A scalable solid-state nanoporous network with atomic-level interaction design for carbon dioxide capture

Mao, Haiyan; Tang, Jing; Day, Gregory S.; Peng, Yucan; Wang, Haoze; Xiao, Xin; Yang, Yufei; Jiang, Yuanwen; Chen, Shuo; Halat, David M.; Lund, Alicia; Lv, Xudong; Zhang, Wenbo; Yang, Chongqing; Lin, Zhou; Zhou, Hong-Cai; Pines, Alexander; Cui, Yi; Reimer, Jeffrey A.

doi:10.1126/sciadv.abo6849

DOE OSTI · 1886938

A scalable solid-state nanoporous network with atomic-level interaction design for carbon dioxide capture

Mao, Haiyan·Tang, Jing·Day, Gregory S.·Peng, Yucan·Wang, Haoze·Xiao, Xin·Yang, Yufei·Jiang, Yuanwen·Chen, Shuo·Halat, David M.·Lund, Alicia·Lv, Xudong·Zhang, Wenbo·Yang, Chongqing·Lin, Zhou·Zhou, Hong-Cai·Pines, Alexander·Cui, Yi·Reimer, Jeffrey A.

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Abstract

Carbon capture and sequestration reduces carbon dioxide emissions and is critical in accomplishing carbon neutrality targets. Here, we demonstrate new sustainable, solid-state, polyamine-appended, cyanuric acid–stabilized melamine nanoporous networks (MNNs) via dynamic combinatorial chemistry (DCC) at the kilogram scale toward effective and high-capacity carbon dioxide capture. Polyamine-appended MNNs reaction mechanisms with carbon dioxide were elucidated with double-level DCC where two-dimensional heteronuclear chemical shift correlation nuclear magnetic resonance spectroscopy was performed to demonstrate the interatomic interactions. We distinguished ammonium carbamate pairs and a mix of ammonium carbamate and carbamic acid during carbon dioxide chemisorption. The coordination of polyamine and cyanuric acid modification endows MNNs with high adsorption capacity (1.82 millimoles per gram at 1 bar), fast adsorption time (less than 1 minute), low price, and extraordinary stability to cycling by flue gas. This work creates a general industrialization method toward carbon dioxide capture via DCC atomic-level design strategies.

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Mao, Haiyan, Tang, Jing, Day, Gregory S., Peng, Yucan, Wang, Haoze, Xiao, Xin, Yang, Yufei, Jiang, Yuanwen, Chen, Shuo, Halat, David M., Lund, Alicia, Lv, Xudong, Zhang, Wenbo, Yang, Chongqing, Lin, Zhou, Zhou, Hong-Cai, Pines, Alexander, Cui, Yi, Reimer, Jeffrey A.. 2022-08-03. A scalable solid-state nanoporous network with atomic-level interaction design for carbon dioxide capture. https://doi.org/10.1126/sciadv.abo6849

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