Protecting and Enhancing the Photoelectrocatalytic Performance of InGaN Nanowires toward Nitrogen Reduction to Ammonia Synthesis

Paulraj Gnanasekar; Karthik Peramaiah; Huafan Zhang; Mathan Kumar Eswaran; Rakesh Rosan Pradhan; Udo Schwingenschlögl; Tien Khee Ng; Qiaoqiang Gan; Jeganathan Kulandaivel; Kuo Wei Huang; Boon S. Ooi

doi:10.1021/acsaem.3c01277

Protecting and Enhancing the Photoelectrocatalytic Performance of InGaN Nanowires toward Nitrogen Reduction to Ammonia Synthesis

Paulraj Gnanasekar, Karthik Peramaiah, Huafan Zhang, Mathan Kumar Eswaran, Rakesh Rosan Pradhan, Udo Schwingenschlögl, Tien Khee Ng, Qiaoqiang Gan, Jeganathan Kulandaivel^*, Kuo Wei Huang^*, Boon S. Ooi^*

^*Corresponding author for this work

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

3 Scopus citations

Abstract

The photoelectrochemical (PEC) reduction of nitrogen (N₂) to ammonia (NH₃) has emerged as a potential alternative to the conventional Haber-Bosch approach as the solar energy-driven process reduces energy consumption. In this work, PEC N₂ reduction is demonstrated with indium gallium nitride (InGaN) nanowires deposited with molybdenum carbide (Mo₂C) co-catalyst. Interestingly, the incorporation of a GaN buffer layer between InGaN and Mo₂C forms a suitable band alignment for rapid photogenerated charge carrier separation for the N₂ reduction reaction (NRR). Impressively, a maximum NH₃ production yield and Faradaic efficiency of 7.93 μg·h^-1·cm^-2 and 15.39%, respectively, is achieved at −0.2 V vs the reversible hydrogen electrode with the unique band structure of the Mo₂C/GaN/InGaN photoelectrode. Density functional theory calculations reveal the favorable Gibbs free energy and efficient charge transfer process of the unique band structure of Mo₂C/GaN/InGaN for effective NRR.

Original language	English (US)
Pages (from-to)	10784-10793
Number of pages	10
Journal	ACS Applied Energy Materials
Volume	6
Issue number	21
DOIs	https://doi.org/10.1021/acsaem.3c01277
State	Published - Nov 13 2023

Keywords

ammonia
III−V nitrate
molecular beam epitaxy
molybdenum carbide
nitrate reduction

ASJC Scopus subject areas

Chemical Engineering (miscellaneous)
Energy Engineering and Power Technology
Electrochemistry
Materials Chemistry
Electrical and Electronic Engineering

UN SDGs

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

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10.1021/acsaem.3c01277

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Gnanasekar, P., Peramaiah, K., Zhang, H., Eswaran, M. K., Pradhan, R. R., Schwingenschlögl, U., Ng, T. K., Gan, Q., Kulandaivel, J., Huang, K. W., & Ooi, B. S. (2023). Protecting and Enhancing the Photoelectrocatalytic Performance of InGaN Nanowires toward Nitrogen Reduction to Ammonia Synthesis. ACS Applied Energy Materials, 6(21), 10784-10793. https://doi.org/10.1021/acsaem.3c01277

@article{5953733605064cf0a3530082114a80e8,

title = "Protecting and Enhancing the Photoelectrocatalytic Performance of InGaN Nanowires toward Nitrogen Reduction to Ammonia Synthesis",

abstract = "The photoelectrochemical (PEC) reduction of nitrogen (N2) to ammonia (NH3) has emerged as a potential alternative to the conventional Haber-Bosch approach as the solar energy-driven process reduces energy consumption. In this work, PEC N2 reduction is demonstrated with indium gallium nitride (InGaN) nanowires deposited with molybdenum carbide (Mo2C) co-catalyst. Interestingly, the incorporation of a GaN buffer layer between InGaN and Mo2C forms a suitable band alignment for rapid photogenerated charge carrier separation for the N2 reduction reaction (NRR). Impressively, a maximum NH3 production yield and Faradaic efficiency of 7.93 μg·h-1·cm-2 and 15.39%, respectively, is achieved at −0.2 V vs the reversible hydrogen electrode with the unique band structure of the Mo2C/GaN/InGaN photoelectrode. Density functional theory calculations reveal the favorable Gibbs free energy and efficient charge transfer process of the unique band structure of Mo2C/GaN/InGaN for effective NRR.",

keywords = "ammonia, III−V nitrate, molecular beam epitaxy, molybdenum carbide, nitrate reduction",

