Co-reporter:Dr. Liang Zhao;Jianwei Wei;Junhua Lu; Cheng He; Chunying Duan
Angewandte Chemie International Edition 2017 Volume 56(Issue 30) pp:8692-8696
Publication Date(Web):2017/07/17
DOI:10.1002/anie.201702926
AbstractUsing small molecules with defined pockets to catalyze chemical transformations resulted in attractive catalytic syntheses that echo the remarkable properties of enzymes. By modulating the active site of a nicotinamide adenine dinucleotide (NADH) model in a redox-active molecular flask, we combined biomimetic hydrogenation with in situ regeneration of the active site in a one-pot transformation using light as a clean energy source. This molecular flask facilitates the encapsulation of benzoxazinones for biomimetic hydrogenation of the substrates within the inner space of the flask using the active sites of the NADH models. The redox-active metal centers provide an active hydrogen source by light-driven proton reduction outside the pocket, allowing the in situ regeneration of the NADH models under irradiation. This new synthetic platform, which offers control over the location of the redox events, provides a regenerating system that exhibits high selectivity and efficiency and is extendable to benzoxazinone and quinoxalinone systems.
Co-reporter:Dr. Liang Zhao;Jianwei Wei;Junhua Lu; Cheng He; Chunying Duan
Angewandte Chemie 2017 Volume 129(Issue 30) pp:8818-8822
Publication Date(Web):2017/07/17
DOI:10.1002/ange.201702926
AbstractUsing small molecules with defined pockets to catalyze chemical transformations resulted in attractive catalytic syntheses that echo the remarkable properties of enzymes. By modulating the active site of a nicotinamide adenine dinucleotide (NADH) model in a redox-active molecular flask, we combined biomimetic hydrogenation with in situ regeneration of the active site in a one-pot transformation using light as a clean energy source. This molecular flask facilitates the encapsulation of benzoxazinones for biomimetic hydrogenation of the substrates within the inner space of the flask using the active sites of the NADH models. The redox-active metal centers provide an active hydrogen source by light-driven proton reduction outside the pocket, allowing the in situ regeneration of the NADH models under irradiation. This new synthetic platform, which offers control over the location of the redox events, provides a regenerating system that exhibits high selectivity and efficiency and is extendable to benzoxazinone and quinoxalinone systems.
Co-reporter:Lu Yang;Liang Zhao;Zhen Zhou;Hui Sun;Chunying Duan
Dalton Transactions 2017 vol. 46(Issue 12) pp:4086-4092
Publication Date(Web):2017/03/21
DOI:10.1039/C6DT04299F
A discrete tetranuclear thiourea-based metal–organic macrocycle (MOM) with a large size was constructed by a well-designed organic ligand and nickel(II) ions via self-assembly. Incorporating thiourea groups as hydrogen-bond donors into a metal–organic complex system leads to a new approach for synthesizing functionalized heterogeneous catalysts, as this not only introduces coordination sites serving as chelators, but also overcomes the issues of self-association via intermolecular H-bonding, often occurring in homogeneous systems. The packing structure of this material formed a confined environment suitable for the access of substrate molecules dragged by the strong hydrogen-bond interactions from the thiourea groups, thus achieving a high catalytic performance in Michael additions of nitrostyrenes to nitroalkanes, with remarkable yields and size-selectivity in heterogeneous phase. Moreover, a comparison of the IR spectrum of Ni–SPT with the spectra of dimethyl malonate- and β-nitrostyrene-impregnated Ni–SPT indicated that both substrate molecules, β-nitrostyrene and dimethyl malonate, were able to access the cavity of the trimeric subunit.
