SHORT COMMUNICATION
DOI:10.1002/ejic.201402395
A Luminescent Ruthenium Azide Complex as a Substrate
for Copper-Catalyzed Click Reactions
Anne Kroll,
[a]
Katharina Monczak,
[a]
Dieter Sorsche,
[a]
and
Sven Rau*
[a]
Keywords: Ruthenium / Click chemistry / Copper / Azides / Photodynamic therapy
A new ligand and its luminescent polypyridyl–Ru
II
complex
were synthesized and characterized. Both provide two azide
functionalities in their periphery, which are electronically
separated from the π-system of the 2,2'-bipyridine ligands
by a methylene group. This azide-functionalized ruthenium
complex provides access to the formerly inaccessible sub-
strate spectrum of alkynyl-functionalized coupling substrates
by using the copper(I)-catalyzed azide–alkyne cycloaddition
Introduction
Coupling of luminescent molecules to biological targets
such as proteins is of increasing importance for detailed
analysis of biological processes.
[1]
An efficient method
towards this aim is the copper(I)-catalyzed azide–alkyne cy-
cloaddition (CuAAC), which was invented in 2002 by
Sharpless and Medal; it is probably one of the most well-
known reactions in the wide field of coupling chemistry
based on Claisen–Huisgen cycloadditions.
[2,3]
Products of
this click reaction possess a 1,4-disubstituted-1,2,3-triazole
bridge that is selectively formed under copper(I) catalysis.
Polypyridyl–ruthenium complexes are very interesting chro-
mophores owing to their highly relevant photophysical
properties such as large Stokes shift, long lifetimes of the
luminescent excited state, and their interesting electrochemi-
cal properties.
[4,5]
Furthermore, they may possess thera-
peutic potential based on their photochemistry.
[6]
Very re-
cently, it was shown that polypyridyl–Ru
II
complexes them-
selves could be used as substrates in click reactions.
[7–9]
However, only alkynyl-substituted luminescent ruthenium
complexes have been utilized so far because of the instabil-
ity of the azide-substituted complexes.
[7]
Interestingly, the
newly formed triazole moiety, the product of the CuAAC,
may be used as a complexation site itself. This was recently
exploited for the formation of various polypyridyl–metal
complexes.
[10–14]
To develop the applicability of CuAAC
[a] The University of Ulm, Institute of Inorganic Chemistry 1,
Materials and Catalysis,
Albert-Einstein-Allee 11, 89081 Ulm, Germany
E-mail: sven.rau@uni-ulm.de
http://www.uni-ulm.de/nawi/nawi-anorg1/startseite.html
Supporting information for this article is available on the
WWW under http://dx.doi.org/10.1002/ejic.201402395.
Eur. J. Inorg. Chem. 2014, 3462–3466 © 2014 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 3462
(CuAAC). Test CuAAC reactions were performed on the li-
gand and directly on the Ru
II
complex by using phenylacetyl-
ene as a model substrate, and relatively high yields of the
products were obtained under mild conditions. Transforma-
tion of the azide into the triazole had only minor influences
on the photophysical properties of the polypyridyl–ruth-
enium core.
further it is necessary to design azide-containing polypyri-
dyl ligands that form stable luminescent polypyridyl–ruth-
enium complexes and to establish their suitability as click
substrates. To the best of our knowledge, only one report
exists in which a ruthenium azide complex, non-lumines-
cent [Ru(p-cymene)(4-azido-2,2'-bipyridine)Cl]
+
, was suc-
cessfully linked through CuAAC.
[9]
Recently published az-
ide-functionalized Ir
III
complexes were converted success-
fully in click reactions. The very low extinction coefficients
of these compounds below 400 nm limit their applicability
as sensors in biological systems.
[15]
Furthermore, it would
be desirable if the photophysical properties of the lumines-
cent ruthenium complex would not change significantly af-
ter the CuAAC reaction. The results of Baron et al. for click
reactions on their alkyne-functionalized complex show that
there is a very small difference in the emission maxima for
the precursor alkyne complex in comparison to that of the
clicked products (up to 13 nm).
[7,16]
Importantly, one of the
“clicked” systems of Chitre et al., in which aromatic azide
functionalities were bound to the bipyridine ligand precur-
sor, showed no luminescence at all.
[8]
To the best of our
knowledge, there are difficulties in performing click reac-
tions on polypyridyl–Ru
II
complexes that bear azide func-
tionalities because of the instability of aromatic azides on
2,2'-bipyridine ligands.
[7]
Accordingly, all alkynyl-function-
alized substrates known to date are not accessible for the
introduction of luminescent metal cores with CuAAC. An
approach towards solving this problem could be to separate
the azide electronically from the π-system of the 2,2'-bipyr-
idine ligands by methylene groups in the sterically opti-
mized 4,4'-positions. Recent results on the successful click
chemistry with the corresponding 5,5' isomer at copper
complexes support the assumption that the 4,4' isomer