An iron-nitrogen doped carbon and CdS hybrid catalytic system for efficient CO photochemical reduction.

Iron porphyrin and carbon black (CB) were utilized to fabricate an iron-nitrogen doped carbon (Fe-N-C) catalyst to create a new heterogeneous catalytic system with CdS to drive CO2 reduction to CO under UV/vis light (AM 1.5G) irradiation. The system delivers a high CO production yield of 111 mmol gcat-1 and a large turnover number (TON) of 1.

Two Polyoxometalate-Based Hybrid Compounds Modified by Iron Schiff Base Complexes: Syntheses, Crystal structures, Cyclic Voltametric Studies and Nonlinear Optical Properties.

Two new polyoxometalate (POM)-based hybrid compounds modified by a Schiff base, [Fe(DAPSC)(H O) ] [HPMo Mo O ] ⋅ 5H O (1) and [Fe(DAPSC)(H O)] [HPV Mo Mo O ] ⋅ 6H O (2), (DAPSC=2,6-diacetylpyridine bis-(semicarbazone)), have been successfully constructed from typical Keggin POMs, iron ions, and DAPSC ligands under hydrothermal condition. Structural analysis demonstrates that the Fe-Schiff base ligand units are free from polyacid anions in compound 1. While in compound 2, the Fe-Schiff base ligand units are bridged with polyacid anions via Fe-O bonds to emerge a stable double-supported skeleton.

Luminescent silver(i) complexes with pyrazole-tetraphenylethene ligands: turn-on fluorescence due to the coordination-driven rigidification and solvent-oriented structural transformation.

A new tetrapyrazole-modified tetraphenylethene (TPE) ligand L was designed and found to display "turn-on" fluorescence when it combines with Ag ions in dilute solution by restricting intramolecular rotation of TPE. A series of Ag complexes 1-7 were obtained, and they exhibit excellent fluorescence properties in the solid state. Compared with PF, the silver complex with the CFSO anion can further enhance its fluorescence due to the transformation of its structure from AgL (2) to AgL (3).

Cobalt-Based Metal-Organic Frameworks for Adsorption of CO and C Hydrocarbons: Effect of Auxiliary Ligands with Different Functional Groups.

Recently, metal-organic frameworks (MOFs) have been investigated as potential materials for CO capture and light hydrocarbon storage/separation due to their high porosity, large surface area, and tunable skeleton structures. In this work, the six cobalt-based MOFs - were successfully synthesized under solvothermal conditions by a mixed-ligand strategy. and have the same framework structure with a topology of {4·5}{4·5·6·7·8}, while the structures of the - frameworks are the same with a topology of {4·5}{4·5·6·7·8}.

Rh-Catalyzed C-H (Het)arylation/Vinylation of -2,6-Difluoroaryl Acrylamides.

Rh-catalyzed sp C-H cross-coupling of acrylamides with organoboron reactants has been accomplished using a commercially available -2,6-difluoroaryl acrylamide auxiliary. A broad range of aryl and vinyl boronates as well as a variety of heterocyclic boronates with strong coordinating ability can serve as the coupling partners. This transformation proceeds under moderate reaction conditions with excellent functional group tolerance and high regioselectivity.

Iron(iii)-bipyridine incorporated metal-organic frameworks for photocatalytic reduction of CO with improved performance.

Metal-organic frameworks (MOFs) represent an emerging class of platforms to assemble single site photocatalysts for artificial photosynthesis. In this work, we report a new CO reduction photocatalyst (UiO-68-Fe-bpy) based on a robust Zr(iv)-MOF platform with incorporated Fe(bpy)Cl (bpy refers to the 4'-methyl-[2,2'-bipyridine] moiety) via amine-aldehyde condensation. We show that this hybrid catalyst can reduce CO to form CO under visible light illumination with excellent selectivity and enhanced activity with respect to its parent MOF and corresponding homogeneous counterpart.