author = "Paulraj Gnanasekar and Karthik Peramaiah and Huafan Zhang and Eswaran, {Mathan Kumar} and Pradhan, {Rakesh Rosan} and Udo Schwingenschl{\"o}gl and Ng, {Tien Khee} and Qiaoqiang Gan and Jeganathan Kulandaivel and Huang, {Kuo Wei} and Ooi, {Boon S.}",

note = "Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society",

year = "2023",

month = nov,

day = "13",

doi = "10.1021/acsaem.3c01277",

language = "English (US)",

volume = "6",

pages = "10784--10793",

journal = "ACS Applied Energy Materials",

issn = "2574-0962",

publisher = "American Chemical Society",

number = "21",

}

Gnanasekar, P, Peramaiah, K, Zhang, H, Eswaran, MK, Pradhan, RR, Schwingenschlögl, U, Ng, TK, Gan, Q, Kulandaivel, J, Huang, KW & Ooi, BS 2023, 'Protecting and Enhancing the Photoelectrocatalytic Performance of InGaN Nanowires toward Nitrogen Reduction to Ammonia Synthesis', ACS Applied Energy Materials, vol. 6, no. 21, pp. 10784-10793. https://doi.org/10.1021/acsaem.3c01277

TY - JOUR

T1 - Protecting and Enhancing the Photoelectrocatalytic Performance of InGaN Nanowires toward Nitrogen Reduction to Ammonia Synthesis

AU - Gnanasekar, Paulraj

AU - Peramaiah, Karthik

AU - Zhang, Huafan

AU - Eswaran, Mathan Kumar

AU - Pradhan, Rakesh Rosan

AU - Schwingenschlögl, Udo

AU - Ng, Tien Khee

AU - Gan, Qiaoqiang

AU - Kulandaivel, Jeganathan

AU - Huang, Kuo Wei

AU - Ooi, Boon S.

PY - 2023/11/13

Y1 - 2023/11/13

N2 - The photoelectrochemical (PEC) reduction of nitrogen (N2) to ammonia (NH3) has emerged as a potential alternative to the conventional Haber-Bosch approach as the solar energy-driven process reduces energy consumption. In this work, PEC N2 reduction is demonstrated with indium gallium nitride (InGaN) nanowires deposited with molybdenum carbide (Mo2C) co-catalyst. Interestingly, the incorporation of a GaN buffer layer between InGaN and Mo2C forms a suitable band alignment for rapid photogenerated charge carrier separation for the N2 reduction reaction (NRR). Impressively, a maximum NH3 production yield and Faradaic efficiency of 7.93 μg·h-1·cm-2 and 15.39%, respectively, is achieved at −0.2 V vs the reversible hydrogen electrode with the unique band structure of the Mo2C/GaN/InGaN photoelectrode. Density functional theory calculations reveal the favorable Gibbs free energy and efficient charge transfer process of the unique band structure of Mo2C/GaN/InGaN for effective NRR.

AB - The photoelectrochemical (PEC) reduction of nitrogen (N2) to ammonia (NH3) has emerged as a potential alternative to the conventional Haber-Bosch approach as the solar energy-driven process reduces energy consumption. In this work, PEC N2 reduction is demonstrated with indium gallium nitride (InGaN) nanowires deposited with molybdenum carbide (Mo2C) co-catalyst. Interestingly, the incorporation of a GaN buffer layer between InGaN and Mo2C forms a suitable band alignment for rapid photogenerated charge carrier separation for the N2 reduction reaction (NRR). Impressively, a maximum NH3 production yield and Faradaic efficiency of 7.93 μg·h-1·cm-2 and 15.39%, respectively, is achieved at −0.2 V vs the reversible hydrogen electrode with the unique band structure of the Mo2C/GaN/InGaN photoelectrode. Density functional theory calculations reveal the favorable Gibbs free energy and efficient charge transfer process of the unique band structure of Mo2C/GaN/InGaN for effective NRR.

KW - ammonia

KW - III−V nitrate

KW - molecular beam epitaxy

KW - molybdenum carbide

KW - nitrate reduction

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U2 - 10.1021/acsaem.3c01277

DO - 10.1021/acsaem.3c01277

M3 - Article

AN - SCOPUS:85177496963

SN - 2574-0962

VL - 6

SP - 10784

EP - 10793

JO - ACS Applied Energy Materials

JF - ACS Applied Energy Materials

IS - 21

ER -

Protecting and Enhancing the Photoelectrocatalytic Performance of InGaN Nanowires toward Nitrogen Reduction to Ammonia Synthesis

Abstract

Keywords

ASJC Scopus subject areas

UN SDGs

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