Discovery of Novel SIRT3 Inhibitors for the Cancer Differentiation Therapy by Structural Modification.

Inhibition of SIRT3 triggered differentiation of multiple myeloma (MM) cells. In discovery of potent SIRT3 inhibitors for cancer differentiation therapy, structural modification was performed on the previously developed lead compound S27. A total of 49 compounds divided into two series were designed and synthesized.

Electromagnetic Mill-Promoted Palladium-Catalyzed Heck-Type Cyclization/Decarboxylative Coupling of ()-1-Iodo-1,6-diene with Propiolic Acids.

Electromagnetic mill (EMM)-promoted solid-state cascade Heck-type cyclization/decarboxylative coupling of propiolic acid with (Z)-1-iodo-1,6-diene derivate was demonstrated. The reaction was realized via palladium catalysis, which is solvent-free and involves no additional heating. The collision between ferromagnetic rods could not only be a favor to the mixing between the solid substrates and the catalyst system, but also the thermogenic action could accelerate this transformation.

Accurate Matching of a Secondary Amino-Functionality Metal-Organic Cage for Selective Recognition and Supramolecular Binding during Photoinduced Hydrogen Evolution.

Accurate matching of the active sites between the host and guest molecules has a great effect on the selective recognition of different but similar guest molecules or different binding abilities toward the same molecule. Herein, a pseudotetrahedral metal-organic cage (MOC, Co) that contains secondary amino groups designed as guest-interacting sites was achieved. Co exhibits the selective recognition of uridine over other similar natural molecules via a fluorescent response.

A self-powered photoelectrochemical biosensing platform for H-FABP monitoring mediated by CsPbBr@COF-V.

Advanced bioelectronic detection based on the integration of modern optical electronics and biological systems has a broad prospect. The strategy of cathode signal amplification in self-powered photoelectrochemical (PEC) immunosensors with excellent performance is rarely reported in the field of immune analysis. Herein, the work demonstrates a self-powered PEC biosensor formed with BiOI photocathode and WO/SnS/ZnS photoanode, and CsPbBr@COF-V was used as the photocathode signal quenching source for the quantitative monitoring of heart fatty acid binding protein (H-FABP).

Structural Self-Assembly and Applications of Metal-Organic Molecular Containers with Flexible Backbones.

Supramolecular chemistry has become an interdisciplinary discipline of chemistry, physics, and biology. As a huge subunit of supramolecular compounds, the functional metal-organic supramolecular systems with well-defined cavities which are able to accommodate size-suitable guests via benign host-guest behavior, have been known as "metal-organic molecular containers" (MOMCs) and attracted much attentions for their rich chemical properties and wide potential applications in molecular recognition, catalysis, bio-medical and other fields. In particular, the MOMCs with flexible backbones exhibit a unique feature both in the aspect of structural construction and applications, due to the free rotation and self-adaptively of the specific functional groups in the skeletons.

Structural Regulation of Two Polyoxometalate-Based Metal-Organic Frameworks for the Heterogeneous Catalysis of Quinazolinones.

Two dimeric {ε-}-based metal-organic frameworks (MOFs), [ε-PMoMoO(OH)Zn][LO] (, LO = [5-((4'-carboxybenzyl)oxy)isophthalic acid]) and [TBA][ε-PMoMoO(OH)Zn][LN] (, TBA = tetrabutylammonium ion, LN = [5-((4-carboxybenzyl)imino)isophthalic acid]), combining the advantages of polyoxometalates (POMs) and MOFs, were synthesized by the one-pot assembly strategy. The dimeric {ε-} units act as nodes that are linked by the flexible ligands and extended into two- or three-dimensional frameworks. The cyclic voltammetry and proton conductivity measurements of and were performed and indicated the high electron and proton transfer abilities.

A label-free electrochemical immunosensor based on PtCoCu PNPs/NB-rGO as a dual signal amplification platform for sensitive detection of β-Amyloid.

