高等学校化学学报 ›› 2023, Vol. 44 ›› Issue (10): 20230227.doi: 10.7503/cjcu20230227
收稿日期:
2023-05-06
出版日期:
2023-10-10
发布日期:
2023-06-06
通讯作者:
孟祥举
E-mail:mengxj@zju.edu.cn
基金资助:
Received:
2023-05-06
Online:
2023-10-10
Published:
2023-06-06
Contact:
MENG Xiangju
E-mail:mengxj@zju.edu.cn
Supported by:
摘要:
中国分子筛基础研究近年来进入了飞速发展阶段, 在分子筛的合成新策略、 新结构与表征, 特别是新的功能应用等方面取得了系列突破性进展. 本文将总结自由基加速沸石分子筛晶化、 稳定超大孔硅铝沸石分子筛的合成、 应用新兴电子显微技术对沸石分子筛周期晶格和局域结构的原子级分辨率观察及对其孔道内限域小分子的电子显微镜成像、 沸石分子筛在低碳分子吸附与催化转化过程中的性能以及沸石分子筛在锂电池中的应用等方面取得的突破性进展, 并对沸石分子筛未来的发展方向和面临的挑战进行展望.
中图分类号:
TrendMD:
戚刚刚, 孟祥举. 中国沸石分子筛基础研究近年来的突破性进展. 高等学校化学学报, 2023, 44(10): 20230227.
QI Ganggang, MENG Xiangju. Recent Breakthrough Progresses in the Fundamental Research of Zeolites in China. Chem. J. Chinese Universities, 2023, 44(10): 20230227.
Fig.1 Radicals’ identification from UV irradiation[6](A—C) EPR spectra of the initial reaction mixture containing DMPO under the UV irradiation for 90 s(A), 30 s(B), and 0 s(C); (D—F) comparison of the experimental and the simulated EPR spectra of DMPO-•OH adduct(D), DMPO-•Si adduct(E), and oxidized DMPO radicals(F); (G) EPR spectrum of the initial reaction mixture containing the spin-trapping agent of BMPO after 10 h of dark incubation. The EPR signals are marked as following: red circles, hydroxyl free radicals; green rectangles, oxidized DMPO radicals; blue arrows, silicon-based radicals.
Fig.2 Three supercages and channel system in ZEO⁃1[9](A—D) Pore system contains three supercages with 16MR(A), 16-12MR(B), and 12MR(C) apertures that are compared here with FAU 12MR supercage(D); (E) structure viewed along a axis; (F) the 3D channel system with the structure model superimposed. Purple arrows, 16MR; yellow arrows, 12MR; orange ball and stick, silicon; red ball and stick, oxygen.
Fig.3 Imaging the huge local deformation of zeolite channels in the in situ STEM system during benzene adsorption[12](A) Schematic of the in situ STEM experimental setup. The benzene adsorption-desorption process was carried out in an enclosed environment chamber made of Si3N4 solid membranes in an atmosphere system. (B—D) iDPC-STEM images and profile analysis of an empty MFI zeolite specimen from the [010] projection. The magnified image shows a nearly round pore. The profile analysis gives the aspect ratio of Dmax to Dmin, which was used to estimate the local deformation of straight channels. (E—G) iDPC-STEM images and profile analysis of a saturated benzene@MFI specimen from the [010] projection at 473 K and 450 torr(1 torr=133 Pa)(90% N2 and 10% benzene). The 10-ring opening pore shows a distinctly elliptical shape stretched along the parallel direction of the benzene plane. (H—J) Further comparison of imaging differences between the empty(H) and saturated states(I) of benzene@MFI, showing clearer imaging of O atoms in the MFI framework, which are highlighted in (J). Forty opening pores were measured to obtain each statistical result. Scale bars, 2 nm[(B) and (E)], 500 pm[(C), (F), (H) and (I)].
Fig.4 OXZEO bifunctional catalyst concept for syngas conversion to light olefins[7](A) Scheme and (B) hydrocarbon distribution in comparison to the ASF distribution in conventional FTS and FTTO-1 over a Fe-based catalyst and FTTO-2 over a Co-based catalyst.
