TY - JOUR
T1 - Dissolution-Recrystallization
T2 - A Novel Mechanism for Fluorochromic Detection of Th4+ Using Color-Tunable Luminescent Metal–Organic Frameworks
AU - Cui, Yunyi
AU - Lu, Huangjie
AU - Hou, Huiliang
AU - Bai, Yaoyao
AU - Yang, Junpu
AU - Li, Yarui
AU - Qiu, Jie
AU - Wang, Shuao
AU - Lin, Jian
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024/11/11
Y1 - 2024/11/11
N2 - Thorium, a predominant actinide in the Earth's crust, presents significant environmental and health risks due to its radioactive nature. These risks are particularly pronounced during the mining and processing of monazite for rare earth elements (REEs), which contain substantial thorium concentrations. Current instrumental analysis methods for thorium, offer high accuracy but require laborious sample preparations and expensive instruments, making them unsuitable for on-site analysis. Herein, we present a class of color-tunable luminescent lanthanide-based metal–organic frameworks (Ln-MOFs) as fluorochromic sensors for Th4+ cations. Utilizing a heterobimetallic Eu3+/Tb3+ doping strategy, the luminescence colors of EuxTb1-x-BDC-OH can be finely tuned from red, to orange, and to green. More intriguingly, the higher Lewis acidity of Th4+ facilitates the transformation of EuxTb1-x-BDC-OH into a UiO-type Th-MOF via a dissolution-recrystallization mechanism. This process results in a gradual reduction of characteristic Ln3+ emissions and the emergence of blue color ligand-based fluorescence, thereby leading to selective fluorochromic responses with increasing Th4+ concentrations and enabling visible detection of Th4+ cations. Additionally, a custom-built portable optoelectronic device is fabricated, which directly converts luminescence colors into red-green-blue (RGB) values. This device enables easy quantification of Th4+ concentrations without the need for complex instrumentation.
AB - Thorium, a predominant actinide in the Earth's crust, presents significant environmental and health risks due to its radioactive nature. These risks are particularly pronounced during the mining and processing of monazite for rare earth elements (REEs), which contain substantial thorium concentrations. Current instrumental analysis methods for thorium, offer high accuracy but require laborious sample preparations and expensive instruments, making them unsuitable for on-site analysis. Herein, we present a class of color-tunable luminescent lanthanide-based metal–organic frameworks (Ln-MOFs) as fluorochromic sensors for Th4+ cations. Utilizing a heterobimetallic Eu3+/Tb3+ doping strategy, the luminescence colors of EuxTb1-x-BDC-OH can be finely tuned from red, to orange, and to green. More intriguingly, the higher Lewis acidity of Th4+ facilitates the transformation of EuxTb1-x-BDC-OH into a UiO-type Th-MOF via a dissolution-recrystallization mechanism. This process results in a gradual reduction of characteristic Ln3+ emissions and the emergence of blue color ligand-based fluorescence, thereby leading to selective fluorochromic responses with increasing Th4+ concentrations and enabling visible detection of Th4+ cations. Additionally, a custom-built portable optoelectronic device is fabricated, which directly converts luminescence colors into red-green-blue (RGB) values. This device enables easy quantification of Th4+ concentrations without the need for complex instrumentation.
KW - Detection
KW - Dissolution-recrystallization
KW - Fluorochromic
KW - Metal–organic framework
KW - Thorium
UR - https://www.scopus.com/pages/publications/85208073305
U2 - 10.1002/anie.202410453
DO - 10.1002/anie.202410453
M3 - 文章
C2 - 39037423
AN - SCOPUS:85208073305
SN - 1433-7851
VL - 63
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 46
M1 - e202410453
ER -