Boosting electrosynthesis of ammonia on surface-engineered MXene Ti3C2

Jiexiang Xia; Shi Ze Yang; Bin Wang; Peiwen Wu; Ilja Popovs; Huaming Li; Stephan Irle; Sheng Dai; Huiyuan Zhu

doi:10.1016/j.nanoen.2020.104681

Boosting electrosynthesis of ammonia on surface-engineered MXene Ti₃C₂

Jiexiang Xia, Shi Ze Yang, Bin Wang, Peiwen Wu, Ilja Popovs, Huaming Li, Stephan Irle, Sheng Dai, Huiyuan Zhu

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

100 Scopus citations

Abstract

Seeking a breakthrough in the development of efficient nitrogen fixation catalysts has become the frontier of energy and chemical conversion schemes. Here, we report that the MXene Ti₃C₂ can serve as a promising catalyst for the electrochemical N₂ reduction reaction (NRR) under ambient conditions. The electrocatalytic performance of Ti₃C₂ can be further optimized through surface engineering. Specifically, Ti₃C₂ with the increased surface hydroxyl moieties demonstrates enhanced production of NH₃ with a yield rate of 1.71 μg h⁻¹ cm⁻², a Faradaic efficiency of 7.01% at −0.2 V vs. RHE at 20 °C and an even higher yield rate of 12.46 μg h⁻¹ cm⁻² together with a Faradaic efficiency of 9.03% at −0.2 V vs. RHE at 60 °C. The detailed electrochemical analysis suggests that the surface hydroxyl modification can effectively facilitate the electron transfer, surface adsorption and activation of dinitrogen. Our work sheds light on the development of efficient NRR catalysts based on earth-abundant elements.

Original language	English
Article number	104681
Journal	Nano Energy
Volume	72
DOIs	https://doi.org/10.1016/j.nanoen.2020.104681
State	Published - Jun 2020

Funding

J. X. was financially supported by the International Postdoctoral Exchange Fellowship Program of China Postdoctoral Council (No. 20150060 ). H. Z., S.I. and S. D. were supported by Fluid Interface Reactions, Structures and Transport (FIRST) Center , an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences . I.P. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division . The electron microscopy (S.Z.Y.) was supported in part by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division and through a user proposal supported by ORNL’s Center for Nanophase Materials Sciences, which is sponsored by the Scientific User Facilities Division of U.S. Department of Energ y. The authors would like to thank Prof. Yury Gogotsi from Drexel University for the helpful discussions. J. X. was financially supported by the International Postdoctoral Exchange Fellowship Program of China Postdoctoral Council (No.20150060). H. Z. S.I. and S. D. were supported by Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences. I.P. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. The electron microscopy (S.Z.Y.) was supported in part by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division and through a user proposal supported by ORNL's Center for Nanophase Materials Sciences, which is sponsored by the Scientific User Facilities Division of U.S. Department of Energy. The authors would like to thank Prof. Yury Gogotsi from Drexel University for the helpful discussions.

Funders	Funder number
Energy Frontier Research Center
International Postdoctoral Exchange Fellowship Program of China Postdoctoral Council	20150060
Materials Science and Engineering Division
ORNL's Center for Nanophase Materials Sciences
ORNL’s Center for Nanophase Materials Sciences
Office of Basic Energy Sciences
U.S. Department of Energ y.
US Department of Energy
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Drexel University
Division of Materials Sciences and Engineering

Keywords

Electrocatalysis
MXene
Nitrogen fixation
Surface engineering
TiC

Access to Document

10.1016/j.nanoen.2020.104681

Cite this

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title = "Boosting electrosynthesis of ammonia on surface-engineered MXene Ti3C2 ",

abstract = "Seeking a breakthrough in the development of efficient nitrogen fixation catalysts has become the frontier of energy and chemical conversion schemes. Here, we report that the MXene Ti3C2 can serve as a promising catalyst for the electrochemical N2 reduction reaction (NRR) under ambient conditions. The electrocatalytic performance of Ti3C2 can be further optimized through surface engineering. Specifically, Ti3C2 with the increased surface hydroxyl moieties demonstrates enhanced production of NH3 with a yield rate of 1.71 μg h−1 cm−2, a Faradaic efficiency of 7.01% at −0.2 V vs. RHE at 20 °C and an even higher yield rate of 12.46 μg h−1 cm−2 together with a Faradaic efficiency of 9.03% at −0.2 V vs. RHE at 60 °C. The detailed electrochemical analysis suggests that the surface hydroxyl modification can effectively facilitate the electron transfer, surface adsorption and activation of dinitrogen. Our work sheds light on the development of efficient NRR catalysts based on earth-abundant elements.",

keywords = "Electrocatalysis, MXene, Nitrogen fixation, Surface engineering, TiC",

author = "Jiexiang Xia and Yang, {Shi Ze} and Bin Wang and Peiwen Wu and Ilja Popovs and Huaming Li and Stephan Irle and Sheng Dai and Huiyuan Zhu",

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year = "2020",

month = jun,

doi = "10.1016/j.nanoen.2020.104681",

language = "English",

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AU - Yang, Shi Ze

AU - Wang, Bin

AU - Wu, Peiwen

AU - Popovs, Ilja

AU - Li, Huaming

AU - Irle, Stephan

AU - Dai, Sheng

AU - Zhu, Huiyuan

PY - 2020/6

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N2 - Seeking a breakthrough in the development of efficient nitrogen fixation catalysts has become the frontier of energy and chemical conversion schemes. Here, we report that the MXene Ti3C2 can serve as a promising catalyst for the electrochemical N2 reduction reaction (NRR) under ambient conditions. The electrocatalytic performance of Ti3C2 can be further optimized through surface engineering. Specifically, Ti3C2 with the increased surface hydroxyl moieties demonstrates enhanced production of NH3 with a yield rate of 1.71 μg h−1 cm−2, a Faradaic efficiency of 7.01% at −0.2 V vs. RHE at 20 °C and an even higher yield rate of 12.46 μg h−1 cm−2 together with a Faradaic efficiency of 9.03% at −0.2 V vs. RHE at 60 °C. The detailed electrochemical analysis suggests that the surface hydroxyl modification can effectively facilitate the electron transfer, surface adsorption and activation of dinitrogen. Our work sheds light on the development of efficient NRR catalysts based on earth-abundant elements.

AB - Seeking a breakthrough in the development of efficient nitrogen fixation catalysts has become the frontier of energy and chemical conversion schemes. Here, we report that the MXene Ti3C2 can serve as a promising catalyst for the electrochemical N2 reduction reaction (NRR) under ambient conditions. The electrocatalytic performance of Ti3C2 can be further optimized through surface engineering. Specifically, Ti3C2 with the increased surface hydroxyl moieties demonstrates enhanced production of NH3 with a yield rate of 1.71 μg h−1 cm−2, a Faradaic efficiency of 7.01% at −0.2 V vs. RHE at 20 °C and an even higher yield rate of 12.46 μg h−1 cm−2 together with a Faradaic efficiency of 9.03% at −0.2 V vs. RHE at 60 °C. The detailed electrochemical analysis suggests that the surface hydroxyl modification can effectively facilitate the electron transfer, surface adsorption and activation of dinitrogen. Our work sheds light on the development of efficient NRR catalysts based on earth-abundant elements.

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