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ACS Yao Yuan Award of Medicinal Chemistry

ACS Yao Yuan Award of Medicinal Chemistry 04-29-2017: Dr. Xiaopin Duan's poster entitled "Photodynamic Therapy Mediated by Non-toxic Core-Shell Nanoparticles Synergize with Immune Checkpoint Blockade to Elicit Antitumor Immunity and Antimetastasis Effect on Breast Cancer" was chosen as a first place winner by the Yao Yuan-Academy for Pharma Innovation. Dr. Duan was invited to present her work which can be found here at the recent symposium as part of her ACS Yao Yuan Award of Medicinal Chemistry. Congratulations also to Dr. Kuangda Lu for his second place poster entitled "Chlorin-Based Nanoscale Metal-Organic Framework Systemically Rejects Colorectal Cancers via Synergistic Photodynamic Therapy and Checkpoint Blockade Immunotherapy" which can be found here

 

2017 Young Investigator Award

04-06-2017: Dr. Kuangda Lu, a recent graduate and current postdoctoral fellow in the Lin Group, has been selected for the 2017 Young Investigator Award for the ACS Inorganic Chemistry Division. As an awardee, Kuangda will present his work on nanoscale metal organic frameworks for biomedical applications at the upcoming ACS meeting.

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New Member of UChicago Medicine's Comprehensive Cancer Center

02-10-2017: Prof Wenbin Lin has been added to the Comprehensive Cancer Center for his nanoplatforms enhancing currently existing chemotherapy, radiotherapy, and immunotherapy.

 

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Innovations in Fuel Cycle Research

08-28-2016: Congratulations to Marek Piechowicz for receiving a First Prize in the U.S. Department of Energy's Innovations in Fuel Cycle Research Awards for his work on uranium recovery from seawater simulant. The Innovations in Fuel Cycle Research Awards program recognizes students who develop innovative solutions fueling nuclear technology. The research for which he won this prize can be found here.

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Congratulations Drs. Lu and Poon

Five years together08-20-2016: Congratulations to Kuangda Lu and Christopher Poon for receiving their PhDs! Dr. Kuangda Lu successfully defended his thesis "Nanoscale Metal Organic Frameworks for Biomedical Applications" and Dr. Chris Poon successfully defended his thesis "Nanoscale Coordination Polymers Co-Deliver Multiple Therapeutics for Combination Therapy of Cancer" earlier this summer.

 

 

 

Graduate Awards

05-23-2016: Congratulations to Kuangda Lu for receiving the Elizabeth R. Norton Prize for Excellence in Research and Zekai Lin for receiving the Otto & Valerie Windt Memorial Graduate Fellowship for the upcoming year.

 

NCI Grant

10-04-2015: The Lin group just received a five-year U01 grant from the National Cancer Institute (NCI) through the Innovative Research in Cancer Nanotechnology (IRCN) program. This IRCN grant will allow the Lin group to continue exploring the applications of nanoscale metal-organic frameworks (NMOFs) in cancer therapy, a research effort his group initiated more than a decade ago. The $2.88 million dollar U01 grant will allow the Lin group to refine the successful strategies to identify prototype NMOFs for clinical translation. Congratulations!

 

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Baxter's Young Investigator Award

Lin Group08-25-2015: Dr. Chunbai He, a postdoctoral fellow in the Lin group, has been chosen as a winner of Baxter's Young Investigator Awards for her hard work and innovative spirit. As a recipient of this award, Dr. He will be highlighted at Baxter.com

 

 

 

 

Group Picnic

Lin Group08-15-2015: The Lin group enjoyed a group outing to Promontory Point where they enjoyed a barbecue and some soccer.

 

 

 

 

Congratulations, Carter

Carter's Convocation Group Picture07-16-2015: Dr. Carter Abney, a graduate of the Lin Lab, has left the group to start his career at Oak Ridge National Laboratory. Congratulations, Carter.

 

 
 

 

Happy Birthday, Professor Lin

Prof Lin's Birthday CakeHappy Birthday Professor Lin. The group celebrated Prof Lin's recent birthday with a cake.

 

 

 

 

Fuel Cycle Research Award

10-30-2014: Carter Abney was featured by UChicago News for his work on extracting uranium from seawater, for which he was a first-place winner in the Department of Energy's Innovations in Fuel Cycle Research Awards Competition.

