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<p>Transforming CO<sub>2</sub> into valuable products presents a promising route for reducing emissions across various industry sectors. However, conventional methods, including sequential CO<sub>2</sub> electrolysis or reverse water–gas shift reaction, depend on energy-intensive CO<sub>2</sub> purification; while emerging reactive CO<sub>2</sub> capture strategies still face challenges in designing optimal system components that enable efficient electrochemical regeneration without compromising catalytic performance. Here we systematically screen a broad library of amine-based absorbents to establish a design rationale for tandem amine scrubbing and CO<sub>2</sub> electrolysis. We identify piperazine as an optimal capture medium and show that its carbamate form can be directly reduced using a nickel single-atom catalyst. This charge-neutral intermediate facilitates spontaneous adsorption, rapid transport and efficient C–N bond cleavage, enabling stable carbon monoxide production alongside in situ amine regeneration. The process achieves an energy efficiency of ~48.8 GJ per tonne CO, offering a scalable and energy efficient pathway towards carbon-neutral chemical feedstocks.</p>

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Tandem amine scrubbing and CO2 electrolysis via direct piperazine carbamate reduction

  • 期刊论文

  • 发表日期：

    2025年9月11日

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  • Peng Li,
  • Yu Mao,
  • Heejong Shin,
  • Qi Yang,
  • Xuan Cheng,
  • Yitong Li,
  • Kangkang Li,
  • Hai Yu,
  • Roger Mulder,
  • Wei Kong Pang,
  • Huanyu Jin,
  • Yong Zhao,
  • Zhi Zheng,
  • Emily Finch,
  • Kyle Hearn,
  • Baohua Jia,
  • Geoffrey I. N. Waterhouse,
  • Ziyun Wang,
  • Tianyi Ma

摘要

Transforming CO2 into valuable products presents a promising route for reducing emissions across various industry sectors. However, conventional methods, including sequential CO2 electrolysis or reverse water–gas shift reaction, depend on energy-intensive CO2 purification; while emerging reactive CO2 capture strategies still face challenges in designing optimal system components that enable efficient electrochemical regeneration without compromising catalytic performance. Here we systematically screen a broad library of amine-based absorbents to establish a design rationale for tandem amine scrubbing and CO2 electrolysis. We identify piperazine as an optimal capture medium and show that its carbamate form can be directly reduced using a nickel single-atom catalyst. This charge-neutral intermediate facilitates spontaneous adsorption, rapid transport and efficient C–N bond cleavage, enabling stable carbon monoxide production alongside in situ amine regeneration. The process achieves an energy efficiency of ~48.8 GJ per tonne CO, offering a scalable and energy efficient pathway towards carbon-neutral chemical feedstocks.