Co-reporter:Kai Wei, Zongchun Gao, Huarong Liu, Xiaojun Wu, Feng Wang, and Hangxun Xu
ACS Macro Letters October 17, 2017 Volume 6(Issue 10) pp:1146-1146
Publication Date(Web):September 29, 2017
DOI:10.1021/acsmacrolett.7b00487
Harnessing mechanical forces to activate latent catalysts has emerged as a novel approach to control the catalytic reactions in organic syntheses and polymerization processes. However, using polymer mechanochemistry to activate platinum-based catalysts, a class of important organometallic catalysts in industry, has not been demonstrated so far. Here we show that the platinum–acetylide complex is mechanoresponsive and can be incorporated into a polymer backbone to form a new mechanophore. The mechanically induced chain scission was demonstrated to be able to release catalytically active platinum species which could catalyze the olefin hydrosilylation process. Various control experiments were conducted to confirm that the chain scission and catalytic reaction were originated from the ultrasound-induced dissociation of platinum–acetylide complex. This work further exemplifies the utilization of organometallic complexes in design and synthesis of latent catalysts for mechanocatalysis and development of self-healing materials based on silicone polymers.
Co-reporter:Zijian Li, Yifei Han, Zongchun Gao, and Feng Wang
ACS Catalysis July 7, 2017 Volume 7(Issue 7) pp:4676-4676
Publication Date(Web):June 6, 2017
DOI:10.1021/acscatal.7b00709
Visible-light photosensitizers have emerged as a sustainable and environmentally friendly medium for organic transformation. Herein, we have developed a supramolecular strategy for manipulating visible-light photosensitization and photocatalytic efficiencies. With the elaborate manipulation of aggregated Pt(II)···Pt(II) interactions, the discrete tetranuclear Pt complexes not only show high binding affinity (Ka ∼ 106 M–1) but also feature bathochromic-shifted metal–metal-to-ligand charge transfer transitions. Both factors are crucial for their 1O2 generation capability upon low-energy visible-light irradiation (λ ≥ 590 nm). More interestingly, when a terpyridine moiety is embedded in the structure of a supramolecular photosensitizer, breakup of tetranuclear Pt(II)···Pt(II) complexation can be realized upon addition of Zn(OTf)2. As a consequence, photo-oxidation of a secondary amine to the corresponding imine can be deactivated and reactivated, via the sequential addition of Zn(OTf)2 and unsubstituted terpyridine as the competitive ligand. Hence, the current study proves that intelligent visible-light photocatalysts can be achieved via rational supramolecular design.Keywords: organometallic chemistry; photocatalysis; photosensitizer; Pt(II)···Pt(II) metal−metal bonds; supramolecular chemistry;
Co-reporter:Xiao Wang;Yifei Han;Yingying Liu; Gang Zou;Zhao Gao; Feng Wang
Angewandte Chemie International Edition 2017 Volume 56(Issue 41) pp:12466-12470
Publication Date(Web):2017/10/02
DOI:10.1002/anie.201704294
AbstractOne-dimensional organic structures with well-oriented π-aggregation, strong emission, and ease of processability are desirable for optoelectronic waveguiding devices. Herein, a strategy is developed to attain this objective by self-assembling platinum(II) acetylides into fluorescent supramolecular polymers via cooperative mechanism. The resulting high-molecular-weight supramolecular polymers are capable of forming electrospun microfibers with uniform geometry and smooth surface, which enable light propagation with extremely low scattering loss (0.008 dB μm−1). With the elaborate combination of bottom-up supramolecular polymerization and top-down electrospinning techniques, this work offers a novel and versatile avenue toward high-performance optical waveguiding materials.
Co-reporter:Jiangjun Chen;Zhongxin Zhang;Chengming Wang;Zhao Gao;Zongchun Gao
Chemical Communications 2017 vol. 53(Issue 84) pp:11552-11555
Publication Date(Web):2017/10/19
DOI:10.1039/C7CC05613C
With the synergistic combination of intermolecular Au(I)–Au(I) and hydrogen bonding interactions, a rod–coil alkynyl–gold(I)–isocyanide monomer tends to form supramolecular fibers and gels via a cooperative nucleation–elongation self-assembly mechanism, which display Ag(I) ion-triggered responsiveness.
Co-reporter:Peng Wang, Zhao Gao, Ming Yuan, Junlong Zhu and Feng Wang
Polymer Chemistry 2016 vol. 7(Issue 22) pp:3664-3668
Publication Date(Web):12 Apr 2016
DOI:10.1039/C6PY00494F
Mechanically linked poly[2]rotaxanes have been designed and synthesized on the basis of the benzo-21-crown-7/secondary ammonium salt recognition motif, which displays interesting thermal and rheological properties due to the integration of [2]rotaxane moieties into the polycaprolactone chains.
