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<p>Systems that sequentially capture and upgrade CO<sub>2</sub> from air to fuels/fuel-intermediates, such as syngas and ethylene, rely on an energy-intensive CO<sub>2</sub> release process. Electrified reactive capture systems transform CO<sub>2</sub> obtained directly from carbonate capture liquid into products. Previous reactive capture systems show a decline in Faradaic efficiencies (FE) at current densities above 200 mA/cm<sup>2</sup>. Here we show the chemical origins of this problem, finding that prior electrocatalyst designs failed to arrest, activate, and reduce in situ-generated CO<sub>2</sub> (<i>i</i>-CO<sub>2</sub>) before it traversed the catalyst layer and entered the tailgas stream. We develop a templated synthesis to define pore structures and the sites of Ni single atoms, and find that carbon-nitrogen-based nanopores are effective in accumulating <i>i</i>-CO<sub>2</sub> via short-range, non-electrostatic interactions between CO<sub>2</sub> molecules and the nanochannel walls. These interactions confine and enrich <i>i</i>-CO<sub>2</sub> within the pores, enhancing its binding and activation. We report as a result carbonate electrolysis at 300 mA/cm<sup>2</sup> with FE to CO of 50% ± 3%, and with &lt;1% CO<sub>2</sub> in the tailgas outlet stream. This corresponds to a projected energy efficiency (EE) to 2:1 syngas of 46% at 300 mA/cm<sup>2</sup> when H<sub>2</sub> is added using a water electrolyzer.</p>

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Interconnected nanoconfining pore networks enhance catalyst CO2 interaction in electrified reactive capture

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月4日

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  • Hengzhou Liu,
  • Lun An,
  • Peiyao Wang,
  • Christine Yu,
  • Jie Zhang,
  • Heejong Shin,
  • Bosi Peng,
  • Jiantao Li,
  • Matthew Li,
  • Hongmin An,
  • Jiaqi Yu,
  • Yuanjun Chen,
  • Peiying Wang,
  • Kug-Seung Lee,
  • Kanika Lalit,
  • Zeyan Liu,
  • Omar K. Farha,
  • Wenyu Huang,
  • Jefferson Zhe Liu,
  • Long Qi,
  • Ke Xie,
  • Edward H. Sargent

摘要

Systems that sequentially capture and upgrade CO2 from air to fuels/fuel-intermediates, such as syngas and ethylene, rely on an energy-intensive CO2 release process. Electrified reactive capture systems transform CO2 obtained directly from carbonate capture liquid into products. Previous reactive capture systems show a decline in Faradaic efficiencies (FE) at current densities above 200 mA/cm2. Here we show the chemical origins of this problem, finding that prior electrocatalyst designs failed to arrest, activate, and reduce in situ-generated CO2 (i-CO2) before it traversed the catalyst layer and entered the tailgas stream. We develop a templated synthesis to define pore structures and the sites of Ni single atoms, and find that carbon-nitrogen-based nanopores are effective in accumulating i-CO2 via short-range, non-electrostatic interactions between CO2 molecules and the nanochannel walls. These interactions confine and enrich i-CO2 within the pores, enhancing its binding and activation. We report as a result carbonate electrolysis at 300 mA/cm2 with FE to CO of 50% ± 3%, and with <1% CO2 in the tailgas outlet stream. This corresponds to a projected energy efficiency (EE) to 2:1 syngas of 46% at 300 mA/cm2 when H2 is added using a water electrolyzer.