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2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 1 wileyonlinelibrary.com
1. Introduction
Detecting the concentration of oxygen is of great practical sig-
nificance,
[1]
and high-sensitivity sensors are highly demanded for
trace oxygen analyses in many environments that must be oxygen-
free such as metallurgy, chemical industry, and so on.
[2]
Optical
Porous Cu(I) Triazolate Framework and Derived Hybrid
Membrane with Exceptionally High Sensing Efficiency for
Gaseous Oxygen
Si-Yang Liu, Xiao-Lin Qi, Rui-Biao Lin, Xiao-Ning Cheng, Pei-Qin Liao, Jie-Peng Zhang,*
and Xiao-Ming Chen
Phosphorescent complexes of precious metal ions are widely studied as
optical sensing materials for molecular oxygen. Combining the advan-
tages of luminescent complexes and porous matrixes, porous coordination
polymers show great potential for oxygen-sensing, although their sensitivity,
requirement of precious metal, and device fabrication remain challenging
issues. In this work, the photoluminescence and oxygen-sensing proper-
ties of the porous Cu(I) triazolate framework [Cu(detz)] (MAF-2, Hdetz =
3,5-diethyl-1,2,4-trizole) is studied in detail, which shows high chemical
stability in moisture and water, very long phosphorescent lifetime (116
μs) and large Stokes shift (14562 cm
-1
), as well as considerable oxygen
permeability (1.7 × 10
-11
mol cm
-1
s
-1
bar
-1
) at ambient conditions, giving
rise to exceptionally high luminescence quenching efficiency of 99.7% at 1
bar O
2
( I
0
/ I
100
= 356) with a perfectly linear Stern-Volmer plot ( K
SV
= 356 bar
-1
,
R
2
= 0.9998), fast response and good reversibility. Further, a counter-diffusion
crystal-growth method was developed to fabricate MAF-2 thin films protected
by silicone rubbers as the first example of soft membrane oxygen sensor
based on coordination polymer or metal-organic framework, which exhibited
extraordinary oxygen-sensing performance (limit of detection = 0.047 mbar)
and outstanding mechanical property, as well as outstanding chemical sta-
bility even in an acidic atmosphere.
DOI: 10.1002/adfm.201401125
S.-Y. Liu, Dr. X.-L. Qi, R.-B. Lin, P.-Q. Liao,
Prof. Dr. J.-P. Zhang, Prof. Dr. X.-M. Chen
MOE Key Laboratory of Bioinorganic
and Synthetic Chemistry
State Key Laboratory of Optoelectronic
Materials and Technologies
School of Chemistry and Chemical Engineering
Sun Yat-Sen University
Guangzhou 510275, China
E-mail: zhangjp7@mail.sysu.edu.cn
Dr. X.-N. Cheng
Instrumental Analysis and Research Center
Sun Yat-Sen University
Guangzhou 510275, China
oxygen sensors based on luminescence
quenching have attracted a great deal of
attention for their high sensitivity and capa-
bility of online detections and non-invasion
measurements.
[3]
To fabricate a lumines-
cence sensor, luminescent dyes should be
immobilized on gas-permeable substrates,
most of which are in the membrane form.
[4]
It is worth pointing out that oxygen-sensing
luminescent dyes usually perform very dif-
ferently in the solution, bulk-solid, and thin-
film states,
[5]
and most sensing compounds
have never become sensors.
[3]
Although some florescent materials
have demonstrated high oxygen-sensing
efficiencies,
[6]
phosphorescent dyes, espe-
cially coordination complexes of precious
metal ions (Pt, Ru, Au, Ir, Re, etc.), are still
the most preferred choices for lumines-
cent sensing,
[7]
because phosphorescence
based on triplet excited state has high
quantum yield and luminescent intensity
(for high sensitivity), long lifetime (for
reducing the interference from scattered
light and fluorescence background, by
using time-resolved luminescence meas-
urement), and large Stokes shift (for easy
separation of excitation and emission).
[8]
Porous coordination polymers (PCPs) are highly ordered
arrays of metal complexes containing guest-accessible chan-
nels.
[9]
Various functionalities, such as luminescent building
blocks, can be rationally incorporated into PCPs.
[10]
By virtue
of their diverse and tunable structures, luminescent PCPs have
emerged as promising sensing materials for solvent, vapor, and
ion species.
[11]
Recently, a few oxygen-sensing PCPs have been
reported, which are mostly based on phosphorescent Ru(II)
or Ir(III) metalloligands.
[12]
So far, it is still very challenging
to reduce the precious metal content and increase the oxygen-
sensitivity of luminescent PCPs.
[6]
In addition, bulk PCP crys-
tals cannot be used directly in practical applications, especially
as gas sensors. The loose powders are difficult to handle as a
sensor unless they are processed or molded into applicable
configurations such as membranes.
[13]
Unlike molecular and
macromolecular luminescent dyes, PCPs are generally fragile,
crystalline and insoluble materials, which can be hardly made
into soft membrane devices for sensing.
[14]
Adv. Funct. Mater. 2014,
DOI: 10.1002/adfm.201401125
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