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