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0 260228

DOI: https://doi.org/10.6023/A25120420

Rapid and Green Mechanochemical Synthesis of UTSA-16(Zn) for High-Performance CO2 Capture

  • Wang Zhitao ,
  • Lin Yuke ,
  • Wan Yan ,
  • Huang Xinwei ,
  • Li Yunbin ,
  • Ji Dinghao ,
  • Xiang Shengchang ,
  • Zhang Zhangjing
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  • aFujian Key Laboratory of Polymer Materials, College of Chemistry and Materials Science, Fujian Normal University, Fuzhou 350117, China;
    bChina Astronaut Research and Training Center, No. 1 Yuanming-yuan West Road, Haidian District, Beijing 100094, China
†These authors contributed equally to this work.
*E-mail: jidh.2008@tsinghua.org.cn; scxiang@fjnu.edu.cn; zzhang@fjnu.edu.cn.

Received date: 2025-12-25

  Online published: 2026-02-28

Supported by

National Science Fund for Distinguished Young Scholars of China (Grant No. 22425102), the National Natural Science Foundation of China (Grant No. 22271046, 22373015, 22501044 and W2431013) and the Foundation of National Key Laboratory of Human Factors Engineering (Grant No. HFNKL2023WW04).

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Abstract

Addressing the pressing challenge of high energy consumption and solvent waste in the industrial-scale production of metal-organic frameworks (MOFs), we report a rapid, green, and scalable mechanochemical strategy for the mass preparation of the highly efficient CO2 adsorbent, UTSA-16(Zn). Unlike conventional solvothermal methods, this protocol using zinc acetate and potassium citrate dramatically shortens the synthesis time from 48 hours to just 6 hours. This achieves a remarkable 48-fold enhancement in space-time yield while reducing solvent consumption by approximately 90%. Crucially, we identify that the in-situ accumulation of acidic byproducts during grinding inhibits framework assembly. Precise pH modulation using 0.2 equivalents of triethylamine (TEA) is essential to buffer the reaction environment, preventing defect formation and ensuring high product crystallinity. The resulting material is structurally isomorphous to its hydrothermally synthesized counterpart, possessing a consistent pore environment with a high BET surface area of 817 m2/g. In terms of performance, the mechanochemically derived UTSA-16(Zn) exhibits exceptional CO2 uptake (3.68 mmol/g at 296 K and 1 atm) and an ultra-high IAST selectivity of 388 for CO2/N2 mixtures, driven by a significant difference in isosteric heat of adsorption. Dynamic breakthrough experiments further validate a robust dynamic capacity of 1.94 mmol/g and stable recyclability under simulated flue gas conditions. This work not only provides a practical manufacturing route for UTSA-16(Zn) but also underscores the pivotal role of pH regulation in the green synthesis of advanced porous materials.

Key words： UTSA-16; MOFs; Separation; Mechanochemical Synthesis; Carbon Dioxide Capture

Cite this article

Wang Zhitao , Lin Yuke , Wan Yan , Huang Xinwei , Li Yunbin , Ji Dinghao , Xiang Shengchang , Zhang Zhangjing . Rapid and Green Mechanochemical Synthesis of UTSA-16(Zn) for High-Performance CO2 Capture[J]. Acta Chimica Sinica, 0 : 260228 . DOI: 10.6023/A25120420