In this work, a label-free electrochemical immunosensor based on popcorn-shaped PtCoCu nanoparticles supported on N- and B-codoped reduced graphene oxide (PtCoCu PNPs/NB-rGO) was constructed to sensitively detect concentration level of β-Amyloid oligomers (Aβ). The PtCoCu PNPs exhibits excellent catalytic ability due to its popcorn structure which improves the specific surface area and porosity, resulting in more active sites being exposed and fast transport paths for ion/electron. NB-rGO with large surface area and unique pleated structure could disperse PtCoCu PNPs through electrostatic adsorption and formation of d-p dative bonds between the metal ion and pyridinic N of NB-rGO.

Ultrasensitive electrochemiluminescent aptasensor for trace detection of kanamycin based-on novel semi-sandwich gadolinium phthalocyanine complex and dysprosium metal-organic framework.

This research developed a signal amplification strategy to construct a highly sensitive electrochemiluminescent (ECL) aptasensor by incorporating dysprosium metal-organic framework (Dy-MOF) as a co-reaction accelerator (CRA) in gadolinium (Gd) luminescent complex based ECL system. A new Gd(III) complex GdPc(acac) (Pc = phthalocyanine, acac = acetylacetonate) with semi-sandwich structure was rationally selected as ECL emitter, exhibiting excellent luminescence performance owing to the "antenna effect" from the conjugated macrocyclic ligand. For further improving the sensitivity of the ECL biosensor, Dy-MOF was introduced into the ECL system as CRA.

Split-Type Photoelectrochemical/Visual Sensing Platform Based on SnO/MgInS/ZnCdS Composites and Au@FeO Nanoparticles for Ultrasensitive Detection of Neuron Specific Enolase.

Herein, a novel dual mode detection system of split-type photoelectrochemical (PEC) and visual immunoassay was developed to detect neuron specific enolase (NSE), which achieved simultaneous and reliable NSE detection due to the completely different signal readouts and transduction mechanism. Specifically, specific reactions of antigens and antibodies were performed in 96-microwell plates. Gold nanoparticle (Au NP)-loaded FeO (Au@FeO) NPs were used as secondary antibody markers and signal regulators, which could produce a blue-colored solution in the presence of 3,3',5,5'-tetramethylbenzidine (TMB) and HO because of its peroxidase-like activity.

The Paramagnetic or Spin Crossover Iron(III) Complexes Based-on Pentadentate Schiff Base Ligand: Crystal Structure, and Magnetic Property Investigation.

A series of bi- or mononuclear hexacoordinate iron(III) complexes, [Fe(L)][Fe(bpb)(CN)2]·CH3OH·0.5H2O (1), [Fe(L)][Co(bpb)(CN)2]·CH3OH (2) [(Fe (L))2(4,4'-bipy)](BPh4)2 (3), [Fe(L)(py)](BPh4) (4) and [Fe(L)(dmap)](BPh4) (5) (bpb = 1,2-bis(pyridine-2-carboxamido)benzenate, L = N,N'-bis(2-hydroxybenzyliden)-1,7-diamino-4-azaheptane, dmap = 4-dimethylaminopyridine), have been prepared with the pentadentate Schiff base iron(III) compound as assemble precursor and characterized by element analysis, IR and X-ray diffraction. Single crystal structural determination revealed the neutral cyanide-bridged binuclear entity for complexes 1 and 2 and the cationic di- or mononuclear structure for complexes 3-5 with the positive charge(s) balanced by BPh4- ion(s).

Pd/EtN·HI-Catalyzed Intramolecular C-H Alkylation to Access []-Annulated Indoles via Highly Regioselective Ring-Opening of Epoxides.

A Pd/EtN·HI-catalyzed intramolecular C-H alkylation of indoles with epoxides was achieved to furnish -fused indole frameworks (5-, 6-, and 7-membered rings) bearing an alcohol group. The conversion proceeded smoothly in the presence of a catalytic amount of EtN·HI together with a palladium catalyst and exhibited great functional group tolerance. The employment of EtN·HI not only avoids the prior preparation of alkyl halide substrates but also is the key to the high chemoselective ring-opening of epoxides.

Series of Stable Anionic Lanthanide Metal-Organic Frameworks as a Platform for Pollutant Separation and Efficient Nanoparticle Catalysis.

