Spin conversion of positronium of ZIFs nanocrystalline

Li Chong-Yang; Li Meng-De; Wang Mei; Li Tao; Liu Jian-Dang; Ye Bang-Jiao; Chen Zhi-Quan

doi:10.7498/aps.71.20220305

Abstract

ZIFs crystal is composed of imidazolidyl bridging single metal ions, and its structure can be adjusted by flexibly selecting functional groups of imidazolidyl ligands, thereby possessing more new properties and functions. While, the pore structure and chemical environment of ZIFs crystals are closely related to their properties. In this work, ZIF nanocrystals are prepared by static reaction. The X-ray diffraction results confirm that the prepared crystals are typical of ZIF-8 crystals, and the regular rhomboidal structure can be observed by scanning electron microscopy. The N₂ adsorption-desorption test indicates that the ZIF crystal exhibits the larger specific surface area (2966.26 m²/g) and pore volume (3.01 cm³/g) . With the increase of Co content, specific surface area and pore volume of ZIFs crystal decrease, while the pore size remains nearly unchanged (around 12 Å). However, the pore size distribution calculated by N₂ adsorption/desorption isothermal curve does not show the ultra-micropore information of the six-membered ring composed of imidazole ligands (3.4 Å). The microstructure and surface properties of the crystal are investigated by positron annihilation lifetime and Doppler broadening. The positron lifetime spectrum has four components. The longer lifetimes $ {\tau }_{3} $ and $ {\tau }_{4} $ are the annihilation lifetimes of o-Ps in the microporous region and the regular angular gap of the crystal, respectively. With the increase of Co content, the lifetime $ {\tau }_{3} $ hardly changes, while the longer lifetime $ {\tau }_{4} $ decreases from 30.89 ns to 12.57 ns, and the corresponding intensities $ {I}_{3} $ and $ {I}_{4} $ decrease sharply from 12.93% and 8.15% to 3.68% and 0.54%, respectively. With the increase of Co content, the S parameter obtained by doppler broadening shows a continuous upward trend, and the p-Ps intensity also increases gradually, which is mainly due to the self-rotation effect of the electron element. Therefore, the decrease of $ {\tau }_{4} $ in ZIFs nanocrystal is probably due to the self-rotation effect of positronium and Co ion on the crystal surface.

Keywords:

Authors and contacts

1.
College of Electric Power, North China University of Water Resources and Electric Power, Zhengzhou 450045, China
2.
School of Physics Science and Technology, Wuhan University, Wuhan 430072, China
3.
School of Physics, University of Science and Technology of China, Hefei 230026, China
4.
School of Physics and Engineering, Zhengzhou University of Light Industry, Zhengzhou 450002, China

Corresponding author: Liu Jian-Dang, liujd@ustc.edu.cn ; Chen Zhi-Quan, chenzq@whu.edu.cn

Funds: Project supported by the National Key R & D Program of China (Grant No. 2019YFA0210000) and the National Natural Science Foundation of China (Grant Nos. 11875248, 12175232).

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References

[1]	彭雨, 吴依, 杨紫微, 李琳钰, 蒋华麟, 陈萍华 2020 广州化工 48 4 Google Scholar Peng Y, Wu Y, Yang Z W, Li L Y, Jiang H L, Chen P H 2020 Guangzhou Chem. Indus. 48 4 Google Scholar
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[11]	马生花, 马芙莲, 解玉龙 2020 硅酸盐通报 39 2993 Google Scholar Ma S H, Ma F L, Xie Y L 2020 Bull. Chin. Ceramic Soc. 39 2993 Google Scholar
[12]	Jin C X, Shang H B 2021 J. Solid State Chem. 297 122040 Google Scholar
[13]	Nagarjun N, Arthy K, Dhakshinamoorthy A 2021 Eur. J. Inorg. Chem. 2021 2108 Google Scholar
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[25]	Jean Y C, Lu X, Lou Y, Bharathi A, Sundar C S, Lyu Y, Hor P H, Chu C W 1992 Phys. Rev. B 45 12126 Google Scholar
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[33]	Zhang H J, Liu Z W, Chen Z Q, Wang S J 2011 Chin. Phys. Lett. 28 017802 Google Scholar
[34]	Chen Z Q, Kawasuso A, Xu Y, Naramoto H, Yuan X L, Sekiguchi T, Suzuki R, Ohdaira T 2005 Phys. Rev. B 71 115213 Google Scholar
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图 1 ZIF-Zn, ZIF-Co_0.05Zn_0.95, ZIF-Co_0.3Zn_0.7和ZIF-Co的X射线衍射谱图

Figure 1. X-ray diffraction patterns measured for ZIF-Zn, ZIF-Co_0.05Zn_0.95, ZIF-Co_0.3Zn_0.7 and ZIF-Co.

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图 2 ZIF-Co-Zn纳米晶体的扫描电子显微镜图　(a) ZIF-Zn; (b) ZIF-Co_0.05Zn_0.95; (c) ZIF-Co_0.3Zn_0.7; (d) ZIF-Co

Figure 2. Scanning electron microscopy of ZIF-Co-Zn: (a) ZIF-Zn; (b) ZIF-Co_0.05Zn_0.95; (c) ZIF-Co_0.3Zn_0.7; (d) ZIF-Co.

