Publications by authors named "Qisheng Huo"

53 Publications

Solvent-Induced Self-Assembly Strategy to Synthesize Well-Defined Hierarchically Porous Polymers.

Adv Mater 2019 Mar 25;31(11):e1806254. Epub 2019 Jan 25.

Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.

Porous polymers with well-orchestrated nanomorphologies are useful in many fields, but high surface area, hierarchical structure, and ordered pores are difficult to be satisfied in one polymer simultaneously. Herein, a solvent-induced self-assembly strategy to synthesize hierarchical porous polymers with tunable morphology, mesoporous structure, and microporous pore wall is reported. The poly(ethylene oxide)-b-polystyrene (PEO-b-PS) diblock copolymer micelles are cross-linked via Friedel-Crafts reaction, which is a new way to anchor micelles into porous polymers with well-defined structure. Varying the polarity of the solvent has a dramatic effect upon the oleophobic/oleophylic interaction, and the self-assembly structure of PEO-b-PS can be tailored from aggregated nanoparticles to hollow spheres even mesoporous bulk. A morphological phase diagram is accomplished to systematically evaluate the influence of the composition of PEO-b-PS and the mixed solvent component on the pore structure and morphology of products. The hypercrosslinked hollow polymer spheres provide a confined microenvironment for the in situ reduction of K PdCl to ultrasmall Pd nanoparticles, which exhibit excellent catalytic performance in solvent-free catalytic oxidation of hydrocarbons and alcohols.
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http://dx.doi.org/10.1002/adma.201806254DOI Listing
March 2019

Mesoporous Hexanuclear Copper Cluster-Based Metal-Organic Framework with Highly Selective Adsorption of Gas and Organic Dye Molecules.

ACS Appl Mater Interfaces 2018 Sep 7;10(37):31233-31239. Epub 2018 Sep 7.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry , Jilin University , Changchun 130012 , P. R. China.

Despite many advances in the design and assembly of mesoporous metal-organic frameworks (meso-MOFs), it is still a challenge to obtain the desired structure. Here, we utilized an effective cluster cooperative assembly strategy by introducing SO ions as chelating binding sites to construct a novel mesoporous MOF, [Cu(SO)(TBA)(OH)( N,N-dimethylacetamide (DMA))]·12DMA·12CHOH [JLU-MOF51, HTBA = 4-(1 H-tetrazol-5-yl)-benzoic acid]. Remarkably, the cooperative assembly of the infrequent hexanuclear [CuSO(OH)] cluster and the classical paddlewheel [Cu(CO)] via linear hetero-N, O donor ligand results in an open three-dimensional framework, which possesses one-dimensional nanometer tube channels with the diameter of 24 and 28 Å. Fascinatingly, JLU-MOF51 displays an exceptionally large Langmuir surface area (5443 m g) and exhibits a high capacity for selective adsorption of CH (CH: 348 cm g at 273 K; CH/CH = 220 at 298 K). In addition, JLU-MOF51 can selectively adsorb fluorescein disodium salt dye among numerous organic dyes. An extremely high surface area and unique structural characteristics make JLU-MOF51 a promising meso-MOF material for the adsorption and separation of hydrocarbon gases and organic dyes. Moreover, this strategy will provide an effective means for constructing meso-MOFs via one-step synthesis.
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http://dx.doi.org/10.1021/acsami.8b06340DOI Listing
September 2018

Multiple dye-doped silica cross-linked micellar nanoparticles for colour-tuneable sensing of cysteine in an aqueous media and living cells.

J Colloid Interface Sci 2018 Nov 22;529:531-537. Epub 2018 Jun 22.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, PR China.

This work demonstrated the design and synthesis of multiple dye-doped silica cross-linked micellar nanoparticles (MD-SCMNPs) by encapsulating three organic dyes (fluorescein derivative (FCD), coumarin derivative (HCE) and Rhodamine b (RhB)) in SCMNPs cores for colour-tuneable sensing of cysteine (Cys) in aqueous media and in living cells. In the presence of Cys, HCE exhibited blue emission, and RhB exhibited purple emission, while FCD reacted with Cys and exhibited green fluorescence "turn-on" in the core of MD-SCMNPs. This green-light-emitting sensing product may cause "step by step" fluorescent resonance energy transfer (FRET) from HCE to the sensing product and then to RhB. Based on the FRET process in the core, MD-SCMNPs can quantitatively detect Cys by a colour change with a low limit of detection (LOD) of 0.3 μM in living cells. Furthermore, MD-SCMNPs exhibited ultrasmall size (∼12 nm) and excellent dispersity and biocompatibility, which could potentially be used as a visualized Cys sensor for health monitoring and disease prediction in the human body.
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http://dx.doi.org/10.1016/j.jcis.2018.06.060DOI Listing
November 2018

Architecture of yolk-shell structured mesoporous silica nanospheres for catalytic applications.