Eight new stable porous lanthanide metal-organic frameworks (Ln-OFs), namely, [Ln(BPTC)][(CH)NH] [Ln = Ho (), Eu (), Gd (), Dy (), Er (), Tm (), Yb (), Lu ()], were prepared by 3,3',5,5'-biphenyltetracarboxylic acid (HBPTC) and lanthanide ions by solvothermal reactions. Complexes - show a three-dimensional (3D) 6,6-connected network {4·6}·{4·6·8} topology based on binuclear (Ln) clusters and feature a one-dimensional curving porous channel occupied by exchangeable dimethylamine cations ([(CH)NH]) in the 3D anionic frameworks. The occupied [(CH)NH] in the anionic channels exhibited excellent ion-exchange ability, which is favorable to Pd and cationic dye adsorption.

Ultrasensitive Photochemical Immunosensor Based on Flowerlike SnO/BiOI/AgS Composites for Detection of Procalcitonin.

Based on the necessity and urgency of detecting infectious disease marker procalcitonin (PCT), a novel unlabeled photoelectrochemical (PEC) immunosensor was prepared for the rapid and sensitive detection of PCT. Firstly, SnO porous nanoflowers with good photocatalytic performance were prepared by combining hydrothermal synthesis and calcining. BiOI nanoflowers were synthesized by facile ultrasonic mixed reaction.

Ligand-Regulated Palladium-Catalyzed Regiodivergent Hydroarylation of the Distal Double Bond of Allenamides with Aryl Boronic Acid.

The ligand-regulated regiodivergent hydroarylation of the distal double bond of allenamides with aryl boronic acid was achieved in the presence of palladium(II) catalysts, delivering a variety of functionalized enamide with excellent E selectivity and Markovnikov/anti-Markovnikov selectivity. Two possible coordination intermediates were proposed to be responsible for the regiodivergent hydroarylation: (1) The coordination , which was proposed to be formed through the coordination of MeCN, distal double bond, phenyl to palladium, led to the aryl group away from the , inducing excellent E selectivity and anti-Markovnikov selectivity. (2) A switch of regioselectivity to 1,2- hydroarylation was obtained using bidentate phosphine ligand (dppf or Xantphos).

Spin Crossover in a Series of Non-Hofmann-Type Fe(II) Coordination Polymers Based on [Hg(SeCN)] or [Hg(SeCN)] Building Blocks.

Self-assembly of [Hg(SeCN)] tetrahedral building blocks, iron(II) ions, and a series of bis-monodentate pyridyl-type bridging ligands has afforded the new heterobimetallic Hg-Fe coordination polymers {Fe[Hg(SeCN)](4,4'-bipy)} (), {Fe[Hg(SeCN)](tvp)} (), {Fe[Hg(SeCN)](4,4'-azpy)} (), {Fe[Hg(SeCN)](4,4'-azpy)(MeOH)} (), {Fe[Hg(SeCN)](3,3'-bipy)} () and {Fe[Hg(SeCN)](3,3'-azpy)} () (4,4-bipy = 4,4'-bipyridine, tvp = -1,2-bis(4-pyridyl)ethylene, 4,4'-azpy = 4,4'-azobispyridine, 3,3-bipy = 3,3'-bipyridine, 3,3'-azpy = 3,3'-azobispyridine). Single-crystal X-ray analyses show that compounds and display a two-dimensional robust sheet structure made up of infinite linear [(FeL)] (L = 4,4'-bipy or 4,4'-azpy) chains linked by formed {[Hg(L)(SeCN)]} anionic dimeric bridges. Complexes and - define three-dimensional networks with different topological structures, indicating, in combination with complexes and , that the polarity, length, rigidity, and conformation of the bridging organic ligand play important roles in the structural nature of the products reported here.

Cyanide-Bridged Polynuclear and One-Dimensional FeIII-MnIII/II Bimetallic Complexes Based-on Pentacyanoferrite(III) Building Block: Synthesis, Crystal Structures, and Magnetic Properties.