 

 

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sal-MOFs for Catalysis of Olefin Hydrogenation

Catalysis of Olefin Hydrogenation

 

 

 

 

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NMOFs for Real-Time Intracellular pH Sensing

pH Sensing08-22-2014: Real-time measurement of intracellular pH in live cells is of great importance for understanding physiological/pathological processes and developing intra-cellular drug delivery systems. As reported in in Journal of American Chemical Society (2014, DOI: 10.1021/ja507333c), the Lin group has demonstrated the first use of nanoscale metal−organic frameworks (NMOFs) for intracellular pH sensing in live cells. UiO NMOFs conjugated to flourescein isothiocyanate (F-UiO) not only showed excellent ratiometric pH-sensing properties but also remained structurally intact inside endosomes, allowing for live cell imaging studies. F-UiO allowed the real time observation of endo- and exocytosis of F-UiO and endosome acidification. Fluorescently labeled NMOFs thus represent a new class of nanosensors for intracellular pH sensing and studying NMOF-cell interactions. This work has been featured in JACS Spotlight for the probe's ability to retain the benefits of fluorescent pH sensors without dye leaching and clumping.

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Group Picnic

Lin Group08-08-2014: The Lin group enjoyed a group outing to Promontory Point where they enjoyed a barbecue and some soccer.

 

 

 

 

 

 

Innovation Fund Award

07-22-2014: The Lin group's work on siRNA grafted nanoscale coordination polymers containing chemotherapeutic drugs has been awarded $100,000 by the Innovation Fund to prepare the NCP for pre-clinical testing in platinum-resistant ovarian cancer. The Innovation Fund, which invests in early development of new ventures created by University of Chicago affiliates, has chosen this technology because it increases progression-free survival benefits and reduces side effects of platinum-based drugs, among other benefits.

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NCPs for Cancer Therapy

NCP CompositionThe Lin group recently designed self-assembled nanoscale coordination polymers (NCPs) for highly effective cancer therapy. As reported in Nature Communications (2014, DOI: 10.1038), the NCPs carry 48±3 wt% cisplatin prodrug (1) and 45±5 wt% oxaliplatin prodrug (2) with selective and substantial accumulation of chemotherapeutics in solid tumours via the passive targeting pathways. In vivo pharmacokinetic studies in mice showed minimal uptake of pegylated NCPs by the mononuclear phagocyte system and excellent blood circulation half-lives of 16.4±2.9 h and 12.0±3.9 h for pegylated 1 and 2, respectively. In several tumor xenograft models evaluated, pegylated NCPs showed superior potency and efficacy compared to free drugs. NCPs have thus been demonstrated as a highly effective drug delivery platform for cancer therapy by virtue of tunable compositions, sizes, and shapes; high drug loadings; ease of surface modification; and intrinsic biodegradability.

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Congratulations, Demin

Demin Liu07-16-2014: Dr. Demin Liu, a graduate of the Lin Lab, has left the group to start his career at Baxter Healthcare. Congratulations, Demin.

 

 

 

 

 

 

Innovations in Fuel Cycle Research

Carter Abney06-02-2014: Carter Abney is the First Place winner in the Separations and Waste Forms division of the Open Competition for the Innovations in Fuel Cycle Research awards competition. His research is in developing sorbent materials for extraction of uranium from seawater and decontamination of nuclear wastes. As an awardee, he will be presenting his paper "Metal-Organic Framework Materials as Nanostructured Sorbents for the Nuclear Fuel Cycle" at the American Nuclear Society Winter meeting in addition to receiving a monetary prize.

 

 

Congratulations, Michael

Mike 05-09-2014: Dr. Michael Carboni has left the group to start his appointment as a permanent research scientist at Commissariat à l'énergie atomique et aux énergies alternatives (CEA, the French Alternative Energies and Atomic Energy Commission). Congratulations, Michael.

 

 

 

Congratulations also to Chris Poon for finishing 10 McChickens in two hours!

