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Nano Research 2024, 17(3): 1151-1164 https://doi.org/10.1007/s12274-023-5943-0
Research Article | Issue | Published: 13 September 2023

Applying heteroatom co-doped carbon nanotube for manifesting high performance in the electrochemical reduction of aqueous nitrogen oxide by gold nanoparticles

Show Author's Information Jane Chung1,2,§,  Haibo Yin1,§,  Rong Wang1,  Yunlong Wang1,  Junyang Zhang1,  Yue Peng1,  Joung Woo Han2,  Seongyun Ryu2,  Junhua Li1( )
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
EHS Research Center, Samsung Electronics Co., Ltd., Gyeonggi-do 18448, Republic of Korea

§ Jane Chung and Haibo Yin contributed equally to this work.

Keywords:
gold nanoparticles, nitrogen defect, electrochemical NO-to-NH3, boron heteroatom, valence states of gold
Topics:
Nanocatalysts
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Chung J, Yin H, Wang R, et al. Applying heteroatom co-doped carbon nanotube for manifesting high performance in the electrochemical reduction of aqueous nitrogen oxide by gold nanoparticles. Nano Research, 2024, 17(3): 1151-1164. https://doi.org/10.1007/s12274-023-5943-0
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Abstract Full text Electronic supplementary material About this article

Electrochemical NO-to-NH3 under ambient conditions could be a viable alternative having advantages in terms of energy consumption and exhaust gas recycling of NO, replacing a traditional ammonia synthesis method of the Haber–Bosch process. In synthesizing boron (B-) and nitrogen (N-) co-doped carbon nanotube (CNT) based gold (Au) catalysts, B-dopants elevate the conductivity of carbon nanotube by sp2 hybridization on graphene and implant B–N domains within the graphene layer, and result in facilitating the embedding amount of Au accompanied by high dispersibility with low particle size. Theoretical density functional theory (DFT) calculations elucidate that the electron cloud transmitted from B-dopant to the active site of Au induces the Lewis acidic site, and the O-distal pathway occurs following a spontaneous reaction. Increment of the electron-deficient B-doping area accompanied by N-defects and B–O edges retains the major valence state of Au as Auδ+, and suppresses hydrogen evolution reaction (HER) by repulsing the hindrance of H*. This record exhibits the highest faradaic efficiency (FE) of 94.7%, and NH3 yield rate of 1877.4 μg·h−1·mgcat−1, which is the optimal yield over energy consumption in the field of the ambient reduction of aqueous NO.


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Electronic supplementary material
About this article

Applying heteroatom co-doped carbon nanotube for manifesting high performance in the electrochemical reduction of aqueous nitrogen oxide by gold nanoparticles

Show Author's information Jane Chung1,2,§, Haibo Yin1,§, Rong Wang1, Yunlong Wang1, Junyang Zhang1, Yue Peng1, Joung Woo Han2, Seongyun Ryu2, Junhua Li1( )
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
EHS Research Center, Samsung Electronics Co., Ltd., Gyeonggi-do 18448, Republic of Korea

§ Jane Chung and Haibo Yin contributed equally to this work.

Abstract

Electrochemical NO-to-NH3 under ambient conditions could be a viable alternative having advantages in terms of energy consumption and exhaust gas recycling of NO, replacing a traditional ammonia synthesis method of the Haber–Bosch process. In synthesizing boron (B-) and nitrogen (N-) co-doped carbon nanotube (CNT) based gold (Au) catalysts, B-dopants elevate the conductivity of carbon nanotube by sp2 hybridization on graphene and implant B–N domains within the graphene layer, and result in facilitating the embedding amount of Au accompanied by high dispersibility with low particle size. Theoretical density functional theory (DFT) calculations elucidate that the electron cloud transmitted from B-dopant to the active site of Au induces the Lewis acidic site, and the O-distal pathway occurs following a spontaneous reaction. Increment of the electron-deficient B-doping area accompanied by N-defects and B–O edges retains the major valence state of Au as Auδ+, and suppresses hydrogen evolution reaction (HER) by repulsing the hindrance of H*. This record exhibits the highest faradaic efficiency (FE) of 94.7%, and NH3 yield rate of 1877.4 μg·h−1·mgcat−1, which is the optimal yield over energy consumption in the field of the ambient reduction of aqueous NO.

Keywords: gold nanoparticles, nitrogen defect, electrochemical NO-to-NH3, boron heteroatom, valence states of gold

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Publication history
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Acknowledgements

Publication history

Received: 04 May 2023
Revised: 19 June 2023
Accepted: 20 June 2023
Published: 13 September 2023
Issue date: March 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22206096 and 21936005) and China Postdoctoral Science Foundation (Nos. 2020TQ0166 and 2021M691771).

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