Boosting Electrocatalytic Ammonia Production through Mimicking “π Back-Donation”

Chade Lv; Lixiang Zhong; Yao Yao; Daobin Liu; Yi Kong; Xiaoli Jin; Zhiwei Fang; Wenjie Xu; Chunshuang Yan; Khang Ngoc Dinh; Minhua Shao; Li Song; Gang Chen; Shuzhou Li; Qingyu Yan; Guihua Yu

doi:10.1016/j.chempr.2020.07.006

Boosting Electrocatalytic Ammonia Production through Mimicking “π Back-Donation”

Chade Lv, Lixiang Zhong, Yao Yao, Daobin Liu, Yi Kong, Xiaoli Jin, Zhiwei Fang, Wenjie Xu, Chunshuang Yan, Khang Ngoc Dinh, Minhua Shao, Li Song, Gang Chen, Shuzhou Li, Qingyu Yan^*, Guihua Yu^*

^*Corresponding author for this work

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

123 Citations (Scopus)

Abstract

Electrocatalytic dinitrogen reduction reaction (N₂RR) is an emerging route for ammonia synthesis at ambient conditions. Albeit the “π back-donation” process enables N₂RR activity on transition metals with empty d-orbitals, given its dilemma in overcoming hydrogen evolution reaction (HER) competition, exploring p-block-element-based catalysts with relatively inferior HER activity is achievable for high selectivity. The challenge lies in designing rational structure to improve N₂RR activity. Here, we synergistically integrate oxygen vacancy (V_O) with hydroxyl on Bi₄O₅I₂ (V_O-Bi₄O₅I₂-OH), which render this p-block-element-based material active to mimic “π back-donation” behavior because of sufficient vacant orbitals. In neutral media, the electrocatalytic N₂RR performance of V_O-Bi₄O₅I₂-OH in terms of splendid faradic efficiency (32.4%) is superior to most of the prior reports using p-block-element-based catalysts. Our findings show a new strategy toward standout N₂RR activity, which holds great potential in exploiting other p-block-element-based electrocatalysts.

Original language	English
Pages (from-to)	2690-2702
Number of pages	13
Journal	Chem
Volume	6
Issue number	10
DOIs	https://doi.org/10.1016/j.chempr.2020.07.006
Publication status	Published - Oct 8 2020
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2020 Elsevier Inc.

ASJC Scopus Subject Areas

General Chemistry
Biochemistry
Environmental Chemistry
General Chemical Engineering
Biochemistry, medical
Materials Chemistry

Keywords

ammonia synthesis
electrocatalysis
mimicking “π back-donation”
N reduction reaction (NRR)
p-block-element catalysts
SDG7: Affordable and clean energy

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10.1016/j.chempr.2020.07.006

Cite this

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title = "Boosting Electrocatalytic Ammonia Production through Mimicking “π Back-Donation”",

abstract = "Electrocatalytic dinitrogen reduction reaction (N2RR) is an emerging route for ammonia synthesis at ambient conditions. Albeit the “π back-donation” process enables N2RR activity on transition metals with empty d-orbitals, given its dilemma in overcoming hydrogen evolution reaction (HER) competition, exploring p-block-element-based catalysts with relatively inferior HER activity is achievable for high selectivity. The challenge lies in designing rational structure to improve N2RR activity. Here, we synergistically integrate oxygen vacancy (VO) with hydroxyl on Bi4O5I2 (VO-Bi4O5I2-OH), which render this p-block-element-based material active to mimic “π back-donation” behavior because of sufficient vacant orbitals. In neutral media, the electrocatalytic N2RR performance of VO-Bi4O5I2-OH in terms of splendid faradic efficiency (32.4%) is superior to most of the prior reports using p-block-element-based catalysts. Our findings show a new strategy toward standout N2RR activity, which holds great potential in exploiting other p-block-element-based electrocatalysts.",

keywords = "ammonia synthesis, electrocatalysis, mimicking “π back-donation”, N reduction reaction (NRR), p-block-element catalysts, SDG7: Affordable and clean energy",

author = "Chade Lv and Lixiang Zhong and Yao Yao and Daobin Liu and Yi Kong and Xiaoli Jin and Zhiwei Fang and Wenjie Xu and Chunshuang Yan and Dinh, {Khang Ngoc} and Minhua Shao and Li Song and Gang Chen and Shuzhou Li and Qingyu Yan and Guihua Yu",

note = "Publisher Copyright: {\textcopyright} 2020 Elsevier Inc.",

year = "2020",

month = oct,

day = "8",

doi = "10.1016/j.chempr.2020.07.006",

language = "English",

volume = "6",

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T1 - Boosting Electrocatalytic Ammonia Production through Mimicking “π Back-Donation”

AU - Lv, Chade

AU - Zhong, Lixiang

AU - Yao, Yao

AU - Liu, Daobin

AU - Kong, Yi

AU - Jin, Xiaoli

AU - Fang, Zhiwei

AU - Xu, Wenjie

AU - Yan, Chunshuang

AU - Dinh, Khang Ngoc

AU - Shao, Minhua

AU - Song, Li

AU - Chen, Gang

AU - Li, Shuzhou

AU - Yan, Qingyu

AU - Yu, Guihua

PY - 2020/10/8

Y1 - 2020/10/8

N2 - Electrocatalytic dinitrogen reduction reaction (N2RR) is an emerging route for ammonia synthesis at ambient conditions. Albeit the “π back-donation” process enables N2RR activity on transition metals with empty d-orbitals, given its dilemma in overcoming hydrogen evolution reaction (HER) competition, exploring p-block-element-based catalysts with relatively inferior HER activity is achievable for high selectivity. The challenge lies in designing rational structure to improve N2RR activity. Here, we synergistically integrate oxygen vacancy (VO) with hydroxyl on Bi4O5I2 (VO-Bi4O5I2-OH), which render this p-block-element-based material active to mimic “π back-donation” behavior because of sufficient vacant orbitals. In neutral media, the electrocatalytic N2RR performance of VO-Bi4O5I2-OH in terms of splendid faradic efficiency (32.4%) is superior to most of the prior reports using p-block-element-based catalysts. Our findings show a new strategy toward standout N2RR activity, which holds great potential in exploiting other p-block-element-based electrocatalysts.

AB - Electrocatalytic dinitrogen reduction reaction (N2RR) is an emerging route for ammonia synthesis at ambient conditions. Albeit the “π back-donation” process enables N2RR activity on transition metals with empty d-orbitals, given its dilemma in overcoming hydrogen evolution reaction (HER) competition, exploring p-block-element-based catalysts with relatively inferior HER activity is achievable for high selectivity. The challenge lies in designing rational structure to improve N2RR activity. Here, we synergistically integrate oxygen vacancy (VO) with hydroxyl on Bi4O5I2 (VO-Bi4O5I2-OH), which render this p-block-element-based material active to mimic “π back-donation” behavior because of sufficient vacant orbitals. In neutral media, the electrocatalytic N2RR performance of VO-Bi4O5I2-OH in terms of splendid faradic efficiency (32.4%) is superior to most of the prior reports using p-block-element-based catalysts. Our findings show a new strategy toward standout N2RR activity, which holds great potential in exploiting other p-block-element-based electrocatalysts.

KW - ammonia synthesis

KW - electrocatalysis

KW - mimicking “π back-donation”

KW - N reduction reaction (NRR)

KW - p-block-element catalysts

KW - SDG7: Affordable and clean energy

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Boosting Electrocatalytic Ammonia Production through Mimicking “π Back-Donation”

Abstract

Bibliographical note

ASJC Scopus Subject Areas

Keywords

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