 

 

MOFs for Highly Efficient Catalytic Organic Transfermations

MOFs for Highly Efficient Catalytic Organic Transfermations04-23-2014: The Lin group recently designed and developed highly stable and recyclable single-site solid catalysts via post-synthetic metalation of the 2,2'-bipyridyl-derived metal-organic framework (MOF) of the UiO structure (bpy-UiO) with iridium or palladium precursors. As reported in the Journal of the American Chemical Society (2014, 136 (18), pp 6566–6569), the Ir-functionalized MOF (bpy-UiO-Ir) is a highly active catalyst for both borylation of aromatic C-H bonds using B2(pin)2 (pin = pinacolate) and ortho-silylation of benzylic¬silyl ethers; the ortho-silylation activity of the bpy-UiO-Ir is at least three orders of magnitude higher than that of the homogeneous control. The Pd-functionalized MOF (bpy-UiO-Pd) catalyzes the dehydrogenation of substituted cyclohexenones to afford phenol derivatives with oxygen as the oxidant. Most impressively, the bpy-UiO-Ir was recycled and reused 20 times for the borylation reaction without loss of catalytic activity or MOF crystallinity. This work highlights the opportunity in designing highly stable and active catalysts based on MOFs containing nitrogen donor ligands for important organic transformations.

 

MOF for Highly Efficient X-ray Scintillation

Highly Efficient X-ray Scintillation04-14-2014: As published in the Journal of the American Chemical Society (2014, 136 (17), pp 6171–6174), the Lin Group reported two metal-organic frameworks (MOFs) capable of efficiently converting X-ray radiation to visible-light luminescence. The MOFs are constructed from M6(µ3-O)4(µ3-OH)4(carboxylate)12 (M = Hf or Zr) secondary building units (SBUs) and anthracene-based dicarboxylate bridging ligands. The high atomic number Zr and Hf in the SBUs serve as effective X-ray antenna by absorbing X-ray photons and converting them to fast electrons through the photoelectric effect. The generated electrons then excite multiple anthracene-based emitters in the MOF through inelastic scattering, leading to efficient generation of detectable photons in the visible spectrum. The MOF materials thus serve as efficient X-ray scintillators via synergistic X-ray absorption by the metal-cluster SBUs and optical emission by the bridging ligands. This work was performed in collaboration with the research group of Lei Xing at the Stanford University School of Medicine.

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Privileged Phosphine-Based Metal-Organic Frameworks for Broad-Scope Asymmetric Catalysis

Asymmetric Catalysis03-31-2014: As published in the Journal of the American Chemical Society (2014, 136 (14), pp 5213–5216) and highlighted in Science, the Lin group developed a robust and porous Zr metal-organic framework (MOF) based on a BINAP-derived dicarboxylate linker, BINAP-MOF. Post-synthetic metalation with Ru and Rh complexes afforded highly enantioselective catalysts for important organic transformations. Notably, the Rh-functionalized MOF is not only highly enantioselective (up to >99% e.e.) but also 3 times as active as the homogeneous control. Extended x-ray absorption fine structure spectroscopy (EXAFS), performed in collaboration with the Lockard group of Rutgers University, revealed that the Ru-functionalized MOF contains Ru-BINAP precatalysts with the same coordination environment as the homogeneous Ru complex. The post-synthetically metalated BINAP-MOFs provide a versatile family of single-site solid catalysts for catalyzing a broad scope of asymmetric organic transformations, including the addition of aryl and alkyl groups to α,β-unsaturated ketones as well as the hydrogenation of substituted alkenes and carbonyl compounds.

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Nanoscale Metal-Organic Frameworks for Treating Drug-Resistant Ovarian Cancer Cells

siRNANMOF03-26-2014: Acquired resistance to chemotherapy is a major limitation for ovarian cancer treatment. The Lin group recently reported in the Journal of the American Chemical Society (2014, 136 (14), pp 5181–5184) the first use of nanoscale metal-organic frameworks (NMOFs) for the co-delivery of cisplatin and pooled small interfering RNAs (siRNAs) to enhance therapeutic efficacy in cisplatin-resistant ovarian cancer. UiO NMOFs with hexagonal-plate morphologies were loaded with cisplatin and MDR gene-silencing siRNAs (Bcl-2, P-glycoprotein [P-gp], and survivin) via encapsulation and surface coordination, respectively. Co-delivery of cisplatin and siRNAs with NMOFs led to an order of magnitude enhancement in chemotherapeutic efficacy in vitro by silencing multiple drug resistance (MDR) genes and re-sensitizing resistant ovarian cancer cells to cisplatin treatment.