Co-reporter:Xiao Wang, Zongchun Gao, Junlong Zhu, Zhao Gao and Feng Wang
Polymer Chemistry 2016 vol. 7(Issue 33) pp:5217-5220
Publication Date(Web):26 Jul 2016
DOI:10.1039/C6PY01109H
A rod-coil cyanostilbene amphiphile, which is prone to form self-assembled micelles with aggregation induced emission properties, serves as a novel platform for the fabrication of a FRET-based ratiometric sensor, leading to highly sensitive and specific detection of mercury ions in water.
Co-reporter:Huaqing Liu;Xiaohang Han;Zongchun Gao;Zhao Gao
Macromolecular Rapid Communications 2016 Volume 37( Issue 8) pp:718-724
Publication Date(Web):
DOI:10.1002/marc.201500695
Co-reporter:Jianlin Peng, Yonggang Shi, Zhishuai Yang, Meiling Qi, Feng Wang
Journal of Chromatography A 2016 Volume 1466() pp:129-135
Publication Date(Web):30 September 2016
DOI:10.1016/j.chroma.2016.08.070
•Unique amphiphilic selectivity for apolar to polar analytes.•High-resolution capability for structural and positional isomers.•Good column inertness for analytes prone to peak tailing.Dicyanuric-functionalized polycaprolactone (DPCL) was explored for its separation performance in gas chromatography (GC). The statically coated DPCL capillary column (0.25 mm, i.d.) showed column efficiency of 3460 plates/m determined by naphthalene at 120 °C. McReynolds constants and Abrahaḿs system constants were also determined to evaluate the polarity and possible molecular interactions of the stationary phase. As a result, DPCL column exhibited excellent separation performance for diverse types of analytes with good peak shapes. Most interestingly, it shows unique amphiphilic selectivity and high-resolution capability for both apolar to polar isomers. In addition, DPCL column had good column repeatability with the RSD values below 0.06% for run-to-run, 0.09–0.40% for day-to-day and 1.7–3.6% for column-to-column, and good thermal stability up to 280 °C. The high selectivity and resolving capability demonstrate the great advantages of the DPCL stationary phase for simultaneous determination of analytes of great variety in complex samples.
Co-reporter:Xiaoqin Lv, Yifei Han, Zhishuai Yang, Zijian Li, Zhao Gao, Feng Wang
Tetrahedron Letters 2016 Volume 57(Issue 18) pp:1971-1975
Publication Date(Web):4 May 2016
DOI:10.1016/j.tetlet.2016.03.080
•The designed molecular tweezer is pre-organized by intramolecular hydrogen bonds.•It shows moderate binding affinity towards the organometallic guests.•The molecular tweezer/guest complexes display interesting optical behaviours.•Addition of HFIP leads to the release of guest from the molecular tweezer receptor.A novel molecular tweezer consisting of 2,2′-iminodibenzoyl backbone and alkynylplatinum(II) terpyridine pincers is designed and synthesized. It shows moderate binding strengths towards two neutral organometallic guests, accompanying with interesting optical behaviours due to the involvement of donor–acceptor and metal–metal interactions. Notably, addition of polar solvent, hexafluoroisopropanol, cleavages intramolecular NH⋯O hydrogen bonds and thereby triggers conformational change for the molecular tweezer receptor. Consequently, molecular tweezer/guest complexation could be significantly influenced, benefiting for further construction of intelligent molecular machines and devices.
Co-reporter:Teng-Fei Fu, Lei Ao, Zong-Chun Gao, Xiao-Long Zhang, Feng Wang
Chinese Chemical Letters 2016 Volume 27(Issue 8) pp:1147-1154
Publication Date(Web):August 2016
DOI:10.1016/j.cclet.2016.06.054
Organoplatinum(II) compounds have received enormous attention over the past decades due to their square-planar geometry as well as intriguing photo-physical properties. Self-assembly has emerged as an excellent approach to create well-ordered supramolecular architectures with tunable properties, which underpin the role of solvent-directed approach for the design of functional materials. In this mini-review, the recent advances on supramolecular self-assembly of cyclometalated platinum(II) complexes have been discussed. During the self-assembly process, non-covalent Pt–Pt and π–π interactions play crucial roles in controlling the structures and functions of the resulting assemblies.Schematic representation for the self-assembly of cyclometalated platinum(II) complexes into various morphologies.