A dual-labeling probe to track functional mitochondria-lysosome interactions in live cells.

Mitochondria-lysosome interactions are essential for maintaining intracellular homeostasis. Although various fluorescent probes have been developed to visualize such interactions, they remain unable to label mitochondria and lysosomes simultaneously and dynamically track their interaction. Here, we introduce a cell-permeable, biocompatible, viscosity-responsive, small organic molecular probe, Coupa, to monitor the interaction of mitochondria and lysosomes in living cells.

Rhodium(III)-Catalyzed C(sp)-H Chemoselective Annulation to O-Cyclized Isochromen-imines from Benzamides.

Through the development of ligands and reaction conditions, the Rh(III)-catalyzed selective annulation of benzamides with internal alkynes has been achieved to the formation of -cyclized isochromen-imines. Various substituents are well-tolerated under mild reaction conditions. Density functional theory calculations indicate that silver carbonate could act as a Lewis acid to assist the ligand to improve the chemical selectivity of the reaction in a catalytic system.

Potential Applications of Cucurbit[n]urils and Their Derivatives in the Capture of Hazardous Chemicals.

Cucurbit[n]urils (Q[n]s) are a relatively young family of macrocycles, consisting of glycoluril units bridged by methylene groups, and their unique structures have attracted extensive attention from chemists in recent decades. Due to the presence of a rigid hydrophobic inner cavity and two polar outer portals lined with carbonyl groups, Q[n]s not only encapsulate guest species into the cavity, but also coordinate with metal ions/clusters. Considerable achievements have been obtained in the fields of Q[n]s-based host-guest chemistry, coordination chemistry, as well as the combination of host-guest and coordination chemistry.

Dual Functionalization of Electron Transport Layer Tailoring Molecular Structure for High-Performance Perovskite Light-Emitting Diodes.

Great progress in modification and optimization of emission layer (EML) in perovskite light-emitting diodes (PeLEDs) results in a significant improvement in device efficiency. However, so far, less attention has been paid to the exploration of hole/electron injection and transporting layers to maximize the utilization of charge carriers for efficient and stable PeLEDs. At present, low electron mobility of electron transport layer (ETL) causes an unbalanced charge injection, and the defects at the ETL/perovskite interface limit the formation and utilization of generated excitons.

Sensitive detection of streptomycin in milk using a hybrid signal enhancement strategy of MOF-based bio-bar code and target recycling.

A MOF-based bio-bar code material was synthesized and firstly applied to develop an electrochemical streptomycin (STR) aptasensor. By using MOF-based bio-bar code and enzyme-assisted target recycling for dual-signal amplification, highly sensitive detection of STR was achieved. The sensing surface was simply fabricated by immobilizing a mixed monolayer of thiolated cDNA/aptamer duplexes (dsDNA) and 6-mercapto-1-hexanol (MCH) on the gold nanoparticle modified screen printed carbon electrode (Au/SPCE).

Rh(III)-Catalyzed C(sp)-H Acetoxylation of 8-Methylquinolines.

A mild and efficient Rh(III)-catalyzed aliphatic C-H acetoxylation directed by quinolines has been developed with widespread functional groups, including various halogens, which usually can provide precursors for further organic synthesis but easily results in selectivity issues in the Pd- and Ni-catalyzed reaction. Interestingly, AcO plays an essential role in promoting the transformation.

A Universal Strategy for Carbon-Supported Transition Metal Phosphides as High-Performance Bifunctional Electrocatalysts towards Efficient Overall Water Splitting.

Exploring cost-effective and general approaches for highly active and stable bifunctional transition metal phosphide (TMP) electrocatalysts towards overall water splitting is greatly desirable and challenging. Herein, a general strategy combining sol-gel and a carbonization-assisted route was proposed to facilely fabricate a series of TMP nanoparticles, including CoP, MoP, FeP, CuP, NiP, PtP, FeNiP, CoNiP, and FeCoNiP, coupled in an amorphous carbon matrix with one-step carbon composite formation. The resultant NiFeP@C exhibits excellent activities as a bifunctional electrocatalyst toward oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) with low overpotentials of 260 and 160 mV, respectively, at 10 mA/cm in 1 M KOH solution.

