High Efficiency Mixed Amine Adsorbents for Directly Capturing Carbon Dioxide from Air

Abstract

The development of effective adsorbents with high amine efficiency and CO₂ adsorption almost unaffected by humidity is extremely challenging. In this study, we introduce an innovative solid amine adsorbent, TETA/DEA@FS, composed of triethylenetetramine (TETA) and diethanolamine (DEA) functionalized fumed silica (FS), which exhibits exceptional capability in selectively capturing trace CO₂ from N₂. TETA/DEA@FS shows an exceptionally high capacity of CO₂ adsorption of 1.13 mmol/g at the temperature of 298 K and the pressure of 0.0004 bar (1 bar=100 kPa), and achieves an unprecedented CO₂/N₂ IAST selectivity of 1.70×10¹². TETA/DEA@FS exhibits high amine efficiency, with breakthrough experiments demonstrating that CO₂ adsorption remains nearly unaffected by humidity. Meanwhile, TETA/DEA@FS demonstrates rapid CO₂ adsorption kinetics and outstanding cyclic stability.

References

[1] AlivandM S, McQuillanR V, MomeniA, ZavabetiA, StevensG W, MumfordK A. Small, 2023, 19: 2300150

[2] KumarR, BandyopadhyayM, PandeyM, TsunojiN. Microporous Mesoporous Mater., 2022, 338: 111956

[3] ShiX, XiaoH, AzarabadiH, SongJ, WuX, ChenX, LacknerK S. Angew. Chem. Int. Ed., 2020, 59: 6984

[4] SongM, RimG, KongF, PriyadarshiniP, RosuC, LivelyR P, JonesC W. Ind. Eng. Chem. Res., 2022, 61: 13624

[5] WangX, ZhaoZ, ZahraK, LiJ, ZhangZ. Chem. Res. Chinese Universities, 2023, 39: 580

[6] WangH, YangZ, ZhouY, CuiH, ChengZ, ZhouZ. Ind. Eng. Chem. Res., 2023, 62: 16579

[7] Pangapanga, PhiriI, MungatanaE D. Int. J. Disaster Risk Reduct., 2021, 61: 102322

[8] KumarA, MaddenD G, LusiM, ChenK J, DanielsE A, CurtinT, PerryJ J IV, ZaworotkoM J. Angew. Chem. Int. Ed., 2015, 54: 14372

[9] EransM, Sanz PérezE S, HanakD P, ClulowZ, ReinerD M, MutchG A. Energy Environ. Sci., 2022, 15: 1360

[10] TsiotsiasA I, CharisiouN D, ItalianoC, FerranteG D, PinoL, VitaA, SebastianV, HinderS J, BakerM A, SharanA, SinghN. Appl. Surf. Sci., 2024, 646: 158945

[11] BalasubramaniamB M, ThierryP T, LethierS, PugnetV, LlewellynP, RajendranA. Chem. Eng. J., 2024, 485: 149568

[12] JiaX, SunP, LiuA, ChenJ, WangJ, ZhangH, ZhuW. Chem. Res. Chinese Universities, 2023, 39: 680

[13] RaganatiF, MiccioF, AmmendolaP. Energy Fuels, 2021, 35: 12845

[14] ChenY, LvD, WuJ, XiaoJ, XiH, XiaQ, LiZ. Chem. Eng. J., 2017, 308: 1065

[15] XianS, PengJ, ZhangZ, XiaQ, WangH, LiZ. Chem. Eng. J., 2015, 270: 385

[16] FuD, ParkY, DavisM E. PNAS, 2022, 119: e2211544119

[17] TaoZ, TianY, OuS Y, GuQ, ShangJ. AlChE J., 2023, 69: e18139

[18] McDonaldT M, LeeW R, MasonJ A, WiersB M, HongC S, LongJ R. J. Am. Chem. Soc., 2012, 134: 7056

[19] GoeppertA, CzaunM, MayR B, PrakashG K S, OlahG A, NarayananS R. J. Am. Chem. Soc., 2011, 133: 20164

[20] LvD, ChenJ, YangK, WuH, ChenY, DuanC, WuY, XiaoJ, XiH, LiZ, XiaQ. Chem. Eng. J., 2019, 375: 122074

[21] YangJ, ZhaoQ, XuH, LiL, DongJ, LiJ. J. Chem. Eng. Data, 2012, 57: 3701

[22] WuL, SunJ, ZhuW, WangC, ZhangL, NiuR, HouR, PanY. Ind. Eng. Chem. Res., 2024, 63: 7760

[23] NugentP, BelmabkhoutY, BurdS D, CairnsA J, LuebkeR, ForrestK, PhamT, MaS, SpaceB, WojtasL, EddaoudiM. Nature, 2013, 495: 80

[24] WangQ, ChenY, LiuP, WangY, YangJ, LiJ, LiL. Molecules, 2022, 27: 5608

[25] LiZ, ZhiY, FengX, DingX, ZouY, LiuX, MuY. Chemistry-A European Journal, 2015, 21: 12079

[26] WuY, LvZ, ZhouX, PengJ, TangY, LiZ. Chem. Eng. J., 2019, 355: 815

[27] CavenatiS, GrandeC A, RodriguesA E. J. Chem. Eng. Data, 2004, 49: 1095

[28] SuF, LuC, ChenH S. Langmuir, 2011, 27: 8090

[29] QuangD V, DindiA, RayerA V, HadriN E, AbdulkadirA, Abu ZahraM R M. Energy Procedia, 2014, 63: 2122

[30] LiK, JiangJ, YanF, TianS, ChenX. Appl. Energy, 2014, 136: 750

[31] GrayM L, HoffmanJ S, HrehaD C, FauthD J, HedgesS W, ChampagneK J, PennlineH W. Energy Fuels, 2009, 23: 4840

[32] SrikanthC S, ChuangS S C. J. Phys. Chem. C, 2013, 117: 9196

[33] WilfongW C, SrikanthC S, ChuangS S C. ACS Appl. Mater. Interfaces, 2014, 6: 13617

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