Academic literature on the topic 'Criminology, n.e.c'

Abstract SYNTHESIS OF THE FIRST INTERNATIONAL SYMPOSIUM FOR RESEARCH IN COMPARATIVE CRIMINOLOGY Introduction At the beginning of the development of the social sciences there was a considerable vogue for comparative research. A long period of empirical studies and almost total preoccupation with methodological problems followed. Once again, however, psychology, political science, sociology, and above all anthropology, have taken up the thread of this tradition, and the bibliography in these fields is becoming ever more abundant. The study of deviance, of various manifestations of criminality, and of social reaction against crime are, however, noticeably missing in the picture, even though there is nothing in the nature of criminology which precludes the development of comparative research. To many research workers in criminology, the time seemed ripe to take up the comparative tradition once again. Two imperatives were considered : the generalization of norms of deviance which are tied to the standard of living set by industrial civilization, thus putting the problem of criminality in a global light ; and, second, the development and standardization of methods of studying these phenomena, drawing on the experience of allied disciplines. The response of the participants in this Symposium and the results of their discussions were not unexpected. A consensus was arrived as to the problems it was thought important to study, and agreement was reached about the strategies of research to be undertaken. Priorities, however, were not established since too much depends on the availability of research teams, funds, etc. But the broad, overall look at the main problems in comparative criminology will, hopefully, open a new chapter in the history of crimino-logical research and in our continuing search for knowledge of man and society. The brief resume which follows should give the reader an idea of the extent of the problems tackled. The detailed proceedings of the Symposium will be published at a later date, in mimeographed form. Sectors of research proposed In a sense, this Symposium was prepared by all the participants. The organizers had requested that each person invited prepare a memorandum setting out the problems in comparative criminology which he considered to be most important. The compilation of their replies, reported to the plenary session at the opening of the Symposium, produced the following results : Summary of suggestions for research activities Note : In all that follows, it should be understood that all of these topics should be studied in a cross-cultural or international context. 1) Definitions and concepts : a) Social vs legal concept of deviance ; b) Distinction between political and criminal crimes ; c) The law : a moral imperative or a simple norm ; d) The concepts used in penal law : how adequate ? e.g. personality of criminal ; e) Who are the sinners in different cultures and at different times. 2) Procedures : a) Working concepts of criminal law and procedure ; b) Differentiating between factors relating to the liability-finding process and the sentencing process ; c) Behavioural manifestations of the administration of criminal justice ; d) Judicial decisions as related to the personality of the judges and of the accused ; e) Sentencing in the cross-national context (2 proposals) ; f) In developing countries, the gap between development of the legal apparatus and social behaviour ; g) Determination of liability ; h) The problem of definition and handling of dangerous offenders ; i) Decision-making by the sentencing judges, etc. (2 proposals) ; ;) Medical vs penal committals ; k) Law-enforcement, policing. 3) Personnel : a) Professionalization in career patterns ; b) Criteria for personnel selection ; c) Greater use of female personnel. 4) Causation. Situations related to criminality : a) How international relations and other external factors affect crime ; 6) Hierarchy of causes of crime ; c) Migrants. Minorities in general ; d) Relation to socio-economic development in different countries ; e) A biological approach to criminal subcultures, constitutional types, twin studies, etc. ; f) Cultural and social approach : norms of moral judgment, ideals presented to the young, etc. ; g) Effect of social change : crime in developing countries, etc. (6 proposals) ; h) Effects of mass media, rapid dissemination of patterns of deviant behaviour (2 proposals). 5) Varieties of crime and criminals : a) Traffic in drugs ; b) Prison riots ; c) Violence particularly in youth (7 proposals) ; d) Dangerousness ; e) Relation to the rights of man (including rights of deviants); f) Female crime (2 proposals) ; g) Prostitution ; i) The mentally ill offender ; ;) Cultural variations in types of crime ; k) Organized crime ; /) Use of firearms ; m) Gambling ; n) Victims and victimology. 6) Treatment : evaluation : a) Social re-adaptation of offenders ; b) Statistical research on corrections, with possible computerization of data ; c) Comparisons between prisons and other closed environments ; d) Extra-legal consequences of deprivation of liberty ; e) Rehabilitation in developing countries ; f ) Criteria for evaluation of programs of correction ; g) Biochemical treatment (2 proposals) ; i) Differential treatment of different types of offense. Evaluation ; /) Prisons as agencies of treatment ; k) Effects of different degrees of restriction of liberty ; /) Environments of correctional institutions ; m) Study of prison societies ; n) Crime as related to the total social system. 