Selective conversion of carbon dioxide into heavy olefins over Ga modified delafossite-CuFeO2.

Ga-modified CuFeO2 used as an efficient catalyst for CO2 hydrogenation to heavy olefins (C=5+) can achieve a high heavy olefin selectivity of 53.5%, which lies at a high level among reported catalysts, at a single pass CO2 conversion of 41.5%. It also displays an excellent long-term stability over 100 h, exhibiting its promising potential for industrial applications.

A nitrogen-doped carbon nanotube confined CuCo nanoalloy catalyzing one-pot conversion of levulinic acid to 1,4-pentanediol.

Nitrogen-doped carbon nanotube confined CuCo nanoalloy catalysts are fabricated by using ZIF-67 as a sacrificial template for the one-pot selective hydrogenation of levulinic acid (LA) to 1,4-pentanediol (1,4-PDO). The optimal catalyst achieves a high 1,4-PDO yield of 87.8% at full LA conversion. It also exhibits good recycling stability and can be reused at least 5 times.

Self-Polymerized Dopamine-Decorated Au NPs and Coordinated with Fe-MOF as a Dual Binding Sites and Dual Signal-Amplifying Electrochemical Aptasensor for the Detection of CEA.

Fabrication of functional electrochemical biosensor is a hot topic; however, precise and sensitive cancer detection in early clinical diagnosis is still a great challenge. Continuous efforts have been devoted to explore functional materials for this issue. In this work, we developed a dual binding sites and dual signal-amplifying electrochemical aptasensor of self-polymerized dopamine-decorated Au and coordinated with Fe-MOF (Au@PDA@Fe-MOF) for the detection of carcinoembryonic antigen (CEA). Remarkably, Au@PDA@Fe-MOF features high sensitivity, multiple active sites, good biocompatibility, and excellent selectivity, which is attributed to abundant -COOH in porous Fe-MOF and unsaturated Fe3+ sites on the surface of Fe-MOF as the active binding sites grafting more NH2-functionalized CEA-specific aptamer and redox PDA and Fe-MOF accelerating the movement of electrons for dual signal amplifying. Meanwhile, the electrochemical aptasensor shows favorable repeatability with 1.82% relative standard deviation (RSD) under five independent aptasensors and strong stability with only 3.3% degradation after 12 days of storage. In addition, the aptasensor has wide CEA detection range from 1 fg mL-1 to 1 µg mL-1 with a low detection limit of 0.33 fg mL-1 (S/N = 3). Furthermore, the aptasensor is feasible for accurate and quantitative detection of CEA in serum samples with RSD below 2.32%. The satisfying results demonstrate promising applications of the CEA aptasensor in practical sample analysis and lay an important foundation for other biomarker detection in early clinical diagnosis.

Cobalt-promoted fabrication of 3D carbon with a nanotube-sheet mutual support structure: scalable preparation of a high-performance anode material for Li-ion batteries.

Currently, the design of carbon-based composite as a high-performance anode material for lithium-ion batteries (LIBs) presents challenges for commercial application. Herein, we developed a three-dimensional carbon-based material with a nanotube-sheet mutual support structure (MS-CNTS) engineered by the catalytic effect of Co species. The present work highlights a concise 'solvent-free' synthetic method allowing for large-scale output, which is potentially available for low cost commercial use. With the readily available acetylacetonate and cobalt (II) acetylacetonate as starting chemicals, this nanostructured carbonaceous material is fabricated with aldol condensation to construct a Co-contained carbon-link network polymer precursor followed by annealing under argon. It is composed of brim-curled graphene-like carbon nanosheets and carbon nanotubes, which support each other's structures to effectively avoid agglomeration. Therefore, it enables high performance in LIBs. In spite of the trace amount of cobalt, the carbon-based MS-CNTS anode delivers a high charge capacity of 1028 mAh g-1 at 0.1 A g-1, high rate capacity of 495 mAh g-1 at 2 A g-1, and ultra-long cycling life with a very low capacity decay of 0.008% per cycle over 1000 cycles at 0.5 A g-1, accompanied by 100% Coulombic efficiency. From full cell measurements, we further confirm the considerable promise of MS-CNTS as anodes with a long cycling life.