Co-reporter:Xuezhao Li, Jinguo Wu, Liyong Chen, Xiaoming Zhong, Cheng He, Rong Zhang and Chunying Duan
Chemical Communications 2016 vol. 52(Issue 62) pp:9628-9631
Publication Date(Web):14 Jun 2016
DOI:10.1039/C6CC04647A
By introducing photoactive fac-tris(2-phenylpyridine)iridium moieties as a ligand backbone to constrain the coordination geometry of cobalt ions, a multifunctional Ir2Co3-type capsule was achieved and showed induced-fit capsule–capsule conversion by cooperative binding one carbonate anion with the equatorial Co(II) centers. The capsule combined photocatalysis and transition metal activation synergistically and exhibited efficient catalytic ability on visible light-activated α-trichloromethylation.
Co-reporter:Xuezhao Li, Jinguo Wu, Cheng He, Rong Zhang and Chunying Duan
Chemical Communications 2016 vol. 52(Issue 29) pp:5104-5107
Publication Date(Web):24 Feb 2016
DOI:10.1039/C6CC00064A
By incorporating a fac-tris(4-(2-pyridinyl)phenylamine)iridium as the backbone of the tripodal ligand to constrain the coordination geometry of Zn(II) ions, a pentanuclear Ir–Zn heterometal–organic luminescent polyhedron was obtained via a subcomponent self-assembly for carbon dioxide fixation and sulfite sequestration.
Co-reporter:Pengyan Wu, Xiangyang Guo, Linjuan Cheng, Cheng He, Jian Wang, and Chunying Duan
Inorganic Chemistry 2016 Volume 55(Issue 16) pp:8153
Publication Date(Web):August 1, 2016
DOI:10.1021/acs.inorgchem.6b01267
The design of a new photocatalytic system and integrating the essential components in a structurally controlled manner to create artificially photosynthetic systems is high desirable. By incorporating a photoactive triphenylamine moiety to assemble a Gd-based metal–organic framework as a heterogeneous photosensitizer, new artificial systems were constructed for the proton and carbon dioxide reduction under irradiation. The assembled MOFs exhibited a one-dimensional metal-oxygen pillar that was connected together by the depronated TCA3– ligands to form a three-dimensional noninterpenetrating porous framework. The combining of proton reduction and/or the carbon dioxide reduction catalysts, i.e., the Fe-Fe hydrogenase active site models and the Ni(Cyclam) complexes, initiated a photoinduced single electron transfer from its excited state to the substrate. The system exhibited an initial TOF of 320 h–1 of hydrogen per catalyst and an overall quantum yield of about 0.21% and is able to reduce carbon dioxide under irradiation. The deposit of the photoactive Gd-TCA into the film of an α-Al2O3 plate provided a platform for the practical applications through prolonging the lifetime of the artifical system and allowed the easily operated devices being recyclable as a promising photocatalytic system.
Co-reporter:Lu Yang; Cheng He;Dr. Xin Liu;Jing Zhang;Hui Sun ;Dr. Huimin Guo
Chemistry - A European Journal 2016 Volume 22( Issue 15) pp:5253-5260
Publication Date(Web):
DOI:10.1002/chem.201504975
Abstract
By using redox-active nickel(II) ions as the connect nodes, a hexanuclear metal–organic cylinder (Ni-YL) was achieved through self-assembly with a large cavity and an opening windows capable to accommodate guest molecules. The suitable cavity of Ni-YL provides an opportunity to encapsulate the anionic ruthenium bipyridine derivative [Ru(dcbpy)3] (dcbpy=2,2′-bipyridine-4,4′-dicarboxylic acid) as the photosensitizer for light-driven reactions. The host–guest behavior between Ni-YL and [Ru(dcbpy)3] was investigated by mass spectrometry, NMR spectroscopy, and computational studies, revealing an effective binding of the guest [Ru(dcbpy)3] within the cavity of Ni-YL. Optical experiments suggested a pseudo-intramolecular photoinduced electron transfer (PET) process between the [Ru(dcbpy)3] and the host Ni-YL, leading to an efficient light-driven hydrogen production based on this system. Control experiments with a mononuclear Ni complex as a reference photocatalyst and the inactive [Fe(dcbpy)3] as an inhibitor for comparison were also performed to confirm such a supramolecular photocatalysis process.