Dalton Trans 2018 Jul;47(27):9072-9078

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

We report the design and realization of yolk-shell structured nanospheres with periodic mesoporous organosilica (PMO) nanospheres or noble metal nanoparticles encapsulated in mesoporous silica shells via a selective etching method. These architectures have well controlled structure, size and morphology. The yolk-shell structured PMO@SiO2 nanoparticles can be precisely functionalized with different catalytic functionalities, even incompatible acidic and basic groups: the PMO core with amino (-NH2) groups and the mesoporous silica shell with sulfonic acid (-SO3H) groups. As a nanoreactor, the as-synthesized Au@SiO2 nanospheres show faster reduction of 4-nitrophenol than that of nitrobenzene. Furthermore, the prepared PMO-NH2@SiO2-SO3H nanoparticles can be used as bifunctional catalysts with highly efficient catalytic performance for catalyzing the deacetalization-Henry cascade reaction.
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http://dx.doi.org/10.1039/c8dt02254bDOI Listing
July 2018

A Topotactic Synthetic Methodology for the Synthesis of Nanosized MFI Zeolites with Hierarchical Structures.

Chemistry 2018 Aug 24;24(48):12600-12606. Epub 2018 Jul 24.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun, 130012, P.R. China.

Much effort has been invested in the designed synthesis of zeolites with nanosized and hierarchical structures in recent decades, on account of increasing demands in practical applications, especially catalysis. Herein, a new topotactic synthetic strategy is demonstrated to synthesize nanosized and hierarchical zeolites in a one-step procedure. By using silica spheres as the adjustable amorphous precursors and tetrapropylammonium hydroxide as a structure-directing agent, effortless control of both size and porosity can be achieved in this system with no extra templates. With a simple hydrothermal process, hierarchical zeolite spheres can be modified with acid cites (Al species incorporated in the framework). Benefitting from its mesoporosity, palladium nanoparticles are incorporated into the nanosized hierarchical zeolite, which makes the materials suitable for use in a cascade catalysis reaction of benzimidazole derivatives, including independent acid catalysis and hydrogenation sites. The nanocomposites show exceptional activity and stability in catalysis and recycling reaction. This strategy can be developed into other versatile and practicable scaffolds for advanced zeolite catalytic nanoreactor systems.
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http://dx.doi.org/10.1002/chem.201801185DOI Listing
August 2018

Synthesis of hierarchical hollow sodium titanate microspheres and their application for selective removal of organic dyes.

J Colloid Interface Sci 2018 Oct 22;528:109-115. Epub 2018 May 22.

College of Liberal Arts and Sciences, National University of Defense Technology, Changsha 410073, PR China. Electronic address:

Titanate-based materials are attractive inorganic adsorbents for wastewater treatment. In this study, hierarchical hollow sodium titanate microspheres (HHSTMs) were successfully synthesized via a template-assisted method. Silica microspheres were selected as hard templates, with a uniformly smooth TiO shell first grown onto the surface of the SiO cores. Then, through an alkaline hydrothermal process, the silica core was removed and the TiO shell gradually converted into a sodium titanate shell with a preserved morphology. The as-synthesized HHSTMs are constructed from twined nanobelts, with a high surface area of 308 m g. A typical organic dye, methylene blue, was employed to investigate the adsorption properties of the HHSTMs. The adsorption process matched well with the Langmuir isothermal model, with the maximum adsorption capacity of methylene blue reaching 443 mg g. Moreover, the resulting HHSTMs can be used to selectively capture of methylene blue from a cationic-anionic dye binary system due to their negatively charged surface. All adsorption processes were very fast and could complete in ten minutes.
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http://dx.doi.org/10.1016/j.jcis.2018.05.069DOI Listing
October 2018

A chelation-induced cooperative self-assembly methodology for the synthesis of mesoporous metal hydroxide and oxide nanospheres.

Nanoscale 2018 Mar 14;10(12):5731-5737. Epub 2018 Mar 14.

Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.