Magnetically Hollow Pt Nanocages with Ultrathin Walls as a Highly Integrated Nanoreactor for Catalytic Transfer Hydrogenation Reaction.

Fabricating efficient and stable nanocatalysts for chemoselective hydrogenation of nitroaromatics is highly desirable because the amines hold tremendous promise for the synthesis of nitrogen containing chemicals. Here, a highly reactive and stable porous carbon nitride encapsulated magnetically hollow platinum nanocage is developed with subnanometer thick walls (Fe3O4@snPt@PCN) for this transformation. This well-controlled nanoreactor is prepared via the following procedures: the preparation of core template, the deposition of platinum nanocage with subnanometer thick walls, oxidative etching, and calcination. This highly integrated catalyst demonstrates excellent performance for the catalytic transfer hydrogenation of various nitroaromatics and the reaction can reach >99% conversion and >99% selectivity. With the ultrathin wall structure, the atom utilization of platinum atoms is highly efficient. The X-ray photoelectron spectroscopy results indicate that partial electrons transfer from the iron oxides to Pt nanowalls, and this increases the electron density of snPt nanoparticles, thus promoting the catalytic activity for the transfer hydrogenation of nitroaromatics. For the reduction of 4-nitrophenol, the reaction rate constant K app is 0.23 min-1 and the turnover frequency (TOF) is up to 3062 h-1. Additional reaction results illustrate that this magnetic nanoreactor can be reused more than eight times and it is a promising catalytic nanoplatform in heterogeneous catalysis.

Direct Production of 2,5-Dimethylfuran with High Yield from Fructose over a Carbon-Based Solid Acid-Coated CuCo Bimetallic Catalyst.

A carbon-based solid acid, which functionalized with p-toluenesulfonic acid (TsOH), an encapsulated non-noble CuCo multifunctional heterogeneous catalyst was for the first time developed and used to catalyze the one-pot direct conversion of fructose into 2,5-dimethylfuran (2,5-DMF) without purification of 5-hydroxymethylfurfural (5-HMF) from the reaction solutions. Fructose was first transformed into intermediate 5-HMF over the outer shell carbon-based solid acid sites via dehydration, and subsequently 5-HMF was further converted to produce 2,5-DMF over the non-noble metal active sites in the core. As high as 71.1 mol % yield of 2,5-DMF was achieved in tetrahydrofuran at 220 °C and 3 MPa H2 for 10 h, which is higher than the yield reported for the direct conversion of fructose to 2,5-DMF. Besides, the carbon-based solid acid-coated CuCo catalyst could be reused up to five times.

Facile and Large-Scale Fabrication of Sub-3†nm PtNi Nanoparticles Supported on Porous Carbon Sheet: A Bifunctional Material for the Hydrogen Evolution Reaction and Hydrogenation.

Facile and large-scale preparation of materials with uniform distributions of ultrafine particles for catalysis is a challenging task, and it is even more difficult to obtain catalysts that excel in both the hydrogen evolution reaction (HER) and hydrogenation, which are the corresponding merging and splitting procedures of hydrogen, respectively. Herein, the fabrication of ultrafine bimetallic PtNi nanoparticles embedded in carbon nanosheets (CNS) by means of in situ self-polymerization and annealing is reported. This bifunctional catalyst shows excellent performance in the hydrogen evolution reaction (HER) and the hydrogenation of p-nitrophenol. Remarkably PtNi bimetallic catalyst with low metal loading (PtNi2 @CNS-600, 0.074 wt % Pt) exhibited outstanding HER activity with an overpotential as low as 68 mV at a current density of 10 mA cm-2 with a platinum loading of only 0.612 µgPt cm-2 and Tafel slope of 35.27 mV dec-1 in a 0.5 m aqueous solution of H2 SO4 , which is comparable to that of the 20 % Pt/C catalyst (31 mV dec-1 ). Moreover, it also shows superior long-term electrochemical durability for at least 30 h with negligible degradation compared with 20 % Pt/C. In addition, the material with increased loading (mPtNi2 @CNS-600, 2.88 % Pt) showed robust catalytic activity for hydrogenation of p-nitrophenol at ambient pressure and temperature. The catalytic activity towards hydrogen splitting is a circumstantial evidence that agrees with the Volmer-Tafel reaction path in the HER.