Co-reporter:Xu Jing, Pengyan Wu, Xin Liu, Linlin Yang, Cheng He and Chunying Duan
New Journal of Chemistry 2015 vol. 39(Issue 2) pp:1051-1059
Publication Date(Web):26 Nov 2014
DOI:10.1039/C4NJ01540A
The photocatalytic hydrogen evolution inspired by the highly evolved, finely tuned molecular photo-synthetic systems in nature represents an important process in sustainable solar energy conversion for the near future. By incorporating a phosphine donor within a thiosemicarbazone moiety, a new proton reduction catalyst Ni−thioP, featuring Ni⋯H interactions was synthesized and structurally characterized. Single crystal structure analysis revealed that the C–S, C–N and N–N bond lengths were all within the normal range of the single and double bonds, suggesting the extensive electron delocalization over the ligand skeleton. The presence of Ni⋯H interactions relative to the amide group coupled with the easy proton migration pathway involving thioamide/thiolate exchange suggested that the thiosemicarbazone complexes could serve as promising candidates for proton reduction. Luminescence titrations exhibited that Ni−thioP served as efficient luminescent quenchers for the photosensitizer Fl, providing the possibilities for the excited state of Fl to activate these catalysts for proton reduction. The direct generation of hydrogen was achieved by carrying out the photolysis of a solution containing fluorescein as the photosensitizer, and triethylamine as the sacrificial and the redox catalysts. Ni−thioP exhibited high activity with a turnover number (TON) of 8000 moles of H2 per mole of the catalyst after 24 hours and an initial TOF larger than 500 moles of H2 per catalyst per hour. To further investigate the potential mechanism for proton reduction, calculations were also performed using density functional theory.
Co-reporter:Liang Zhao, Yang Liu, Cheng He, Jian Wang and Chunying Duan
Dalton Transactions 2014 vol. 43(Issue 1) pp:335-343
Publication Date(Web):08 Oct 2013
DOI:10.1039/C3DT51900G
Novel cerium-based ‘Molecular Lanterns’ Ce-DBDS, Ce-DBBS and Ce-DBOS were achieved via self-assembly from bis-tridentate ligands H4DBDS, H4DBBS and H4DBOS, respectively. Structure analysis of Ce-DBDS shows that six oxygen atoms of the ether bond groups on the ligands form a lantern-like cavity inside the compound. Thus the ‘Molecular Lanterns’ exhibit crown ether recognition behavior and could be applied in luminescent magnesium chemosensors. The restricted geometry constraints of the internal cavities provide high selectivities of the lantern-like probes towards the Mg2+ ion over other different-sized metal ions such as Al3+, Li+, Ca2+, Na+, Ba2+ and K+. Ce-DBBS which contains three fully substituted benzyl groups exhibited better sensitivity by the cation–π interaction between Mg2+ and the benzyl group, compared to the Ce-DBDS. However, Ce-DBOS can work as an artificial chemosensor for selective fluorescent detection of Al3+ rather than Mg2+, due to its cavity being much smaller than Ce-DBDS and Ce-DBBS.
Co-reporter:Jing Zhang, Hao Yu, Caixia Zhang, Cheng He and Chunying Duan
New Journal of Chemistry 2014 vol. 38(Issue 7) pp:3137-3145
Publication Date(Web):26 Mar 2014
DOI:10.1039/C4NJ00062E
The application of metal–organic polyhedrons as “molecular flasks” has resulted in a surge of interest in the reactivity and properties of molecules within their well-defined cavity. Inspired by the structures of the natural enzymatic pockets, two neutral metal–organic tetrahedrons, Ce-TBMN and Ce-TBAS, were achieved via self-assembly by incorporating triamine-triazine and amide groups as hydrogen bond sites into the fragments of the ligands respectively. Both of them could act as molecular flasks to prompt the Knoevenagel condensation reactions of salicylaldehyde derivatives and cyanosilylation reactions of aromatic aldehydes. Experiments of catalysts with different cavity radii and substrates with different sizes and shapes, as well as competitive experiments using nonreactive guests as inhibitors demonstrated that the tetrahedrons exhibited enzymatically catalytic behavior and the catalytic reactions occurred in the “molecular flasks”. Control experiments with the H6TMBN or H6TBAS ligands themselves as the catalyst in the Knoevenagel condensation were carried out under the same conditions. For the smaller substrates, their conversions catalyzed by the ligands were significantly lower than those catalyzed by Ce-TBMN or Ce-TBAS, respectively, suggesting that metal–organic polyhedrons could effectively fix multi hydrogen bond groups to avoid the “self-quenching” effect, enhancing the catalytic activity of the multi-hydrogen bond groups in the homogeneous state.
