Boron-Modulated Electronic-Configuration Tuning of Cobalt for Enhanced Nitric Oxide Fixation to Ammonia

Bichao Wu; Lei Huang; Lvji Yan; Haiyin Gang; Yiyun Cao; Dun Wei; Haiying Wang; Zaiping Guo; Wenchao Zhang

doi:10.1021/acs.nanolett.3c01994

Boron-Modulated Electronic-Configuration Tuning of Cobalt for Enhanced Nitric Oxide Fixation to Ammonia

Bichao Wu, Lei Huang, Lvji Yan, Haiyin Gang, Yiyun Cao, Dun Wei, Haiying Wang^*, Zaiping Guo^*, Wenchao Zhang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

30 Citations (Scopus)

Abstract

Electrocatalytic nitric oxide reduction (eNORR) to ammonia (NH₃) provides an environmental route to alleviate NO pollution and yield great-value chemicals. The evolution of eNORR has been primarily hindered, however, by the poor reaction kinetics and low solubility of the NO in aqueous electrolytes. Herein, we have rationally designed a cobalt-based composite with a heterostructure as a highly efficient eNORR catalyst. In addition, by integrating boron to modulate the electronic structure, the catalyst CoB/Co@C delivered a significant NH₃ yield of 315.4 μmol h^-1 cm^-2 for eNORR and an outstanding power density of 3.68 mW cm^-2 in a Zn-NO battery. The excellent electrochemical performance of CoB/Co@C is attributed to the enrichment of NO by cobalt and boron dual-site adsorption and fast charge-transfer kinetics. It is demonstrated that the boron is pivotal in the enhancement of NO, the suppression of hydrogen evolution, and Co oxidation to boost eNORR performance. © 2023 American Chemical Society.

Original language	English
Pages (from-to)	7120-7128
Journal	Nano Letters
Volume	23
Issue number	15
Online published	25 Jul 2023
DOIs	https://doi.org/10.1021/acs.nanolett.3c01994
Publication status	Published - 9 Aug 2023
Externally published	Yes

Funding

This work was supported by the National Key Research and Development Program of China (2020YFC1909200, 2022YFC3900200), the National Natural Science Foundation of China (52104315), and the Hunan Provincial Science and Technology Innovation Leading Talent Program (2021RC4010).

Research Keywords

ammonia production
boron modulation
NO enrichment
NO reduction reaction

UN SDGs

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

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abstract = "Electrocatalytic nitric oxide reduction (eNORR) to ammonia (NH3) provides an environmental route to alleviate NO pollution and yield great-value chemicals. The evolution of eNORR has been primarily hindered, however, by the poor reaction kinetics and low solubility of the NO in aqueous electrolytes. Herein, we have rationally designed a cobalt-based composite with a heterostructure as a highly efficient eNORR catalyst. In addition, by integrating boron to modulate the electronic structure, the catalyst CoB/Co@C delivered a significant NH3 yield of 315.4 μmol h-1 cm-2 for eNORR and an outstanding power density of 3.68 mW cm-2 in a Zn-NO battery. The excellent electrochemical performance of CoB/Co@C is attributed to the enrichment of NO by cobalt and boron dual-site adsorption and fast charge-transfer kinetics. It is demonstrated that the boron is pivotal in the enhancement of NO, the suppression of hydrogen evolution, and Co oxidation to boost eNORR performance. {\textcopyright} 2023 American Chemical Society.",

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year = "2023",

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doi = "10.1021/acs.nanolett.3c01994",

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T1 - Boron-Modulated Electronic-Configuration Tuning of Cobalt for Enhanced Nitric Oxide Fixation to Ammonia

AU - Wu, Bichao

AU - Huang, Lei

AU - Yan, Lvji

AU - Gang, Haiyin

AU - Cao, Yiyun

AU - Wei, Dun

AU - Wang, Haiying

AU - Guo, Zaiping

AU - Zhang, Wenchao

PY - 2023/8/9

Y1 - 2023/8/9

N2 - Electrocatalytic nitric oxide reduction (eNORR) to ammonia (NH3) provides an environmental route to alleviate NO pollution and yield great-value chemicals. The evolution of eNORR has been primarily hindered, however, by the poor reaction kinetics and low solubility of the NO in aqueous electrolytes. Herein, we have rationally designed a cobalt-based composite with a heterostructure as a highly efficient eNORR catalyst. In addition, by integrating boron to modulate the electronic structure, the catalyst CoB/Co@C delivered a significant NH3 yield of 315.4 μmol h-1 cm-2 for eNORR and an outstanding power density of 3.68 mW cm-2 in a Zn-NO battery. The excellent electrochemical performance of CoB/Co@C is attributed to the enrichment of NO by cobalt and boron dual-site adsorption and fast charge-transfer kinetics. It is demonstrated that the boron is pivotal in the enhancement of NO, the suppression of hydrogen evolution, and Co oxidation to boost eNORR performance. © 2023 American Chemical Society.

AB - Electrocatalytic nitric oxide reduction (eNORR) to ammonia (NH3) provides an environmental route to alleviate NO pollution and yield great-value chemicals. The evolution of eNORR has been primarily hindered, however, by the poor reaction kinetics and low solubility of the NO in aqueous electrolytes. Herein, we have rationally designed a cobalt-based composite with a heterostructure as a highly efficient eNORR catalyst. In addition, by integrating boron to modulate the electronic structure, the catalyst CoB/Co@C delivered a significant NH3 yield of 315.4 μmol h-1 cm-2 for eNORR and an outstanding power density of 3.68 mW cm-2 in a Zn-NO battery. The excellent electrochemical performance of CoB/Co@C is attributed to the enrichment of NO by cobalt and boron dual-site adsorption and fast charge-transfer kinetics. It is demonstrated that the boron is pivotal in the enhancement of NO, the suppression of hydrogen evolution, and Co oxidation to boost eNORR performance. © 2023 American Chemical Society.

KW - ammonia production

KW - boron modulation

KW - NO enrichment

KW - NO reduction reaction

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Boron-Modulated Electronic-Configuration Tuning of Cobalt for Enhanced Nitric Oxide Fixation to Ammonia

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