Co-reporter:Yu-Kui Tian, Yi-Fei Han, Zhi-Shuai Yang, and Feng Wang
Macromolecules 2016 Volume 49(Issue 17) pp:6455-6461
Publication Date(Web):August 26, 2016
DOI:10.1021/acs.macromol.6b01032
Molecular tweezer/guest recognition has emerged as a novel motif for the construction of supramolecular polymers. However, the overwhelming majority of ADA- or DAD-type (D = donor, A = acceptor) molecular tweezer/guest recognition systems suffer from relatively low binding affinities and inconspicuous variations toward external stimuli. To address this issue, herein a novel heterodimeric DADA-type complex has been designed and constructed. By engineering of donor–acceptor and hydrogen-bonding interactions, it demonstrates 1000 times enhancement for the complexation strength (Ka = 2.23 × 106 M–1) than the ADA-type counterpart. Moreover, by modulating the intermolecular hydrogen bonds involved in the system, its binding affinity exhibits significantly large variations toward external stimuli (∼102–103-fold change for Ka). The robust yet adaptive heterodimeric complex is employed as a tecton for the fabrication of high-molecular-weight donor–acceptor-type supramolecular polymers, demonstrating the efficiency and versatility to develop self-assembled materials via rational engineering of fundamental noncovalent recognition motifs.
Co-reporter:Zhao Gao;Yifei Han;Jiangjun Chen;Xiao Wang ;Dr. Feng Wang
Chemistry – An Asian Journal 2016 Volume 11( Issue 12) pp:1775-1779
Publication Date(Web):
DOI:10.1002/asia.201600364
Abstract
Trimethylammonium-derived alkynylplatinum(II) terpyridine molecular tweezers have been designed and synthesized in this manuscript. They show moderate binding affinity towards the complementary organoplatinum guest in polar media, such as DMSO, methanol, and water, even though the guest itself is sparingly soluble in the latter two solvents. Responsive guest encapsulation/release from the cavity of molecular tweezers can be achieved by successive addition and removal of trifluoroacetic acid, accompanying with remarkable switching of the photophysical signals, which would benefit for the fabrication of intelligent supramolecular materials with tailored functionalities.
Co-reporter:Tengfei Fu, Yifei Han, Lei Ao, and Feng Wang
Organometallics 2016 Volume 35(Issue 17) pp:2850-2853
Publication Date(Web):August 16, 2016
DOI:10.1021/acs.organomet.6b00429
The binding affinity between alkynylplatinum(II) terpyridine molecular tweezer and naphthol-derived guests can be significantly enhanced by embedding an intermolecular O–H---N hydrogen bond, facilitating the achievement of a responsive host–guest recognition system via the photolabile “caging” strategy.
Co-reporter:Zhishuai Yang, Yonggang Shi, Wen Chen and Feng Wang
Polymer Chemistry 2015 vol. 6(Issue 31) pp:5540-5544
Publication Date(Web):12 Feb 2015
DOI:10.1039/C4PY01591F
Two architecturally controlled supramolecular polymers have been fabricated via the concurrent integration of orthogonal Hamilton receptor/cyanuric acid and benzo-21-crown-7/secondary ammonium salt recognition motifs, demonstrating significant chain topological-dependent supramolecular polymerization behaviours.
Co-reporter:Entai Shi, Zhao Gao, Ming Yuan, Xiaoyu Wang and Feng Wang
Polymer Chemistry 2015 vol. 6(Issue 31) pp:5575-5579
Publication Date(Web):26 Jun 2015
DOI:10.1039/C5PY00239G
Benzothiadiazole-functionalized dinuclear platinum(II) acetylide bolaamphiphiles have been demonstrated to form nanoparticles in protic solvents, serving as novel fluorescent labels for bio-imaging applications with good biocompatibility and sufficient stability.
Co-reporter:Yonggang Shi, Zhishuai Yang, Huaqing Liu, Zijian Li, Yukui Tian, and Feng Wang
ACS Macro Letters 2015 Volume 4(Issue 1) pp:6
Publication Date(Web):December 10, 2014
DOI:10.1021/mz500659f
Mechanically linked poly[2]rotaxanes have been successfully constructed via the hierarchical self-assembly strategy. The integration of two noninterfering noncovalent recognition motifs facilitates chain extension of the B21C7-based [2]rotaxane monomer, demonstrating the capabilities to form self-standing films with preferable transparency and softness.