7) Research methodology : a) Publication of what is known regarding methodology ; b) Methods of research ; c) Culturally-comparable vs culturally-contrasting situations ; d) Development of a new clearer terminology to facilitate communication ; e) Actual social validity of the penal law. 8) Statistics : epidemiology : a) Need for comparable international statistics ; standardized criteria (3 proposals) ; b) Difficulties. Criminologists must collect the data themselves. 9) Training of research workers : Recruiting and training of « com-paratists ». 10) Machinery : Committee of co-ordination. Discussions The discussions at the Symposium were based on these suggestions, the main concentration falling on problems of manifestations of violence in the world today, the phenomenon of student contestation, and on human rights and the corresponding responsibilities attached thereto. Although the participants did not come to definite conclusions as to the respective merits of the problems submitted for consideration, they did discuss the conditions under which comparative studies of these problems should be approached, the techniques appropriate to obtaining valid results, and the limitations on this type or work. Four workshops were established and studied the various problems. The first tackled the problems of the definition of the criteria of « danger » represented by different type of criminals ; the problem of discovering whether the value system which underlies the Human Rights Declaration corresponds to the value system of today's youth; the problem of the treatment of criminals ; of female criminality ; and, finally, of violence in the form of individual and group manifestations. The second workshop devoted its main consideration to the revolt of youth and to organized crime, also proposing that an international instrument bank of documentation and information be established. The third workshop considered problems of theory : how the police and the public view the criminal ; the opportunity of making trans-cultural comparisons on such subjects as arrest, prison, etc. ; and the role of the media of information in the construction of value systems. The fourth workshop blazed a trail in the matter of methodology appropriate to research in comparative criminology. The period of discussions which followed the report of the four workshops gave rise to a confrontation between two schools of thought within the group of specialists. The question arose as to whether the problem of student contestation falls within the scope of the science of criminology. Several experts expressed the opinion that criminologists ought not to concern themselves with a question which really belongs in the realm of political science. On the other hand, the majority of the participants appeared to feel that the phenomenon of student contestation did indeed belong in the framework of criminological research. One of the experts in particular took it upon himself to be the spokesman of this school of thought. There are those, he said, who feel that criminology should confine itself and its research to known criminality, to hold-ups, rape, etc. However, one should not forget that penal law rests on political foundations, the legality of power, a certain moral consensus of the population. Today, it is exactly this « legitimate » authority that is being contested. Is it not to be expected, therefore, that criminology should show interest in all sociological phenomena which have legal and criminal implications ? Contestation and violence have consequences for the political foundations of penal law, and therefore are fit subjects for the research of the criminologist. International Centre {or Comparative Criminology The First International Symposium for Research in Comparative Criminology situated itself and its discussions within the framework and in the perspectives opened by the founding of the International Centre for Comparative Criminology. The Centre is sponsored jointly by the University of Montreal and the International Society for Criminology, with headquarters at the University of Montreal. As one of the participants emphasized, criminologists need a place to retreat from the daily struggle, to meditate, to seek out and propose instruments of research valid for the study of problems common to several societies. Viewing the facts as scientists, we are looking for operational concepts. Theoreticians and research workers will rough out the material and, hopefully, this will inspire conferences and symposiums of practitioners, jurists, sociologists, penologists, and other specialists. Above all, it will give common access to international experience, something which is lacking at present both at the level of documentation and of action. A bank of instruments of method- ology in the field of comparative criminology does not exist at the present time. The Centre will undertake to compile and analyse research methods used in scientific surveys, and it will establish such an instrument bank. It will also gather and analyse information pertaining to legislative reforms now in progress or being contemplated in the field of criminal justice. Through the use of computers, the Centre will be able to put these two projects into effect and make the results easily accessible to research workers, and to all those concerned in this field. The participants at the Symposium were given a view of the extent of the problems envisaged for research by the future Centre. It is hoped that this initiative will be of concrete use to research workers, private organizations, public services and governments at many levels, and in many countries.

