Highly enantioselective resolution of terminal epoxides using polymeric catalysts

Poly-salen-Co(III) complexes were employed in the hydrolytic kinetic resolution (HKR) of terminal epoxides and ee's up to 98% were obtained. In the HKR of epichlorohydrin, the polymeric catalysts can be recovered and modified for recycling. The recovered polymer catalyst shows good activity and selectivity. (C) 2002 Elsevier Science Ltd. All rights reserved.

A high-resolution solid-state NMR study on nano-structured HZSM-5 zeolite

Variations in the structure and acidity properties of HZSM-5 zeolites with reduction in crystal sizes down to nanoscale (less than 100 nm) have been investigated by XRD, TEM and solid-state NMR with a system capable of in situ sample pretreatment. As evidenced by a combination of Al-27 MAS NMR, Si-29 MAS, CP/MAS NMR and H-1 MAS NMR techniques, the downsize of the zeolite crystal leads to an obvious line broadening of the Al-27, Si-29 MAS NMR spectrum, an increasing of the silanol concentration on the external surface, and a pronounced alteration of the acidity distribution between the external and internal surfaces of the zeolite. In a HZSM-5 zeolite with an average size at about 70 nm, the nonacidic hydroxyl groups (silanols) are about 14% with respect to the total amount of Si, while only 4% of such hydroxyl groups exist in the same kind of zeolite at 1000 nm crystal size. The result of H-1 MAS NMR obtained using Fluorinert(R) FC-43 (perfluorotributyl amine) as a probe molecule demonstrates that most of the silanols are located on the external surface of the zeolite. Moreover, the concentration of Bronsted acid sites on the external surface of the nano-structured zeolite appears to be distinctly higher than that of the microsized zeolite.

Multiple Resolution Image Classification

Binary image classifiction is a problem that has received much attention in recent years. In this paper we evaluate a selection of popular techniques in an effort to find a feature set/ classifier combination which generalizes well to full resolution image data. We then apply that system to images at one-half through one-sixteenth resolution, and consider the corresponding error rates. In addition, we further observe generalization performance as it depends on the number of training images, and lastly, compare the system's best error rates to that of a human performing an identical classification task given teh same set of test images.

The stability of nanosized HZSM-5 zeolite: a high-resolution solid-state NMR study

The thermal and hydrothermal stabilities of HZSM-5 zeolites with crystal sizes less than 100 nm have been studied by multinuclear solid-state NMR, combined with BET and XRD. As evidenced by Al-27 and Si-29 MAS as well as their corresponding cross-polarization/MAS NMR investigations, the thermal stability of nanosized HZSM-5 is not so good as that of microsized HZSM-5. This is due to two processes concerning dealumination and desilicification involved in the calcination of nanosized HZSM-5, while only the dealumination process is conducted in microsized HZSM-5 under the similar calcination process. The hydrothermal stability of nanosized HZSM-5 is, contrary to what was expected, not so bad as that of the microsized HZSM-5 in the course of steam treatment. The actual resistance of the hydrothermal stability to the crystal size of HZSM-5 can be ascribed to an active reconstruction of zeolitic framework through an effective filling of amorphous Si species into nanosized HZSM-5 during hydrothermal treatment. (C) 2001 Published by Elsevier Science B.V.

High resolution time-of-flight spectrometer for crossed molecular beam study of elementary chemical reactions

In this article, we describe an apparatus in our laboratory for investigating elementary chemical reactions using the high resolution time-of-flight Rydberg tagging method. In this apparatus, we have adopted a rotating source design so that collision energy can be changed for crossed beam studies of chemical reactions. Preliminary results on the HI photodissociation and the F atom reaction with H-2 are reported here. These results suggest that the experimental apparatus is potentially a powerful tool for investigating state-to-state dynamics of elementary chemical reactions. (c) 2005 American Institute of Physics.

Resolution prediction and optimization of temperature programme in comprehensive two-dimensional gas chromatography

A model is developed for predicting the resolution of interested component pair and calculating the optimum temperature programming condition in the comprehensive two-dimensional gas chromatography (GC x GC). Based on at least three isothermal runs, retention times and the peak widths at half-height on both dimensions are predicted for any kind of linear temperature-programmed run on the first dimension and isothermal runs on the second dimension. The calculation of the optimum temperature programming condition is based on the prediction of the resolution of "difficult-to-separate components" in a given mixture. The resolution of all the neighboring peaks on the first dimension is obtained by the predicted retention time and peak width on the first dimension, the resolution on the second dimension is calculated only for the adjacent components with un-enough resolution on the first dimension and eluted within a same modulation period on the second dimension. The optimum temperature programming condition is acquired when the resolutions of all components of interest by GC x GC separation meet the analytical requirement and the analysis time is the shortest. The validity of the model has been proven by using it to predict and optimize GC x GC temperature programming condition of an alkylpyridine mixture. (c) 2005 Elsevier B.V. All rights reserved.

