We present the synthesis and characterization of novel square planar transition metal complexes of Schiff base ligands,which act as guanine quadruplex binders and stabilizers.The complexes stabilize quadruplexes relat...We present the synthesis and characterization of novel square planar transition metal complexes of Schiff base ligands,which act as guanine quadruplex binders and stabilizers.The complexes stabilize quadruplexes related to telomere stability or present in oncogene regulatory sequences,as determined by optical spectroscopy,pointing out the emergence of selectivity towards specific structures or sequences.These results are supported and rationalized by molecular modeling simulations.Furthermore,we show that the treatment of cancer cell lines with our complexes is associated with the increase in the number of nuclear guanine quadruplexes and the downregulation in the expression of the considered oncogenes.Remarkably,only very moderate cytotoxicity can be observed for all complexes.These results pave the way for the development of selective anticancer treatment by metal compounds targeting the expression of specific oncogenes.展开更多
It is a widely held view that the continuous hydrogen bonding network plays a crucial role in proton transport.Herein,we report the cyclic single-crystal-to-single-crystal transformation of three hydrogenbonded organi...It is a widely held view that the continuous hydrogen bonding network plays a crucial role in proton transport.Herein,we report the cyclic single-crystal-to-single-crystal transformation of three hydrogenbonded organic frameworks(HOFs),BPPA,BPPA-azo,and BPPA-gua,induced by the change of auxiliary ligands,which explicitly demonstrates that the hydrophilic interlayers of BPPA possess good self-adaptability to vip molecules.Their proton conducting performance was studied under different humidities at varying temperatures,indicating that the proton conductivity of BPPA with continuous hydrogen bonding networks formed by water molecules reaches 5.14×10^(−2)S cm^(−1) under 80℃ and 95% relative humidity(RH),which is four orders of magnitude higher than those of BPPA-azo and BPPA-gua with their continuous hydrogen bonding networks formed by 1,2,4-triazole and guanidine molecules,respectively,under the same conditions.The evidence from this study suggests that the rotational degrees of freedom of hydrogen bonding donors and acceptors play the most important role in the construction of efficient proton conduction pathways.展开更多
基金support of this work through Labex SEAM ANR 11 LABEX 086,ANR 11 IDEX 0502The authors thank Prof A.Palumbo Piccionello,University of Palermo,for his support with mass spectrometry,and Prof C.Kowol and Dr W.Kandioller,University of Vienna,and Dr Y.Bernhard,L2CM-UMR CNRS 7053,University of Lorraine,for their support with elemental analysis+1 种基金The support of the IdEx“Universite Paris 2019”ANR-18-IDEX-0001 is also acknowledgedThe financial support of the European Union-NextGenerationEU through the Italian Ministry of University and Research under PNRR-M4C2-I1.3 Project PE_00000019“HEAL ITALIA”CUP(B73C22001250006)is gratefully acknowledged.
文摘We present the synthesis and characterization of novel square planar transition metal complexes of Schiff base ligands,which act as guanine quadruplex binders and stabilizers.The complexes stabilize quadruplexes related to telomere stability or present in oncogene regulatory sequences,as determined by optical spectroscopy,pointing out the emergence of selectivity towards specific structures or sequences.These results are supported and rationalized by molecular modeling simulations.Furthermore,we show that the treatment of cancer cell lines with our complexes is associated with the increase in the number of nuclear guanine quadruplexes and the downregulation in the expression of the considered oncogenes.Remarkably,only very moderate cytotoxicity can be observed for all complexes.These results pave the way for the development of selective anticancer treatment by metal compounds targeting the expression of specific oncogenes.
基金supported by the National Natural Science Foundation of China(NSFC,Grant No.21771193,22275210,and 22201305)the Fundamental Research Funds for the Central Universities(22CX06024A)the Outstanding Youth Science Fund Projects of Shandong Province(2022HWYQ-070).
文摘It is a widely held view that the continuous hydrogen bonding network plays a crucial role in proton transport.Herein,we report the cyclic single-crystal-to-single-crystal transformation of three hydrogenbonded organic frameworks(HOFs),BPPA,BPPA-azo,and BPPA-gua,induced by the change of auxiliary ligands,which explicitly demonstrates that the hydrophilic interlayers of BPPA possess good self-adaptability to vip molecules.Their proton conducting performance was studied under different humidities at varying temperatures,indicating that the proton conductivity of BPPA with continuous hydrogen bonding networks formed by water molecules reaches 5.14×10^(−2)S cm^(−1) under 80℃ and 95% relative humidity(RH),which is four orders of magnitude higher than those of BPPA-azo and BPPA-gua with their continuous hydrogen bonding networks formed by 1,2,4-triazole and guanidine molecules,respectively,under the same conditions.The evidence from this study suggests that the rotational degrees of freedom of hydrogen bonding donors and acceptors play the most important role in the construction of efficient proton conduction pathways.