Co-reporter:Yu-Jing Tian, En-Tai Shi, Yu-Kui Tian, Ri-Sheng Yao, and Feng Wang
Organic Letters 2014 Volume 16(Issue 12) pp:3180-3183
Publication Date(Web):June 3, 2014
DOI:10.1021/ol500752b
A platinum(II) acetylide-based bolaamphiphile equipped with two peripheral B18C6 moieties has been successfully prepared, which demonstrates cooperative recognition behavior toward l-alanine ester salt in chloroform. In a polar methanol/chloroform (3/1, v/v) medium, the amino acid additives influence the aggregation of the bolaamphiphile significantly, leading to the morphological transition from nanospherical to disordered structures. The adaptive properties of the current host–guest binary system will benefit the development of stimuli-responsive supramolecular materials.
Co-reporter:Yu-Kui Tian, Zhi-Shuai Yang, Xiao-Qin Lv, Ri-Sheng Yao and Feng Wang
Chemical Communications 2014 vol. 50(Issue 67) pp:9477-9480
Publication Date(Web):02 Jun 2014
DOI:10.1039/C4CC03158J
A bis-alkynylplatinum(II) terpyridine tweezer–alkynylgold(III) diphenylpyridine guest is shown to maintain the specific complexation in the presence of a B21C7–secondary ammonium salt recognition motif, which facilitates the formation of supramolecular hyperbranched polymers via the “tweezering directed self-assembly” strategy.
Co-reporter:Yangyang Xu, Hao Jiang, Qijin Zhang, Feng Wang and Gang Zou
Chemical Communications 2014 vol. 50(Issue 3) pp:365-367
Publication Date(Web):29 Oct 2013
DOI:10.1039/C3CC47245K
Herein the enantio-selective polymerization of diacetylene (DA) units in the discotic hydrogen-bonding complex is carried out in an asymmetric reaction field consisting of the lamellar columnar LC phase and CPUL stimulus.
Co-reporter:Yu-Kui Tian
Macromolecular Rapid Communications 2014 Volume 35( Issue 3) pp:337-343
Publication Date(Web):
DOI:10.1002/marc.201300742
Co-reporter:Yu-Kui Tian;Yong-Gang Shi;Zhi-Shuai Yang ;Dr. Feng Wang
Angewandte Chemie 2014 Volume 126( Issue 24) pp:6204-6208
Publication Date(Web):
DOI:10.1002/ange.201402192
Abstract
Supramolecular polymers are constructed based on the novel bis[alkynylplatinum(II)] terpyridine molecular tweezer/pyrene recognition motif. Successive addition of anthracene as the diene and cyano-functionalized dienophile triggers the reversible supramolecular polymerization process, thus advancing the concept of utilizing Diels–Alder chemistry to access stimuli-responsive materials in compartmentalized systems.
Co-reporter:Yu-Kui Tian;Yong-Gang Shi;Zhi-Shuai Yang ;Dr. Feng Wang
Angewandte Chemie International Edition 2014 Volume 53( Issue 24) pp:6090-6094
Publication Date(Web):
DOI:10.1002/anie.201402192
Abstract
Supramolecular polymers are constructed based on the novel bis[alkynylplatinum(II)] terpyridine molecular tweezer/pyrene recognition motif. Successive addition of anthracene as the diene and cyano-functionalized dienophile triggers the reversible supramolecular polymerization process, thus advancing the concept of utilizing Diels–Alder chemistry to access stimuli-responsive materials in compartmentalized systems.
Co-reporter:Yue Ding, Peng Wang, Yu-Kui Tian, Yu-Jing Tian and Feng Wang
Chemical Communications 2013 vol. 49(Issue 53) pp:5951-5953
Publication Date(Web):13 May 2013
DOI:10.1039/C3CC42511H
Linear supramolecular polymers, assembled via the combination of orthogonal terpyridine–Zn2+ and benzo-21-crown-7/secondary ammonium salt recognition motifs, exhibit dynamic properties responsive to various external stimuli.
Co-reporter:Yu-Jing Tian, E. W. Meijer and Feng Wang
Chemical Communications 2013 vol. 49(Issue 80) pp:9197-9199
Publication Date(Web):07 Aug 2013
DOI:10.1039/C3CC44997A
Rod-like platinum(II) acetylide complexes have been demonstrated to form one-dimensional helical supramolecular polymers by the cooperative growth mechanism, leading to supramolecular gels by bundling single fibrils into entangled networks.
Co-reporter:Yu-Kui Tian, Long Chen, Yu-Jing Tian, Xiao-Yu Wang and Feng Wang
Polymer Chemistry 2013 vol. 4(Issue 3) pp:453-457
Publication Date(Web):30 Nov 2012
DOI:10.1039/C2PY20984E
A novel supramolecular polymer network has been successfully constructed using a heterometallic coordination-driven self-assembly strategy. Moreover, triggered by a variety of competitive ligands, the supramolecular network could be reversibly assembled/disassembled and thereby demonstrates dynamic properties.