With unique physical and chemical properties and porous architectures, mesoporous transition metal hydroxide (MMHO) and oxide (MMO) nanospheres hold great potential for various applications in drug delivery, catalysis, energy storage and conversion. However, synthesizing MMHO and MMO with well-defined mesostructures remains a great challenge because of the weak interaction between surfactants and metal precursors. Herein we describe a chelation-induced cooperative self-assembly system in which the weak interaction can be cooperatively amplified through the use of a chelating ligand acting as a co-template. Both MMHO and MMO nanospheres with tunable diameters and high surface areas can be readily synthesized via this strategy. The as-synthesized mesoporous ZnO nanospheres exhibit excellent photoelectric performance, and as a highly efficient oxygen evolution reaction (OER) catalyst of low cost, the calcined Cu(OH) nanospheres exhibit one of the best activities for the OER. Moreover, this cooperative method gives rise to an alternative to "classical" self-assembly methods for the preparation of mesostructured nanomaterials and, in some cases, the only viable synthetic route toward MMHO and MMO nanostructures.
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http://dx.doi.org/10.1039/c7nr07883hDOI Listing
March 2018

An anionic single-walled metal-organic nanotube with an armchair (3,3) topology as an extremely smart adsorbent for the effective and selective adsorption of cationic carcinogenic dyes.

Chem Commun (Camb) 2018 Mar 6;54(24):3006-3009. Epub 2018 Mar 6.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China.

A novel discrete single-walled metal-organic nanotube (JLU-MONT1) with a rare armchair (3,3) carbon nanotube topology is successfully synthesized, which is further linked by hydrogen-bonds forming a 3D supramolecular architecture. Benefiting from its anionic skeletal features and open mesoporous channels (21 Å), JLU-MONT1 exhibits extremely high efficiency and capability to adsorb carcinogens basic red 9 and basic violet 14.
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http://dx.doi.org/10.1039/c8cc00542gDOI Listing
March 2018

Hydrogen bond-induced bright enhancement of fluorescent silica cross-linked micellar nanoparticles.

J Colloid Interface Sci 2018 Jun 24;519:224-231. Epub 2018 Feb 24.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

This work demonstrated the synthesis and design of ultra-bright and ultra-small fluorescent nanoparticles, which were prepared by encapsulating 4-(diphenylamino)benzaldehyde (DPB) in silica cross-linked micellar nanoparticles (SCMNPs). The DPB-doped SCMNPs (DPB-SCMNPs) exhibited ultra-bright fluorescence in an aqueous medium that was 22 times brighter than that of free DPB molecules in an organic solvent. For the first time, density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations were used to confirm that the enhanced brightness of the DPB-SCMNPs was due to a hydrogen bond-induced mechanism. In addition, the 3D fluorescence spectra and the Commission Internationale de L'Eclairage (CIE) diagram were employed to determine the optical properties and emission colour of the DPB-SCMNPs. Moreover, the DPB-SCMNPs were water-soluble, monodisperse and ultra-small (∼12 nm) and should be robust and stable in aqueous media and biological systems.
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http://dx.doi.org/10.1016/j.jcis.2018.02.064DOI Listing
June 2018

Novel Schiff base (DBDDP) selective detection of Fe (III): Dispersed in aqueous solution and encapsulated in silica cross-linked micellar nanoparticles in living cell.

J Colloid Interface Sci 2018 Mar 20;514:357-363. Epub 2017 Dec 20.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

This work demonstrated the synthesis of (4E)-4-(4-(diphenylamino)benzylideneamino)-1,2-dihydro-1,5- dimethyl-2-phenylpyrazol-3-one (DBDDP) for Fe (III) detection in aqueous media and in the core of silica cross-linked micellar nanoparticles in living cells. The free DBDDP performed fluorescence enhancement due to Fe (III)-promoted hydrolysis in a mixed aqueous solution, while the DBDDP-doped silica cross-linked micellar nanoparticles (DBDDP-SCMNPs) performed an electron-transfer based fluorescence quenching of Fe (III) in living cells. The quenching fluorescence of DBDDP-SCMNPs and the concentration of Fe (III) exhibited a linear correlation, which was in accordance with the Stern-Volmer equation. Moreover, DBDDP-SCMNPs showed a low limit of detection (LOD) of 0.1 ppm and an excellent selectivity against other metal ions. Due to the good solubility and biocompatibility, DBDDP-SCMNPs could be applied as fluorescence quenching nanosensors in living cells.
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http://dx.doi.org/10.1016/j.jcis.2017.12.050DOI Listing
March 2018

Knitting N-doped Hierarchical Porous Polymers to Stabilize Ultra-small Pd Nanoparticles for Solvent-Free Catalysis.