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POM Molecular Catalysts for Visible Light-Driven Water Oxidation

A Biomimetic Copper Water Oxidation Catalyst with Low Overpotential03-24-2014: As reported by the Lin Group in the Journal of the American Chemical Society (2014, 136 (14), pp 5359–5366), a series of all-inorganic, abundant-metal-based, high-nuclearity cobalt-phosphate (Co-Pi) molecular catalysts were synthesized and shown to be highly effective at photocatalytic water oxidation. The Co-Pi cluster contains a Co4O4 cubane which is structurally analogous to the [Mn3CaO4] core of the oxygen-evolving complex (OEC) in photosystem II (PSII). Four distinct compounds were investigated and shown to be the first POM-based Co−Pi-cluster molecular catalysts for visible light-driven water oxidation, thus serving as a functional model of the OEC in PSII. The systematic synthesis of four isostructural analogues allowed for investigating the influence of different heteroatoms in the POM ligands on the photocatalytic activities of these Co−Pi cluster WOCs. Further study shows that these oxidatively resistant catalysts were not only highly effective at photocatalytic water oxidation, but could also maintain their structural integrity under photocatalytic conditions.

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Biomimetic Copper Water Oxidation Catalyst with Low Overpotential

A Biomimetic Copper Water Oxidation Catalyst with Low Overpotential12-10-2013: In the Journal of the American Chemical Society (2014, 136 (1), pp 273–281), researchers in the Lin group reported a highly active water oxidation catalyst (WOC) from simply mixing a Cu(II) salt and 6,6'-dihydroxy-2,2'-bipyridine in a basic aqueous solution. Cyclic voltammetry of the solution at pH = 12-14 shows irreversible catalytic current with an onset potential of ~0.8 V vs. NHE. Catalytic oxygen evolution takes place in controlled potential electrolysis at a relatively low overpotential of 640 mV. Through collaboration with computational chemists at UNC-Chapel Hill Research Computing, DFT calculations were performed to further investigate the catalytic system. Experimental and computational studies suggest that the ligand participates in electron transfer processes to facilitate the oxidation of the Cu center to lead to an active WOC with low overpotential, akin to the use of the tyrosine radical by Photosystem II to oxidize the CaMn4 center for water oxidation.

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Soaking Up Uranium

Soaking up uraniumPublished in Chemical Science, and also highlighted in C&EN, the Lin Group prepared three metal–organic frameworks (MOFs) of the UiO-68 network topology and investigated for sorption of uranium from water and artificial seawater. The stable and porous phosphorylurea-derived MOFs were shown to be highly efficient in sorbing uranyl ions, with saturation sorption capacities as high as 217 mg U g-1; which is equivalent to binding one uranyl ion for every two sorbent groups. Coordination modes between uranyl groups and simplified phosphorylurea motifs were investigated by DFT calculations, revealing a thermodynamically favorable monodentate binding of two phosphorylurea ligands to one uranyl ion. Convergent orientation of phosphorylurea groups at appropriate distances inside the MOF cavities is believed to facilitate their cooperative binding with uranyl ions. This work represents the first application of MOFs as novel sorbents to extract actinide elements from aqueous media.

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2013 Young Investigator Award

cheng wangCheng "Wave" Wang, a graduate student in the Lin Group, has been selected for a 2013 Young Investigator Awards given by the ACS Division of Inorganic Chemistry. As an awardee, Wave will be giving an award presentation at the 2013 Fall ACS National meeting in Indianapolis, where he will receive $1000 and a plaque at the special oral presentation session. Wave's research focuses on developing novel metal organic frameworks for solar energy related applications and heterogeneous asymmetric catalysis.






Exceptional Methane Uptake Capacity

methane uptakeResearchers in the Lin Group have constructed a 6,8-connected 3-dimensional metal–organic framework, MOF, of the tph topology from a new aromatic-rich, tetraphenylmethane-derived octa-carboxylate bridging ligand and trizinc cluster secondary building units, SBUs, which exhibited exceptionally high hydrogen and methane uptake capacities. This MOF has the highest hydrogen uptake among all of the MOFs that have been examined to date. As described in the journal Chemical Science, the gravimetric and volumetric methane uptake capacities for this new framework are the highest among thousands of MOFs that have been evaluated. The Lin Group attribute the exceptionally high gas uptake capacities to the highly branched, aromatic-rich nature of the bridging ligand, optimal pore size, and the open metal sites in the trizinc SBUs in a stable high-connectivity MOF.

