Electrochemically active surface area controls HER activity for FexNi100–x films in alkaline electrolyte

Bakovic, Sergio I. Perez; Acharya, Prashant; Watkins, Morgan; Thornton, Hannah; Hou, Shixuan; Greenlee, Lauren F.

doi:10.1016/j.jcat.2020.12.037

Electrochemically active surface area controls HER activity for Fe_xNi_100–x films in alkaline electrolyte

Journal Article · Thu Jan 07 23:00:00 EST 2021 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2020.12.037· OSTI ID:1755862

Bakovic, Sergio I. Perez ^[1]; Acharya, Prashant ^[2]; Watkins, Morgan ^[2]; Thornton, Hannah ^[2]; ^[2]; ^[2]

Univ. of Arkansas, Fayetteville, AR (United States); University of Arkansas
Univ. of Arkansas, Fayetteville, AR (United States)

We report the synthesis and electrocatalytic activity of Fe_xNi_100-x electrochemically deposited films were investigated. Films were evaluated for the hydrogen evolution reaction (HER) in alkaline media with respect to composition and electrochemically active surface area (ECSA). Results demonstrate that films of higher or equal Fe content had an ECSA tenfold greater than films with higher Ni. When normalized by geometric surface area, Fe₅₀Ni₅₀ films required the lowest overpotential of -390 mV to reach a current density of -10 mA cm^-2. However, when normalized by the ECSA, intrinsic HER activity increases as Ni content increases. Tafel slope, ECSA, microscopy, and impedance spectroscopy analyses allow a decoupled analysis of surface area versus activity effects on overall measured HER activity. Furthermore, these analyses collectively demonstrate that the increase in electrocatalytic activity is attributed to the increase in ECSA and not to an enhancement in the intrinsic activity by Fe and Ni component interactions.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Arkansas, Fayetteville, AR (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0016529

OSTI ID:: 1755862

Alternate ID(s):: OSTI ID: 1775874

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 394; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (48)