Fig.5 Models(A, D) and tomographic section TEM images(B, C, E, F) of the AuPd@ZSM⁃5⁃R(A—C) and AuPd/ZSM⁃5(D—F) catalysts[14]Scale bars: (B) 100 nm; (C) 10 nm(5 nm in inset); (E) 200 nm; (F) 50 nm.
Fig.6 Identification of boron hydroxyl groups in BS⁃1[15](A) 1H MAS NMR spectra of BS-1 and B/S-1; (B) different H species and their chemical shifts; (C) 2D 1H-1H DQ MAS NMR of BS-1 before(blue) and after(red) ODHP; (D) transition state structure of —B[OH…O(H)—Si]2 reacting with oxygen and propane.
Fig.7 Schematic view of faujasite supercage along [110] direction(A) and packing of C2D2 in the supercage of Ni@FAU along [110] direction(B)[17]Si/Al: yellow; O: red; Ni: green; C: brown; D: white.
Fig.8 Structure, performance, safety, abuse tolerance and flexibility of the SSLAB with C⁃LiXZM[19](A) SEM image of the integrated structure of carbon nanotube cathode-solid zeolite electrolyte(C-LiXZM) and TEM image of the cathode/electrolyte interface(inset); (B) the cycle life comparison of Li-air batteries with different solid electrolytes; (C) the optical photograph of C-LiXZM-based solid-state Li-air battery with a thickness of merely 0.33 mm; (D, E) the flexibility tests of the integrated solid-state Li-air battery based on C-LiXZM under different bending(D) and torsion conditions(E); (F) safety and environmental adaptability of C-LiXZM-based solid-state Li-air batteries; (G) superior shape modifiability of C-LiXZM-based solid-state Li-air battery; (H) the application of the integrated solid-state Li-air batteries based on C-LiXZM in powering an unmanned aerial vehicle.
1 | Xu R. R., Pang W. Q., Yu J. H., Huo Q. S., Chen J. S., Chemistry of Zeolite and Related Porous Materials,Wiley, Singapore, 2007 |
2 | Jin S. Q., Sun H. M., Yang W. M., Chem. J. Chinese Universities, 2021, 42(1), 217—226 |
金少青, 孙洪敏, 杨为民. 高等学校化学学报, 2021, 42(1), 217—226 | |
3 | Yan W. F., Natl. Sci. Rev., 2022, 9(9), nwac056 |
4 | Luo Y., Smeet S., Peng F., Etman A., Wang Z. D., Sun J. L., Yang W. M., Chem. Eur. J., 2017, 23(66), 16829—16834 |
5 | Luo Y., Smeet S., Wang Z. D., Sun J. L., Yang W. M., Chem. Eur. J., 2019, 25(9), 2184—2188 |
6 | Feng G. D., Cheng P., Yan W. F., Boronat M., Li X., Su J. H., Wang, J. Y., Li, Y., Corma A., Xu R. R., Yu J. H., Science, 2016, 351(6278), 1188—1191 |
7 | Jiao F., Li J. J., Pan X. L., Xiao J. P., Li H. B., Ma H., Wei M. M., Pan Y., Zhou Z. Y., Li M. R., Miao S., Li J., Zhu Y., Xiao D., He T., Yang J., Qi F., Fu Q., Bao X. H., Science, 2016, 351(6277), 1065—1068 |
8 | Jiao F., Bai B., Li G., Pan X. L., Ye Y. H., Qu S. C., Xu C. Q., Xiao J. P., Jia Z. H., Liu W., Peng T., Ding Y. L., Liu C., Li J. J., Bao X. H., Science, 2023, 380(6646), 727—730 |
9 | Lin Q. F., Gao Z. R., Lin C., Zhang S. Y., Chen J., Li Z., Liu X., Fan W., Li J., Chen X., Camblor M. A., Chen F. J., Science, 2021, 379(6575), 1605—1608 |