Co-reporter:Yang Jiao, Jing Zhang, Lejie Zhang, Zhihua Lin, Cheng He and Chunying Duan
Chemical Communications 2012 vol. 48(Issue 48) pp:6022-6024
Publication Date(Web):24 Apr 2012
DOI:10.1039/C2CC30497J
An octa-nuclear bicoronal Ce-based triangular prism and tetra-nuclear molecular tetrahedron containing 36 and 24 folds amides within their main backbones were achieved and structurally characterized for the selective luminescent recognition of lactose and sucrose, respectively, over other related natural mono- and disaccharides.
Co-reporter:Xiao Wu, Zhihua Lin, Cheng He and Chunying Duan
New Journal of Chemistry 2012 vol. 36(Issue 1) pp:161-167
Publication Date(Web):15 Nov 2011
DOI:10.1039/C1NJ20736A
Channel-like and cage-like porous molecular materials Tb–PT1 and Sm–PT1 were constructed through packing and stacking of the amide-containing lanthanide-based octahedra [Tb6(H3L)4 (NO3)9-3H+]6+ and [Sm6(H3L)4(NO3)12]6+, respectively, where H3L is N′,N′,N′′-tris(pyridin-2-ylmethylene)benzene-1,3,5-tricarbohydrazide. Catalytic experiments on cyanosilylation reactions exhibited that the loading of only 1 mol% of Tb–PT1 leads to >90% conversion of the products with all the three nitrobenzaldehydes (NBA), but less than 10% conversion in the case of large size 3-formyl-1-phenylene-3 and 5-di-tert-butylbenzoate (BA) substrates. Adsorption of the substrates in the catalyst demonstrated a 3:1 mole ratio (per octahedron) of these nitrobenzaldehydes, but no adsorption of BA could be observed. Luminescent detection of the suspension of Tb–PT1 in CH2Cl2 solution exhibited that the presence of nitrobenzaldehydes quenched the emissions efficiently, whereas the addition of BA did not cause any significant spectra variations. All these results revealed that the catalytic performance of Tb–PT1 was size-selective and the interactions corresponding to the Tb3+ sites were dominant in activating the aldehydes. The catalytic experiments on aldol reactions between cyclohexanone and these aldehydes exhibited that the smallest 4-NBA substrate has the largest conversion (80%) over the others. The presence of cyclohexanone led to absorption spectral changes and luminescence enhancements of the catalyst. These results suggested that interactions between cyclohexanone and the amide groups were dominant in activating the cyclohexanone and the aldol reactions possibly occurred within the cavities of the octahedron. Evaluation of catalytic performance of Sm–PT1 in which those channels in Tb–PT1 were blocked upon cyanosilylation and aldol reactions as well as the adsorption experiments were also carried out for a comparison.
Co-reporter:Jian Wang ; Cheng He ; Pengyan Wu ; Jing Wang ;Chunying Duan
Journal of the American Chemical Society 2011 Volume 133(Issue 32) pp:12402-12405
Publication Date(Web):July 12, 2011
DOI:10.1021/ja2048489
Metal–organic polyhedra represent a unique class of functional molecular containers that display interesting molecular recognition properties and fascinating reactivity reminiscent of the natural enzymes. By incorporating a triphenylamine moiety as a bright blue emitter, a robust cerium-based tetrahedron was developed as a luminescent detector of nitronyl nitroxide (PTIO), a specific spin-labeling nitric oxide (NO) trapper. The tetrahedron encapsulates molecules of NO and PTIO within the cavity to prompt the spin-trapping reaction and transforms the normal EPR responses into a more sensitively luminescent signaling system with the limit of detection improved to 5 nM. Twelve-fold amide groups are also functionalized within the tetrahedron to modify the hydrophilic/lipophilic environment, ensuring the successful application of biological imaging in living cells.