Chem Asian J 2017 Dec 7;12(23):3039-3045. Epub 2017 Nov 7.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, Jilin, 130012, China.

Hierarchical porous polymers with more than one pore size distributions can effectively support noble metal catalysts and circumvent the limitation of the diffusion of the reactants, and thus exhibit both excellent catalytic activity and superior diffusive properties. Herein, we report a simple one-step Friedel-Crafts reaction to knit a series of benzene heterocycle monomers, such as indane, indoline, indole and tetrahydronaphthalene to obtain hierarchical porous polymers with high surface areas and/or abundant N sites. These polymers can be directly used to immobilize Pd ions, and stabilize Pd nanoparticles during the thermal reduction process to obtain Pd/polymer catalysts. In particular, indoline- and indole-based polymers with high N content up to 7 wt % exhibit outstanding ability to stabilize uniform ultrasmall Pd nanoparticles. The obtained Pd-polymers exhibit excellent catalytic activity in the solvent-free oxidation of benzyl alcohol with O .
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http://dx.doi.org/10.1002/asia.201701104DOI Listing
December 2017

Two Analogous Polyhedron-Based MOFs with High Density of Lewis Basic Sites and Open Metal Sites: Significant CO Capture and Gas Selectivity Performance.

ACS Appl Mater Interfaces 2017 Sep 15;9(38):32820-32828. Epub 2017 Sep 15.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University , Changchun 130012, PR China.

By means of modulating the axial ligand and adopting supermolecular building blocks (SBBs) strategy, two polyhedron-based metal-organic frameworks (PMOFs) have been successfully synthesized [Cu(CONH)(CHN)(HO)(DMF)]·3DMF·8HO (JLU-Liu46) and [Cu(CONH)(CHN)(HO)(DMF)]·3DMF·8HO (JLU-Liu47), which possess a high density of Lewis basic sites (LBSs) and open metal sites (OMSs). Since the size of axial ligand in JLU-Liu47 is smaller than that in JLU-Liu46, JLU-Liu47 shows larger pore volume and higher BET surface area. Then, the adsorption ability of JLU-Liu47 for some small gases is better than JLU-Liu46. It is worthwhile to mention that both of the two compounds exhibit outstanding adsorption capability for CO ascribed to the introducing of urea groups. In addition, the theoretical ideal adsorbed solution theory (IAST) calculation and transient breakthrough simulation indicate that JLU-Liu46 and JLU-Liu47 should be potential materials for gas storage and separation, particularly for CO/N, CO/CH, and CH/CH separation.
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http://dx.doi.org/10.1021/acsami.7b10795DOI Listing
September 2017

Tuning Gas Adsorption Properties of Zeolite-like Supramolecular Assemblies with gis Topology via Functionalization of Isoreticular Metal-Organic Squares.

ACS Appl Mater Interfaces 2017 Oct 11;9(39):33521-33527. Epub 2017 Jul 11.

Division of Physical Sciences and Engineering, Advanced Membranes & Porous Materials Center, Functional Materials Design, Discovery & Development (FMD3), King Abdullah University of Science and Technology (KAUST) , 4700, Thuwal 23955-6900, Kingdom of Saudi Arabia.

A strategy based on metal-ligand directed assembly of metal-organic squares (MOSs), built-up from four-membered ring (4MR) secondary building units (SBUs), has been employed for the design and construction of isoreticular zeolite-like supramolecular assemblies (ZSAs). Four porous Co-based ZSAs having the same underlying gis topology, but differing only with respect to the capping and bridging linkers, were successfully isolated and fully characterized. In this series, each MOS in ZSA-3-ZSA-6 possess an ideal square geometry and is connected to four neighboring MOS via a total of 16 hydrogen bonds to give a 3-periodic porous network.To systematically assess the effect of the pore system (size and functionality) on the gas adsorption properties, we evaluated the MOSs for their affinity for different probe molecules such as CO and light hydrocarbons. ZSA-3-ZSA-6 showed high thermal stability (up to 300 °C) and was proven highly porous as evidenced by gas adsorption studies. Notably, alkyl-functionalized MOSs were found to offer potential for selective separation of CO, CH, and CH from CH and H containing gas stream, such as natural gas and refinery-off gases.
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http://dx.doi.org/10.1021/acsami.7b06010DOI Listing
October 2017

A Flexible Doubly Interpenetrated Metal-Organic Framework with Breathing Behavior and Tunable Gate Opening Effect by Introducing Co into ZnO Clusters.