Pd-CuFe Catalyst for Transfer Hydrogenation of Nitriles: Controllable Selectivity to Primary Amines and Secondary Amines.

A multicomponent nanocatalyst system was fabricated for the transfer hydrogenation of nitrile compounds. This catalyst system contains palladium, copper, and iron, which are supported on the magnetite nanospheres, and the loading of palladium could be at the parts per million level. Palladium and copper contribute to the transformation of nitrile, and the product distribution highly depends on the alloying of Fe to Cu. The nitriles could be converted to primary amine by the Pd-Cu catalyst in the absence of Fe, whereas in the presence of Fe the products are secondary amines with high selectivity. This could be attributed to the electronic modulation of iron to copper. A variety of nitriles have been transformed to the corresponding primary or secondary amines with high selectivity, and the TOF reaches 2,929 hr-1 for Pd. Furthermore, the catalyst could be recycled by an external magnetic field and reused five times without severe activity loss.

Evaluation of carotid atherosclerotic plaque surface characteristics utilizing simultaneous noncontrast angiography and intraplaque hemorrhage (SNAP) technique.

PURPOSE: To evaluate the feasibility of the Simultaneous Noncontrast Angiography and intraPlaque hemorrhage (SNAP) technique in identification of carotid plaque surface characteristics compared with the conventional multicontrast vessel wall imaging protocol. MATERIALS AND METHODS: Thirty symptomatic patients with carotid plaque were recruited and underwent carotid artery magnetic resonance imaging (MRI) (3.0T) using a conventional multicontrast protocol and SNAP sequence. As an intrinsic multicontrast sequence, SNAP could generate a gray blood reference (Ref) image set, a black blood corrected real (CR) image set, and a bright blood MR angiography (MRA) image set. A bright blood SNAP Ref2 image was implemented by combining Ref and MRA images for facilitating plaque surface characteristics evaluation. The presence/absence of calcification (CA), juxtaluminal calcification (JCA), and ulceration was assessed. The agreement between SNAP and multicontrast vessel wall protocol in identifying CA, JCA, and ulceration was analyzed using Cohen's kappa analysis. The interreader and intrareader reproducibility of SNAP imaging in identifying plaque surface characteristics was also assessed. RESULTS: Good to excellent agreement was found between SNAP and conventional multicontrast protocol in identifying CA (κ = 0.74, 95% confidence interval [CI]: 0.54-0.93), JCA (κ = 0.81, 95% CI: 0.66-0.97), and ulceration (κ = 0.82, 95% CI: 0.65-0.99). In addition, excellent intrareader and interreader reproducibility was found for SNAP imaging in identification of CA, JCA, and ulceration. CONCLUSION: SNAP imaging showed excellent agreement with multicontrast imaging and high reproducibility in identification of both JCA and ulceration, suggesting that SNAP imaging may be a time-efficient, alternative tool in identification of plaque surface characteristics in carotid arteries. LEVEL OF EVIDENCE: 4 Technical Efficacy: Stage 1 J. Magn. Reson. Imaging 2018;47:634-639.

Carrageenan/MIV-150 (PC-815), a combination microbicide.

OBJECTIVE: The objective of this article is to study the effect of PC-815, a novel combination microbicide containing carrageenan and the nonnucleoside reverse transcriptase inhibitor (NNRTI) MIV-150, in blocking HIV-1 and HIV-2 infections in vitro as compared with Carraguard alone. GOAL: The goal of this study was to develop a combination microbicide that is more efficacious than Carraguard against HIV-1 and HIV-2. STUDY DESIGN: The microtiter syncytial assay was used to evaluate: 1) the antiviral and virucidal activity of MIV-150 against HIV-1MN; 2) the additive effect of MIV-150 when combined with carrageenan; and 3) a possible interference of seminal fluid in the antiviral activity of these compounds. RESULTS: MIV-150 effectively inactivated free virus. Combination of MIV-150 and Carraguard demonstrated an additive antiviral effect. Seminal fluid had no effect on the antiviral activity of MIV-150 or Carraguard. The average concentration that blocks 50% of infection (EC50) for PC-815 was approximately 10 times stronger than Carraguard for the different clinical isolates used in the study. CONCLUSION: Theoretically, PC-815 is likely to be a more efficacious microbicide than Carraguard.