Resumen: El objetivo de la presente investigación es explorar la estructura y el contenido de una red de usuarios de abuso sexual basado en imágenes en Twitter. Para ello se analizaron los perfiles de Twitter que contienen la palabra "Quemón o “Nudes” utilizando análisis de redes, técnicas de procesamiento natural del lenguaje. Entre 2017 y 2018 hubo una comunidad de abuso sexual basado en imágenes en Twitter. Al menos 329 usuarios se dedicaron y se auto describieron como cuentas sexualmente explícitas, vengativas, y en donde contenido sexual no consensual podía ser compartido de forma anónima. Ya con seguidores, la red comprende a más de 130,000 personas. Esta es una estimación conservadora, más cuentas podrían utilizar diferentes palabras clave, no tener ninguna descripción, o formar parte de comunidades privadas. Estos resultados sugieren que los consumidores de contenido de abuso sexual basado en imágenes son los principales responsables de su propagación. Abstract: This study aimed to explore the structure and content of an image-based sexual abuse user network on Twitter. For this purpose, Twitter profiles containing the word “Quemones” or "Nudes" were analyzed using network analysis, natural language processing techniques. Between 2017 and 2018 there was a community of image-based sexual abuse on Twitter. At least 329 users engaged in and self- described themselves as sexually explicit, vindictive accounts, and where nonconsensual sexual content could be shared anonymously. Already with followers, the network comprises more than 130,000 people. This is a conservative estimate; more accounts could use different keywords, have no description, or be part of private communities. These results suggest that consumers of image-based sexual abuse content are primarily responsible for its spread. Fuentes de Consulta: Allen, W. D. (2007). The Reporting and Underreporting of Rape. 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Bullying behaviour can have a negative impact on a child's physical and psychological health. Bullying in the classroom is a challenge for early-childhood educators. Preschool is the first place outside the home where children face social challenges when interacting with their classmates. Child-Friendly Class is the first step and part of the Children Friendly School (CSF) as a UNICEF program and an important Indonesian government policy to prevent the emergence of child bullying behaviour. This study aims to identify needs in the process of developing a Child-Friendly Classroom Management model to anticipate bullying behaviour. This research and development method uses an adaptation of the Rowntree model which includes three stages of the process and data collection techniques using interviews, questionnaires, and observation. The results of this study indicate that the preparation of an effective classroom management guidebook to create child-friendly classes needs to be followed up immediately. Several findings related to teachers' perceptions of classroom management, and child-friendly classes prove that child-friendly classes have not been implemented properly in PAUD institutions, with bullying behaviour still appearing in early childhood in PAUD institutions. PAUD teachers understand that it is important to implement classroom management but so far there has been no manual on how to manage effective classrooms as well as training related to the implementation of effective classroom management. The creation of child-friendly classes is believed to be able to help teachers suppress the emergence of bullying behaviour in early childhood. Keywords: Child-Friendly Classroom Management, Bullying Prevention, Early Childhood Education References: Allday, R. A., Hinkson-Lee, K., Hudson, T. 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(2011). An Examination of New Zealand Teachers’ Attributions and Perceptions of Behaviour, Classroom Management, and the Level of Formal Teacher Training Received in Behaviour Management. King, E. (2020). Implications for the child friendly schools policy within Cambodia’s cultural and primary school context. Asia-Pacific Journal of Teacher Education, 48(4), 375–388. https://doi.org/10.1080/1359866X.2019.1645811 Kirves, L., & Sajaniemi, N. (2012). Bullying in early educational settings. Early Child Development and Care,182(3–4), 383–400. https://doi.org/10.1080/03004430.2011.646724 MacSuga, A. S., & Simonsen, B. (2011). Increasing Teachers’ Use of Evidence-Based Classroom Management Strategies through Consultation: Overview and Case Studies. Beyond Behavior, 20, 4–12. Maida, P. (2006). Child-Friendly-School-Manual. UNICEF. Modipane, M., & Themane, M. (2014). Teachers’ social capital as a resource for curriculum development: Lessons learnt in the implementation of a Child-Friendly Schools programme. South African Journal of Education, 34(4), 1–8. https://doi.org/10.15700/201412052105 