Inorg Chem 2017 Jun 19;56(11):6645-6651. Epub 2017 May 19.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University , Changchun 130012, People's Republic of China.

A ZnO clusters based flexible doubly interpenetrated metal-organic framework [(ZnO)(DCPB)DMF]·2DMF·8HO (JLU-Liu33, HDCPB = 1,3-di(4-carboxyphenyl)benzene, DMF = N,N-dimethylformamide) with pcu topology has been solvothermally synthesized. Because of its flexible structure, JLU-Liu33 exhibits a breathing behavior upon N and CO adsorption at low temperature, and CH and CH adsorption at 273 and 298 K. Furthermore, by adopting the direct synthesis method, two isomorphic compounds-JLU-Liu33L and JLU-Liu33H-have been obtained by partial substituting Zn with different amounts of Co into the JLU-Liu33 framework. The gas adsorption study of Co-doped materials reveals that the gate opening effect of JLU-Liu33 can be modulated by introducing different contents of Co into ZnO clusters. Meanwhile, with the increasing amount of Co, the adsorption amount and isosteric enthalpy values for CO have been improved. It is worth mentioning that JLU-Liu33H exhibits commendable selectivity for CO over CH which may be a good candidate for industrial gas purification and air separation applications.
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http://dx.doi.org/10.1021/acs.inorgchem.7b00744DOI Listing
June 2017

Transformation from single-mesoporous to dual-mesoporous organosilica nanoparticles.

Nanoscale 2017 May;9(19):6362-6369

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

Transformation from single-mesoporous to dual-mesoporous structured organosilica nanoparticles can be achieved by simply varying the volume fraction of ethanol in the synthesis system, using lauryl sulfonate betaine and sodium dodecyl sulfonate as dual-templates. Core-shell structured dual-mesoporous organosilica nanoparticles possess smaller mesopores (4.0 nm) in the shell and flower-like larger mesopores (46 nm) in the core. Owing to the unique mesostructure, dual-mesoporous organosilica nanoparticles show a high loading capacity and a slow release rate for cargo molecules. The large mesopores on the inside can provide a large storage space for the guest molecules and the small mesopores in the outer shell act as a natural valve, slowing the release. In addition, both single-mesoporous and dual-mesoporous organosilica nanoparticles, exhibit low cell toxicity and excellent cell permeability.
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http://dx.doi.org/10.1039/c7nr00363cDOI Listing
May 2017

Two Finite Binuclear [M(μ-OH)(COO)] (M = Co, Ni) Based Highly Porous Metal-Organic Frameworks with High Performance for Gas Sorption and Separation.

Inorg Chem 2017 Apr 17;56(7):4141-4147. Epub 2017 Mar 17.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University , Changchun 130012, P. R. China.

Two highly porous MOFs, [Co(μ-OH)(bpdc)(Htpim)][SiF]·3.5DMA·2.5CHOH (JLU-Liu37, Hbpdc = biphenyl-4,4'-dicarboxylate, Htpim = 2,4,5-tri(4-pyridyl)imidazole) and [Ni(μ-OH)(bpdc)(Htpim)][SiF]·7.5DMA·6CHOH (JLU-Liu38), have been solvothermally synthesized by using the mixed ligand strategy. Both of the compounds possess finite binuclear [M(μ-OH)(COO)] (M = Co, Ni) secondary building units (SBUs) which formed with a polar functional group, μ-OH. JLU-Liu37 and JLU-Liu38 exhibit notable adsorption capacities for CO and light hydrocarbons (CH, CH, and CH). Moreover, both of the materials exhibit arrestive natural gas selective separation ability, especially for CH/CH (206 for an equimolar mixture under 1 bar and 298 K, for JLU-Liu37). Both of the MOFs may be effectively applied in the separation of industrial light hydrocarbons.
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http://dx.doi.org/10.1021/acs.inorgchem.7b00156DOI Listing
April 2017

An anionic metal-organic framework with ternary building units for rapid and selective adsorption of dyes.

Dalton Trans 2017 Mar;46(10):3332-3337

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China.

