Atom-level Interaction Design Between Amines and Support for Achieving Efficient and Stable CO Capture

Overview

Journal Nat Commun

Specialty Biology

Date 2024 Jun 13

PMID 38871697

Authors

Xin Sun

Xuehua Shen

Hao Wang

Feng Yan

Jiali Hua

Guanghuan Li

Zuotai Zhang

Affiliations

Soon will be listed here.

Abstract

Amine-functionalized adsorbents offer substantial potential for CO capture owing to their selectivity and diverse application scenarios. However, their effectiveness is hindered by low efficiency and unstable cyclic performance. Here we introduce an amine-support system designed to achieve efficient and stable CO capture. Through atom-level design, each polyethyleneimine (PEI) molecule is precisely impregnated into the cage-like pore of MIL-101(Cr), forming stable composites via strong coordination with unsaturated Cr acid sites within the crystal lattice. The resulting adsorbent demonstrates a low regeneration energy (39.6 kJ/mol), excellent cyclic stability (0.18% decay per cycle under dry CO regeneration), high CO adsorption capacity (4.0 mmol/g), and rapid adsorption kinetics (15 min for saturation at 30 °C). These properties stem from the unique electron-level interaction between the amine and the support, effectively preventing carbamate products' dehydration. This work presents a feasible and promising cost-effective and sustainable CO capture strategy.

Citing Articles

Design of Ultra-Stable Solid Amine Adsorbents and Mechanisms of Hydroxyl Group-Dependent Deactivation for Reversible CO Capture from Flue Gas.

Zhao M, Huang L, Gao Y, Wang Z, Liang S, Zhu X Nanomicro Lett. 2025; 17(1):170.

PMID: 40019639 PMC: 11871205. DOI: 10.1007/s40820-025-01664-w.

Organic and Metal-Organic Polymer-Based Catalysts-Enfant Terrible Companions or Good Assistants?.

Kralik M, Koos P, Markovic M, Lopatka P Molecules. 2024; 29(19).

PMID: 39407552 PMC: 11477782. DOI: 10.3390/molecules29194623.

Atom-level interaction design between amines and support for achieving efficient and stable CO capture.

Sun X, Shen X, Wang H, Yan F, Hua J, Li G Nat Commun. 2024; 15(1):5068.

PMID: 38871697 PMC: 11176289. DOI: 10.1038/s41467-024-48994-8.

References

Rim G, Kong F, Song M, Rosu C, Priyadarshini P, Lively R . Sub-Ambient Temperature Direct Air Capture of CO using Amine-Impregnated MIL-101(Cr) Enables Ambient Temperature CO Recovery. JACS Au. 2022; 2(2):380-393. PMC: 8889612. DOI: 10.1021/jacsau.1c00414. View

Shi X, Xiao H, Azarabadi H, Song J, Wu X, Chen X . Sorbents for the Direct Capture of CO from Ambient Air. Angew Chem Int Ed Engl. 2019; 59(18):6984-7006. DOI: 10.1002/anie.201906756. View

Pang S, Lee L, Sakwa-Novak M, Lively R, Jones C . Design of Aminopolymer Structure to Enhance Performance and Stability of CO Sorbents: Poly(propylenimine) vs Poly(ethylenimine). J Am Chem Soc. 2017; 139(10):3627-3630. DOI: 10.1021/jacs.7b00235. View

Dutcher B, Fan M, Russell A . Amine-based CO2 capture technology development from the beginning of 2013-a review. ACS Appl Mater Interfaces. 2015; 7(4):2137-48. DOI: 10.1021/am507465f. View

Moon H, Carrillo J, Leisen J, Sumpter B, Osti N, Tyagi M . Understanding the Impacts of Support-Polymer Interactions on the Dynamics of Poly(ethyleneimine) Confined in Mesoporous SBA-15. J Am Chem Soc. 2022; 144(26):11664-11675. DOI: 10.1021/jacs.2c03028. View

