Rational Electrode-Electrolyte Design for Efficient Ammonia Electrosynthesis under Ambient Conditions

Bryan H.R. Suryanto; Colin S.M. Kang; Dabin Wang; Changlong Xiao; Fengling Zhou; Luis Miguel Azofra; Luigi Cavallo; Xinyi Zhang; Douglas R. Macfarlane

doi:10.1021/acsenergylett.8b00487

Rational Electrode-Electrolyte Design for Efficient Ammonia Electrosynthesis under Ambient Conditions

Bryan H.R. Suryanto, Colin S.M. Kang, Dabin Wang, Changlong Xiao, Fengling Zhou, Luis Miguel Azofra, Luigi Cavallo, Xinyi Zhang, Douglas R. Macfarlane

School of Chemistry

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

235 Citations (Scopus)

Abstract

Renewable energy-driven ammonia electrosynthesis by N₂ reduction reaction (NRR) at ambient conditions is vital for sustainability of both the global population and energy demand. However, NRR under ambient conditions to date has been plagued with a low yield rate and selectivity (<10%) due to the more favorable hydrogen evolution reaction (HER) in aqueous media. Herein, surface area enhanced α-Fe nanorods grown on carbon fiber paper were used as NRR cathodes in an aprotic fluorinated solvent-ionic liquid mixture. Through this design, significantly enhanced NRR activity with an NH₃ yield rate of ∼2.35 × 10^-11 mol s^-1 cm_GSA^-2, (3.71 × 10^-13 mol s^-1 cm_ECSA^-2) and selectivity of ∼32% has been achieved under ambient conditions. This study reveals that the use of hydrophobic fluorinated aprotic electrolyte effectively limits the availability of protons and thus suppresses the competing HER. Therefore, electrode-electrolyte engineering is essential in advancing the NH₃ electrosynthesis technology.

Original language	English
Pages (from-to)	1219-1224
Number of pages	6
Journal	ACS Energy Letters
Volume	3
Issue number	6
DOIs	https://doi.org/10.1021/acsenergylett.8b00487
Publication status	Published - 8 Jun 2018

UN SDGs

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

SDG 7 Affordable and Clean Energy

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10.1021/acsenergylett.8b00487

240848215-oaFinal published version, 2.95 MB

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title = "Rational Electrode-Electrolyte Design for Efficient Ammonia Electrosynthesis under Ambient Conditions",

abstract = "Renewable energy-driven ammonia electrosynthesis by N2 reduction reaction (NRR) at ambient conditions is vital for sustainability of both the global population and energy demand. However, NRR under ambient conditions to date has been plagued with a low yield rate and selectivity (<10\%) due to the more favorable hydrogen evolution reaction (HER) in aqueous media. Herein, surface area enhanced α-Fe nanorods grown on carbon fiber paper were used as NRR cathodes in an aprotic fluorinated solvent-ionic liquid mixture. Through this design, significantly enhanced NRR activity with an NH3 yield rate of ∼2.35 × 10-11 mol s-1 cmGSA-2, (3.71 × 10-13 mol s-1 cmECSA-2) and selectivity of ∼32\% has been achieved under ambient conditions. This study reveals that the use of hydrophobic fluorinated aprotic electrolyte effectively limits the availability of protons and thus suppresses the competing HER. Therefore, electrode-electrolyte engineering is essential in advancing the NH3 electrosynthesis technology.",

author = "Suryanto, \{Bryan H.R.\} and Kang, \{Colin S.M.\} and Dabin Wang and Changlong Xiao and Fengling Zhou and Azofra, \{Luis Miguel\} and Luigi Cavallo and Xinyi Zhang and Macfarlane, \{Douglas R.\}",

year = "2018",

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doi = "10.1021/acsenergylett.8b00487",

language = "English",

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T1 - Rational Electrode-Electrolyte Design for Efficient Ammonia Electrosynthesis under Ambient Conditions

AU - Suryanto, Bryan H.R.

AU - Kang, Colin S.M.

AU - Wang, Dabin

AU - Xiao, Changlong

AU - Zhou, Fengling

AU - Azofra, Luis Miguel

AU - Cavallo, Luigi

AU - Zhang, Xinyi

AU - Macfarlane, Douglas R.

PY - 2018/6/8

Y1 - 2018/6/8

N2 - Renewable energy-driven ammonia electrosynthesis by N2 reduction reaction (NRR) at ambient conditions is vital for sustainability of both the global population and energy demand. However, NRR under ambient conditions to date has been plagued with a low yield rate and selectivity (<10%) due to the more favorable hydrogen evolution reaction (HER) in aqueous media. Herein, surface area enhanced α-Fe nanorods grown on carbon fiber paper were used as NRR cathodes in an aprotic fluorinated solvent-ionic liquid mixture. Through this design, significantly enhanced NRR activity with an NH3 yield rate of ∼2.35 × 10-11 mol s-1 cmGSA-2, (3.71 × 10-13 mol s-1 cmECSA-2) and selectivity of ∼32% has been achieved under ambient conditions. This study reveals that the use of hydrophobic fluorinated aprotic electrolyte effectively limits the availability of protons and thus suppresses the competing HER. Therefore, electrode-electrolyte engineering is essential in advancing the NH3 electrosynthesis technology.

AB - Renewable energy-driven ammonia electrosynthesis by N2 reduction reaction (NRR) at ambient conditions is vital for sustainability of both the global population and energy demand. However, NRR under ambient conditions to date has been plagued with a low yield rate and selectivity (<10%) due to the more favorable hydrogen evolution reaction (HER) in aqueous media. Herein, surface area enhanced α-Fe nanorods grown on carbon fiber paper were used as NRR cathodes in an aprotic fluorinated solvent-ionic liquid mixture. Through this design, significantly enhanced NRR activity with an NH3 yield rate of ∼2.35 × 10-11 mol s-1 cmGSA-2, (3.71 × 10-13 mol s-1 cmECSA-2) and selectivity of ∼32% has been achieved under ambient conditions. This study reveals that the use of hydrophobic fluorinated aprotic electrolyte effectively limits the availability of protons and thus suppresses the competing HER. Therefore, electrode-electrolyte engineering is essential in advancing the NH3 electrosynthesis technology.

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JO - ACS Energy Letters

JF - ACS Energy Letters

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Rational Electrode-Electrolyte Design for Efficient Ammonia Electrosynthesis under Ambient Conditions

Abstract

UN SDGs

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Efficient ionic liquid-based reduction of nitrogen to ammonia

Monash Centre for Electron Microscopy (MCEM)

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Rational Electrode-Electrolyte Design for Efficient Ammonia Electrosynthesis under Ambient Conditions

Abstract

UN SDGs

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Projects

Efficient ionic liquid-based reduction of nitrogen to ammonia

Equipment

Monash Centre for Electron Microscopy (MCEM)

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