Pre-Adsorbed H-Assisted N2 Activation on Single-Atom Cadmium-O5 Decorated In2O3 for Efficient NH3 Electrosynthesis

Zhibo Yao; Shiqiang Liu; Honghong Liu; Yukun Ruan; Song Hong; Tai Sing Wu; Leiduan Hao; Yun Liang Soo; Pei Xiong; Molly Meng Jung Li; Alex W. Robertson; Qineng Xia; Liang Xin Ding; Zhenyu Sun

doi:10.1002/adfm.202209843

Pre-Adsorbed H-Assisted N₂ Activation on Single-Atom Cadmium-O₅ Decorated In₂O₃ for Efficient NH₃ Electrosynthesis

Zhibo Yao
, Shiqiang Liu
, Honghong Liu
, Yukun Ruan
, Song Hong
, Tai Sing Wu
, Leiduan Hao
, Yun Liang Soo
, Pei Xiong
, Molly Meng Jung Li
, Alex W. Robertson
, Qineng Xia
, Liang Xin Ding
, Zhenyu Sun

Research output: Journal article publication › Journal article › Academic research › peer-review

68 Citations (Scopus)

Abstract

The electrocatalytic nitrogen reduction reaction (NRR) provides a promising avenue for sustainable and decentralized green ammonia (NH₃) synthesis. To promote the NRR, the design and synthesis of efficient electrocatalysts with an elucidated reaction mechanism is critically important. Here, surface hydrogenation-facilitated NRR is demonstrated to yield NH₃ at low overpotentials on oxygen-deficient In₂O₃ plates decorated with single atom CdO₅ that have a weak N₂-binding capability. Adsorbed ^*H is calculated to be first produced via the Volmer reaction (H₂O + e⁻ → ^*H + OH⁻) and then reacts with dissolved N₂ to generate ^*N₂H₂, which is likely the rate determining step (RDS) of the whole process. Cd atoms and oxygen vacancies in In₂O₃ jointly enhance the activation of N₂ and accelerate the RDS, boosting the NRR. An NH₃ production rate of as high as 57.5 µg h⁻¹ mg_cat⁻¹ is attained at a mild potential, which is retained to a large extent even after 44 h of continuous polarization.

Original language	English
Article number	2209843
Journal	Advanced Functional Materials
Volume	33
Issue number	5
DOIs	https://doi.org/10.1002/adfm.202209843
Publication status	Published - 27 Nov 2022

Keywords

electrocatalyses
N reduction
NH
reaction mechanisms
single-atom catalysts

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Chemistry
Biomaterials
General Materials Science
Condensed Matter Physics
Electrochemistry

More information

10.1002/adfm.202209843

Cite this

Yao, Z., Liu, S., Liu, H., Ruan, Y., Hong, S., Wu, T. S., Hao, L., Soo, Y. L., Xiong, P., Li, M. M. J., Robertson, A. W., Xia, Q., Ding, L. X., & Sun, Z. (2022). Pre-Adsorbed H-Assisted N₂ Activation on Single-Atom Cadmium-O₅ Decorated In₂O₃ for Efficient NH₃ Electrosynthesis. Advanced Functional Materials, 33(5), Article 2209843. https://doi.org/10.1002/adfm.202209843

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title = "Pre-Adsorbed H-Assisted N2 Activation on Single-Atom Cadmium-O5 Decorated In2O3 for Efficient NH3 Electrosynthesis",

abstract = "The electrocatalytic nitrogen reduction reaction (NRR) provides a promising avenue for sustainable and decentralized green ammonia (NH3) synthesis. To promote the NRR, the design and synthesis of efficient electrocatalysts with an elucidated reaction mechanism is critically important. Here, surface hydrogenation-facilitated NRR is demonstrated to yield NH3 at low overpotentials on oxygen-deficient In2O3 plates decorated with single atom CdO5 that have a weak N2-binding capability. Adsorbed *H is calculated to be first produced via the Volmer reaction (H2O + e− → *H + OH−) and then reacts with dissolved N2 to generate *N2H2, which is likely the rate determining step (RDS) of the whole process. Cd atoms and oxygen vacancies in In2O3 jointly enhance the activation of N2 and accelerate the RDS, boosting the NRR. An NH3 production rate of as high as 57.5 µg h−1 mgcat−1 is attained at a mild potential, which is retained to a large extent even after 44 h of continuous polarization.",