Monks, C. P., Smith, P. K., & Swettenham, J. (2005). Psychological correlates of peer victimisation in preschool: Social cognitive skills, executive function and attachment profiles. Aggressive Behavior, 31(6), 571–588. https://doi.org/10.1002/ab.20099 Olweus, D. (1994). Bullying at School: Basic Facts and Effects of a School Based Intervention Program. Journal of Child Psychology and Psychiatry, 35(7), 1171–1190. https://doi.org/10.1111/j.1469-7610.1994.tb01229.x O’Neill, S. C., & Stephenson, J. (2011). Classroom behaviour management preparation in undergraduate primary teacher education in Australia: A web-based investigation. Australian Journal of Teacher Education, 36(10). https://doi.org/10.14221/ajte.2011v36n10.3 O’Neill, S., & Stephenson, J. (2012). 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ARCH GEN PSYCHIATRY, 66(9), 9. Tauber, R. T. (2007). Classroom Management: Sound Theory and Effective Practice. Praeger Publishers. https://books.google.la/books?id=XiQFyR41kysC Ttofi, M. M., & Farrington, D. P. (2011). Effectiveness of school-based programs to reduce bullying: A systematic and meta-analytic review. Journal of Experimental Criminology, 7(1), 27–56. https://doi.org/10.1007/s11292-010-9109-1 Ttofi, M. M., & Farrington, D. P. (2012). Bullying prevention programs: The importance of peer intervention, disciplinary methods and age variations. Journal of Experimental Criminology, 8(4), 443–462. https://doi.org/10.1007/s11292-012-9161-0 Unal, Z., & Unal, A. (2012). The Impact of Years of Teaching Experience on the Classroom Management Approaches of Elementary School Teachers. International Journal of Instruction, 5, 41–60. UNICEF. (2007). Implementation Handbook for The Convention on The Rights of The Child (3th Edition). UNICEF. Vaillancourt, T., McDougall, P., Hymel, S., Krygsman, A., Miller, J., Stiver, K., & Davis, C. (2008). Bullying: Are researchers and children/youth talking about the same thing? International Journal of Behavioral Development, 32(6), 486–495. https://doi.org/10.1177/0165025408095553 Vlachou, M., Andreou, E., Botsoglou, K., & Didaskalou, E. (2011). Bully/Victim Problems Among Preschool Children: A Review of Current Research Evidence. Educational Psychology Review, 23(3), 329–358. https://doi.org/10.1007/s10648-011-9153-z Vlachou, M., Botsoglou, K., & Andreou, E. (2014). Bullying/Victimization in Preschool Children. https://doi.org/10.13140/2.1.5086.1764 Vreeman, R. C., & Carroll, A. E. (2007). A systematic review of school-based interventions to prevent bullying. Archives of Pediatrics & Adolescent Medicine, 161 1, 78–88. Witvliet, M., Olthof, T., Hoeksma, J. B., Goossens, F. A., Smits, M. S. I., & Koot, H. M. (2010). Peer Group Affiliation of Children: The Role of Perceived Popularity, Likeability, and Behavioral Similarity in Bullying. Social Development, 19(2), 285–303. https://doi.org/10.1111/j.1467-9507.2009.00544.x Yaşar, M. (2017). Adaptation of General System Theory and Structural Family Therapy Approach to Classroom Management in Early Childhood Education* *. 32.

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El presente trabajo, vinculado a la l?nea de investigaci?n Sistemas Jur?dico-Penales Contempor?neos del Programa de P?s Graduaci?n en Ciencias Criminales (PPGCCRIM) de la Pontif?cia Universidade Cat?lica do Rio Grande do Sul, trata de una investigaci?n cr?tica acerca de las medidas cautelares alternativas al encarcelamiento, tras la creaci?n de la Ley n? 12.403, de 04 de Mayo de 2011. Para esto, fijase en la (innegable) crises por la que pasan todas las cuestiones referentes a las prisiones cautelares y sus efectos, fundamentalmente en lo que dice respecto a la manera como est?n ocurriendo tales juzgamientos si hay la utilizaci?n pr?ctica de la nueva ley por los juzgadores, y caso las haga, si los mismos, tras la nueva ley, mudaran su manera de juzgar - parti?ndose, para esto, de una premisa anterior, cuando las decisiones estaban pautadas solamente en la bipolaridad cautelar (prisi?n/libertad), utilizando e introduciendo en sus juzgamientos las nuevas medidas cautelares alternativas. Es importante subrayar la actualidad del eje en que se centra ese trabajo, dado que, como la nueva Ley empez? a regirse en 2011, a?n necesita desarrollarse en su aplicaci?n por parte de los juzgadores que van a utilizarla. En ese sentido, es fundamental analizar, en un primer momento, la principiologia, adem?s de los fundamentos de la prisi?n colectiva y, en un seg?n momento, presentar propiamente las medidas cautelares alternativas al c?rcel. La disertaci?n de maestr?a se concluye con un estudio cr?tico acerca de la utilizaci?n de tales medidas cautelares en casos concretos, por medio de habeas corpus juzgados por las C?maras Criminales del Tribunal de Justicia de Rio Grande del Sur, siendo que, despu?s, es realizada una cr?tica con relaci?n a la utilizaci?n de las referidas medidas en los juzgamientos ante aquella Corte.