In this contribution, based-on the structurally confirmed pentacyanometallate (PPh4)2[Fe(CN)5(imidazole)]·(imidazole)·H2O (1) and the manganese compounds [Mn(L)(H2O)2]ClO4 (L = N,N-ethylenebis(3-methoxysalicylideneiminate) or [Mn(MAC)(H2O)Cl]ClO4 (MAC = 2,13-dimethyl-3,6,9,12,18-pentaazabicyclo-[12.3.1]octadeca-1(18),2,12,14,16-pentaene), two new cyanide-bridged bimetallic FeIII-MnIII/II complexes [Mn(L)(H2O)]3[Fe(CN)5(imidazole)](ClO4) (2) and [Mn(MAC)][Fe(CN)5(imidazole)]·CH3OHn (3) were successfully synthesized and characterized by elemental analysis, IR spectroscopy and X-ray structure determination.

A Lanthanide-Containing Coordination Polymer Using Tetraphenylethene-Based Linkers with Selective Fe Sensing and Efficient Iodine Adsorption Activities.

As a star ligand, the construction of coordination polymers (CPs) based on tetrakis(4-carboxyphenyl)ethylene (H) has drawn much attention, due to not only the various coordination configurations but also the intriguing chromophore feature causing aggregation-induced emission (AIE). Herein, by the solvothermal reaction of H as connected nodes with lanthanide La(III) salts, the first example of the La(III)--based CP () has been obtained. The structural analyses indicate that exhibits a 3D framework connected by the sharing carboxylate groups with two kinds of 1D rhombic channels when viewed along the direction.

A rare octacoordinated mononuclear iron(III) spin-crossover compound: synthesis, crystal structure and magnetic properties.

The chemistry of transition-metal complexes with unusually high coordination numbers has been of interest because of their application in catalytic and biological systems. Deprotonation of the ionogenic tetradentate ligand 6,6'-bis(1H-tetrazol-5-yl)-2,2'-bipyridine [Hbipy(ttr)] in the presence of iron(III) and tetra-n-butylammonium bromide, [n-BuN]Br, in solution resulted in the synthesis of a rare octacoordinated anionic mononuclear complex, tetra-n-butylammonium bis[6,6'-bis(tetrazol-1-id-5-yl)-2,2'-bipyridine]iron(III) methanol hemisolvate dihydrate, (CHN)[Fe(CHN)]·0.5CHOH·2HO or [n-BuN][Fe{bipy(ttr)}]·0.

Intramolecular Photoelectrochemical System Using Tyrosine-Modified Antibody-Targeted Peptide as Electron Donor for Detection of Biomarkers.

An intramolecular photoelectrochemical (PEC) system is designed from the novel electron donor YYYHWRGWV (Y3-H) peptide ligand for the first time. The bifunctional nonapeptide cannot only rely on the HWRGWV sequence as a site-oriented immobilizer to recognize the crystallizable fragment (Fc) domains of the antibody but also acts as electron donors for PEC generation via three tyrosine (Y) of the N-terminal. The BiWO/AgInS heterojunction with a significant visible-light absorption is utilized as a photoelectric generator, and the motivation is ascribed to a proven proposition, namely, that short-wavelength illuminant radiates proteins, causing a decline in bioactivity of immune protein.

Nickel-Catalyzed Reductive Aryl Thiocarbonylation of Alkene via Thioester Group Transfer Strategy.

Herein reported is a nickel-catalyzed reductive aryl thiocarbonylation of alkene via thioester group transfer strategy by using simple and readily available thioesters. In contrast to traditional activation of weaker C(acyl)-S bond, the C(acyl)-C bond of thioester was selectively cleaved to enable this reaction under mild conditions. Furthermore, this approach features operational simplicity and broad substrate scope, providing a complementary and practical route for thioester synthesis without requiring toxic thiol or CO gas.

Self-assembly of a cobalt(II)-based metal-organic framework as an effective water-splitting heterogeneous catalyst for light-driven hydrogen production.