keywords = "electrocatalyses, N reduction, NH, reaction mechanisms, single-atom catalysts",

author = "Zhibo Yao and Shiqiang Liu and Honghong Liu and Yukun Ruan and Song Hong and Wu, \{Tai Sing\} and Leiduan Hao and Soo, \{Yun Liang\} and Pei Xiong and Li, \{Molly Meng Jung\} and Robertson, \{Alex W.\} and Qineng Xia and Ding, \{Liang Xin\} and Zhenyu Sun",

note = "Funding Information: Z.Y. and S.L. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (no. 21972010, 22022503) and Beijing Natural Science Foundation (no. 2192039). Publisher Copyright: {\textcopyright} 2022 Wiley-VCH GmbH.",

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doi = "10.1002/adfm.202209843",

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T1 - Pre-Adsorbed H-Assisted N2 Activation on Single-Atom Cadmium-O5 Decorated In2O3 for Efficient NH3 Electrosynthesis

AU - Yao, Zhibo

AU - Liu, Shiqiang

AU - Liu, Honghong

AU - Ruan, Yukun

AU - Hong, Song

AU - Wu, Tai Sing

AU - Hao, Leiduan

AU - Soo, Yun Liang

AU - Xiong, Pei

AU - Li, Molly Meng Jung

AU - Robertson, Alex W.

AU - Xia, Qineng

AU - Ding, Liang Xin

AU - Sun, Zhenyu

N1 - Funding Information: Z.Y. and S.L. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (no. 21972010, 22022503) and Beijing Natural Science Foundation (no. 2192039). Publisher Copyright: © 2022 Wiley-VCH GmbH.

PY - 2022/11/27

Y1 - 2022/11/27

N2 - The electrocatalytic nitrogen reduction reaction (NRR) provides a promising avenue for sustainable and decentralized green ammonia (NH3) synthesis. To promote the NRR, the design and synthesis of efficient electrocatalysts with an elucidated reaction mechanism is critically important. Here, surface hydrogenation-facilitated NRR is demonstrated to yield NH3 at low overpotentials on oxygen-deficient In2O3 plates decorated with single atom CdO5 that have a weak N2-binding capability. Adsorbed *H is calculated to be first produced via the Volmer reaction (H2O + e− → *H + OH−) and then reacts with dissolved N2 to generate *N2H2, which is likely the rate determining step (RDS) of the whole process. Cd atoms and oxygen vacancies in In2O3 jointly enhance the activation of N2 and accelerate the RDS, boosting the NRR. An NH3 production rate of as high as 57.5 µg h−1 mgcat−1 is attained at a mild potential, which is retained to a large extent even after 44 h of continuous polarization.

AB - The electrocatalytic nitrogen reduction reaction (NRR) provides a promising avenue for sustainable and decentralized green ammonia (NH3) synthesis. To promote the NRR, the design and synthesis of efficient electrocatalysts with an elucidated reaction mechanism is critically important. Here, surface hydrogenation-facilitated NRR is demonstrated to yield NH3 at low overpotentials on oxygen-deficient In2O3 plates decorated with single atom CdO5 that have a weak N2-binding capability. Adsorbed *H is calculated to be first produced via the Volmer reaction (H2O + e− → *H + OH−) and then reacts with dissolved N2 to generate *N2H2, which is likely the rate determining step (RDS) of the whole process. Cd atoms and oxygen vacancies in In2O3 jointly enhance the activation of N2 and accelerate the RDS, boosting the NRR. An NH3 production rate of as high as 57.5 µg h−1 mgcat−1 is attained at a mild potential, which is retained to a large extent even after 44 h of continuous polarization.

KW - electrocatalyses

KW - N reduction

KW - NH

KW - reaction mechanisms

KW - single-atom catalysts

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DO - 10.1002/adfm.202209843

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