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图 3 ZIF-Co-Zn纳米晶体的(a) N₂吸附-脱附等温线(STP, 标准状况)及其(b)孔径分布

Figure 3. N₂ adsorption and desorption isothermal (a) and its pore size distribution (b) of ZIF-Co-Zn nanocrystalline. STP, standard temperature and pressure.

DownLoad: Full-Size Img PowerPoint

图 4 经归一化峰处理后ZIF-Zn, ZIF-Co_0.05Zn_0.95和ZIF-Co的正电子湮没寿命谱图

Figure 4. Peak-normalized positron lifetime spectrum measured for ZIF-Zn, ZIF-Co_0.05Zn_0.95, ZIF-Co.

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图 5 ZIF-Co-Zn中正电子寿命随Co摩尔含量的变化　(a) $ {\tau }_{1} $, $ {\tau }_{2} $; (b) $ {\tau }_{3} $, $ {\tau }_{4} $

Figure 5. Variation of positron lifetime as a function of Co molar content: (a) $ {\tau }_{1} $, $ {\tau }_{2} $; (b) $ {\tau }_{3} $, $ {\tau }_{4} $.

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图 6 ZIF-Co-Zn中o-Ps强度$ {I}_{3} $, $ {I}_{4} $随Co摩尔含量的变化

Figure 6. Variation of o-Ps intensity $ {I}_{3} $, $ {I}_{4} $ of ZIF-Co-Zn as a function of Co molar content.

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图 7 ZIF-Co-Zn中多普勒展宽S参数随Co摩尔含量的变化

Figure 7. Variation of doppler broadening S-parameter of ZIF-Co-Zn as a function of Co molar content.

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图 8 ZIF-Co-Zn中o-Ps和p-Ps强度随Co摩尔含量的变化

Figure 8. Variation of o-Ps and p-Ps intensity of ZIF-Co-Zn as a function of Co molar content.

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图 9 ZIF-Co-Zn中S-W曲线

Figure 9. S-W plot measured for the ZIF-Co-Zn porous material.

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表 1 ZIF-Co-Zn纳米晶体中孔结构信息

Table 1. Pore structure parameters of ZIF-Co-Zn crystals

Sample	$ {S}_{\mathrm{B}\mathrm{E}\mathrm{T}}/ $ $({\mathrm{m} }^{2}{\cdot}{\mathrm{g} }^{-1})$	$ {S}_{\mathrm{m}\mathrm{i}\mathrm{c}\mathrm{r}\mathrm{o}}/ $ $({\mathrm{m} }^{2}{\cdot}{\mathrm{g} }^{-1})$	$ {V}_{\mathrm{t}\mathrm{o}\mathrm{t}\mathrm{a}\mathrm{l}} $/ $\left({\mathrm{c}\mathrm{m} }^{3}{\cdot\mathrm{g} }^{-1}\right)$
B1	2966.26	2523.56	3.01
B2	2644.63	2330.56	2.39
B3	3110.94	2734.41	2.96
B4	3101.99	2684.39	2.99
B5	3149.70	2798.98	2.71
B6	3019.41	2753.46	1.70
B7	2250.85	2139.03	1.00
注: B1—B7依次代表制备的ZIF-Zn, ZIF-Co_0.025-Zn_0.975, ZIF-Co_0.5-Zn_0.95, ZIF-Co_0.15-Zn_0.85, ZIF-Co_0.3-Zn_0.7, ZIF-Co_0.7-Zn_0.3及ZIF-Co.

