Reduction of Transition-Metal Columbite-Tantalite as a Highly Efficient Electrocatalyst for Water Splitting

Patrick M. Bacirhonde; Nelson Y. Dzade; Carmen Chalony; Jeesoo Park; Eun Suk Jeong; Emmanuel O. Afranie; Sunny Lee; Cheol Sang Kim; Do Hwan Kim; Chan Hee Park

doi:10.1021/acsami.1c21742

Reduction of Transition-Metal Columbite-Tantalite as a Highly Efficient Electrocatalyst for Water Splitting

Patrick M. Bacirhonde, Nelson Y. Dzade, Carmen Chalony, Jeesoo Park, Eun Suk Jeong, Emmanuel O. Afranie, Sunny Lee, Cheol Sang Kim, Do Hwan Kim, Chan Hee Park

John and Willie Leone Department of Energy & Mineral Engineering (EME)

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

We successfully report a liquid-liquid chemical reduction and hydrothermal synthesis of a highly stable columbite-tantalite electrocatalyst with remarkable hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance in acidic media. The reduced Fe_0.79Mn_0.21Nb_0.16Ta_0.84O₆(CTr) electrocatalyst shows a low overpotential of 84.23 mV at 10 mA cm^-2and 103.7 achieved at 20 mA cm^-2current density in situ for the HER and OER, respectively. The electrocatalyst also exhibited low Tafel slopes of 104.97 mV/dec for the HER and 57.67 mV/dec for the OER, verifying their rapid catalytic kinetics. The electrolyzer maintained a cell voltage of 1.5 V and potential-time stability close to that of Pt/C and RuO₂. Complementary first-principles density functional theory calculations identify the Mn sites as most active sites on the Fe_0.75Mn_0.25Ta_1.875Nb_0.125O₆(100) surface, predicting a moderate Gibbs free energy of hydrogen adsorption (δG_H*≈ 0.08 eV) and a low overpotential of η = 0.47 V. The |δGMn_H*| = 0.08 eV on the Fe_0.75Mn_0.25Ta_1.875Nb_0.125O₆(100) surface is similar to that of the well-known and highly efficient Pt catalyst (|δGPt_H*| ≈ 0.09 eV).

Original language	English (US)
Pages (from-to)	15090-15102
Number of pages	13
Journal	ACS Applied Materials and Interfaces
Volume	14
Issue number	13
DOIs	https://doi.org/10.1021/acsami.1c21742
State	Published - Apr 6 2022

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Materials Science(all)

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10.1021/acsami.1c21742

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@article{8008902b88634ed58e87ce4cbab36ad2,

title = "Reduction of Transition-Metal Columbite-Tantalite as a Highly Efficient Electrocatalyst for Water Splitting",

abstract = "We successfully report a liquid-liquid chemical reduction and hydrothermal synthesis of a highly stable columbite-tantalite electrocatalyst with remarkable hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance in acidic media. The reduced Fe0.79Mn0.21Nb0.16Ta0.84O6(CTr) electrocatalyst shows a low overpotential of 84.23 mV at 10 mA cm-2and 103.7 achieved at 20 mA cm-2current density in situ for the HER and OER, respectively. The electrocatalyst also exhibited low Tafel slopes of 104.97 mV/dec for the HER and 57.67 mV/dec for the OER, verifying their rapid catalytic kinetics. The electrolyzer maintained a cell voltage of 1.5 V and potential-time stability close to that of Pt/C and RuO2. Complementary first-principles density functional theory calculations identify the Mn sites as most active sites on the Fe0.75Mn0.25Ta1.875Nb0.125O6(100) surface, predicting a moderate Gibbs free energy of hydrogen adsorption (δGH*≈ 0.08 eV) and a low overpotential of η = 0.47 V. The |δGMnH*| = 0.08 eV on the Fe0.75Mn0.25Ta1.875Nb0.125O6(100) surface is similar to that of the well-known and highly efficient Pt catalyst (|δGPtH*| ≈ 0.09 eV).",

author = "Bacirhonde, {Patrick M.} and Dzade, {Nelson Y.} and Carmen Chalony and Jeesoo Park and Jeong, {Eun Suk} and Afranie, {Emmanuel O.} and Sunny Lee and Kim, {Cheol Sang} and Kim, {Do Hwan} and Park, {Chan Hee}",

note = "Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (2019R1A2C1003988) and also partially supported by the Regional Leading Research Center Program (2019R1A5A8080326) through the National Research Foundation funded by the Ministry of Science and ICT of the Republic of Korea. NYD acknowledges the UK Engineering and Physical Sciences Research Council (EPSRC) for funding (Grant No. EP/S001395/1) and support from the College of Earth and Minerals Sciences and the John and Willie Leone Family Department of Energy and Mineral Engineering of the Pennsylvania State University. The computational resources used are the Advanced Research Computing at Cardiff (ARCCA) Division, Cardiff University, and HPC Wales and ARCHER ( http://www.archer.ac.uk ), the UK{\textquoteright}s national supercomputing service, via the membership of the UK{\textquoteright}s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202). Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

