Chemical assay-guided natural product isolation via solid-supported chemodosimetric fluorescent probe

As a new model of chemical assay-guided natural product isolation, an effective chemodosimetric assay system was devised. Our chemical assay system features a fluorogenic chemodosimeter immobilized on a solid support, which offers advantages in identifying the desired compounds in complex natural product mixtures. To isolate only compounds with the target functional groups, the click chemistry concept was adopted. The model system presented here was developed for natural products with a terminal alkyne. Using our newly designed alkyne sensing beads with the aforementioned features, we have readily identified, quantified, and isolated compounds with a terminal alkyne group from plant extracts.     

Two dimensional inorganic electride-promoted electron transfer efficiency in transfer hydrogenation of alkynes and alkenes

A simple and highly efficient transfer hydrogenation of alkynes and alkenes by using a two-dimensional electride, dicalcium nitride ([Ca₂N]⁺·e^–), as an electron transfer agent is disclosed. Excellent yields in the transformation are attributed to the remarkable electron transfer efficiency in the electride-mediated reactions. It is clarified that an effective discharge of electrons from the [Ca₂N]⁺·e^– electride in alcoholic solvents is achieved by the decomposition of the electride via alcoholysis and the generation of ammonia and Ca(OⁱPr)₂. We found that the choice of solvent was crucial for enhancing the electron transfer efficiency, and a maximum efficiency of 80% was achieved by using a DMF mixed isopropanol co-solvent system. This is the highest value reported to date among single electron transfer agents in the reduction of C–C multiple bonds. The observed reactivity and efficiency establish that electrides with a high density of anionic electrons can readily participate in the reduction of organic functional groups.     

The impact of conditions mimicking physiological environment on the thermal stability of aliphatic polycarbonate-based polyurethane elastomers

Journal of Thermal Analysis and Calorimetry - Thermal stabilities of all-aliphatic thermoplastic polyurethane (PU) films, either three-component (made from polycarbonate-based macrodiol,...     

Ultra-high surface area and mesoporous N-doped carbon derived from sheep bones with high electrocatalytic performance toward the oxygen reduction reaction

A nitrogen (N)-doped mesoporous carbon material exhibiting ultra-high surface area was successfully synthesized from sheep bones via a facile and low-cost method. The obtained carbon material had an ultra-high specific surface area of 1961 m² g^?1 and provided rich active sites for the oxygen reduction reaction (ORR), which in turn resulted in high electrocatalytic activity. It was found that the pore size distribution for the newly prepared carbonaceous material fell in the range of 1–4 nm. Benefiting from its high surface area and the presence of pyridine-N and quaternary-N species, the as-prepared carbon material exhibited excellent ORR activity in an oxygen-saturated 0.1 M KOH solution, compared to commercial Pt/C (10 wt%). Due to its high ORR catalytic activity, stability and low-cost, using sheep bone as C and N precursors to produce N-doped carbon provides an encouraging step toward the goal of replacing commercial Pt/C as fuel cell cathode electrocatalyst.     

Highly Ordered Mesoporous Cobalt-Copper Composite Oxides for Preferential CO Oxidation

Highly ordered mesoporous cobalt-copper composite oxides were prepared by the nanocasting method with various Co and Cu ratios. The catalysts obtained were characterized by X-ray diffraction, N₂ adsorption–desorption, H₂-temperature programmed reduction, CO-temperature programmed desorption and X-ray photoelectron spectroscopy. All of the catalysts had uniform mesopores and high surface areas. The distinct catalytic properties of these well-characterized mesoporous materials were demonstrated for preferential CO oxidation. It is found that the mesoporous cobalt-copper composite oxides, exhibited the higher catalytic activity for CO conversion and selectivity compared with the mesoporous Co₃O₄ and mesoporous CuO. Among these catalysts the mesoporous cobalt-copper catalyst with Co:Cu molar ratio of 70:30, shows the best catalytic activity and the broadest operating temperature “window” for the high CO conversion in the range of 125–200^oC. The higher catalytic activity was attributed to the higher CO adsorption and oxygen vacancies.     

