Layered Uranyl Phosphonate as A Dual-response Luminescence Thermometer★

doi:10.6023/A23050242

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (10): 1311-1317.DOI: 10.6023/A23050242 Previous Articles Next Articles

Special Issue: 庆祝《化学学报》创刊90周年合辑

Original article

层状铀酰膦酸配位聚合物作为双响应光致发光温度计^★

温哥华^a, 温都日娜^b, 陈秀梅^c, 麻秀芳^a, 翁果果^a, 韦依凡^a, 鲍松松^a, 谢小吉^c, 胡淑贤^b^,^*(), 郑丽敏^a^,^*()

a 南京大学化学化工学院配位化学国家重点实验室人工微结构科学与技术协同创新中心南京 210023
b 北京科技大学数理学院北京 100083
c 南京工业大学柔性电子(未来技术)学院&先进材料研究院南京 211816

投稿日期:2023-05-19 发布日期:2023-07-14
作者简介:
^★庆祝《化学学报》创刊90周年.
基金资助:
国家自然科学基金(21731003); 国家自然科学基金(21976014); 国家自然科学基金(22276013); 国家重点研究计划(2021YFB3501501)

Layered Uranyl Phosphonate as A Dual-response Luminescence Thermometer^★

Ge-Hua Wen^a, Wendurina^b, Xiumei Chen^c, Xiu-Fang Ma^a, Guo-Guo Weng^a, Yi-Fan Wei^a, Song-Song Bao^a, Xiaoji Xie^c, Shu-Xian Hu^b(), Li-Min Zheng^a()

a School of Chemistry and Chemical Engineering, Nanjing University, State Key Laboratory of Coordination Chemistry, Collaborative Innovation Center of Advanced Microstructures, Nanjing 210023, China
b School of Mathematics and Physics, University of Science and Technology Beijing, Beijing 100083, China
c School of Flexible Electronics (Future Technologies) & Institute of Advanced Materials (IAM), Nanjing Tech University (NanjingTech), Nanjing 211816, China

Received:2023-05-19 Published:2023-07-14
Contact: *E-mail: hushuxian@csrc.ac.cn; lmzheng@nju.edu.cn
About author:
^★Dedicated to the 90th anniversary of Acta Chimica Sinica.
Supported by:
National Natural Science Foundation of China(21731003); National Natural Science Foundation of China(21976014); National Natural Science Foundation of China(22276013); National Key Research Program(2021YFB3501501)

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Abstract

Luminescent uranyl phosphonate coordination polymers have been used for temperature sensing but have not yet been used for dual-response luminescence thermometers. Herein we report a luminescent uranyl phosphonate based on 2-(phosphonomethyl)benzoic acid (2-pmbH₃), namely, (α-C₈H₁₂N)[UO₂(2-pmb)] (1). This compound crystallizes in monoclinic space group C2/c and shows a layered structure. Within the layer, the uranyl ions are doubly bridged by O—P—O and O—C—O unis forming chains. The equivalent chains are cross-linked through corner-sharing of UO₇ pentagonal bipyramids and PO₃C tetrahedra forming a layer. The adjacent U···U distances within the layer are 0.5414 and 0.5743 nm. The organic groups of the 2-pmb³⁻ ligand reside on the two sides of the layer. The interlayer space is filled with the racemic protonated phenethylamine cations to charge-balance the anionic layer. The shortest U···U distance between the layers is 1.239 nm. Compound 1 exhibits high thermal and water stability, especially in aqueous solution at pH 5~11 and in boiling water. The UV-Vis spectrum of 1 shows two broad bands peaking at 320 and 412 nm. The scalar-relativistic density functional calculations reveal that the two bands are associated with ligand-to-metal charge transfer (LMCT) transitions from ligand orbitals to metal orbitals lower-f_δ (f_z(x2−y2)). Photoluminescence properties show that 1 emits green-light at room temperature with six emission peaks at 481, 500, 516, 540, 564 and 591 nm, assigned to the electronic and vibronic transitions of S₁₁-S₀₀ and S₁₀-S₀_ν (ν=0~4). Interestingly, both the emission intensity and the lifetime of compound 1 are temperature-dependent, making it possible to be used as a dual-response luminescence thermometer in the temperature range of 200~360 K. The intensity-dependent maximum sensitivity is 2.96%•K⁻¹ (330 K) and the lifetime-dependent maximum sensitivity is 2.51%•K⁻¹ (350 K), which are comparable to some lanthanide-based luminescent thermometers. This work provides a rare example of uranyl coordination polymers that can be used as a dual-response luminescence thermometer with wide operating temperature and good sensitivity.

