Building Electron/Proton Nanohighways for Full Utilization of Water Splitting Catalysts

Yang, Gaoqiang; Yu, Shule; Kang, Zhenye; Li, Yifan; Bender, Guido; Pivovar, Bryan S.; Green, Johney B.; Cullen, David A.; Zhang, Feng‐Yuan

doi:10.1002/aenm.201903871

Title: Building Electron/Proton Nanohighways for Full Utilization of Water Splitting Catalysts

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Abstract

Low electron/proton conductivities of electrochemical catalysts, especially earth-abundant nonprecious metal catalysts, severely limit their ability to satisfy the triple-phase boundary (TPB) theory, resulting in extremely low catalyst utilization and insufficient efficiency in energy devices. Here, an innovative electrode design strategy is proposed to build electron/proton transport nanohighways to ensure that the whole electrode meets the TPB, therefore significantly promoting enhance oxygen evolution reactions and catalyst utilizations. It is discovered that easily accessible/tunable mesoporous Au nanolayers (AuNLs) not only increase the electrode conductivity by more than 4000 times but also enable the proton transport through straight mesopores within the Debye length. The catalyst layer design with AuNLs and ultralow catalyst loading (≈0.1 mg cm-2) augments reaction sites from 1D to 2D, resulting in an 18-fold improvement in mass activities. Furthermore, using microscale visualization and unique coplanar-electrode electrolyzers, the relationship between the conductivity and the reaction site is revealed, allowing for the discovery of the conductivity-determining and Debye-length-determining regions for water splitting. These findings and strategies provide a novel electrode design (catalyst layer + functional sublayer + ion exchange membrane) with a sufficient electron/proton transport path for high-efficiency electrochemical energy conversion devices.

Authors:

Yang, Gaoqiang ^[1]; Yu, Shule ^[1]; Kang, Zhenye ^[2]; Li, Yifan ^[1]; Bender, Guido ^[3];

^[3];

^[3]; Cullen, David A. ^[3];

^[1]

Univ. of Tennessee, Knoxville, TN (United States). Dept. of Mechanical, Aerospace and Biomedical Engineering; Univ. of Tennessee Space Inst. (UTSI), Tullahoma, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Mechanical, Aerospace and Biomedical Engineering; Univ. of Tennessee Space Inst. (UTSI), Tullahoma, TN (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Dept.
National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Dept.

Publication Date:: 2020-02-28

Research Org.:: National Renewable Energy Lab. (NREL), Golden, CO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Science (SC); USDOE Office of Nuclear Energy (NE)

OSTI Identifier:: 1660075

Alternate Identifier(s):: OSTI ID: 1602091; OSTI ID: 1706248

Report Number(s):: NREL/JA-5900-77326
Journal ID: ISSN 1614-6832; MainId:26272;UUID:2f616546-4058-47a8-9d48-fc184ba1a566;MainAdminID:14054

Grant/Contract Number:: AC36-08GO28308; EE0008426; FE0011585; AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Advanced Energy Materials

Additional Journal Information:: Journal Volume: 10; Journal Issue: 16; Journal ID: ISSN 1614-6832

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; coplanar electrodes; electrochemical catalysts; electron/proton conductivity; nanolayers; oxygen evolution reaction; straight mesopores; water splitting

Citation Formats


                    Yang, Gaoqiang, Yu, Shule, Kang, Zhenye, Li, Yifan, Bender, Guido, Pivovar, Bryan S., Green, Johney B., Cullen, David A., and Zhang, Feng‐Yuan. Building Electron/Proton Nanohighways for Full Utilization of Water Splitting Catalysts.  United States: N. p., 2020. 
Web.  doi:10.1002/aenm.201903871.

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                    Yang, Gaoqiang, Yu, Shule, Kang, Zhenye, Li, Yifan, Bender, Guido, Pivovar, Bryan S., Green, Johney B., Cullen, David A., & Zhang, Feng‐Yuan. Building Electron/Proton Nanohighways for Full Utilization of Water Splitting Catalysts.  United States.  https://doi.org/10.1002/aenm.201903871

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                    Yang, Gaoqiang, Yu, Shule, Kang, Zhenye, Li, Yifan, Bender, Guido, Pivovar, Bryan S., Green, Johney B., Cullen, David A., and Zhang, Feng‐Yuan. Fri .  
"Building Electron/Proton Nanohighways for Full Utilization of Water Splitting Catalysts".  United States.  https://doi.org/10.1002/aenm.201903871.  https://www.osti.gov/servlets/purl/1660075.

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@article{osti_1660075,

  title        = {Building Electron/Proton Nanohighways for Full Utilization of Water Splitting Catalysts},

  author       = {Yang, Gaoqiang and Yu, Shule and Kang, Zhenye and Li, Yifan and Bender, Guido and Pivovar, Bryan S. and Green, Johney B. and Cullen, David A. and Zhang, Feng‐Yuan},

  abstractNote = {Low electron/proton conductivities of electrochemical catalysts, especially earth-abundant nonprecious metal catalysts, severely limit their ability to satisfy the triple-phase boundary (TPB) theory, resulting in extremely low catalyst utilization and insufficient efficiency in energy devices. Here, an innovative electrode design strategy is proposed to build electron/proton transport nanohighways to ensure that the whole electrode meets the TPB, therefore significantly promoting enhance oxygen evolution reactions and catalyst utilizations. It is discovered that easily accessible/tunable mesoporous Au nanolayers (AuNLs) not only increase the electrode conductivity by more than 4000 times but also enable the proton transport through straight mesopores within the Debye length. The catalyst layer design with AuNLs and ultralow catalyst loading (≈0.1 mg cm-2) augments reaction sites from 1D to 2D, resulting in an 18-fold improvement in mass activities. Furthermore, using microscale visualization and unique coplanar-electrode electrolyzers, the relationship between the conductivity and the reaction site is revealed, allowing for the discovery of the conductivity-determining and Debye-length-determining regions for water splitting. These findings and strategies provide a novel electrode design (catalyst layer + functional sublayer + ion exchange membrane) with a sufficient electron/proton transport path for high-efficiency electrochemical energy conversion devices.},

  doi          = {10.1002/aenm.201903871},

  journal      = {Advanced Energy Materials},

  number       = 16,

  volume       = 10,

  place        = {United States},

  year         = {2020},

  month        = {2}

}

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