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^*

^*Corresponding author for this work

Research output: Contribution to journal › Journal article › peer-review

8 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
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 - 2022.04.6

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

3d-5d transition metals
cation vacancies
columbite-tantalite
electrocatalyst
ionic-electronic conductivity
liquid-liquid chemical reduction
oxygen vacancies
water splitting

Quacquarelli Symonds(QS) Subject Topics

Materials Science

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10.1021/acsami.1c21742

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@article{81774f7edbf649d4ba429018db2cc1fb,

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).",

keywords = "3d-5d transition metals, cation vacancies, columbite-tantalite, electrocatalyst, ionic-electronic conductivity, liquid-liquid chemical reduction, oxygen vacancies, water splitting",

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\}",

year = "2022",

month = apr,

day = "6",

doi = "10.1021/acsami.1c21742",

language = "English",

volume = "14",

pages = "15090--15102",

journal = "ACS Applied Materials and Interfaces",

issn = "1944-8244",

number = "13",

}

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

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).

KW - 3d-5d transition metals

KW - cation vacancies

KW - columbite-tantalite

KW - electrocatalyst

KW - ionic-electronic conductivity

KW - liquid-liquid chemical reduction

KW - oxygen vacancies

KW - water splitting

UR - https://www.scopus.com/pages/publications/85127633097

U2 - 10.1021/acsami.1c21742

DO - 10.1021/acsami.1c21742

M3 - Journal article

C2 - 35324159

AN - SCOPUS:85127633097

SN - 1944-8244

VL - 14

SP - 15090

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

Abstract

UN SDGs

Keywords

Quacquarelli Symonds(QS) Subject Topics

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