year = "2022",

month = apr,

day = "6",

doi = "10.1021/acsami.1c21742",

language = "English (US)",

volume = "14",

pages = "15090--15102",

journal = "ACS Applied Materials and Interfaces",

issn = "1944-8244",

publisher = "American Chemical Society",

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TY - JOUR

T1 - Reduction of Transition-Metal Columbite-Tantalite as a Highly Efficient Electrocatalyst for Water Splitting

AU - Bacirhonde, Patrick M.

AU - Dzade, Nelson Y.

AU - Chalony, Carmen

AU - Park, Jeesoo

AU - Jeong, Eun Suk

AU - Afranie, Emmanuel O.

AU - Lee, Sunny

AU - Kim, Cheol Sang

AU - Kim, Do Hwan

AU - Park, Chan Hee

N1 - Funding Information: This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (2019R1A2C1003988) and also partially supported by the Regional Leading Research Center Program (2019R1A5A8080326) through the National Research Foundation funded by the Ministry of Science and ICT of the Republic of Korea. NYD acknowledges the UK Engineering and Physical Sciences Research Council (EPSRC) for funding (Grant No. EP/S001395/1) and support from the College of Earth and Minerals Sciences and the John and Willie Leone Family Department of Energy and Mineral Engineering of the Pennsylvania State University. The computational resources used are the Advanced Research Computing at Cardiff (ARCCA) Division, Cardiff University, and HPC Wales and ARCHER ( http://www.archer.ac.uk ), the UK’s national supercomputing service, via the membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202). Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/4/6

Y1 - 2022/4/6

N2 - We successfully report a liquid-liquid chemical reduction and hydrothermal synthesis of a highly stable columbite-tantalite electrocatalyst with remarkable hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance in acidic media. The reduced Fe0.79Mn0.21Nb0.16Ta0.84O6(CTr) electrocatalyst shows a low overpotential of 84.23 mV at 10 mA cm-2and 103.7 achieved at 20 mA cm-2current density in situ for the HER and OER, respectively. The electrocatalyst also exhibited low Tafel slopes of 104.97 mV/dec for the HER and 57.67 mV/dec for the OER, verifying their rapid catalytic kinetics. The electrolyzer maintained a cell voltage of 1.5 V and potential-time stability close to that of Pt/C and RuO2. Complementary first-principles density functional theory calculations identify the Mn sites as most active sites on the Fe0.75Mn0.25Ta1.875Nb0.125O6(100) surface, predicting a moderate Gibbs free energy of hydrogen adsorption (δGH*≈ 0.08 eV) and a low overpotential of η = 0.47 V. The |δGMnH*| = 0.08 eV on the Fe0.75Mn0.25Ta1.875Nb0.125O6(100) surface is similar to that of the well-known and highly efficient Pt catalyst (|δGPtH*| ≈ 0.09 eV).

AB - We successfully report a liquid-liquid chemical reduction and hydrothermal synthesis of a highly stable columbite-tantalite electrocatalyst with remarkable hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance in acidic media. The reduced Fe0.79Mn0.21Nb0.16Ta0.84O6(CTr) electrocatalyst shows a low overpotential of 84.23 mV at 10 mA cm-2and 103.7 achieved at 20 mA cm-2current density in situ for the HER and OER, respectively. The electrocatalyst also exhibited low Tafel slopes of 104.97 mV/dec for the HER and 57.67 mV/dec for the OER, verifying their rapid catalytic kinetics. The electrolyzer maintained a cell voltage of 1.5 V and potential-time stability close to that of Pt/C and RuO2. Complementary first-principles density functional theory calculations identify the Mn sites as most active sites on the Fe0.75Mn0.25Ta1.875Nb0.125O6(100) surface, predicting a moderate Gibbs free energy of hydrogen adsorption (δGH*≈ 0.08 eV) and a low overpotential of η = 0.47 V. The |δGMnH*| = 0.08 eV on the Fe0.75Mn0.25Ta1.875Nb0.125O6(100) surface is similar to that of the well-known and highly efficient Pt catalyst (|δGPtH*| ≈ 0.09 eV).

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U2 - 10.1021/acsami.1c21742

DO - 10.1021/acsami.1c21742

M3 - Article

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AN - SCOPUS:85127633097

SN - 1944-8244

VL - 14

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EP - 15102

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 13

ER -

Reduction of Transition-Metal Columbite-Tantalite as a Highly Efficient Electrocatalyst for Water Splitting

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