A novel metal-organic framework, [(CH)NH][CuO(SO)CuL(DMF)(HO)]·9DMF (JLU-Liu39) HL = pyridine-3,5-bis(phenyl-4-carboxylic acid), has been successfully synthesized under solvothermal conditions. Structure analysis indicates that the framework of JLU-Liu39 is constructed by ternary building units which include a rare hexa-nuclear [CuO(SO)] cluster, a classical [Cu(CO)] paddlewheel, and a 3-connected hetero-N, O donor ligand. The whole 3D framework possesses a (3,4,4)-connected fjh topology and a large window size of 25.3 Å with high solvent-accessible volume accounting for approximately 75.8% of the cell volume. On the basis of the anionic framework and large pore volume, JLU-Liu39 can efficiently adsorb cationic dyes such as MLB, MV, RhB and neutral dye NR but exclude anionic dyes such as MO and Orange II. Moreover, JLU-Liu39 also exhibits size-exclusion performance for dyes of different sizes, and the dye adsorption amounts decrease with the increase of dye size. With respect to the proportional mixture dyes with different charges for MO & MLB and Orange II & MLB, JLU-Liu39 can be able to selectively adsorb the cationic dye MLB efficiently. Based on the aforementioned considerations, JLU-Liu39 is a good anionic-skeleton MOF material for the adsorption and separation of organic dyes.
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http://dx.doi.org/10.1039/c7dt00192dDOI Listing
March 2017

Facile synthesis of 3D porous CoVO nanoroses and 2D NiCoVO nanoplates for high performance supercapacitors and their electrocatalytic oxygen evolution reaction properties.

Dalton Trans 2017 Mar;46(10):3295-3302

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

Binary metal oxides have recently attracted extensive attention from researchers in the energy storage and conversion field due to their high energy densities and multiple oxidation states. Novel 3D CoVO porous rose-like structures and 2D NiCoVO nanoplates were facilely synthesized via a solvothermal method, and the morphologies, Ni/Co ratios, and surface area of these samples can be easily tuned in the same procedure. The as-prepared CoVO porous rose-like structure exhibited good electrocatalytic oxygen evolution performance with excellent activity and stability. In addition, 2D NiCoVO nanoplates delivered a high specific capacitance of 1098.9 F g at 4 A g and good cycling stability (remaining 68% after 7000 cycles) in aqueous KOH electrolyte. The NiCoVO nanoplates inherit the pseudocapacitive benefits of both NiVO and CoVO, showing a higher specific capacitance than pure CoVO porous rose-like structures.
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http://dx.doi.org/10.1039/c7dt00435dDOI Listing
March 2017

A controllable asymmetrical/symmetrical coating strategy for architectural mesoporous organosilica nanostructures.

Nanoscale 2016 Jul;8(28):13581-8

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

We describe a facile and controllable asymmetrical/symmetrical coating strategy for the preparation of various novel periodic mesoporous organosilica (PMO) nanostructures, including Au&PMO Janus, Au@PMO yolk-shell and Au@PMO/mSiO2 yolk-double shell nanoparticles, by using Au@SiO2 nanoparticles as seeds. During this process, ammonia first functions as a basic catalyst facilitating the hydrolyzation and condensation of the organosilica precursor, and additionally as an etching agent selectively in situ dissolving the SiO2 shells of Au@SiO2 nanoparticles to form these unique nanostructures. All these three types of nanoparticles have high surface areas, large pore volumes and tailorable cavity structures. Both the Au&PMO and Au@PMO nanoparticles exhibit excellent catalytic activity for the decomposition of H2O2 and the reduction of 4-nitrophenol. Based on these unique structural merits and organic-inorganic hybrid components, the fabricated Janus and hollow PMO nanoparticles show much improved hemocompatibility, which could be further applied in nano-biomedicines without the need for surface modification.
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http://dx.doi.org/10.1039/c6nr03229jDOI Listing
July 2016

Immobilization of Bacillus subtilis lipase on a Cu-BTC based hierarchically porous metal-organic framework material: a biocatalyst for esterification.

Dalton Trans 2016 Apr 18;45(16):6998-7003. Epub 2016 Mar 18.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012, P. R. China.

Bacillus subtilis lipase (BSL2) has been successfully immobilized into a Cu-BTC based hierarchically porous metal-organic framework material for the first time. The Cu-BTC hierarchically porous MOF material with large mesopore apertures is prepared conveniently by using a template-free strategy under mild conditions. The immobilized BSL2 presents high enzymatic activity and perfect reusability during the esterification reaction. After 10 cycles, the immobilized BSL2 still exhibits 90.7% of its initial enzymatic activity and 99.6% of its initial conversion.
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http://dx.doi.org/10.1039/c6dt00677aDOI Listing
April 2016

Significant enhancement of gas uptake capacity and selectivity via the judicious increase of open metal sites and Lewis basic sites within two polyhedron-based metal-organic frameworks.