Conceptual design of ammonia-based energy storage system: System design and time-invariant performance Wang, Ganzhou; Mitsos, Alexander; Marquardt, Wolfgang AIChE Journal, Vol. 63, Issue 5 https://doi.org/10.1002/aic.15660	journal	March 2017
X-ray photoelectron spectroscopic chemical state quantification of mixed nickel metal, oxide and hydroxide systems Biesinger, Mark C.; Payne, Brad P.; Lau, Leo W. M. Surface and Interface Analysis, Vol. 41, Issue 4 https://doi.org/10.1002/sia.3026	journal	April 2009
Verwendung von Schwingquarzen zur W�gung d�nner Schichten und zur Mikrow�gung Sauerbrey, G�nter Zeitschrift f�r Physik, Vol. 155, Issue 2 https://doi.org/10.1007/BF01337937	journal	April 1959
Analytical utility of valence band X-ray photoelectron spectroscopy of iron and its oxides, with spectral interpretation by cluster and band structure calculations Temesghen, W.; Sherwood, P. Analytical and Bioanalytical Chemistry, Vol. 373, Issue 7 https://doi.org/10.1007/s00216-002-1362-3	journal	July 2002
A mini review on nickel-based electrocatalysts for alkaline hydrogen evolution reaction Gong, Ming; Wang, Di-Yan; Chen, Chia-Chun Nano Research, Vol. 9, Issue 1 https://doi.org/10.1007/s12274-015-0965-x	journal	December 2015
Electrochemical Growth of Surface Oxides on Nickel. Part 3: Formation of β-NiOOH in Relation to the Polarization Potential, Polarization Time, and Temperature Alsabet, Mohammad; Grdeń, Michal; Jerkiewicz, Gregory Electrocatalysis, Vol. 6, Issue 1 https://doi.org/10.1007/s12678-014-0214-1	journal	July 2014
Acid promoted Ni/NiO monolithic electrode for overall water splitting in alkaline medium Li, Caicai; Hou, Junxian; Wu, Zexing Science China Materials, Vol. 60, Issue 10 https://doi.org/10.1007/s40843-017-9089-y	journal	September 2017
The potentiodynamic behaviour of iron in alkaline solutions Schrebler Guzmán, R. S.; Vilche, J. R.; Arvía, A. J. Electrochimica Acta, Vol. 24, Issue 4 https://doi.org/10.1016/0013-4686(79)87026-7	journal	April 1979
Bipolar performance of the electroplated iron–nickel deposits for water electrolysis Hu, Chi-Chang; Wu, Yau-Ruen Materials Chemistry and Physics, Vol. 82, Issue 3 https://doi.org/10.1016/S0254-0584(03)00316-X	journal	December 2003
Recent developments in electrode materials for water electrolysis Suffredini, H. International Journal of Hydrogen Energy, Vol. 25, Issue 5 https://doi.org/10.1016/S0360-3199(99)00049-X	journal	May 2000
Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Cr, Mn, Fe, Co and Ni Biesinger, Mark C.; Payne, Brad P.; Grosvenor, Andrew P. Applied Surface Science, Vol. 257, Issue 7, p. 2717-2730 https://doi.org/10.1016/j.apsusc.2010.10.051	journal	January 2011
Fabrication and evaluation of nickel cobalt alloy electrocatalysts for alkaline water splitting Hong, Sung Hoon; Ahn, Sang Hyun; Choi, Insoo Applied Surface Science, Vol. 307 https://doi.org/10.1016/j.apsusc.2014.03.197	journal	July 2014
Synergistic effect: Hierarchical Ni3S2@Co(OH)2 heterostructure as efficient bifunctional electrocatalyst for overall water splitting Wang, Shuaipeng; Xu, Li; Lu, Weixin Applied Surface Science, Vol. 457 https://doi.org/10.1016/j.apsusc.2018.06.253	journal	November 2018
An overview of hydrogen production technologies Holladay, J. D.; Hu, J.; King, D. L. Catalysis Today, Vol. 139, Issue 4 https://doi.org/10.1016/j.cattod.2008.08.039	journal	January 2009
Electroactivity of Ni–Fe cathodes in alkaline water electrolysis and effect of corrosion Flis-Kabulska, I.; Flis, J. Corrosion Science, Vol. 112 https://doi.org/10.1016/j.corsci.2016.07.017	journal	November 2016
Electrochemical and in situ magnetic study of iron/iron oxide films oxidized and reduced in KOH solution for magneto-ionic switching Duschek, K.; Uhlemann, M.; Schlörb, H. Electrochemistry Communications, Vol. 72 https://doi.org/10.1016/j.elecom.2016.09.018	journal	November 2016
The role of iron in the prevention of nickel electrode deactivation in alkaline electrolysis Mauer, Anne E.; Kirk, Donald W.; Thorpe, Steven J. Electrochimica Acta, Vol. 52, Issue 11 https://doi.org/10.1016/j.electacta.2006.10.037	journal	March 2007
Electrochemical deposition and characterization of NiFe coatings as electrocatalytic materials for alkaline water electrolysis Solmaz, Ramazan; Kardaş, Gülfeza Electrochimica Acta, Vol. 54, Issue 14 https://doi.org/10.1016/j.electacta.2009.01.064	journal	May 2009