O presente trabalho, vinculado ? linha de pesquisa Sistemas Jur?dico-Penais Contempor?neos do Programa de P?s-Gradua??o em Ci?ncias Criminais (PPGCCRIM) da Pontif?cia Universidade Cat?lica do Rio Grande do Sul (PUCRS), aborda uma pesquisa cr?tica sobre as medidas cautelares alternativas ao encarceramento, ap?s o advento da Lei n? 12.403, de 04 de maio de 2011. Para tanto, parte-se da (ineg?vel) crise que atravessa todas as quest?es envolvendo as pris?es cautelares e seus efeitos, principalmente no que se refere ? forma como vem ocorrendo tais julgamentos - se h? utiliza??o pr?tica da nova lei pelos julgadores, e se os mesmos, ap?s a nova lei, mudaram sua forma de julgar - partindo-se, para tanto, de uma premissa anterior, quando as decis?es pautavam apenas sobre a bipolaridade cautelar (pris?o/liberdade), passando a utilizar e inserir em seus julgamentos as novas medidas cautelares alternativas. ? importante destacar a atualidade do tema, pois como a nova Lei passou a viger em 2011, ainda necessita de amadurecimento coletivo por parte dos julgadores para sua melhor aplica??o. Nesse sentido, ? fundamental analisar, primeiramente, a principiologia e os fundamentos da pris?o preventiva; e, em um segundo momento, apresentar propriamente as medidas cautelares alternativas ao c?rcere. A disserta??o encerrase com um estudo cr?tico acerca da utiliza??o de tais medidas cautelares em casos concretos, atrav?s de habeas corpus julgados pelas C?maras Criminais do Tribunal de Justi?a do Estado do Rio Grande do Sul, seguidos de uma cr?tica sobre a utiliza??o das referidas medidas nos julgamento perante aquela Corte.

The formation of C-C and C-N bonds in modern organic synthesis is a key target for methodological advancement. Current methods of C-C and C-N bond formation often involve the use of expensive catalysts, or sub-stoichiometric reagents, which can lead to the generation of undesirable waste products. This thesis describes a novel and environmentally benign set of reaction conditions for the formation of C-C and C-N bonds by hydroacylation and this is promoted by mixing two reagents, an aldehyde and an electron-deficient double bond, under freely available atmospheric oxygen at room temperature Chapter 1 will provide an introduction to the thesis and mainly discusses methods for C-C bond formation, in particular, radical chemistry and hydroacylation. Chapter 2 describes the hydroacylation of vinyl sulfonates and vinyl sulfones (C-C double bonds) with aliphatic and aromatic aldehydes with a discussion and evidence for the mechanism of the transformation. Chapter 3 details the synthesis of precursors for intramolecular cyclisations and studies into aerobic intramolecular cyclisations. Chapter 4 describes the hydroacylation of vinyl phosphonates (C-C double bonds) and diazocarboxylates (N-N double bonds) with aliphatic and aromatic aldehydes bearing functional groups. In addition, the hydroacylation of diazocarboxylates with chiral aldehydes will be discussed. In conclusion, a new, facile and clean set of reaction conditions for the formation of C-C and C-N bonds has been developed via aerobic C-H activation of aldehydes providing access to unsymmetrical ketones.

Ce travail de these a permis le déveloippement de nouvelles reactions de couplage catalysées par des sels de cobalt(II) Le premier chapitre décrit l'allylation cobalta catalysée d'halogénures d'alkyles. La méthode est facile à mettre en œuvre, efficace avec une grande variété d'halogénures d'alkyes et des acétates ou carbonates d'allyle substitués. Les rendements vont de bons à excellents et la tolérance fonctionnelle élevée. Dans le cas d'acétates d'allyle substitués le produit linéaire est obtenu majoritairement ou exclusivement. Quelques expériences ont permis de mettre en lumière la formation d'espèce radicalaire lors du cycle catalytique. Les premiers essais pour étendre cette méthodologie aux couplages allyle-allyle et alkyle-alkyle sont également décrits. Le deuxième chapitre porte sur l'amination catalysée au cobalt d'organozinciques fonctionnalisés en utilisant des N-chloroamines. La procédure est simple et générale et demande des conditions plus douces que celles précédemment décrite, tout en tolérant un très large éventail de substrats, avec une bonne tolérance à de nombreux groupes fonctionnels. Les premiers essais pour étendre la méthodologie à la réaction entre un organozincique et une source électrophile de soufre en vue de former des liaisons C-S sont également exposés. Enfin le dernier chapitre décrit la réaction d'organozinciques engendrés par catalyse au cobalt avec une source " verte " de cyanure électrophile, N-cyano-N-phenyl-p-methyl-benzenesulfonamide (NCTS), pour conduire avec de bons rendements aux arylnitriles correspondants. Des sources analogues de CN+ ont également été testées.