A Series Three-Dimensional LnCr (Ln = Gd, Tb, Er) Heterometallic Cluster-Based Coordination Polymers Containing Interesting Nanotubes Exhibiting High Magnetic Entropy.

A series of novel 3D 3d-4f heterometallic cluster-based coordination polymers, [LnCr(μ-O)(μ-O)(NA)(HO)]·HO (Ln = , , ; HNA nicotinic acid; = 13 (), 11.33 (), 15 ()), have been successfully synthesized by hydrothermal method using nicotinic acid as bridging ligand. The single-crystal X-ray diffraction (SCXRD) analysis indicated that the basic unit of LnCr shows a butterfly-shaped structure.

Coordination polymers with a pyridyl-salen ligand for photocatalytic carbon dioxide reduction.

A new ligand HL with pyridine and salen moieties and its coordination polymers (CPs) [Mn(L)Cl]·DMF (1) and [Fe(L)Cl]·DMF (2) were synthesized and their photocatalytic activity for the conversion of CO into CO under visible-light irradiation was investigated. This is the first instance of pyridyl-salen-ligand based CPs for photocatalyzing CO reduction.

Agaric-derived N-doped carbon nanorod arrays@nanosheet networks coupled with molybdenum carbide nanoparticles as highly efficient pH-universal hydrogen evolution electrocatalysts.

Non-precious, stable and efficient catalysts for the pH-universal hydrogen evolution reaction (HER) are highly desirable to meet the vast energy demands. Herein, we report a facile and scalable strategy using agaric as a precursor to construct a Mo2C-based HER electrocatalyst consisting of ultrafine Mo2C nanoparticles embedded within biomass-derived 3D N-doped carbon nanorod arrays@nanosheet networks (Mo2C@N-CANs). This electrocatalyst is highly active for the pH-universal hydrogen evolution reaction and requires overpotentials of only 82 mV, 100 mV and 350 mV to drive a current density of -10 mA cm-2 in acidic, alkaline and neutral media, exhibiting stable operation for 3000 cycles and 24 h long-term stability.

Cucurbit[7]uril-Based Metal-Organic Rotaxane Framework for Dual-Capture of Molecular Iodine and Cationic Potassium Ion.

Metal-organic rotaxane frameworks (MORFs) attracted much attention in the past years for construction of intelligent functional materials. Herein, a one-pot synthesis is reported of a three-dimensional (3D) cucurbit[7]uril (Q[7])-based MORF under hydrothermal conditions, namely Q[7]-MORF-1, formed by encapsulating the anionic benzoate moieties of the tricarboxylate ligand into the cavity of Q[7]. Furthermore, Q[7]-MORF-1 shows dual-capture capacity for iodine and K selectively among the alkali metal ions.

Rapid solvent-evaporation strategy for three-dimensional cobalt-based complex hierarchical architectures as catalysts for water oxidation.

It is a challenging task to seek a highly-efficient electrocatalyst for oxygen evolution reaction (OER) of water splitting. Non-noble Co-based nanomaterials are considered as earth-abundant and effective catalysts to lower overpotential and increase polarization current density of OER. In this work, we reported, for the first time, a "rapid solvent-evaporation" strategy for the synthesis of three-dimensional (3D) cobalt complex hierarchical architectures constructed by two-dimensional (2D) nanosheets.

An Optical/Photoacoustic Dual-Modality Probe: Ratiometric in/ex Vivo Imaging for Stimulated HS Upregulation in Mice.

