Issue 7, Article No. 1604688
  • DOI: 10.1002/adfm.201604688

Facile Synthesis of Iridium Nanocrystals with Well-Controlled Facets Using Seed-Mediated Growth
journal, July 2014

  • Xia, Xiaohu; Figueroa-Cosme, Legna; Tao, Jing
  • Journal of the American Chemical Society, Vol. 136, Issue 31
  • DOI: 10.1021/ja505716v

Shape‐Controlled Synthesis of Colloidal Metal Nanocrystals by Replicating the Surface Atomic Structure on the Seed
journal, April 2018


Seed-Mediated Growth of Colloidal Metal Nanocrystals
journal, December 2016

  • Xia, Younan; Gilroy, Kyle D.; Peng, Hsin-Chieh
  • Angewandte Chemie International Edition, Vol. 56, Issue 1
  • DOI: 10.1002/anie.201604731

Keimvermitteltes Wachstum kolloidaler Metallnanokristalle
journal, December 2016

  • Xia, Younan; Gilroy, Kyle D.; Peng, Hsin-Chieh
  • Angewandte Chemie, Vol. 129, Issue 1
  • DOI: 10.1002/ange.201604731

Platinum-based nanocages with subnanometer-thick walls and well-defined, controllable facets
journal, July 2015


Synthesis and Characterization of Ru Cubic Nanocages with a Face-Centered Cubic Structure by Templating with Pd Nanocubes
journal, August 2016


Facile synthesis of Pd–Ir bimetallic octapods and nanocages through galvanic replacement and co-reduction, and their use for hydrazine decomposition
journal, January 2013

  • Liu, Maochang; Zheng, Yiqun; Xie, Shuifen
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 28
  • DOI: 10.1039/c3cp51950c

High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media
journal, August 2017

  • Kim, Jaemin; Shih, Pei-Chieh; Tsao, Kai-Chieh
  • Journal of the American Chemical Society, Vol. 139, Issue 34
  • DOI: 10.1021/jacs.7b06808

Polyoxometalate electrocatalysts based on earth-abundant metals for efficient water oxidation in acidic media
journal, October 2017

  • Blasco-Ahicart, Marta; Soriano-López, Joaquín; Carbó, Jorge J.
  • Nature Chemistry, Vol. 10, Issue 1
  • DOI: 10.1038/nchem.2874

Iridium-based double perovskites for efficient water oxidation in acid media
journal, August 2016

  • Diaz-Morales, Oscar; Raaijman, Stefan; Kortlever, Ruud
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12363

Ultrathin Laminar Ir Superstructure as Highly Efficient Oxygen Evolution Electrocatalyst in Broad pH Range
journal, June 2016


A highly active and stable IrO x /SrIrO 3 catalyst for the oxygen evolution reaction
journal, September 2016


Atomic-scale insights into surface species of electrocatalysts in three dimensions
journal, March 2018


Oxide-supported Ir nanodendrites with high activity and durability for the oxygen evolution reaction in acid PEM water electrolyzers
text, January 2015


Works referencing / citing this record:

Fine‐Tuning Intrinsic Strain in Penta‐Twinned Pt–Cu–Mn Nanoframes Boosts Oxygen Reduction Catalysis
journal, January 2020

  • Qin, Yuchen; Zhang, Wenlong; Guo, Kai
  • Advanced Functional Materials, Vol. 30, Issue 11
  • DOI: 10.1002/adfm.201910107

Recent Advances on Water‐Splitting Electrocatalysis Mediated by Noble‐Metal‐Based Nanostructured Materials
journal, November 2019

  • Li, Yingjie; Sun, Yingjun; Qin, Yingnan
  • Advanced Energy Materials, Vol. 10, Issue 11
  • DOI: 10.1002/aenm.201903120

HZIF-based hybrids for electrochemical energy applications
journal, January 2019


Theoretical insights into nonprecious oxygen-evolution active sites in Ti–Ir-Based perovskite solid solution electrocatalysts
journal, January 2020

  • Shi, Lei; Chen, Hui; Liang, Xiao
  • Journal of Materials Chemistry A, Vol. 8, Issue 1
  • DOI: 10.1039/c9ta10059h

Laser Synthesis of Iridium Nanospheres for Overall Water Splitting
journal, September 2019

  • Wang, Hai-Bin; Wang, Jia-Qi; Mintcheva, Neli
  • Materials, Vol. 12, Issue 18
  • DOI: 10.3390/ma12183028

Laser Synthesis of Iridium Nanospheres for Overall Water Splitting
journal, September 2019

  • Wang, Hai-Bin; Wang, Jia-Qi; Mintcheva, Neli
  • Materials, Vol. 12, Issue 18
  • DOI: 10.3390/ma12183028