In this thesis, the synthesis, characterisation and complexation chemistry of a series of related NNC and ONC pyridine based pincer ligands, together with some reaction chemistry of the metal complexes is described. The pro-ligands and the metal complexes have been characterised by a combination of multinuclear NMR spectroscopic techniques, IR spectroscopy, mass spectrometry and, for selected examples, by single crystal X-ray crystallography; remarkable spectroscopic and structural data are discussed. In Chapter 2, the synthesis and characterization of thirteen NNC and ONC pyridine based pincer ligands is described, including nine novel pincer ligands and four pyridine based pincers which have been previously reported. In Chapter 3, the palladium/platinum chemistry of NNCaryl and ONCaryl pyridine based pincer ligands is explored. Variation on the donor atoms has allowed an investigation of donor property influences on C-H activation, by giving peri-activated palladium pincer complexes for the ketimine-, aldimine-, amine- and biyridine-armed ligands and generating ortho-activated ONC palladium pincer complexes in the case of the alcohol-armed pro-ligand. Use of different palladium salts also led to different regioselective C-H activations. With the ketimine-armed naphthyl ligand (HL1ket-nap) as the example, the interconversion chemistry between the ortho- and peri-C-H activated products is also explored. In Chapter 4, sp3 C-H activation of the Et-armed ligand HL4Et with both palladium acetate and palladium chlorides has been unsuccessful, giving the N,N-coordinated bidentate species. The reaction of palladium acetate with the iPr-armed pro-ligand HL4iPr has resulted in minor amounts of C-H activated vinyl species with the major product being the non-activated palladium diacetate complex. Noticeably, upon reaction with Na2PdCl4, a mixture of the non-activated bis-chloride palladium complex and the sp3 C-H activated NNC-tridentate palladium species has been obtained, in a ratio of 1:1.5. Moreover, the sp3 C-H activation and the isolation of a rare sp3 C-H activated palladium complex have been achieved by reacting the tBu-armed pro-ligand HL4tBu with palladium acetate. The reaction of this ligand with Na2PdCl4 also resulted in the successful C-H activation of the tBu-arm to give a palladium pincer complex with a yield of 95%. Other than the NMR and FABMS analyses, the solid state X-ray structure of the latter complex confirmed the formation of the material as a rare sp3 C-H activated palladium complex. The stoichiometric reactivity of the (NNC/ONC)PdCl species towards AgBF4/AgPF6, and the subsequent ligand exchange reactions are disclosed in Chapter 5, together with the application of twelve palladium complexes as a series of promising catalysts in the allylic arylation of various allylic acetates with sodium tetraphenylborate.

Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Chemistry, 2003.
Vita.
Includes bibliographical references.
New methods for Pd-catalyzed cross-coupling reactions of aryl halides or arenesulfonates are described. Key to the success of these transformations is the proper choice of ligand and reaction conditions. Palladium catalysts supported by bulky, monodentate phosphine ligands with a biaryl backbone or the bidentate ligand, Xantphos, effectively promote the formation of ca-aryl carbonyl compounds. Base-sensitive functional groups are better tolerated when a weak base, such as K3PO4, is used. One of the most difficult transformations in Pd catalysis, the intermolecular C-O bond formation between primary alcohols and electron-neutral or even electron-rich aryl halides, was effectively promoted by the use of a new generation of ligands, 3-methyl-2-di-t-butylphosphinobiaryl. The one-step synthesis of ligands from cheap starting materials, as well as the mild reaction conditions employed for the coupling reactions, enables the practical use of Pd catalysis to access aryl alkyl ethers for the first time. Continuing study of Pd-catalyzed C-N bond-forming processes using biaryl monophosphine ligands led to the discovery of a structural derivative of these ligands, 2-dicyclohexylphosphino-2',4',6'-triisopropylbiphenyl. This ligand, in combination with a Pd source, produces a catalyst system with both a greater degree of activity and of stability than those that use our previous ligands. Substrates that were not amenable to Pd catalysis previously are reexamined using this new catalyst system, and excellent results are obtained.
by Xiaohua Huang.
Ph.D.

