Interconnected nanoconfining pore networks enhance catalyst CO2 interaction in electrified reactive capture
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 () and
Edward H. Sargent ()
Additional contact information
Hengzhou Liu: Northwestern University
Lun An: Iowa State University
Peiyao Wang: The University of Melbourne
Christine Yu: Northwestern University
Jie Zhang: Iowa State University
Heejong Shin: Northwestern University
Bosi Peng: Northwestern University
Jiantao Li: Northwestern University
Matthew Li: Argonne National Laboratory
Hongmin An: Northwestern University
Jiaqi Yu: Northwestern University
Yuanjun Chen: Northwestern University
Peiying Wang: Northwestern University
Kug-Seung Lee: Pohang University of Science and Technology (POSTECH)
Kanika Lalit: Iowa State University
Zeyan Liu: Northwestern University
Omar K. Farha: Northwestern University
Wenyu Huang: Iowa State University
Jefferson Zhe Liu: The University of Melbourne
Long Qi: Iowa State University
Ke Xie: Northwestern University
Edward H. Sargent: Northwestern University
Nature Communications, 2025, vol. 16, issue 1, 1-13
Abstract:
Abstract 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
Date: 2025
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DOI: 10.1038/s41467-025-61407-8
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