Interconnected nanoconfining pore networks enhance catalyst CO 2 interaction in electrified reactive capture

Liu, Hengzhou [Northwestern Univ., Evanston, IL (United States)]; An, Lun [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)]; Wang, Peiyao [Univ. of Melbourne, Parkville, VIC (Australia)] (ORCID:0000000304064952); Yu, Christine [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000247200363); Zhang, Jie [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)]; Shin, Heejong [Northwestern Univ., Evanston, IL (United States)]; Peng, Bosi [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000193025925); Li, Jiantao [Northwestern Univ., Evanston, IL (United States)]; Li, Matthew [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000190933207); An, Hongmin [Northwestern Univ., Evanston, IL (United States)]; Yu, Jiaqi [Northwestern Univ., Evanston, IL (United States)]; Chen, Yuanjun [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000215603854); Wang, Peiying [Northwestern Univ., Evanston, IL (United States)]; Lee, Kug-Seung [Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)] (ORCID:0000000275708404); Lalit, Kanika [Iowa State Univ., Ames, IA (United States)]; Liu, Zeyan [Northwestern Univ., Evanston, IL (United States)]; Farha, Omar K. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000299049845); Huang, Wenyu [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000323277259); Liu, Jefferson Zhe [Univ. of Melbourne, Parkville, VIC (Australia)] (ORCID:0000000252827945); Qi, Long [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000212132946); Xie, Ke [Northwestern Univ., Evanston, IL (United States)] (ORCID:000000034220272X); Sargent, Edward H. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000303966495)

doi:10.1038/s41467-025-61407-8

DOE OSTI · 2573066

Interconnected nanoconfining pore networks enhance catalyst CO 2 interaction in electrified reactive capture

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Abstract

Systems that sequentially capture and upgrade CO 2 from air to fuels/fuel-intermediates, such as syngas and ethylene, rely on an energy-intensive CO 2 release process. Electrified reactive capture systems transform CO 2 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 2 . Here we show the chemical origins of this problem, finding that prior electrocatalyst designs failed to arrest, activate, and reduce in situ-generated CO 2 (i-CO 2 ) 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-CO 2 via short-range, non-electrostatic interactions between CO 2 molecules and the nanochannel walls. These interactions confine and enrich i-CO 2 within the pores, enhancing its binding and activation. We report as a result carbonate electrolysis at 300 mA/cm 2 with FE to CO of 50% ± 3%, and with <1% CO 2 in the tailgas outlet stream. This corresponds to a projected energy efficiency (EE) to 2:1 syngas of 46% at 300 mA/cm 2 when H 2 is added using a water electrolyzer.

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Liu, Hengzhou [Northwestern Univ., Evanston, IL (United States)], An, Lun [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)], Wang, Peiyao [Univ. of Melbourne, Parkville, VIC (Australia)] (ORCID:0000000304064952), Yu, Christine [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000247200363), Zhang, Jie [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)], Shin, Heejong [Northwestern Univ., Evanston, IL (United States)], Peng, Bosi [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000193025925), Li, Jiantao [Northwestern Univ., Evanston, IL (United States)], Li, Matthew [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000190933207), An, Hongmin [Northwestern Univ., Evanston, IL (United States)], Yu, Jiaqi [Northwestern Univ., Evanston, IL (United States)], Chen, Yuanjun [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000215603854), Wang, Peiying [Northwestern Univ., Evanston, IL (United States)], Lee, Kug-Seung [Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)] (ORCID:0000000275708404), Lalit, Kanika [Iowa State Univ., Ames, IA (United States)], Liu, Zeyan [Northwestern Univ., Evanston, IL (United States)], Farha, Omar K. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000299049845), Huang, Wenyu [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000323277259), Liu, Jefferson Zhe [Univ. of Melbourne, Parkville, VIC (Australia)] (ORCID:0000000252827945), Qi, Long [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000212132946), Xie, Ke [Northwestern Univ., Evanston, IL (United States)] (ORCID:000000034220272X), Sargent, Edward H. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000303966495). 2025-07-04. Interconnected nanoconfining pore networks enhance catalyst CO 2 interaction in electrified reactive capture. https://doi.org/10.1038/s41467-025-61407-8

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