Co-reporter:Xiaoyue Hu, Jian Wang, Xiang Zhu, Dapeng Dong, Xiaolin Zhang, Shuo Wu and Chunying Duan
Chemical Communications 2011 vol. 47(Issue 41) pp:11507-11509
Publication Date(Web):26 Sep 2011
DOI:10.1039/C1CC14032A
A copper(II) complex CuRBT with a ring-closed rhodamine-containing tripodal ligand was synthesized as a highly selective fluorescent imaging agent for nitric oxide (NO). It featured a 700-fold fluorescent enhancement toward NO from a dark-background with the detection limit of NO about 1 nM in aqueous solution and could be applied for monitoring intracellular NO.
Co-reporter:Liang Zhao, Siyi Qu, Cheng He, Rong Zhang and Chunying Duan
Chemical Communications 2011 vol. 47(Issue 33) pp:9387-9389
Publication Date(Web):18 Jul 2011
DOI:10.1039/C1CC12766G
By incorporating NOO tridentate chelators into rationally designed ligand systems, a well-defined molecular cube Ce-TBDS and a bicoronal trigonal prism Ce-TBBS were achieved viaself-assembly and the luminescence recognition of natural saccharides with Ce-TBBS were also investigated.
Co-reporter:Jian Wang;Dr. Hongmei Wu;Liang Zhao ; Chunying Duan
Chemistry – An Asian Journal 2011 Volume 6( Issue 5) pp:1225-1233
Publication Date(Web):
DOI:10.1002/asia.201000733
Abstract
Two trinuclear zinc-based cyclohelicates, Zn–PDB (PDB=[5-(dibenzylamino)-N1′,N3′-bis(pyridin-2-ylmethylene)isophthalohydrazide]) and Zn–PMB (PMB=[5-(bodipy-oxy)-N1′,N3′-bis(pyridin-2-ylmethylene)isophthalohydrazide]) containing dibenzylamino and BODIPY groups, respectively, were generated by incorporating two amide-containing tridentate chelators into meta-positions of a substituted phenyl ring. Single-crystal structure analysis and related spectroscopic characterizations demonstrated the formation of macrocyclic helicals both in the solid state and in solution. The host–guest behavior of the cyclohelical hosts towards γ-glutamyl-cysteinyl-glycine (GSH) and its component amino acids was investigated by spectroscopic titrations. UV/Vis absorption titration and NMR titrations of Zn–PDB and Zn–PMB upon addition of the above-mentioned guests suggested that the Glu residue of GSH was positioned within the cavity. The COO− groups interacted with metal ions through static interactions. The Cys moiety of GSH interacted with the amide groups sited in host molecules through hydrogen-bonding interactions to produce measurable spectral changes. Fluorescent titrations of Zn–PMB upon the addition of GSH and ESI-MS investigations of the titration solutions confirmed the host–guest interaction modes and revealed the possible 1:1 complexation stoichiometry. These results showed that the recognition of a substrate within the cavity of functionalized metal–organic cage-like receptors could be a useful method to produce supramolecular sensors for biomolecules.
Co-reporter:Yang Liu, Zhihua Lin, Cheng He, Liang Zhao and Chunying Duan
Dalton Transactions 2010 vol. 39(Issue 46) pp:11122-11125
Publication Date(Web):29 Sep 2010
DOI:10.1039/C0DT01086C
A well-defined Ce-based molecular tetrahedron and a cube-like architecture were achieved via self-assembly by incorporating NOO tridentate chelators into the rationally designed ligands with C3 or C2v symmetries, respectively.