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NMOFs as Contrast Agents in CT Imaging

CT contrast agentsNanoscale metal–organic frameworks, NMOFs, of the UiO-66 structure containing high Zirconium and Hafnium content, 37% and 57% by weight respectively, were synthesized and characterized in work by the Lin Group, published in and featured on the cover of the Journal of Materials Chemistry. The potential of these NMOFs as contrast agents for X-ray computed tomography, CT, imaging was evaluated. Hf-NMOFs of different sizes were coated with silica and poly(ethylene glycol), PEG, to enhance biocompatibility, and were used for in vivo CT imaging of mice, showing increased attenuation in the liver and spleen.

 

 

 

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Cavity-Induced Enantioselectivity Reversal

enantioselectivityThe Lin Group, in collaboration with Dr. Shubin Lin of the UNC Research Computing Center, reports inChemical Science the first enzyme-like catalysis by a metal-organic framework, MOF. They constructed a pair of highly porous chiral MOFs, 1 and 2, from chiral 1,1'-binaphthyl-2,2'-phosphoric acid-derived 3,3',6,6'- and 4,4'',6,6'-tetra(benzoate) ligands, respectively. Both MOFs are active catalysts for Friedel–Crafts reactions between indole and imines. Interestingly, the 1-catalyzed asymmetric reactions yielded the major enantiomers of the opposite chirality to those afforded by the corresponding homogeneous catalyst. Structural analyses and Quantum Mechanics/Molecular Mechanics calculations revealed that the flip of product handedness results from the chiral environment of the MOF cavity, similar to enzymatic catalysis in which the product stereoselectivity is determined by the enzyme pocket.

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Enantioselective Fluorescence Sensing

fluorescence sensingResearchers in the Lin Group, published in JACS, have built a highly porous and fluorescent metal–organic framework, MOF-1, from a chiral tetracarboxylate bridging ligand derived from 1,1′-bi-2-naphthol, BINOL, and a cadmium carboxylate infinite-chain secondary building unit. The fluorescence of MOF-1 can be effectively quenched by amino alcohols via H-bonding with the binaphthol moieties decorating the MOF, leading to a remarkable chiral sensor for amino alcohols with greatly enhanced sensitivity and enantioselectivity over BINOL-based homogeneous systems. The higher detection sensitivity of MOF-1 is due to a preconcentration effect by which the analytes are absorbed and concentrated inside the MOF channels, whereas the higher enantioselectivity of MOF-1 is believed to result from enhanced chiral discrimination owing to the cavity confinement effect and the conformational rigidity of the BINOL groups in the framework. MOF-1 was quenched by four chiral amino alcohols with unprecedentedly high Stern–Volmer constants of 490–31200 M–1and enantioselectivity ratios of 1.17–3.12.

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Hydrogen Generating MOFs

hydrogen generating mofsMetal-organic frameworks, MOFs, are an interesting class of porous crystalline materials that can be easily functionalized at the molecular level. The Lin Group is interested in using photoactive MOFs as a new platform to integrate different functional components that are needed for solar energy conversion. The group reports in JACS on the design of synergistic hydrogen evolution photocatalysts based on platinum nanoparticle MOF assemblies. Platinum nanoparticles were selectively loaded to the cavities of phosphorescent MOFs (1 and 2) to enable efficient photocatalytic H2 evolution via photo-injection of electrons from the light-harvesting MOF frameworks into the platinum nanoparticles. The Pt@2 assembly showed a hydrogen evolution efficiency increase by approximately five times, compared to the homogeneous control, and could be readily recycled and reused by centrifugation.

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Nanocomposites for Hydrogen Production

nanocomposites for hydrogen productionAs described in Advanced Materials, the Lin Group has developed a new metal-organic framework (MOF)-templated method for the synthesis of a mixed metal oxide nanocomposite with interesting photophysical properties. Fe-containing nanoscale MOFs are coated with amorphous titania, which are then are calcined to produce crystalline composite octahedral nanoshells with hematite Fe2O3 nanoparticles embedded in anatase TiO2. This material enables photocatalytic hydrogen production from water using visible light, which cannot be achieved by either Fe2O3 or TiO2 alone or a mixture of the two. This versatile MOF-templated nanocomposite synthesis procedure could be readily modified, by varying the type of MOF and the coating material, to prepare new materials with desirable synergistic properties.

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