[EN] Heterogeneous catalysis is one of the most important tools in the advancement of green chemistry, understood it as one that efficiently uses (preferably renewable) raw materials, eliminate waste and avoids the use of toxic and/or dangerous reagents and solvents in chemicals production and application. In this thesis we have investigated the reaction mechanisms and the nature of the active centers in C-C, C-N and N-N bond forming reactions over cerium oxide and over gold nanoparticles supported on cerium oxide heterogeneous catalysts. As C-C bond formation reaction, we had been studied Sonogashira reaction catalyzed by a heterogeneous Au/CeO2 catalyst, wherein the CeO2 nanoparticle is about 5 nm in diameter. The second part of the thesis comprises the study of C-N bonds formation during carbamoylation reaction between diaminotoluene and dimethyl carbonate, catalyzed by cerium oxide, studying the effect over the reaction of the crystal planes available for reactants adsorption. In a third part, the N-N bond formation in the reductive coupling reaction of nitrocompounds to obtain azocompounds was studied, using Au/CeO2 as heterogeneous catalyst. Also in this section we report, by first time, an active and selective heterogeneous catalyst for the Mills reaction between nitroso compounds and anilines to obtain symmetric and asymmetric azocompounds.
[ES] La catálisis heterogénea es una de las más importantes herramientas para el desarrollo de la Química Sostenible, entendida como aquella que utiliza eficientemente las materias primas (preferiblemente renovables), elimina los desechos y evita el uso de reactivos y solventes tóxicos y/o peligrosos en la manufactura y aplicación de los productos químicos. En esta tesis doctoral se han investigado los mecanismos de reacción y la naturaleza de los centros activos, en reacciones de formación de enlaces C-C, C-N, y N-N sobre catalizadores heterogéneos de óxido de cerio y de nanopartículas de oro soportadas en óxido de cerio. Como reacción de formación de enlaces C-C se ha estudiado la reacción de Sonogashira catalizada con un catalizador heterogéneo de Au/CeO2, en donde el CeO2 está en forma de nanopartículas de cerca de 5nm de diámetro. En la segunda parte de la tesis se profundiza en el estudio de la formación de enlaces C-N durante la reacción de carbamoilación del diaminotolueno con dimetilcarbonato catalizada por el óxido de cerio, estudiando el efecto que tiene sobre la reacción la naturaleza de los planos cristalinos disponibles para la adsorción de los reactivos. En una tercera parte se estudia la formación de enlaces N-N en la reacción de acoplamiento reductivo de nitrocompuestos para obtener azocompuestos en presencia de un catalizador heterogéneo de Au/CeO2. Es este mismo apartado se reporta por primera vez un catalizador heterogéneo de alta actividad y selectividad para la Reacción de Mills entre un nitrosocompuesto y una anilina para obtener azocompuestos simétricos y asimétricos.
[CAT] La catàlisi heterogènia és una de les ferramentes més importants per al desenvolupament de la Química Sostenible, entesa com aquella que utilitza eficientment les matèries pimes (preferiblement renovables), elimina els rebutjos i evita l'ús de reactius i dissolvents tòxics i/o perillosos en la manufactura i aplicació dels productes químics. En esta tesi doctoral s'han investigat els mecanismes de reacció i la natura dels centres actius, en reaccions de formació d'enllaços C-C, C-N i N-N sobre catalitzadors heterogenis d'òxid de ceri i nanopartícules d'or suportades en òxid de ceri. Com reacció de formació d'enllaços C-C s'ha estudiat la reacció de Sonogashira catalitzada amb un catalitzador heterogeni d'Au/CeO2, on el CeO2 està en forma de nanopartícules amb un diàmetre proper als 5nm. En la segona part de la tesi s'aprofundeix en l'estudi de la formació d'enllaços C-N durant la reacció de carbamilació del diaminotoluè amb dimetilcarbonat catalitzada per l'òxid de ceri, estudiant l'efecte que té sobre la reacció la natura dels plans cristal·lins disponibles per a l'adsorció dels reactius. En una tercera part s'estudia la formació d'enllaços N-N en la reacció d'acoblament reductiu de nitrocompostos per a obtenir azocompostos en presència d'un catalitzador heterogeni d'Au/CeO2. En aquest mateix apartat es reporta per primera vegada un catalitzador heterogeni d'alta activitat i selectivitat per a la Reacció de Mills entre un nitrocompost i una anilina per a obtenir azocompostos simètrics i asimètrics.