Key words: uranyl phosphonate, temperature sensing, dual-response luminescence thermometer, luminescence intensity, lifetime, relativistic density-functional theory

Cite this article

Ge-Hua Wen, Wendurina, Xiumei Chen, Xiu-Fang Ma, Guo-Guo Weng, Yi-Fan Wei, Song-Song Bao, Xiaoji Xie, Shu-Xian Hu, Li-Min Zheng. Layered Uranyl Phosphonate as A Dual-response Luminescence Thermometer^★[J]. Acta Chimica Sinica, 2023, 81(10): 1311-1317.

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Fig. & Tab. 7

Figure 1. (a) Building unit of structure 1; (b) inorganic layer in structure 1; (c) packing diagram of structure 1 viewed along the c-axis (hydrogen atoms are omitted for clarity); (d) the α-C8H12N molecules arranged in the channel between the layers, viewed along the c-axis; (e) hydrogen bond interactions between the protonated amino group of α-C8H12N molecules and the phosphonate and uranyl oxygen atoms

Figure 2. (a) TG-DSC curve of 1; (b) PXRD patterns of 1 after soaked in aqueous solutions for 24 h at various pH and boiling water

Figure 3. (a) Absorption spectrum of 1; (b) solid-state emission spectra of 1

Figure 4. (a) Total density of state (TDOS); (b), (c), (d) projected density of states (PDOS); (e) contour plots (isovalue=0.05 au) of the band edges of 1

Figure 5. (a) Emission spectra of 1 recorded in the range of 80~420 K (λex=310 nm); (b) variation trends of emission peak at 516 nm (gray) and corresponding quenching curve (yellow); (c) plots showing the relative luminescence change (monitored at 516 nm) of 1 in the temperature range of 200~360 K; (d) relative sensitivity of 1 in the 200~360 K range

Materials	Intensity		Lifetime		Ref.
Materials	Temp. range/K	Max.S_r/(%•K⁻¹)	Temp. range/K	Max.S_r/(%•K⁻¹)	Ref.
Eu(bzac)₃(H₂O)₂	83~303	5.25 (303 K)	233~303	1.35 (293 K)	[10]
Eu(CPDK_3-5)₃phen	298~348	2.2 (298 K)	298~348	1.6 (348 K)	[11]
Eu(tta)₃(pyphen)	83~325	1.98 (323 K)	258~323	1.68 (323 K)	[12]
Tb₁₋_xEu_xFTPTC (x=0.05, 0.1, 0.2)	25~125	9.11 (125 K)	25~300	—	[13]
(Y_0.89Tb_0.10Eu_0.01)₆(BDC)₇(OH)₄(H₂O)₄	288~573	1.69 (523 K)	288~573	≈1.5 (523 K)	[14]
Eu_0.6Tb_1.4Pt₃	60~300	2.72 (263 K)	150~300	3.26 (239 K)	[15]
Eu_0.6Tb_1.4Pd₃	60~300	2.78 (279 K)	150~300	3.04 (266 K)	[15]
(UO₂)₂(1,3-pbp)(H₂O)₂•2H₂O	93~293	1.96	—	—	[23]
[BTEA]₂[(UO₂)₂(1,3-pbpH₂)₂F₂]	93~293	1.546	—	—	[24]
[(U^VIO₂)₄(U^VO₂)(μ-O)₄(H₂O)₄(BMBCP)₂]•NO₃	77~197	—	77~197	—	[30]
(UO₂)(2-pmbH₂)₂	120~300	0.9 (215 K)	—	—	[27]
(H₃O)[(UO₂)₂(2-pmb)(2-pmbH)]	100~300	2.16 (205 K)	—	—	[27]
(H₃O)[(UO₂)₂(2-pmb)(2-pmbH)]-ns@PMMA	100~300	1.19 (205 K)	—	—	[27]
1	200~360	2.96 (330 K)	200~360	2.51 (350 K)	This work

Table 1. Comparison of the performance of 1 with other lanthanide and uranyl coordination polymers

Figure 6. (a) Luminescence decay curves measured at various temperatures (200~360 K) for 1 (λem=516 nm); (b) lifetime of 1 at different temperatures; (c) relative sensitivity value Sr calculated at different temperatures; (d) the minimum temperature uncertainty calculated from the sensitivity curve for δΔ/Δ=0.5%

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层状铀酰膦酸配位聚合物作为双响应光致发光温度计^★

Layered Uranyl Phosphonate as A Dual-response Luminescence Thermometer^★

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References 44

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层状铀酰膦酸配位聚合物作为双响应光致发光温度计★

Layered Uranyl Phosphonate as A Dual-response Luminescence Thermometer★

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Supporting Info.

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Abstract

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Fig. & Tab. 7

References 44

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层状铀酰膦酸配位聚合物作为双响应光致发光温度计^★

Layered Uranyl Phosphonate as A Dual-response Luminescence Thermometer^★