A Kriging-based constrained global optimization algorithm for expensive black-box functions with infeasible initial points

In many engineering optimization problems, the objective and the constraints which come from complex analytical models are often black-box functions with extensive computational effort. In this case, it is necessary for optimization process to use sampling data to fit surrogate models so as to reduce the number of objective and constraint evaluations as soon as possible. In addition, it is sometimes difficult for the constrained optimization problems based on surrogate models to find a feasible point, which is the premise of further searching for a global optimal feasible solution. For this purpose, a new Kriging-based Constrained Global Optimization (KCGO) algorithm is proposed. Unlike previous Kriging-based methods, this algorithm can dispose black-box constrained optimization problem even if all initial sampling points are infeasible. There are two pivotal phases in KCGO algorithm. The main task of the first phase is to find a feasible point when there is no feasible data in the initial sample. And the aim of the second phase is to obtain a better feasible point under the circumstances of fewer expensive function evaluations. Several numerical problems and three design problems are tested to illustrate the feasibility, stability and effectiveness of the proposed method.     

VMO Spaces Associated with Operators with Gaussian Upper Bounds on Product Domains

In this paper, we extend the well-known result “the predual of Hardy space \(H^1\) is VMO” to the product setting, associated with differential operators. Let \(L_i\), \(i = 1, 2\), be the infinitesimal generators of the analytic semigroups \(\{e^{-tL_i}\}\) on \(L^2({\mathbb {R}})\). Assume that the kernels of the semigroups \(\{e^{-tL_i}\}\) satisfy the Gaussian upper bounds. We introduce the VMO spaces VMO\(_{L_1, L_2}(\mathbb {R}\times \mathbb {R})\) associated with operators \(L_1\) and \(L_2\) on the product domain \(\mathbb {R}\times \mathbb {R}\), then show that the dual space of VMO\(_{L_1, L_2}(\mathbb {R}\times \mathbb {R})\) is the Hardy space \(H^1_{L_1^*, L_2^*}(\mathbb {R}\times \mathbb {R})\) associated with the adjoint operators \(L^*_1\) and \(L^*_2\).     

The crank moments weighted by the parity of cranks

In this note, we introduce the 2kth crank moment \(\mu _{2k}(-1,n)\) weighted by the parity of cranks and show that \((-1)^n \mu _{2k}(-1,n)>0\) for \(n\ge k \ge 0\). When \(k=0\), the inequality \((-1)^n \mu _{2k}(-1,n)>0\) reduces to Andrews and Lewis’s inequality \((-1)^n(M_e(n)-M_o(n))>0\) for \(n\ge 0\), where \(M_e(n)\) (resp. \(M_o(n)\)) denotes the number of partitions of n with even (resp. odd) crank. Several generating functions of \(\mu _{2k}(-1,n)\) are also studied in order to show the positivity of \((-1)^n\mu _{2k}(-1,n)\).     

Carleson measures,BMO spaces and balayages associated to Schrdinger operators

Let L be a Schrdinger operator of the form L =-? + V acting on L~2(R~n), n≥3, where the nonnegative potential V belongs to the reverse Hlder class B_q for some q≥n. Let BMO_L(R~n) denote the BMO space associated to the Schrdinger operator L on R~n. In this article, we show that for every f ∈ BMO_L(R~n) with compact support, then there exist g ∈ L~∞(R~n) and a finite Carleson measure μ such that f(x) = g(x) + S_(μ,P)(x) with ∥g∥∞ + |||μ|||c≤ C∥f∥BMO_L(R~n), where S_(μ,P)=∫(R_+~(n+1))Pt(x,y)dμ(y, t),and Pt(x, y) is the kernel of the Poisson semigroup {e-~(t(L)~(1/2))}t0 on L~2(R~n). Conversely, if μ is a Carleson measure, then S_(μ,P) belongs to the space BMO_L(R~n). This extends the result for the classical John-Nirenberg BMO space by Carleson(1976)(see also Garnett and Jones(1982), Uchiyama(1980) and Wilson(1988)) to the BMO setting associated to Schrdinger operators.