The solar photocatalysis of water splitting represents a significant branch of enzymatic simulation by efficient chemical conversion and the generation of hydrogen as green energy provides a feasible way for the replacement of fossil fuels to solve energy and environmental issues. We report herein the self-assembly of a Co-based metal-organic framework (MOF) constructed from 4,4',4'',4'''-(ethene-1,1,2,2-tetrayl)tetrabenzoic acid [or tetrakis(4-carboxyphenyl)ethylene, HTCPE] and 4,4'-bipyridyl (bpy) as four-point- and two-point-connected nodes, respectively. This material, namely, poly[(μ-4,4'-bipyridyl)[μ-4,4',4'',4'''-(ethene-1,1,2,2-tetrayl)tetrabenzoato]cobalt(II)], [Co(CHO)(CHN)], crystallized as dark-red block-shaped crystals with high crystallinity and was fully characterized by single-crystal X-ray diffraction, PXRD, IR, solid-state UV-Vis and cyclic voltammetry (CV) measurements.

Tuning of crystallization method and ligand conformation to give a mononuclear compound or two-dimensional SCO coordination polymer based on a new semi-rigid V-shaped bis-pyridyl bis-amide ligand.

With the new semi-rigid V-shaped bidentate pyridyl amide compound 5-methyl-N,N'-bis(pyridin-4-yl)benzene-1,3-dicarboxamide (L) as an auxiliary ligand and the Fe ion as the metal centre, one mononuclear complex, bis(methanol-κO)bis[5-methyl-N,N'-bis(pyridin-4-yl)benzene-1,3-dicarboxamide-κN]bis(thiocyanato-κN)iron(II), [Fe(SCN)(CHNO)(CHOH)] (1), and one two-dimensional coordination polymer, catena-poly[[[bis(thiocyanato-κN)iron(II)]-bis[μ-5-methyl-N,N'-bis(pyridin-4-yl)benzene-1,3-dicarboxamide-κN:N']] methanol disolvate dihydrate], {[Fe(SCN)(CHNO)]·2CHOH·2HO} (2), were prepared by slow evaporation and H-tube diffusion methods, respectively, indicating the effect of the method of crystallization on the structure type of the target product. Both complexes have been structurally characterized by elemental analysis, IR spectroscopy and single-crystal X-ray crystallography. The single-crystal X-ray diffraction analysis shows that L functions as a monodentate ligand in mononuclear 1, while it coordinates in a bidentate manner to two independent Fe(SCN) units in complex 2, with a different conformation from that in 1 and the ligands point in two almost orthogonal directions, therefore leading to a two-dimensional grid-like network.

A label-free immunosensor for the sensitive detection of hepatitis B e antigen based on PdCu tripod functionalized porous graphene nanoenzymes.

Nanomaterials with enzyme properties possess excellent catalytic activity and stability. We prepared new nanoenzymes to construct a label-free electrochemical immunosensor for the detection of hepatitis B e antigen (HBe Ag). In this study, PdCu tripod (PdCu TP) functionalized porous graphene (PG) nanoenzymes (PdCu TPs/PG) were prepared through the in situ reduction of PdCu tripods onto porous graphene.

A Versatile Porous Silver-Coordinated Material for the Heterogeneous Catalysis of Chemical Conversion with Propargylic Alcohols and CO.

The efficient transformation of carbon dioxide into useful chemical feedstock is of great significance, attracting intense research interest. The widely studied porous-coordinated polymers possess large pores to adsorb guest molecules and further allow the contact and to transfer the substrate molecule within their microenvironment. Here we present the synthesis of a silver-based metal-organic frameworks (MOFs) material with a three-dimensional structure by incorporating a tetraphenyl-ethylene moiety as the four-point connected node via the solvothermal method.

A thermal- and light-induced switchable one-dimensional rare loop-like spin crossover coordination polymer.

Rare loop-like isostructural one-dimensional coordination polymer (1D-CP) systems formulated as {Fe(DPIP)(NCSe)}·4DMF (1) and {Fe(DPIP)(NCSe)}·4DMF (2) were obtained by self-assembling Fe and pseudohalide NCX(X = S, Se) ions in presence of the V-shaped bidentate bridging ligand, namely, N,N'-dipyridin-4-ylisophthalamide (DPIP), and were characterized by elemental analysis, IR spectroscopy, TGA, single crystal X-ray diffraction and powder X-ray diffraction. The magnetic studies show that complex 2 undergoes a complete thermally induced spin crossover (SCO) behavior centered at T = 120 K with ca. 5 K thermal hysteresis loop and light-induced excited spin state trapping effect (LIESST) with T = 65 K.