Laser-heated high-temperature NMR - a time-resolution study

Submitted to Appl Magn Reson Sponsorship: EPSRC / EU

Ubuntu, Jesus, and Earth: Integrating African Religion and Christianity in Ecological Ethics

Africa faces problems of ecological devastation caused by economic exploitation, rapid population growth, and poverty. Capitalism, residual colonialism, and corruption undermine Africa's efforts to forge a better future. The dissertation describes how in Africa the mounting ecological crisis has religious, political, and economic roots that enable and promote social and environmental harm. It presents the thesis that religious traditions, including their ethical expressions, can effectively address the crisis, ameliorate its impacts, and advocate for social and environmental betterment, now and in the future. First, it examines African traditional religion and Christian teaching, which together provide the foundation for African Christianity. Critical examination of both religious worldviews uncovers their complementary emphases on human responsibility toward planet Earth and future generations. Second, an analysis of the Gwembe Tonga of Chief Simamba explores the interconnectedness of all elements of the universe in African cosmologies. In Africa, an interdependent, participatory relationship exists between the world of animals, the world of humans, and the Creator. In discussing the annual lwiindi (rain calling) ceremony of Simamba, the study explores ecological overtones of African religions. Such rituals illustrate the involvement of ancestors and high gods in maintaining ecological integrity. Third, the foundation of the African morality of abundant life is explored. Across Sub-Saharan Africa, ancestors' teachings are the foundation of morality; ancestors are guardians of the land. A complementary teaching that Christ is the ecological ancestor of all life can direct ethical responses to the ecological crisis. Fourth, the eco-social implications of ubuntu (what it means to be fully human) are examined. Some aspects of ubuntu are criticized in light of economic inequalities and corruption in Africa. However, ubuntu can be transformed to advocate for eco-social liberation. Fifth, the study recognizes that in some cases conflicts exist between ecological values and religious teachings. This conflict is examined in terms of the contrast between awareness of socioeconomic problems caused by population growth, on the one hand, and advocacy of a traditional African morality of abundant children, on the other hand. A change in the latter religious view is needed since overpopulation threatens sustainable living and the future of Earth. The dissertation concludes that the identification of Jesus with African ancestors and theological recognition of Jesus as the ecological ancestor, woven together with ubuntu, an ethic of interconnectedness, should characterize African consciousness and promote resolution of the socio-ecological crisis.

Cortical Learning of Recognition Categories: A Resolution of the Exemplar Vs. Prototype Debate

Do humans and animals learn exemplars or prototypes when they categorize objects and events in the world? How are different degrees of abstraction realized through learning by neurons in inferotemporal and prefrontal cortex? How do top-down expectations influence the course of learning? Thirty related human cognitive experiments (the 5-4 category structure) have been used to test competing views in the prototype-exemplar debate. In these experiments, during the test phase, subjects unlearn in a characteristic way items that they had learned to categorize perfectly in the training phase. Many cognitive models do not describe how an individual learns or forgets such categories through time. Adaptive Resonance Theory (ART) neural models provide such a description, and also clarify both psychological and neurobiological data. Matching of bottom-up signals with learned top-down expectations plays a key role in ART model learning. Here, an ART model is used to learn incrementally in response to 5-4 category structure stimuli. Simulation results agree with experimental data, achieving perfect categorization in training and a good match to the pattern of errors exhibited by human subjects in the testing phase. These results show how the model learns both prototypes and certain exemplars in the training phase. ART prototypes are, however, unlike the ones posited in the traditional prototype-exemplar debate. Rather, they are critical patterns of features to which a subject learns to pay attention based on past predictive success and the order in which exemplars are experienced. Perturbations of old memories by newly arriving test items generate a performance curve that closely matches the performance pattern of human subjects. The model also clarifies exemplar-based accounts of data concerning amnesia.

Molecular composition of biogenic secondary organic aerosols using ultrahigh resolution mass spectrometry: comparing laboratory and field studies

Numerous laboratory experiments have been performed in an attempt to mimic atmospheric secondary organic aerosol (SOA) formation. However, it is still unclear how close the aerosol particles generated in laboratory experiments resemble atmospheric SOA with respect to their detailed chemical composition. In this study, we generated SOA in a simulation chamber from the ozonolysis of α-pinene and a biogenic volatile organic compound (BVOC) mixture containing α- and β-pinene, Δ3-carene, and isoprene. The detailed molecular composition of laboratory-generated SOA was compared with that of background ambient aerosol collected at a boreal forest site (Hyytiälä, Finland) and an urban location (Cork, Ireland) using direct infusion nanoelectrospray ultrahigh resolution mass spectrometry. Kendrick Mass Defect and Van Krevelen approaches were used to identify and compare compound classes and distributions of the detected species. The laboratory-generated SOA contained a distinguishable group of dimers that was not observed in the ambient samples. The presence of dimers was found to be less pronounced in the SOA from the VOC mixtures when compared to the one component precursor system. The elemental composition of the compounds identified in the monomeric region from the ozonolysis of both α-pinene and VOC mixtures represented the ambient organic composition of particles collected at the boreal forest site reasonably well, with about 70% of common molecular formulae. In contrast, large differences were found between the laboratory-generated BVOC samples and the ambient urban sample. To our knowledge this is the first direct comparison of molecular composition of laboratory-generated SOA from BVOC mixtures and ambient samples.