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Breathing Europium-Terbium Co-doped Luminescent MOF as a Broad-Range Ratiometric Thermometer with a Contrasting Temperature-Intensity Relationship.

ABSTRACT: Solvothermal reactions of lanthanide salts and a semirigid tripodal H₃tatab (4,4',4?-s-triazine-1,3,5-triyltri-p-aminobenzoic acid) ligand in mixed water and N-methyl pyrrolidone (NMP) generated novel breathing MOFs [Ln(tatab)]·solvent (Ln = Eu in 1-Eu, Tb in 1-Tb, Eu_0.015Tb_0.985 in 1-Eu_0.015Tb_0.985). The framework of 1 was contracted upon removal of guests to form partly desolvated [Ln (tatab)]·3.7H₂O·2.5NMP (1'). Single-crystal X-ray analyses demonstrated that 1 has the breathing ability to spontaneously release guests and maintain the same topology. In contrast to as-synthesized 1, the cell volume of 1' decreased markedly upon removal of the guests. Different from linear dicarboxylates, the semirigid tripodal tatab ligand is bridged to an inorganic Ln-O chain, limiting the rotation around the O-O-axis of carboxylate. The breathing mechanism is based on the flexible C-N-C angles of amide bonds in the tatab ligand, causing a change in the solvent-accessible volume in the framework. Interestingly, the luminescence color of breathing co-doped lanthanide MOF 1'-Eu_0.015Tb_0.985 is blue-shifted and turned from orange to green with an increase in temperature, which can be attributed to a change in the relative intensity of Tb and Eu emissions, and is quite different from that observed for the reported related compounds. The breathing co-doped lanthanide MOF 1'-Eu_0.015Tb_0.985 can be applied as a high-sensitivity ratiometric thermometer in a broad temperature from 90 to 300 K.

SUBMITTER: Yao J

PROVIDER: S-EPMC6641742 | biostudies-literature | 2018 May

REPOSITORIES: biostudies-literature

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Breathing Europium-Terbium Co-doped Luminescent MOF as a Broad-Range Ratiometric Thermometer with a Contrasting Temperature-Intensity Relationship.

Yao Jin J Zhao Yan-Wu YW Zhang Xian-Ming XM

ACS omega 20180529 5

Solvothermal reactions of lanthanide salts and a semirigid tripodal H3tatab (4,4',4″-s-triazine-1,3,5-triyltri-p-aminobenzoic acid) ligand in mixed water and N-methyl pyrrolidone (NMP) generated novel breathing MOFs [Ln(tatab)]·solvent (Ln = Eu in 1-Eu, Tb in 1-Tb, Eu0.015Tb0.985 in 1-Eu0.015Tb0.985). The framework of 1 was contracted upon removal of guests to form partly desolvated [Ln (tatab ...[more]

PMID: 31458775

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Project description:Luminescence thermometry is a remote temperature measurement technique that relies on thermally induced changes in spectroscopic properties. Because of its great application potential, even under very demanding conditions where other techniques fail, it has attracted the attention of many researchers in recent years. Unfortunately, most of the existing luminescence thermometers are fraught with large inaccuracies and thus are not reliable enough to be applied in real and demanding applications. However, there is one of the most recent and very promising but insufficiently studied approaches to luminescence thermometry quantification - single-band ratiometric luminescence thermometry. It is based on the analysis of the luminescence intensity ratio of a single emission band being photoexcited in two ways, i.e. by ground (GSA) and excited (ESA) state absorption. It is characterized by high relative sensitivity to temperature changes as well as high measurement precision. However, because ESA-excited luminescence intensity can depend on the type and concentration of dopant ions or the properties of the host material, further more-detailed studies must be conducted to understand the impact of numerous photophysical processes on the relative sensitivity, temperature resolution and useful temperature range of SBR LTs. In this work, the effect of interionic interactions occurring through cross-relaxation on the thermometric properties of single-band ratiometric luminescent thermometers in NaYF4:Nd3+ and NaGdF4:Nd3+ was investigated and discussed. In contrast to the disadvantageous concentration quenching phenomenon that is typically observed at an increased content of dopants, the beneficial role of cross-relaxation in the enhancement of the signal-to-noise ratio of the ESA-excited luminescence at high temperatures was demonstrated. The maximum relative temperature sensitivity reached was equal to S R = 16.9% K-1 at 223 K for NaYF4:50%Nd3+ nanocrystals and its value remained above 1% K-1 throughout the whole analyzed temperature range from 223 K to 473 K.

Dataset Information

Breathing Europium-Terbium Co-doped Luminescent MOF as a Broad-Range Ratiometric Thermometer with a Contrasting Temperature-Intensity Relationship.

Publications

Breathing Europium-Terbium Co-doped Luminescent MOF as a Broad-Range Ratiometric Thermometer with a Contrasting Temperature-Intensity Relationship.

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