Co-reporter:Long Chen, Yu-Kui Tian, Yue Ding, Yu-Jing Tian, and Feng Wang
Macromolecules 2012 Volume 45(Issue 20) pp:8412-8419
Publication Date(Web):October 10, 2012
DOI:10.1021/ma3016486
A facile route is demonstrated to realize the supramolecular cross-linked networks based on the benzo-21-crown-7/secondary ammonium salt recognition motif, which involves the interchain host–guest interactions between the secondary ammonium salt-functionalized polystyrene and the complementary homoditopic benzo-21-crown-7 cross-linker. Reversible addition–fragmentation chain transfer polymerization is utilized to prepare the well-defined secondary ammonium salt-functionalized graft polymer. As determined by 1H NMR and GPC, the molecular weight Mn is 13.3 kDa with polydispersity value of 1.10, suggesting that 15.9 repeating units of secondary ammonium salt moieties exist in a single polymer chain. The properties of the resulting supramolecular cross-linked networks are characterized in solution by means of 1H NMR titration and viscosity measurements, which indicate the growth of entangled polymer chains after the efficient host–guest complexation. At high concentrations of acetonitrile, the interpenetrating three-dimensional networks could entrap large amounts of solvent and thereby lead to the formation of supramolecular gels, which exhibit multistimuli (thermo-, pH-, and chemo-) responsive sol–gel transition behaviors. Such a strategy will benefit for the further development of intelligent supramolecular materials with desired functionalities.
Co-reporter:Zijian Li, Yifei Han, Fan Jin, Zongchun Gao, Zhao Gao, Lei Ao and Feng Wang
Dalton Transactions 2016 - vol. 45(Issue 43) pp:NaN17295-17295
Publication Date(Web):2016/09/26
DOI:10.1039/C6DT03160A
A novel bis[alkynylplatinum(II)] terpyridine molecular tweezer with conformationally-rigid spacer has been designed and synthesized, which shows enhanced binding affinity towards the complementary guests when compared to its semi-rigid counterpart. Moreover, a three-component supramolecular recognition system comprised of the molecular tweezer and two electron-rich guests was established. Reversible switching of the host–guest binding preference can be achieved via adding a trace amount of hexafluoroisopropanol (HFIP) into chloroform. Such a system will be interesting for the future construction of intelligent molecular machines and devices.
Co-reporter:Yu-Kui Tian, Zhi-Shuai Yang, Xiao-Qin Lv, Ri-Sheng Yao and Feng Wang
Chemical Communications 2014 - vol. 50(Issue 67) pp:NaN9480-9480
Publication Date(Web):2014/06/02
DOI:10.1039/C4CC03158J
A bis-alkynylplatinum(II) terpyridine tweezer–alkynylgold(III) diphenylpyridine guest is shown to maintain the specific complexation in the presence of a B21C7–secondary ammonium salt recognition motif, which facilitates the formation of supramolecular hyperbranched polymers via the “tweezering directed self-assembly” strategy.
Co-reporter:Yangyang Xu, Hao Jiang, Qijin Zhang, Feng Wang and Gang Zou
Chemical Communications 2014 - vol. 50(Issue 3) pp:NaN367-367
Publication Date(Web):2013/10/29
DOI:10.1039/C3CC47245K
Herein the enantio-selective polymerization of diacetylene (DA) units in the discotic hydrogen-bonding complex is carried out in an asymmetric reaction field consisting of the lamellar columnar LC phase and CPUL stimulus.
Co-reporter:Yue Ding, Peng Wang, Yu-Kui Tian, Yu-Jing Tian and Feng Wang
Chemical Communications 2013 - vol. 49(Issue 53) pp:NaN5953-5953
Publication Date(Web):2013/05/13
DOI:10.1039/C3CC42511H
Linear supramolecular polymers, assembled via the combination of orthogonal terpyridine–Zn2+ and benzo-21-crown-7/secondary ammonium salt recognition motifs, exhibit dynamic properties responsive to various external stimuli.
Co-reporter:Yu-Jing Tian, E. W. Meijer and Feng Wang
Chemical Communications 2013 - vol. 49(Issue 80) pp:NaN9199-9199
Publication Date(Web):2013/08/07
DOI:10.1039/C3CC44997A
Rod-like platinum(II) acetylide complexes have been demonstrated to form one-dimensional helical supramolecular polymers by the cooperative growth mechanism, leading to supramolecular gels by bundling single fibrils into entangled networks.
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