Tracking signaling HS in live mice demands responsive imaging with fine tissue imaging depth and low interferences from tissue scattering/autofluorescence and probe concentration. With complementary advantages of fluorescence and photoacoustic (PA) imaging, optical/PA dual-modality imaging was suggested for in/ex vivo HS imaging. Therefore, a -benzoyloxyltricarboheptamethine cyanine, , was prepared as the first ratiometric optical/PA dual-modality probe for HS, profiting from a keto-enol transition sensing mechanism.

Series of Cadmium(II) Coordination Polymers Based on a Versatile Multi-N-Donor Tecton or Mixed Carboxylate Ligands: Synthesis, Structure, and Selectively Sensing Property.

Five Cd(II) metal-organic frameworks (MOFs), [Cd(HL)] (), [Cd(HL)(HO)] (), [Cd(HL)(obda)] (), [Cd(HL)(ohmbda)(DMA)(HO)] (), and [Cd(HL)(btc)(HO)]·3HO (), were prepared by reactions of Cd(NO)·4HO with 1-(1-imidazol-4-yl)-4-(4-tetrazol-5-yl)benzene (HL) or mixed carboxylate ancillary ligands of 1,2-benzenedicarboxylic acid (Hobda), 5-hydroxy-1,3-benzenedicarboxylic acid (Hohmbda), and 1,3,5-benzenetricarboxylic acid (Hbtc), respectively. Their structures have been characterized by single-crystal X-ray diffraction, elemental analysis, infrared spectroscopy (IR), thermogravimetric analysis, and powder X-ray diffraction. Compounds and are supramolecular isomeric frameworks without consideration of the solvent molecules.

Water-Stable Coordination Polymers as Dual Fluorescent Sensors for Highly Oxidizing Anions Cr O and MnO.

Due to their striking optical properties, luminescent coordination polymers as sensors for the detection of hazardous species have drawn interest of researchers in consideration of the control of environmental pollution. In this work, the organic ligand 2-(4-((E)-2-(pyridine-2-yl)vinyl)styryl)pyridine (2-bpeb), which possesses a large π-conjugated system, was employed to react with d metal ions to obtain novel luminescent coordination polymers. Three complexes [Cd(2-bpeb) (CNA)(H O)] (CP1), [Cd(2-bpeb) (NDC)] (CP2) and [Zn(2-bpeb)(BDC)] (CP3) were synthesized successfully by introducing carboxylic acids of 4-carboxycinnamic acid (H CNA), 2,6-naphthalene dicarboxylic acid (H NDC) and 1,4-benzenedicarboxylic acid (H BDC) as auxiliary ligands.

Solvent-Free Photoreduction of CO to CO Catalyzed by Fe-MOFs with Superior Selectivity.

It is deemed as a desired approach to utilize solar energy for the conversion of CO into valuable products, and the majority of the MOFs-based photocatalytic reductions of CO have focused on formic acid (HCOOH) production with an organic solvent as the reaction medium. Herein, we report a solvent-free reaction route for the photoreduction of CO catalyzed by Fe-MOFs, namely, NH-MIL-53(Fe) [(Fe(OH)(NH-BDC)]•G, NH-MIL-88B(Fe) [FeO(HO)(NH-BDC)]Cl•G, and NH-MIL-101(Fe) [FeO(HO)(NH-BDC)]Cl•G (NH-BDC = 2-aminoterephthalic acid; G = guest and/or solvent molecules). Compared with the orthodox reaction route, the present out-of-the-way photocatalytic reduction of CO with superior selectivity to CO occurs at the gas-solid interface.

Facet-dependent photocatalytic hydrogen production of metal-organic framework NH-MIL-125(Ti).

Facet-dependent catalytic activity of hard materials such as metals and metal oxides is well recognized in previous works. However, it has rarely been established for metal-organic frameworks (MOFs), possibly because the soft crystals of MOFs are conceptually different from the hard solids. In this work, the surface structure of the MOF NH-MIL-125(Ti) has been investigated by density functional theory (DFT) calculations for the first time.