Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas

Fangqi Yang; Caihong Liang; Weizhen Zhou; Wendi Zhao; Pengfei Li; Zhengyu Hua; Haoming Yu; Shixia Chen; Shuguang Deng; Jing Li; Yeng Ming Lam; Jun Wang

doi:10.1002/smll.202300417

Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas

Fangqi Yang, Caihong Liang, Weizhen Zhou, Wendi Zhao, Pengfei Li, Zhengyu Hua, Haoming Yu, Shixia Chen, Shuguang Deng, Jing Li, Yeng Ming Lam, Jun Wang

Engineering, Ira A. Fulton Schools of (IAFSE)

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

Abstract

Post-combustion flue gas (mainly containing 5–40% CO₂ balanced by N₂) accounts for about 60% global CO₂ emission. Rational conversion of flue gas into value-added chemicals is still a formidable challenge. Herein, this work reports a β-Bi₂O₃-derived bismuth (OD-Bi) catalyst with surface coordinated oxygen for efficient electroreduction of pure CO₂, N_2, and flue gas. During pure CO₂ electroreduction, the maximum Faradaic efficiency (FE) of formate reaches 98.0% and stays above 90% in a broad potential of 600 mV with a long-term stability of 50 h. Additionally, OD-Bi achieves an ammonia (NH₃) FE of 18.53% and yield rate of 11.5 µg h⁻¹ mg_cat⁻¹ in pure N₂ atmosphere. Noticeably, in simulated flue gas (15% CO₂ balanced by N₂ with trace impurities), a maximum formate FE of 97.3% is delivered within a flow cell, meanwhile above 90% formate FEs are obtained in a wide potential range of 700 mV. In-situ Raman combined with theory calculations reveals that the surface coordinated oxygen species in OD-Bi can drastically activate CO₂ and N₂ molecules by selectively favors the adsorption of *OCHO and *NNH intermediates, respectively. This work provides a surface oxygen modulation strategy to develop efficient bismuth-based electrocatalysts for directly reducing commercially relevant flue gas into valuable chemicals.

Original language	English (US)
Journal	Small
DOIs	https://doi.org/10.1002/smll.202300417
State	Accepted/In press - 2023

Keywords

bismuth
CO reduction
electrocatalysts
flue gas reduction
N reduction

ASJC Scopus subject areas

Biotechnology
Chemistry(all)
Biomaterials
Materials Science(all)

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10.1002/smll.202300417

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@article{30904efea0064d6c92349c1cb6945f0b,

title = "Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas",

abstract = "Post-combustion flue gas (mainly containing 5–40% CO2 balanced by N2) accounts for about 60% global CO2 emission. Rational conversion of flue gas into value-added chemicals is still a formidable challenge. Herein, this work reports a β-Bi2O3-derived bismuth (OD-Bi) catalyst with surface coordinated oxygen for efficient electroreduction of pure CO2, N2, and flue gas. During pure CO2 electroreduction, the maximum Faradaic efficiency (FE) of formate reaches 98.0% and stays above 90% in a broad potential of 600 mV with a long-term stability of 50 h. Additionally, OD-Bi achieves an ammonia (NH3) FE of 18.53% and yield rate of 11.5 µg h−1 mgcat−1 in pure N2 atmosphere. Noticeably, in simulated flue gas (15% CO2 balanced by N2 with trace impurities), a maximum formate FE of 97.3% is delivered within a flow cell, meanwhile above 90% formate FEs are obtained in a wide potential range of 700 mV. In-situ Raman combined with theory calculations reveals that the surface coordinated oxygen species in OD-Bi can drastically activate CO2 and N2 molecules by selectively favors the adsorption of *OCHO and *NNH intermediates, respectively. This work provides a surface oxygen modulation strategy to develop efficient bismuth-based electrocatalysts for directly reducing commercially relevant flue gas into valuable chemicals.",

keywords = "bismuth, CO reduction, electrocatalysts, flue gas reduction, N reduction",

author = "Fangqi Yang and Caihong Liang and Weizhen Zhou and Wendi Zhao and Pengfei Li and Zhengyu Hua and Haoming Yu and Shixia Chen and Shuguang Deng and Jing Li and Lam, {Yeng Ming} and Jun Wang",

note = "Funding Information: This research work was supported by the National Natural Science Foundation of China (No. 21908090, 22108243, 22168023, and 22272004) and the Natural Science Foundation of Jiangxi Province (No. 20212BAB213038). F. Yang acknowledges the 2020 Nanchang University Scholarship for Doctoral Visiting Abroad. Y. M. Lam acknowledges the financial support from Ministry of Education (MOE), Singapore (MOE‐T2‐1‐085, MOE‐T1‐RG98/19). J. Li acknowledges the support from the Fundamental Research Funds for the Central Universities (YWF‐22‐L‐1256). The authors acknowledge the use of high‐performance computing facilities in National Supercomputing Centre Singapore and Nanyang Technological University High Performance Computing Centre for the DFT computations performed in this work. F. Yang and C. Liang thank Dr. Yonglu Li (College of Biosystems Engineering and Food Science, Zhejiang University) for assistance with the experiments. Publisher Copyright: {\textcopyright} 2023 Wiley-VCH GmbH.",