References

[1] H. Li, M. Eddaoudi, M. O'Keeffe, O. M. Yaghi, Nature1999, 402, 276-279
[2] H. K. Chae, D. Y. Siberio-Pérez, J. Kim, Y. Go, M. Eddaoudi, A. J. Matzger, M. O'Keeffe, O. M. Yaghi, D. Materials, G. Discovery, Nature2004, 427, 523-527.
[3] S. Horike, S. Shimomura, S. Kitagawa, Nat. Chem. 2009, 1, 695-704;
[4] G. Férey, Chem. Soc. Rev. 2008, 37, 191-214.
[5] Gao C.; Zhang S.; Pang H.;Acta Chim. Sinica 2025, 83(8): 962-980.
[6] O. K. Farha, I. Eryazici, N. C. Jeong, B. G. Hauser, C. E. Wilmer, A. A. Sarjeant, R. Q. Snurr, S. T. Nguyen, A. Ö. Yazaydın, J. T. Hupp, J. Am. Chem. Soc. 2012, 134, 15016-15021.
[7] Z. Chen, K. O. Kirlikovali, P. Li, O. K. Farha, Acc. Chem. Res. 2022, 55, 579-591.
[8] R.-B. Lin, Z. Zhang, B. Chen, Acc. Chem. Res. 2021, 54, 3362-3376.
[9] H. Furukawa, J. Kim, N. W. Ockwig, M. O’Keeffe, O. M. Yaghi, J. Am. Chem. Soc. 2008, 130, 11650-11661.
[10] M. Eddaoudi, J. Kim, N. Rosi, D. Vodak, J. Wachter, M. O'Keeffe, O. M. Yaghi, Science2002, 295, 469-472.
[11] S. Yuan, L. Huang, Z. Huang, D. Sun, J.-S. Qin, L. Feng, J. Li, X. Zou, T. Cagin, H.-C. Zhou, J. Am. Chem. Soc. 2020, 142, 4732-4738.
[12] Y. Han, C. Ji, Y. Lou, R. Li, M. He, D. Yuan, Z. Han, J. Am. Chem. Soc. 2025, 147, 19262-19271.
[13] S. Xiang, W. Zhou, J. M. Gallegos, Y. Liu, B. Chen, J. Am. Chem. Soc. 2009, 131, 12415-12419.
[14] K. M. Carsch, H. Z. H. Jiang, R. A. Klein, A. S. Rosen, P. S. Summerhill, J. L. Peltier, A. J. Huang, R. A. Murphy, M. N. Dods, H. A. Silva, Z. Hasanbasri, H. Kwon, S. L. Karstens, Y. Yabuuchi, J. Börgel, J. W. Taylor, K. R. Meihaus, K. C. Bustillo, A. M. Minor, K. A. Persson, C. M. Brown, R. D. Britt, N. P. Stadie, J. R. Long, Science2025, 390, 808-812.
[15] X.-D. Zhang, Y.-Z. Zhang, T. Li, Y.-X. Zuo, X.-N. Li, D.-S. Zhang, L. Geng, B. Wang, H. Huang, X. Zhang, Inorg. Chem. Front. 2025, 12, 2036-2046.
[16] W. Li, L. Wang, B. E. Keshta, Y. Bi, Y. Zhang, B. Chen, Coord. Chem. Rev. 2025, 545, 217032.
[17] P.-Q. Liao, N.-Y. Huang, W.-X. Zhang, J.-P. Zhang, X.-M. Chen, Science2017, 356, 1193-1196.
[18] J. Cui, Z. Zhang, L. Yang, J. Hu, A. Jin, Z. Yang, Y. Zhao, B. Meng, Y. Zhou, J. Wang, Y. Su, J. Wang, X. Cui, H. Xing, Science2024, 383, 179-183.
[19] H. Zeng, M. Xie, T. Wang, R.-J. Wei, X.-J. Xie, Y. Zhao, W. Lu, D. Li, Nature2021, 595, 542-548.
[20] Y. Zhang, W. Sun, B. Luan, J. Li, D. Luo, Y. Jiang, L. Wang, B. Chen, Angew. Chem. 2023, 62, e202309925.
[21] Zhang H.; Li G.-L.; Zhang K.-G.; Liao C.-Y.;Acta Chim. Sinica 2017, 75(9): 841-859.