Co-reporter:Yang Liu, Xiao Wu, Cheng He, Yang Jiao and Chunying Duan
Chemical Communications 2009 (Issue 48) pp:7554-7556
Publication Date(Web):09 Nov 2009
DOI:10.1039/B915358F
New Ce-based Werner type tetrahedrons were achieved for size-selectively luminescent detection of natural carbohydrates through incorporating amide groups as both the multiple hydrogen bonding triggers and binding-signalling transductor.
Co-reporter:Hongmei Wu, Cheng He, Zhihua Lin, Yang Liu and Chunying Duan
Inorganic Chemistry 2009 Volume 48(Issue 2) pp:408-410
Publication Date(Web):December 12, 2008
DOI:10.1021/ic801350h
Metallohelical triangles consisting of chromophore units and hydrogen-bonding trigger sites were prepared by modulating two tridentate N2O units containing amide groups within a central benzene ring at the meta sites, for the selective detection of adenosine trisphosphate in aqueous media over other ribonucleotides.
Co-reporter:Wei Huang, Xiang Zhu, Dayu Wua, Cheng He, Xiaoyue Hu and Chunying Duan
Dalton Transactions 2009 (Issue 47) pp:10457-10465
Publication Date(Web):14 Oct 2009
DOI:10.1039/B914490K
In virtue of the sulfurphilic nature of Hg2+, three new sensors RN1, RN2 and RST1 that combine a thiophene group and one or two rhodamine choromophores, or a thiospirolactam rhodamine chromophore, were designed and prepared for the selective detection of Hg2+ in aqueous media, respectively. These sensors all displayed good brightness and fluorescence enhancement following Hg2+ coordination with limits of detection for Hg2+ at the ppb level. Thus, they have the potential for distinguishing between safe and toxic levels of inorganic mercury in drinking water. RN1 exhibited chromogenic and fluorogenic selectivity over alkali, alkaline earth metals, divalent first-row transition metal ions as well as heavy metals, but the presence of Cu2+ had a small but significant influence on the absorption detection of Hg2+. Compared to RN1, the introduction of sufficient sulfur atoms could increase the binding capability of RST1 towards Hg2+ relative to the sensor RN1, but decrease its Hg specific ability. The existence of some heavy and transition metal ions, such as Pb2+, Ag+, Cu2+ enhance the silent absorption spectra of RST1. Spectral evidence and X-ray structural investigations of the mercury complex revealed a possible 1:2 complexation behaviour between the Hg2+ ion and the sensor RN1 or RST1. Sensor RN2 which contains two rhodamine carboxhydrazone arms exhibited better selectivity, compared to those of RN1 and RST1. The addition of Cu2+ only caused a small interference for the absorption detection of Hg2+ under the same conditions, demonstrating the efficiency of the robust bis-chelating mode with regard to the selectivity for Hg2+.
Co-reporter:Liang Zhao, Siyi Qu, Cheng He, Rong Zhang and Chunying Duan
Chemical Communications 2011 - vol. 47(Issue 33) pp:NaN9389-9389
Publication Date(Web):2011/07/18
DOI:10.1039/C1CC12766G
By incorporating NOO tridentate chelators into rationally designed ligand systems, a well-defined molecular cube Ce-TBDS and a bicoronal trigonal prism Ce-TBBS were achieved viaself-assembly and the luminescence recognition of natural saccharides with Ce-TBBS were also investigated.