year = "2023",

doi = "10.1002/smll.202300417",

language = "English (US)",

journal = "Small",

issn = "1613-6810",

publisher = "Wiley-VCH Verlag",

}

TY - JOUR

T1 - Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas

AU - Yang, Fangqi

AU - Liang, Caihong

AU - Zhou, Weizhen

AU - Zhao, Wendi

AU - Li, Pengfei

AU - Hua, Zhengyu

AU - Yu, Haoming

AU - Chen, Shixia

AU - Deng, Shuguang

AU - Li, Jing

AU - Lam, Yeng Ming

AU - Wang, Jun

N1 - Funding Information: This research work was supported by the National Natural Science Foundation of China (No. 21908090, 22108243, 22168023, and 22272004) and the Natural Science Foundation of Jiangxi Province (No. 20212BAB213038). F. Yang acknowledges the 2020 Nanchang University Scholarship for Doctoral Visiting Abroad. Y. M. Lam acknowledges the financial support from Ministry of Education (MOE), Singapore (MOE‐T2‐1‐085, MOE‐T1‐RG98/19). J. Li acknowledges the support from the Fundamental Research Funds for the Central Universities (YWF‐22‐L‐1256). The authors acknowledge the use of high‐performance computing facilities in National Supercomputing Centre Singapore and Nanyang Technological University High Performance Computing Centre for the DFT computations performed in this work. F. Yang and C. Liang thank Dr. Yonglu Li (College of Biosystems Engineering and Food Science, Zhejiang University) for assistance with the experiments. Publisher Copyright: © 2023 Wiley-VCH GmbH.

PY - 2023

Y1 - 2023

N2 - Post-combustion flue gas (mainly containing 5–40% CO2 balanced by N2) accounts for about 60% global CO2 emission. Rational conversion of flue gas into value-added chemicals is still a formidable challenge. Herein, this work reports a β-Bi2O3-derived bismuth (OD-Bi) catalyst with surface coordinated oxygen for efficient electroreduction of pure CO2, N2, and flue gas. During pure CO2 electroreduction, the maximum Faradaic efficiency (FE) of formate reaches 98.0% and stays above 90% in a broad potential of 600 mV with a long-term stability of 50 h. Additionally, OD-Bi achieves an ammonia (NH3) FE of 18.53% and yield rate of 11.5 µg h−1 mgcat−1 in pure N2 atmosphere. Noticeably, in simulated flue gas (15% CO2 balanced by N2 with trace impurities), a maximum formate FE of 97.3% is delivered within a flow cell, meanwhile above 90% formate FEs are obtained in a wide potential range of 700 mV. In-situ Raman combined with theory calculations reveals that the surface coordinated oxygen species in OD-Bi can drastically activate CO2 and N2 molecules by selectively favors the adsorption of *OCHO and *NNH intermediates, respectively. This work provides a surface oxygen modulation strategy to develop efficient bismuth-based electrocatalysts for directly reducing commercially relevant flue gas into valuable chemicals.

AB - Post-combustion flue gas (mainly containing 5–40% CO2 balanced by N2) accounts for about 60% global CO2 emission. Rational conversion of flue gas into value-added chemicals is still a formidable challenge. Herein, this work reports a β-Bi2O3-derived bismuth (OD-Bi) catalyst with surface coordinated oxygen for efficient electroreduction of pure CO2, N2, and flue gas. During pure CO2 electroreduction, the maximum Faradaic efficiency (FE) of formate reaches 98.0% and stays above 90% in a broad potential of 600 mV with a long-term stability of 50 h. Additionally, OD-Bi achieves an ammonia (NH3) FE of 18.53% and yield rate of 11.5 µg h−1 mgcat−1 in pure N2 atmosphere. Noticeably, in simulated flue gas (15% CO2 balanced by N2 with trace impurities), a maximum formate FE of 97.3% is delivered within a flow cell, meanwhile above 90% formate FEs are obtained in a wide potential range of 700 mV. In-situ Raman combined with theory calculations reveals that the surface coordinated oxygen species in OD-Bi can drastically activate CO2 and N2 molecules by selectively favors the adsorption of *OCHO and *NNH intermediates, respectively. This work provides a surface oxygen modulation strategy to develop efficient bismuth-based electrocatalysts for directly reducing commercially relevant flue gas into valuable chemicals.

KW - bismuth

KW - CO reduction

KW - electrocatalysts

KW - flue gas reduction

KW - N reduction

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U2 - 10.1002/smll.202300417

DO - 10.1002/smll.202300417

M3 - Article

AN - SCOPUS:85151952424

SN - 1613-6810

JO - Small

JF - Small

ER -

Oxide-Derived Bismuth as an Efficient Catalyst for Electrochemical Reduction of Flue Gas

Abstract

Keywords

ASJC Scopus subject areas

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