10 | Li Z., Gao Z. R., Lin Q. F., Liu C. X., Gao F. X., Lin C., Zhang S. Y., Deng H., Mayoral A., Fan W., Luo S., Chen X., He H., Camblor M. A., Chen F. J., Science, 2023, 374(6629), 283—287 |
11 | Shen B. Y., Chen X., Wang H. Q., Xiong H., Bosch E. G., Lazić I., Cai D., Qian W. Z., Jin S. F., Liu X., Han Y., Wei F., Nature, 2021, 592(7855), 541—544 |
12 | Xiong H., Liu Z. Q., Chen X., Wang H. Q., Qian W. Z., Zhang C. X., Zheng A. M., Wei F., Science, 2022, 376(6592), 491—496 |
13 | Shen B. Y., Wang H. Q., Xiong H., Chen X., Bosch E. G., Lazikć, Qian W. Z., Wei F., Nature, 2022, 607(7920), 703—707 |
14 | Jin Z., Wang L., Zuidema E., Mondal K., Zhang M., Zhang J., Wang C. T., Meng X. J., Yang H. Q., Mesters C., Xiao F. S., Science, 2020, 367(6474), 193—197 |
15 | Zhou H., Yi X. F., Hui Y., Wang L., Chen W., Qin Y. C., Wang M., Ma J. B., Chu X. F., Wang Y. Q., Hong X., Chen Z. F., Meng X. J., Wang H., Zhu Q. Y., Song L. J., Zheng A. M., Xiao F. S., Science, 2021, 372(6537), 76—80 |
16 | Zhao D., Tian X. X., Doronkin D. E., Han S. L., Kondratenko V. A., Grunwaldt J. D., Perechodjuk A., Vuong T. H., Rabeah J., Eckelt R., Rodemerck U., Linke D., Jiang G. Y., Jiao H. J., Kondratenko E. V., Nature, 2021, 599(7884), 234—238 |
17 | Chai Y. C., Han X., Li W. Y., Liu S. S., Yao S. K., Wang C., Shi W., da⁃Silva I., Manuel P., Cheng Y. Q., Daemen L. D., Ramirez⁃Cuesta A. J., Tang C. C., Jiang L., Yang S. H., Guan N. J., Li L. D., Science, 2020, 368(6494), 1002—1006 |
18 | Zhou Y., Zhang J. L., Wang L., Cui X. L., Liu X. L., Wong S. S., An H., Yan N., Xie J. Y., Yu C., Zhang P. X., Du Y. H., Xi S. B., Zheng L. R., Cao X. Z., Wu Y. J., Wang Y. X., Wang C. Q., Wei H. M., Chen L., Xing H. B., Wang J., Science, 2021, 373(6552), 315—320 |
19 | Chi X. W., Li M. L., Di J. C., Bai P., Song L. N., Wang X. X. Li F., Liang S., Xu J. J., Yu J. H., Nature, 2021, 592(7855), 551—557 |
20 | Wen J. L., Zhang J. H., Jiang J X, Chem. J. Chinese Universities, 2021, 42(1), 101—116 |
闻嘉丽, 张钧豪, 姜久兴. 高等学校化学学报, 2021, 42(1), 101—116 | |
21 | Chen X., Shen B. Y., Xiong H., Wei F., Chem. J. Chinese Universities, 2021, 42(1), 133—147 |
陈晓, 申博渊, 熊昊, 魏飞. 高等学校化学学报, 2021, 42(1), 133—147 | |
22 | Liu Y. F., Wang L., Xiao F. S., Chem. Res. Chinese Universities, 2022, 38(3), 671—676 |
23 | Yan W. F., Sun Q. M., Yu J. H., Matter, 2021, 4(8), 2642—2644 |
24 | Liu S. S., Chai Y. C., Guan N. J., Li L. D., Chem. J. Chinese Universities, 2021, 42(1), 268—288 |
刘珊珊, 柴玉超, 关乃佳, 李兰冬. 高等学校化学学报, 2021, 42(1), 268—288 | |
25 | Wu Q. M., Wang Y. Q., Meng X. J., Xiao F. S., Chem. J. Chinese Universities, 2021, 42(1), 21—28 |
吴勤明, 王叶青, 孟祥举, 肖丰收. 高等学校化学学报, 2021, 42(1), 21—28 | |
26 | Wu Q. M., Luan H. M., Xiao F. S., Natl. Sci. Rev., 2022, 9(9), nwac023 |
27 | Jiao M. C., Jiang J. G., Xu H., Wu P., Chem. J. Chinese Universities, 2021, 42(1), 29—39 |
焦美晨, 蒋金刚, 徐浩, 吴鹏. 高等学校化学学报, 2021, 42(1), 29—39 | |
28 | Wang W. Y., Xu J., Deng F., Natl. Sci. Rev., 2022, 9(9), nwac155 |
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