[22] T. Lan, B. Yu, Y. Liu, D. Ning, C. Zhi, Y. Chen, L. Sun, X. Cui, J. Li,L. Li,Chin. J. Chem. 2025, 43, 1141-1147
[23] Wu Z.-L.; Zhang L.; Chen Y.; Li J.-P.; Li L.-B.Acta Chim. Sinica 2025, 83(8): 917-936.
[24] Huang G.; Chen Y.-Z.; Jiang H.-L.Acta Chim. Sinica 2016, 74(2): 113-129.
[25] W. Wang, D. Chen, F. Li, X. Xiao, Q. Xu, Chem2024, 10, 86-133.
[26] S. Wang, X. Zhou, X. Ding, X. Wang, Y. Jin, Z. Zhou, X. Lu, W. Yang, H. Wang, ChemSusChem.2025, 18, e202402648.
[27] B. Yan, J. Song, D. Zhang, Z. Guan, Y. Fang,Chin. J. Chem. 2025, 43, 1078-1089
[28] Liu. Y.; Gao. F.-Q.; Ma. Z.-Y.; Zhang. Y.-L.; Li. W.-W.; Hou. L.; Zhang. X.-J.; Wang. Y.-Y. Acta Chim. Sinica 2024, 82, 152-159.
[29] H. Yuan, N. Li, W. Fan, H. Cai, D. Zhao, Adv. Sci. 2022, 9, 2104374.
[30] H. Roh, D.-H. Kim, Y. Cho, Y.-M. Jo, J. A. del Alamo, H. J. Kulik, M. Dincă, A. Gumyusenge, Adv. Mater. 2024, 36, 2312382.
[31] X. Rao, T. Song, J. Gao, Y. Cui, Y. Yang, C. Wu, B. Chen, G. Qian, J. Am. Chem. Soc. 2013, 135, 15559-15564.
[32] Wang. Y.; Zou. Y.; Zhang. Y.; Zheng. S.-J.; Wang. H.-Y.; Liu. T.-F.; Li. R.-F.Acta Chim. Sinica 2025, 83, 45-51.
[33] S. Xiang, X. Wu, J. Zhang, R. Fu, S. Hu, X. Zhang, J. Am. Chem. Soc. 2005, 127, 16352-16353.
[34] S. Xiang, Y. He, Z. Zhang, H. Wu, W. Zhou, R. Krishna, B. Chen, Nat. Commun. 2012, 3, 954.
[35] S. Gaikwad, S.-J. Kim, S. Han, J. Ind. Eng. Chem. 2020, 87, 250-263.
[36] S. B. Peh, S. Xi, A. Karmakar, J. Y. Yeo, Y. Wang, D. Zhao, Inorg. Chem. 2020, 59, 9350-9355.
[37] C. A. Grande, R. Blom, V. Middelkoop, D. Matras, A. Vamvakeros, S. D. M. Jacques, A. M. Beale, M. Di Michiel, K. Anne Andreassen, A. M. Bouzga, Chem. Eng. J. 2020, 402, 126166.
[38] R. Gaikwad, S. Gaikwad, Y. Kim, S. Han, Microporous and Mesoporous Mater. 2021, 323, 111233.
[39] V. B. López-Cervantes, M. L. Martínez, J. L. Obeso, C. García-Carvajal, N. S. Portillo-Vélez, A. Guzmán-Vargas, R. A. Peralta, E. González-Zamora, I. A. Ibarra, D. Solis-Ibarra, J. L. Woodliffe, Y. A. Amador-Sánchez, Dalton Trans. 2025, 54, 1646-1654.
[40] S. Altarawneh, J. L. Woodliffe, J. Mater. Chem. A 2025, 13, 26610-26626.
[41] J. L. Woodliffe, J. Molinar-Díaz, R. Clowes, O. H. Hussein, E. Lester, R. Ferrari, I. Ahmed, A. Laybourn, J. Environ. Chem. Eng. 2024, 12, 114167.
[42] G. Xu, K. Otsubo, T. Yamada, S. Sakaida, H. Kitagawa,J. Am. Chem. Soc. 2013, 135, 7438-7441.
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