Chem Commun (Camb) 2016 Feb;52(15):3223-6

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China.

Two new isomorphous polyhedron-based MOFs ( and ), with dual functionalities of OMSs and LBSs, have been synthesized by using the SBB strategy. By judiciously avoiding the DABCO axial ligand, possesses more OMSs than , and exhibits a significant enhancement of CO2 uptake capacity 210 versus 162 cm(3) g(-1) for at 273 K under 1 bar.
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http://dx.doi.org/10.1039/c5cc09922fDOI Listing
February 2016

Host-Guest Chirality Interplay: A Mutually Induced Formation of a Chiral ZMOF and Its Double-Helix Polymer Guests.

J Am Chem Soc 2016 Jan 14;138(3):786-9. Epub 2016 Jan 14.

Functional Materials Design, Discovery & Development (FMD3), Advanced Membranes & Porous Materials Center, Division of Physical Sciences and Engineering, 4700 King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900, Kingdom of Saudi Arabia.

A novel homochiral zeolite-like metal-organic framework (ZMOF), [(Cu4I4) (dabco)2]·[Cu2(bbimb)]·3DMF (JLU-Liu23, dabco =1,4-diazabicyclo[2.2.2]-octane, H2bbimb =1,3-bis(2-benzimidazol)benzene, DMF = N,N-dimethylformamide), has been successfully constructed to host unprecedented DNA-like [Cu2(bbimb)]n polymers with double-helicity. The host-guest chirality interplay permitted the induced formation of an unusual gyroid MOF with homochirality and helical channels in the framework for the first time, JLU-Liu23. Importantly, the enantiomeric pairs (23P, 23M) can be promoted and isolated in the presence of appropriate chiral inducing agents, affording enantioselective separation of chiral molecules as well as small gas molecules.
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http://dx.doi.org/10.1021/jacs.5b12516DOI Listing
January 2016

Mixed anionic surfactant-templated mesoporous silica nanoparticles for fluorescence detection of Fe(3.).

Dalton Trans 2016 Jan;45(2):508-14

Division of Materials Science, Luleå University of Technology, SE-97187 Luleå, Sweden.

This work demonstrates a novel method for the synthesis of large pore mesoporous silica nanoparticles (MSNs) with a pore diameter of 10.3 nm and a particle diameter of ∼50 nm based on the incorporation of mixed anionic surfactants sodium dodecyl benzene sulfonate (SDBS) and sodium dodecyl sulphate (SDS) as the template in the synthesis process. The dispersity, morphology, pore structure and size of mesoporous nanoparticles were adjusted by changing the molar ratio of two anionic surfactants, the concentration of the co-structure-directing agent (3-aminopropyltrimethoxysilane) and the reaction temperature. The results of synthesis experiments suggested that the formation of large pore MSNs involved a nucleation and growth process. MSNs were post-grafted with a Schiff base moiety for fluorescence sensing of Fe(3+) in water. The applicability of functionalized MSNs was demonstrated by selective fluorescence detection of Fe(3+) in aqueous media.
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http://dx.doi.org/10.1039/c5dt03052hDOI Listing
January 2016

Ti(IV) oxalate complex-derived hierarchical hollow TiO2 materials with dye degradation properties in water.

Dalton Trans 2016 Jan;45(1):265-70

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

Ti(IV)-based complexes have been demonstrated as candidates for preparing hybrid and functional materials, and have received considerable attention. In this paper, hierarchical hollow titania materials with different surface nanostructures were synthesized successfully using a hydrothermal process via the transformation of a Ti(IV) oxalate complex as a precursor. Different concentrations of ammonia were used to adjust the morphologies and crystalline forms of the hydrothermal products. The hierarchical hollow anatase titania materials, HHTM-1 (cal) and HHTM-2 (cal), have high surface areas of up to 132 m(2) g(-1) and 84 m(2) g(-1), respectively, and show superior performance for dye degradation in water.
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http://dx.doi.org/10.1039/c5dt03291aDOI Listing
January 2016

Mesostructured TiO2 Gated Periodic Mesoporous Organosilica-Based Nanotablets for Multistimuli-responsive Drug Release.

Small 2015 Nov 29;11(44):5907-11. Epub 2015 Sep 29.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, Jilin, 130012, P. R. China.