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[1]	彭雨, 吴依, 杨紫微, 李琳钰, 蒋华麟, 陈萍华 2020 广州化工 48 4 Google Scholar Peng Y, Wu Y, Yang Z W, Li L Y, Jiang H L, Chen P H 2020 Guangzhou Chem. Indus. 48 4 Google Scholar
[2]	韩臻, 陈元涛, 张炜, 许成, 胡广壮, 刘蓉 2021 应用化工 50 638 Google Scholar Han Z, Chen Y T, Zhang W, Xu C, Hu G Z, Liu R 2021 Appl. Chem. Indus. 50 638 Google Scholar
[3]	田龙, 豆维新, 杨玮婷, 王成 2021 应用化学 38 84 Google Scholar Tian L, Dou W X, Yang W T Wang C 2021 Chin. J. Appl. Chem. 38 84 Google Scholar
[4]	Sharma S K, Sudarshan K, Yadav A K, Jha S N, Bhattacharyya D, Pujari P K 2019 J. Phys. Chem. C 123 22273 Google Scholar
[5]	He X, Chen D R, Wang W N 2020 Chem. Eng. J. 382 122825 Google Scholar
[6]	Chu Q, Zhang S, Li X, Guo P, Fu A, Liu B, Wang Y Y 2021 Chem-Asian J. 16 1233 Google Scholar
[7]	Ding R, Zheng W, Yang K, Dai Y, Ruan X, Yan X, He G 2020 Sep. Purif. Technol. 236 116209 Google Scholar
[8]	Kumar S, Srivastava R, Koh J 2020 J. CO₂Util. 41 101251 Google Scholar
[9]	Ralph F S C, Cohen S M, Yan W, Deng H X, Guillerm V, Eddaoudi M, Madden D G, Fairen-Jimenez D, Lyu H, Macreadie L K, Ji Z, Zhang Y Y, Wang B, Haase F, Wçll C, Zaremba O, Andreo J, Wuttke S, Diercks C S 2021 Angew. Chem. Int. Edit. 60 23946 Google Scholar
[10]	Ran J, Jaroniec M, Qiao S Z 2018 Adv. Mater. 30 1704649 Google Scholar
[11]	马生花, 马芙莲, 解玉龙 2020 硅酸盐通报 39 2993 Google Scholar Ma S H, Ma F L, Xie Y L 2020 Bull. Chin. Ceramic Soc. 39 2993 Google Scholar
[12]	Jin C X, Shang H B 2021 J. Solid State Chem. 297 122040 Google Scholar
[13]	Nagarjun N, Arthy K, Dhakshinamoorthy A 2021 Eur. J. Inorg. Chem. 2021 2108 Google Scholar
[14]	邹伦妃, 马振超, 王苏龙, 白宇森, 王亚珍 2021 电源技术 45 512 Google Scholar Zou L F, Ma Z C, Wang S L, Bai Y S, Wang Y Z 2021 Power Technology 45 512 Google Scholar
[15]	Yao B, Lua S K, Lim H S, Zhang Q, Cui X, White T J, Ting V P, Dong Z 2021 Micropor. Mesopor. Mat. 314 110777 Google Scholar
[16]	Barrett E P, Joyner L G, Halenda P P 1951 J. Am. Chem. Soc. 73 373 Google Scholar
[17]	Brunauer S, Emmett P H, Teller E 1938 J. Am. Chem. Soc. 60 309 Google Scholar
[18]	Jean Y C 2003 Principles and Applications of Positron & Positronium Chemistry (World Scientific Pub Co Inc. (March 31)) p267
[19]	Tao S J 1972 J. Chem. Phys. 56 5499 Google Scholar
[20]	Eldrup M, Lightbody D, Sherwood J N 1981 Chem. Phys. 63 51 Google Scholar
[21]	Goworek T, Ciesielski K, Jasinska B, Wawryszczuk J 1998 Chem. Phys. 230 305 Google Scholar
[22]	Dull T L, Frieze W E, Gidley D W 2001 J. Phys. Chem. B 105 4657 Google Scholar
[23]	Li C Y, Qi N, Liu Z W, Zhou B, Chen Z Q, Wang Z 2016 Appl. Surf. Sci. 363 445 Google Scholar
[24]	王少阶, 陈志权, 王波, 吴奕初, 方鹏飞, 张永学 2008 应用正电子谱学 (湖北: 湖北科学技术出版社) 第198页 Wang S J, Chen Z Q, Wang B, Wu Y C, Fang P F, Zhang Y X 2008 Applied Positron Spectroscopy (Hubei: Hubei Science and Technology Press) p198 (in Chinese)
[25]	Jean Y C, Lu X, Lou Y, Bharathi A, Sundar C S, Lyu Y, Hor P H, Chu C W 1992 Phys. Rev. B 45 12126 Google Scholar
[26]	Matthias T, Katsumi K, Alexander V N, James P O, Francisco R R, Jean R, Kenneth S W S 2015 Pure Appl. Chem. 87 1051 Google Scholar
[27]	Davis M E 2002 Nature 417 813 Google Scholar
[28]	Paulin R, Ambrosino G 1968 J. Phys. France 29 263 Google Scholar
[29]	Lahtinen J, Hautojärvi P 1997 J. Phys. Chem. B 101 1609 Google Scholar
[30]	Eldrup M, Vehanen A, Schultz P J, Lynn K G 1984 Phys. Rev. Lett. 53 954 Google Scholar
[31]	Ito K, Nakanishi H, Ujihira Y 1999 J. Phys. Chem. B 103 4555 Google Scholar
[32]	Zhang H J, Chen Z Q, Wang S J, Kawasuso A, Morishita N 2010 Phys. Rev. B 82 035439 Google Scholar
[33]	Zhang H J, Liu Z W, Chen Z Q, Wang S J 2011 Chin. Phys. Lett. 28 017802 Google Scholar
[34]	Chen Z Q, Kawasuso A, Xu Y, Naramoto H, Yuan X L, Sekiguchi T, Suzuki R, Ohdaira T 2005 Phys. Rev. B 71 115213 Google Scholar
[35]	Lazzarini A L F, Lazzarini E, Mariani M 1993 J. Chem. Soc. Faraday Trans. 89 3737 Google Scholar
[36]	Lazzarini A L F, Lazzarini E, Mariani M 1994 J. Chem. Soc. Faraday Trans. 90 423 Google Scholar

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