Co-reporter:Hao Yu, Cheng He, Jing Xu, Chunying Duan and Joost N. H. Reek
Inorganic Chemistry Frontiers 2016 - vol. 3(Issue 10) pp:
Publication Date(Web):
DOI:10.1039/C6QI00211K
Co-reporter:Lu Yang, Liang Zhao, Zhen Zhou, Cheng He, Hui Sun and Chunying Duan
Dalton Transactions 2017 - vol. 46(Issue 12) pp:NaN4092-4092
Publication Date(Web):2017/02/22
DOI:10.1039/C6DT04299F
A discrete tetranuclear thiourea-based metal–organic macrocycle (MOM) with a large size was constructed by a well-designed organic ligand and nickel(II) ions via self-assembly. Incorporating thiourea groups as hydrogen-bond donors into a metal–organic complex system leads to a new approach for synthesizing functionalized heterogeneous catalysts, as this not only introduces coordination sites serving as chelators, but also overcomes the issues of self-association via intermolecular H-bonding, often occurring in homogeneous systems. The packing structure of this material formed a confined environment suitable for the access of substrate molecules dragged by the strong hydrogen-bond interactions from the thiourea groups, thus achieving a high catalytic performance in Michael additions of nitrostyrenes to nitroalkanes, with remarkable yields and size-selectivity in heterogeneous phase. Moreover, a comparison of the IR spectrum of Ni–SPT with the spectra of dimethyl malonate- and β-nitrostyrene-impregnated Ni–SPT indicated that both substrate molecules, β-nitrostyrene and dimethyl malonate, were able to access the cavity of the trimeric subunit.
Co-reporter:Xuezhao Li, Jinguo Wu, Cheng He, Rong Zhang and Chunying Duan
Chemical Communications 2016 - vol. 52(Issue 29) pp:NaN5107-5107
Publication Date(Web):2016/02/24
DOI:10.1039/C6CC00064A
By incorporating a fac-tris(4-(2-pyridinyl)phenylamine)iridium as the backbone of the tripodal ligand to constrain the coordination geometry of Zn(II) ions, a pentanuclear Ir–Zn heterometal–organic luminescent polyhedron was obtained via a subcomponent self-assembly for carbon dioxide fixation and sulfite sequestration.
Co-reporter:Xuezhao Li, Jinguo Wu, Liyong Chen, Xiaoming Zhong, Cheng He, Rong Zhang and Chunying Duan
Chemical Communications 2016 - vol. 52(Issue 62) pp:NaN9631-9631
Publication Date(Web):2016/06/14
DOI:10.1039/C6CC04647A
By introducing photoactive fac-tris(2-phenylpyridine)iridium moieties as a ligand backbone to constrain the coordination geometry of cobalt ions, a multifunctional Ir2Co3-type capsule was achieved and showed induced-fit capsule–capsule conversion by cooperative binding one carbonate anion with the equatorial Co(II) centers. The capsule combined photocatalysis and transition metal activation synergistically and exhibited efficient catalytic ability on visible light-activated α-trichloromethylation.
Co-reporter:Yang Jiao, Jing Zhang, Lejie Zhang, Zhihua Lin, Cheng He and Chunying Duan
Chemical Communications 2012 - vol. 48(Issue 48) pp:NaN6024-6024
Publication Date(Web):2012/04/24
DOI:10.1039/C2CC30497J
An octa-nuclear bicoronal Ce-based triangular prism and tetra-nuclear molecular tetrahedron containing 36 and 24 folds amides within their main backbones were achieved and structurally characterized for the selective luminescent recognition of lactose and sucrose, respectively, over other related natural mono- and disaccharides.
Co-reporter:Yang Liu, Xiao Wu, Cheng He, Yang Jiao and Chunying Duan
Chemical Communications 2009(Issue 48) pp:
Publication Date(Web):
DOI:10.1039/B915358F
Co-reporter:Xiaoyue Hu, Jian Wang, Xiang Zhu, Dapeng Dong, Xiaolin Zhang, Shuo Wu and Chunying Duan
Chemical Communications 2011 - vol. 47(Issue 41) pp:NaN11509-11509
Publication Date(Web):2011/09/26
DOI:10.1039/C1CC14032A
A copper(II) complex CuRBT with a ring-closed rhodamine-containing tripodal ligand was synthesized as a highly selective fluorescent imaging agent for nitric oxide (NO). It featured a 700-fold fluorescent enhancement toward NO from a dark-background with the detection limit of NO about 1 nM in aqueous solution and could be applied for monitoring intracellular NO.