Electrocatalytic activation of Ni electrode for hydrogen production by electrodeposition of Co and V species Marcetakaninski, M.; Nikolic, V.; Tasic, G. International Journal of Hydrogen Energy, Vol. 34, Issue 2 https://doi.org/10.1016/j.ijhydene.2008.09.024	journal	January 2009
Assessment of the roughness factor effect and the intrinsic catalytic activity for hydrogen evolution reaction on Ni-based electrodeposits Herraiz-Cardona, I.; Ortega, E.; Antón, J. García International Journal of Hydrogen Energy, Vol. 36, Issue 16 https://doi.org/10.1016/j.ijhydene.2011.05.047	journal	August 2011
3D hierarchical network NiCo 2 S 4 nanoflakes grown on Ni foam as efficient bifunctional electrocatalysts for both hydrogen and oxygen evolution reaction in alkaline solution Yin, Xucai; Sun, Gang; Wang, Lixin International Journal of Hydrogen Energy, Vol. 42, Issue 40 https://doi.org/10.1016/j.ijhydene.2017.08.129	journal	October 2017
The activity of nanocrystalline Fe-based alloys as electrode materials for the hydrogen evolution reaction Müller, Christian Immanuel; Sellschopp, Kai; Tegel, Marcus Journal of Power Sources, Vol. 304 https://doi.org/10.1016/j.jpowsour.2015.11.008	journal	February 2016
Characterization of Ni, NiMo, NiW and NiFe electroactive coatings as electrocatalysts for hydrogen evolution in an acidic medium Navarro-Flores, Elisa; Chong, Zhiwen; Omanovic, Sasha Journal of Molecular Catalysis A: Chemical, Vol. 226, Issue 2 https://doi.org/10.1016/j.molcata.2004.10.029	journal	February 2005
Self-assembled ultrathin NiCo2S4 nanoflakes grown on Ni foam as high-performance flexible electrodes for hydrogen evolution reaction in alkaline solution Ma, Lianbo; Hu, Yi; Chen, Renpeng Nano Energy, Vol. 24 https://doi.org/10.1016/j.nanoen.2016.04.024	journal	June 2016
Recent progress in alkaline water electrolysis for hydrogen production and applications Zeng, Kai; Zhang, Dongke Progress in Energy and Combustion Science, Vol. 36, Issue 3 https://doi.org/10.1016/j.pecs.2009.11.002	journal	June 2010
Current status of water electrolysis for energy storage, grid balancing and sector coupling via power-to-gas and power-to-liquids: A review Buttler, Alexander; Spliethoff, Hartmut Renewable and Sustainable Energy Reviews, Vol. 82 https://doi.org/10.1016/j.rser.2017.09.003	journal	February 2018
New interpretations of XPS spectra of nickel metal and oxides Grosvenor, Andrew P.; Biesinger, Mark C.; Smart, Roger St. C. Surface Science, Vol. 600, Issue 9 https://doi.org/10.1016/j.susc.2006.01.041	journal	May 2006
Three-Dimensional Structures of MoS ₂ @Ni Core/Shell Nanosheets Array toward Synergetic Electrocatalytic Water Splitting Xing, Zhicai; Yang, Xiurong; Asiri, Abdullah M. ACS Applied Materials & Interfaces, Vol. 8, Issue 23 https://doi.org/10.1021/acsami.6b02331	journal	May 2016
Facile Synthesis of Nickel–Iron/Nanocarbon Hybrids as Advanced Electrocatalysts for Efficient Water Splitting Zhang, Xing; Xu, Haomin; Li, Xiaoxiao ACS Catalysis, Vol. 6, Issue 2 https://doi.org/10.1021/acscatal.5b02291	journal	December 2015
MoS ₂ –Ni ₃ S ₂ Heteronanorods as Efficient and Stable Bifunctional Electrocatalysts for Overall Water Splitting Yang, Yaqing; Zhang, Kai; Lin, Huanlei ACS Catalysis, Vol. 7, Issue 4 https://doi.org/10.1021/acscatal.6b03192	journal	February 2017
Electrochemical Hydrogen Evolution at Ordered Mo ₇ Ni ₇ Csernica, Peter M.; McKone, James R.; Mulzer, Catherine R. ACS Catalysis, Vol. 7, Issue 5 https://doi.org/10.1021/acscatal.7b00344	journal	April 2017
Ambient Electrochemical Ammonia Synthesis with High Selectivity on Fe/Fe Oxide Catalyst Hu, Lin; Khaniya, Asim; Wang, Jun ACS Catalysis, Vol. 8, Issue 10 https://doi.org/10.1021/acscatal.8b02585	journal	August 2018
Self-Supported FeNi-P Nanosheets with Thin Amorphous Layers for Efficient Electrocatalytic Water Splitting Yan, Qing; Wei, Tong; Wu, Jun ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 8 https://doi.org/10.1021/acssuschemeng.7b04743	journal	June 2018
An Investigation of Thin-Film Ni–Fe Oxide Catalysts for the Electrochemical Evolution of Oxygen Louie, Mary W.; Bell, Alexis T. Journal of the American Chemical Society, Vol. 135, Issue 33 https://doi.org/10.1021/ja405351s	journal	August 2013
Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction McCrory, Charles C. L.; Jung, Suho; Peters, Jonas C. Journal of the American Chemical Society, Vol. 135, Issue 45 https://doi.org/10.1021/ja407115p	journal	October 2013
