Efficient amino-acid-based reactive capture of CO2 via nickel molecular catalyst

Reactive capture integrates CO<sub>2</sub> capture and electrochemical conversion into CO - a key building block in the synthesis of industrial chemicals and fuels - avoiding costly regeneration steps and improving efficiency. Amino acid salt solutions, which offer rapid CO<sub>2</sub> capture, facile CO<sub>2</sub> release, O<sub>2</sub> tolerance, and low toxicity, are promising sorbents for reactive capture. However, we find that amino acids can adsorb to common CO-producing catalysts, covering the active sites and deactivating the catalyst, and that they bind less to nickel phthalocyanine (NiPc). Still, when tested for reactive capture systems - where CO<sub>2</sub> supply is inherently limited - NiPc's performance is constrained by its weak CO<sub>2</sub> adsorption and activation. Here we develop a nickel molecular catalyst supported on carbon nanotubes with a conjugated NiPc framework that resists amino acid adsorption and a coordinatively unsaturated Ni-N<sub>3</sub> structure that promotes CO<sub>2</sub> adsorption and enhances CO selectivity. As a result, we achieve 94% CO Faradaic efficiency at 100 mA cm<sup>-2</sup> with an energy efficiency of 42% and an energy cost of 25 GJ t<sub>CO</sub><sup>-1</sup>.

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Publication Details

Journal
Nature Communications
Published
2025-11-24
DOI
https://doi.org/10.1038/s41467-025-65331-9
Citations
2
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
0.73

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article

Efficient amino-acid-based reactive capture of CO2 via nickel molecular catalyst

Yurou Celine Xiao, Zahra Azimi Dijvejin, Paul J. Corbett, Mengyang Fan et al.
2 citations
Nature Communications
CO2 Reduction Techniques and Catalysts
0.73
article

Efficient amino-acid-based reactive capture of CO2 via nickel molecular catalyst

Yurou Celine Xiao, Zahra Azimi Dijvejin, Paul J. Corbett, Mengyang Fan, Jieyuan Liu, Rui Kai Miao, Panagiotis Papangelakis, Drew Higgins, Sung‐Fu Hung, Siyu Sonia Sun, Ali Shayesteh Zeraati, Zunmin Guo, David Sinton, Yuanyuan Che, Ying‐Rui Lu, Kai Han, Amir Foroozan, Yucheng Liu, Yong Wang, Shijie Liu, Feng Li, Min Liu, Yuke Li, Cai Wang, Qiyou Wang, Kang‐Shun Peng
article en
2 citations

Abstract

Reactive capture integrates CO<sub>2</sub> capture and electrochemical conversion into CO - a key building block in the synthesis of industrial chemicals and fuels - avoiding costly regeneration steps and improving efficiency. Amino acid salt solutions, which offer rapid CO<sub>2</sub> capture, facile CO<sub>2</sub> release, O<sub>2</sub> tolerance, and low toxicity, are promising sorbents for reactive capture. However, we find that amino acids can adsorb to common CO-producing catalysts, covering the active sites and deactivating the catalyst, and that they bind less to nickel phthalocyanine (NiPc). Still, when tested for reactive capture systems - where CO<sub>2</sub> supply is inherently limited - NiPc's performance is constrained by its weak CO<sub>2</sub> adsorption and activation. Here we develop a nickel molecular catalyst supported on carbon nanotubes with a conjugated NiPc framework that resists amino acid adsorption and a coordinatively unsaturated Ni-N<sub>3</sub> structure that promotes CO<sub>2</sub> adsorption and enhances CO selectivity. As a result, we achieve 94% CO Faradaic efficiency at 100 mA cm<sup>-2</sup> with an energy efficiency of 42% and an energy cost of 25 GJ t<sub>CO</sub><sup>-1</sup>.

Nature CommunicationsVol. 16(1)
National Yang Ming Chiao Tung University (TW), University of Toronto (CA), National Synchrotron Radiation Research Center (TW), Shell (Netherlands) (NL), McMaster University (CA)
Shell, McMaster University, Shell Global Solutions International, Government of Canada, Canada Research Chairs, Natural Sciences and Engineering Research Council of Canada
Openalex Percentile: Top 27%
CO2 Reduction Techniques and Catalysts
0.73
DOIOpen Access PDFOpenAlex
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