Co-reporter:Yang Liu, Zhihua Lin, Cheng He, Liang Zhao and Chunying Duan
Dalton Transactions 2010 - vol. 39(Issue 46) pp:NaN11125-11125
Publication Date(Web):2010/09/29
DOI:10.1039/C0DT01086C
A well-defined Ce-based molecular tetrahedron and a cube-like architecture were achieved via self-assembly by incorporating NOO tridentate chelators into the rationally designed ligands with C3 or C2v symmetries, respectively.
Co-reporter:Wei Huang, Xiang Zhu, Dayu Wua, Cheng He, Xiaoyue Hu and Chunying Duan
Dalton Transactions 2009(Issue 47) pp:NaN10465-10465
Publication Date(Web):2009/10/14
DOI:10.1039/B914490K
In virtue of the sulfurphilic nature of Hg2+, three new sensors RN1, RN2 and RST1 that combine a thiophene group and one or two rhodamine choromophores, or a thiospirolactam rhodamine chromophore, were designed and prepared for the selective detection of Hg2+ in aqueous media, respectively. These sensors all displayed good brightness and fluorescence enhancement following Hg2+ coordination with limits of detection for Hg2+ at the ppb level. Thus, they have the potential for distinguishing between safe and toxic levels of inorganic mercury in drinking water. RN1 exhibited chromogenic and fluorogenic selectivity over alkali, alkaline earth metals, divalent first-row transition metal ions as well as heavy metals, but the presence of Cu2+ had a small but significant influence on the absorption detection of Hg2+. Compared to RN1, the introduction of sufficient sulfur atoms could increase the binding capability of RST1 towards Hg2+ relative to the sensor RN1, but decrease its Hg specific ability. The existence of some heavy and transition metal ions, such as Pb2+, Ag+, Cu2+ enhance the silent absorption spectra of RST1. Spectral evidence and X-ray structural investigations of the mercury complex revealed a possible 1:2 complexation behaviour between the Hg2+ ion and the sensor RN1 or RST1. Sensor RN2 which contains two rhodamine carboxhydrazone arms exhibited better selectivity, compared to those of RN1 and RST1. The addition of Cu2+ only caused a small interference for the absorption detection of Hg2+ under the same conditions, demonstrating the efficiency of the robust bis-chelating mode with regard to the selectivity for Hg2+.
Co-reporter:Liang Zhao, Yang Liu, Cheng He, Jian Wang and Chunying Duan
Dalton Transactions 2014 - vol. 43(Issue 1) pp:NaN343-343
Publication Date(Web):2013/10/08
DOI:10.1039/C3DT51900G
Novel cerium-based ‘Molecular Lanterns’ Ce-DBDS, Ce-DBBS and Ce-DBOS were achieved via self-assembly from bis-tridentate ligands H4DBDS, H4DBBS and H4DBOS, respectively. Structure analysis of Ce-DBDS shows that six oxygen atoms of the ether bond groups on the ligands form a lantern-like cavity inside the compound. Thus the ‘Molecular Lanterns’ exhibit crown ether recognition behavior and could be applied in luminescent magnesium chemosensors. The restricted geometry constraints of the internal cavities provide high selectivities of the lantern-like probes towards the Mg2+ ion over other different-sized metal ions such as Al3+, Li+, Ca2+, Na+, Ba2+ and K+. Ce-DBBS which contains three fully substituted benzyl groups exhibited better sensitivity by the cation–π interaction between Mg2+ and the benzyl group, compared to the Ce-DBDS. However, Ce-DBOS can work as an artificial chemosensor for selective fluorescent detection of Al3+ rather than Mg2+, due to its cavity being much smaller than Ce-DBDS and Ce-DBBS.
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ACETATE](http://img.cochemist.com/ccimg/360100/360072-54-4.png)
ACETATE](http://img.cochemist.com/ccimg/360100/360072-54-4_b.png)
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