Benchmarking Hydrogen Evolving Reaction and Oxygen Evolving Reaction Electrocatalysts for Solar Water Splitting Devices McCrory, Charles C. L.; Jung, Suho; Ferrer, Ivonne M. Journal of the American Chemical Society, Vol. 137, Issue 13 https://doi.org/10.1021/ja510442p	journal	March 2015
Studies of the Hydrogen Evolution Reaction on Raney Nickel–Molybdenum Electrodes Birry, L.; Lasia, A. Journal of Applied Electrochemistry, Vol. 34, Issue 7 https://doi.org/10.1023/B:JACH.0000031161.26544.6a	journal	July 2004
Powering the planet with solar fuel Gray, Harry B. Nature Chemistry, Vol. 1, Issue 1 https://doi.org/10.1038/nchem.141	journal	April 2009
Insight on Tafel slopes from a microkinetic analysis of aqueous electrocatalysis for energy conversion Shinagawa, Tatsuya; Garcia-Esparza, Angel T.; Takanabe, Kazuhiro Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep13801	journal	September 2015
Nanostructured catalysts for electrochemical water splitting: current state and prospects Li, Xiumin; Hao, Xiaogang; Abudula, Abuliti Journal of Materials Chemistry A, Vol. 4, Issue 31 https://doi.org/10.1039/C6TA02334G	journal	January 2016
Inexpensive electrochemical synthesis of nickel iron sulphides on nickel foam: super active and ultra-durable electrocatalysts for alkaline electrolyte membrane water electrolysis Ganesan, Pandian; Sivanantham, Arumugam; Shanmugam, Sangaraju Journal of Materials Chemistry A, Vol. 4, Issue 42 https://doi.org/10.1039/C6TA04499A	journal	January 2016
Approaches for measuring the surface areas of metal oxide electrocatalysts for determining their intrinsic electrocatalytic activity Wei, Chao; Sun, Shengnan; Mandler, Daniel Chemical Society Reviews, Vol. 48, Issue 9 https://doi.org/10.1039/C8CS00848E	journal	January 2019
Engineering FeNi alloy nanoparticles via synergistic ultralow Pt doping and nanocarbon capsulation for efficient hydrogen evolution Fan, Aixin; Qin, Congli; Zhang, Xin Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/C9TA08594G	journal	January 2019
The role of the Auger parameter in XPS studies of nickel metal, halides and oxides Biesinger, Mark C.; Lau, Leo W. M.; Gerson, Andrea R. Physical Chemistry Chemical Physics, Vol. 14, Issue 7, p. 2434-2442 https://doi.org/10.1039/c2cp22419d	journal	January 2012
Electrodeposited Ni dendrites with high activity and durability for hydrogen evolution reaction in alkaline water electrolysis Ahn, Sang Hyun; Hwang, Seung Jun; Yoo, Sung Jong Journal of Materials Chemistry, Vol. 22, Issue 30 https://doi.org/10.1039/c2jm31439h	journal	January 2012
The Hydrogen Economy Crabtree, George W.; Dresselhaus, Mildred S.; Buchanan, Michelle V. Physics Today, Vol. 57, Issue 12 https://doi.org/10.1063/1.1878333	journal	December 2004
Powering the planet: Chemical challenges in solar energy utilization Lewis, N. S.; Nocera, D. G. Proceedings of the National Academy of Sciences, Vol. 103, Issue 43, p. 15729-15735 https://doi.org/10.1073/pnas.0603395103	journal	October 2006
An Oxalate Method for Measuring the Surface Area of Nickel Electrodes Hall, David S.; Bock, Christina; MacDougall, Barry R. Journal of The Electrochemical Society, Vol. 161, Issue 12 https://doi.org/10.1149/2.0711412jes	journal	January 2014

Similar Records

Electrolytic Synthesis of Ni-W-MWCNT Composite Coating for Alkaline Hydrogen Evolution Reaction

Journal Article · Thu Mar 15 00:00:00 EDT 2018 · Journal of Materials Engineering and Performance · OSTI ID:22858061

Effects of Ni, Fe, Cu, and Cr substitutions for Co in La{sub 0.8}Sr{sub 0.2}CoO{sub 3} on electrocatalytic properties for oxygen evolution

Journal Article · Wed May 01 00:00:00 EDT 1996 · Journal of the Electrochemical Society · OSTI ID:256801

The influence of intercrystalline defects on hydrogen activity and transport in nickel

Journal Article · Tue Aug 01 00:00:00 EDT 1995 · Acta Metallurgica et Materialia · OSTI ID:100600

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
alkaline
electrochemically active surface area
electrodeposition
films
hydrogen evolution reaction
intrinsic activity
iron
nickel

Electrochemically active surface area controls HER activity for FexNi100–x films in alkaline electrolyte

Citation Formats

References (48)

Similar Records

Related Subjects

Electrochemically active surface area controls HER activity for Fe_xNi_100–x films in alkaline electrolyte