层状铀酰膦酸配位聚合物作为双响应光致发光温度计★

doi:10.6023/A23050242

化学学报 ›› 2023, Vol. 81 ›› Issue (10): 1311-1317.DOI: 10.6023/A23050242 上一篇下一篇

所属专题：庆祝《化学学报》创刊90周年合辑

研究论文

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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摘要/Abstract

具有光致发光性质的铀酰膦酸配位聚合物已经用于温度传感, 但尚未用于双响应发光温度计. 本工作报道了一种基于邻羧基苯甲基膦酸配体(2-pmbH₃)的层状铀酰膦酸配位聚合物, 即(α-C₈H₁₂N)[UO₂(2-pmb)] (1). 其中铀酰离子通过2-pmb³⁻配体连接成层, 外消旋且质子化的苯乙胺分子作为抗衡离子占据层间. 层内最近的U1···U1距离为0.541 nm. 化合物1表现出较高的热稳定性和水稳定性. 光致发光性质表明, 化合物1在室温下发出绿光, 可以在200~360 K的温度范围内作为发光强度和寿命的双响应发光温度计, 其强度依赖的最大灵敏度为2.96%•K⁻¹ (330 K), 寿命依赖的最大灵敏度为2.51%•K⁻¹ (350 K), 实现了工作温度更高、灵敏度更高的铀酰基温度计. 相对论密度泛函(DFT)计算证实了该化合物的稳定性来源于铀酰赤道面膦酸氧2p轨道与铀5f_ϕ轨道相互作用. 计算表明, 在320 nm和412 nm附近的两个峰为O=U=O内氧以及膦酸氧2p到铀5f_δ(f_z(x2−y2))的配体到金属电荷转移(LMCT).

关键词: 铀酰膦酸配位聚合物, 温度传感, 双响应发光温度计, 发光强度, 寿命, 相对论密度泛函

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

引用此文

温哥华, 温都日娜, 陈秀梅, 麻秀芳, 翁果果, 韦依凡, 鲍松松, 谢小吉, 胡淑贤, 郑丽敏. 层状铀酰膦酸配位聚合物作为双响应光致发光温度计^★[J]. 化学学报, 2023, 81(10): 1311-1317.

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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图/表 7

图1. (a) 化合物1的构筑单元; (b) 1的无机层结构; (c) 沿c轴方向1的堆积图(为了结构清晰, 氢原子被省略); (d) α-C8H12N分子沿c轴方向有序排列; (e) α-C8H12N分子上质子化的氨基基团与膦酸基团和铀酰离子间存在氢键相互作用

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

图2. (a) 1的热重-差热(TG-DSC)曲线; (b) 1在不同pH值水溶液和沸水浸泡24 h后的PXRD图

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

图3. (a) 1的吸收光谱; (b) 1的固态发射光谱

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

图4. (a) 1的总态密度; (b) 元素分波态密度; (c) 轨道分波态密度; (d) O元素的分波态密度; (e) 带边波函数

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

图5. (a)在80~420 K范围内(λex=310 nm)测试的发射光谱; (b) 516 nm处发射峰的变化趋势(灰色)及对应的猝灭曲线(黄色); (c) 1在200~360 K的温度范围内的相对发光强度变化(在516 nm处监测); (d) 1在200~360 K范围内的相对灵敏度

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

表1. 化合物1与其它稀土和铀酰配位聚合物材料的性能比较

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

图6. (a) 不同温度(200~360 K)下的发光衰减曲线(λem=516 nm); (b) 不同温度下的寿命; (c) 不同温度下寿命的相对灵敏度值; (d) 由δΔ/Δ=0.5%的灵敏度曲线计算最小温度不确定度

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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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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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^★