Nguyen T, Dogan N, Lim H, Yavuz C . Amine Chemistry of Porous CO Adsorbents. Acc Chem Res. 2023; 56(19):2642-2652. DOI: 10.1021/acs.accounts.3c00367. View

Patel H, Byun J, Yavuz C . Carbon Dioxide Capture Adsorbents: Chemistry and Methods. ChemSusChem. 2016; 10(7):1303-1317. DOI: 10.1002/cssc.201601545. View

Choi W, Min K, Kim C, Ko Y, Jeon J, Seo H . Epoxide-functionalization of polyethyleneimine for synthesis of stable carbon dioxide adsorbent in temperature swing adsorption. Nat Commun. 2016; 7:12640. PMC: 5013602. DOI: 10.1038/ncomms12640. View

Lin J, Nguyen T, Vaidhyanathan R, Burner J, Taylor J, Durekova H . A scalable metal-organic framework as a durable physisorbent for carbon dioxide capture. Science. 2021; 374(6574):1464-1469. DOI: 10.1126/science.abi7281. View

10.

Siegelman R, Kim E, Long J . Porous materials for carbon dioxide separations. Nat Mater. 2021; 20(8):1060-1072. DOI: 10.1038/s41563-021-01054-8. View

11.

Ferey G, Mellot-Draznieks C, Serre C, Millange F, Dutour J, Surble S . A chromium terephthalate-based solid with unusually large pore volumes and surface area. Science. 2005; 309(5743):2040-2. DOI: 10.1126/science.1116275. View

12.

Grimme S, Antony J, Ehrlich S, Krieg H . A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J Chem Phys. 2010; 132(15):154104. DOI: 10.1063/1.3382344. View

13.

Lashaki M, Khiavi S, Sayari A . Stability of amine-functionalized CO adsorbents: a multifaceted puzzle. Chem Soc Rev. 2019; 48(12):3320-3405. DOI: 10.1039/c8cs00877a. View

14.

Lin L, Meng Y, Ju T, Han S, Meng F, Li J . Characteristics, application and modeling of solid amine adsorbents for CO capture: A review. J Environ Manage. 2022; 325(Pt A):116438. DOI: 10.1016/j.jenvman.2022.116438. View

15.

Xia R, Tian D, Kattel S, Hasa B, Shin H, Ma X . Electrochemical reduction of acetonitrile to ethylamine. Nat Commun. 2021; 12(1):1949. PMC: 8007591. DOI: 10.1038/s41467-021-22291-0. View

16.

Rong X, Ettelaie R, Lishchuk S, Cheng H, Zhao N, Xiao F . Liquid marble-derived solid-liquid hybrid superparticles for CO capture. Nat Commun. 2019; 10(1):1854. PMC: 6478824. DOI: 10.1038/s41467-019-09805-7. View

17.

Sayari A, Heydari-Gorji A, Yang Y . CO2-induced degradation of amine-containing adsorbents: reaction products and pathways. J Am Chem Soc. 2012; 134(33):13834-42. DOI: 10.1021/ja304888a. View

18.

Perdew , Burke , Ernzerhof . Generalized Gradient Approximation Made Simple. Phys Rev Lett. 1996; 77(18):3865-3868. DOI: 10.1103/PhysRevLett.77.3865. View

19.

Sun X, Shen X, Wang H, Yan F, Hua J, Li G . Atom-level interaction design between amines and support for achieving efficient and stable CO capture. Nat Commun. 2024; 15(1):5068. PMC: 11176289. DOI: 10.1038/s41467-024-48994-8. View

20.

Lin Y, Yan Q, Kong C, Chen L . Polyethyleneimine incorporated metal-organic frameworks adsorbent for highly selective CO2 capture. Sci Rep. 2013; 3:1859. PMC: 3656390. DOI: 10.1038/srep01859. View