A multistimuli-responsive drug carrier is designed and successfully synthesized by self-assembly of thiol-modified periodic mesoporous organosilica (PMO) nanoparticles, coated gold nanoparticles (AuNPs), and mesostructured titanium dioxide (TiO2). Dye-loaded PMO-Au@TiO2 nanotablets are shown to respond to environmental changes (pH, temperature, and light) to achieve controlled release.
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http://dx.doi.org/10.1002/smll.201501835DOI Listing
November 2015

A polyhedral metal-organic framework based on the supermolecular building block strategy exhibiting high performance for carbon dioxide capture and separation of light hydrocarbons.

Chem Commun (Camb) 2015 Oct 4;51(83):15287-9. Epub 2015 Sep 4.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China.

By using the supermolecular building block (SBB) strategy, a polyhedron-based metal-organic framework (PMOF), which features three types of cages with multiple sizes and shapes, has been synthesized. It exhibits high performance for CO2 capture (170 cm(3) g(-1) at 273 K under 1 bar) and selectivity of CO2/CH4 (9.4) and C3H8/CH4 (271.5).
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http://dx.doi.org/10.1039/c5cc06162hDOI Listing
October 2015

Luminescence and energy-transfer properties of color-tunable Ca2Mg0.25Al1.5Si1.25O7:Ce(3+)/Eu(2+)/Tb(3+) phosphors for ultraviolet light-emitting diodes.

Luminescence 2016 Mar 6;31(2):453-461. Epub 2015 Aug 6.

College of Chemistry, Jilin University, Changchun, 130012, People's Republic of China.

A series of Ca2Mg0.25Al1.5Si1.25O7:Ce(3+)/Eu(2+)/Tb(3+) phosphors was been prepared via a conventional high temperature solid-state reaction and their luminescence properties were studied. The emission spectra of Ca2Mg0.25Al1.5Si1.25O7:Ce(3+),Eu(2+) and Ca2Mg0.25Al1.5Si1.25O7:Ce(3+),Tb(3+) phosphors show not only a band due to Ce(3+) ions (409 nm) but also as a band due to Eu(2+) (520 nm) and Tb(3+) (542 nm) ions. More importantly, the effective energy transfer from Ce(3+) to Eu(2+) and Tb(3+) ions was confirmed and investigated by emission/excitation spectra and luminescent decay behaviors. Furthermore, the energy level scheme and energy transfer mechanism were investigated and were demonstrated to be of resonant type via dipole-dipole (Ce(3+) to Eu(2+)) and dipole-quadrupole (Ce(3+) to Tb(3+)) reactions, respectively. Under excitation at 350 nm, the emitting color could be changed from blue to green by adjusting the relative doping concentration of Ce(3+) and Eu(2+) ions as well as Ce(3+) and Tb(3+) ions. The above results indicate that Ca2Mg0.25Al1.5Si1.25O7:Ce(3+),Eu(2+)/Tb(3+) are promising single-phase blue-to-green phosphors for application in phosphor conversion white-light-emitting diodes.
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http://dx.doi.org/10.1002/bio.2981DOI Listing
March 2016

Correction: Enzyme and voltage stimuli-responsive controlled release system based on β-cyclodextrin-capped mesoporous silica nanoparticles.

Dalton Trans 2015 May;44(17):8300

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, China.

Correction for 'Enzyme and voltage stimuli-responsive controlled release system based on β-cyclodextrin-capped mesoporous silica nanoparticles' by Yu Xiao et al., Dalton Trans., 2015, 44, 4355-4361.
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http://dx.doi.org/10.1039/c5dt90068aDOI Listing
May 2015

Megranate-like nanoreactor with multiple cores and an acidic mesoporous shell for a cascade reaction.

Nanoscale 2015 Feb;7(8):3719-25

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

Megranate-like nanoparticles possess a unique structure that is composed of multiple cores and shells, which is different from simple yolk-shell nanoparticles. Megranate-like nanoparticles can combine the properties of each component and be used as nanoreactors. This study describes the preparation of bifunctional megranate-like nanoreactors, consisting of multiple metal cores and thiol modified mesoporous SiO2 shells. Different metal nanoparticles (Pd, Pt, Au) can be incorporated into the structure as cores, and the thiol group in the shells can be oxidized to acidic -SO3H. The megranate-like nanoparticles show good bifunctional catalytic properties and recyclability in a cascade catalytic reaction for the desired benzimidazole derivative. Moreover, the individual components of the megranate-like nanoparticles also show good catalytic activities in the hydrogenation reduction of nitro-aromatics and the deprotection reaction of benzaldehyde dimethyl acetal.
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http://dx.doi.org/10.1039/c4nr06341dDOI Listing
February 2015