Cómbita Merchán, DF. (2016). Formación de enlaces C-C, C-N y N-N con catalizadores de óxido de cerio y de oro/óxido de cerio [Tesis doctoral no publicada]. Universitat Politècnica de València. https://doi.org/10.4995/Thesis/10251/62780
TESIS

This work is foremost a study of various palladium-bearing N-heterocyclic carbenes complexes and their catalytic potential to form C-N bonds. Both alkyl amination and aryl amination are considered. Further elucidation on the mechanism of such catalytic activity is investigated. The viability of alkyl amination using palladium complexes bearing the ligands, ITMe, 1,2,3,4- tetramethylimidazol-2-ylidene, and ICy, 1,3- bis-cyclohexylimidazol-2-ylidene, as catalysts, is investigated. This includes the synthesis of [Pd(ITMe)(neopentyl)Cl]2,[Pd(ITMe)2(neopentyl)Cl], [Pd(ITMe)(neopentyl)(tbutylamine)Cl], [Pd(ITMe)(neopentyl)(hexylamine)Cl], with successful elimination of the alkyl-amination reaction product in low yield from the latter complex. [Pd(ICy)(neopentyl)Cl]2, [Pd(ICy)2(neopentyl)Cl] are also isolated. Unsuccessful attempts were made to vary the electronic properties of the complexes by replacing the amine with a hydrazine. Work was also done on indirect alkylation using tBuLi which led to a new method for synthesis of [Pd(ItBu)2] and novel complex, [Pd(ItBu)Cl3. ItBuH] (ItBu = 1,3- bis-tertbutylimidazol-2-ylidene). Aryl amination catalysed by complexes of palladium bearing the ligand, ITMe, is considered. This includes an improved synthesis of [Pd(ITMe)2] and synthesis of [Pd(ITMe)2(anisole)Cl]. Unsuccessful attempts at the elucidation of the mechanism of [Pd(ITMe)2(anisole)] formation led to the unexpected formation of [Pd(ITMe)2(SiMe3)(Si(SiMe3)3)] and [Pd(ITMe)2(SiMe3)2]. Aryl amination with using [Pd(ITMe)2(SiMe3)2] led to two aryl amination products, 4-ortho-methoxyphenyl morpholine as well as the expected para isomer. The use of complexes [Pd(ItBu)2] and [Pd(SIPr)2] (SIPr = 1,3-bis(2,6-diisopropylphenyl)imidazolin-2-ylidene) in C-S bond formation was explored. Addition of mesityl magnesium bromide to Pd(1,5-COD)Cl2 led to addition of mesityl substrate across 1,5-COD double bond and the addition of ITMe formed the Heck cycle intermediate [Pd(8-mesityl-1,4,5-η3 – C8H12)X2] (X=Cl, Br). Addition of 4-tolyl magnesium chloride resulting in the formation of Pd(ItBu)2(tolyl)Cl via an indirect route.

The radioactive nucleus ¹³N (t½ = 10 min, Jπ = ½) contains one loosely bound proton (Sp = 1.94 MeV) which can be considered to be bound to a core of ¹²C. Taking advantage of the recent availability of beams of radioactive nuclei at Louvain-la-Neuve, Belgium, a beam of ¹³N has been used to investigate the transfer reaction ¹¹B(¹³N,¹²C)¹²C. Particle-γ coincidence data was taken, using the LEDA silicon strip array and BaF₂ modules, gating on the 15.11 MeV γ-decay from the T = 1 state in ¹²C*. Two final states, corresponding to ¹²Cgs + ¹²C*(15.11 MeV) and ¹²C*(4.44 MeV)+ ¹²C*(15.11 MeV) have been observed and angular distributions have been measured for both transitions at each of two beam energies, 29.5 MeV and 45 MeV. The results are discussed with special reference to the loosely bound nature of the valence proton in ¹³N; the transfer reaction has been modelled using a DWBA code, with the ¹³N ground state constructed as a mixture of states: a p½ proton bound to ¹²Cgs , or a p3/2 proton bound to ¹²C*₂₊ (4.44 MeV). Fits to the experimental data have been obtained using a very shallow set of optical potentials, which are found to be energy dependent. The agreement with experiment is good, with the exception of the ¹²C*(4.44)+¹²C*(15.11) transition at the lower beam energy, which is significantly underestimated by the calculations, suggesting a contribution from a different reaction mechanism.

En une veriable complexe, l'image d'une fonction meromorphe evite au plus deux points de la sphere de rieman: c'est le theoreme de picard. De plus, grace a la theorie de nevanlinna, nous savons que chaque valeur est prise dans le disque de rayon r avec la meme frequence asymptotique sauf pour un ensemble denombrable de valeurs. En plusieurs variables, on observe un phenomene different. Il existe en effet des applications holomorphes, injectives, de c#n dans c#n dont l'image n'est pas dense dans c#n: ce sont les applications de fatou-bieberbach. Rosay et rudin ont montre qu'il existe pourtant des ensembles discrets qui doivent rencontrer l'image de toute application holomorphe non degeneree ; nous les appellerons ensembles inevitables. L. Gruman a construit explicitement une famille de tels ensembles e(a) parametres par a dans c*#n. Nous montrons que chaque ensemble e(a) est rencontre dans la boule de rayon r avec la meme frequence asymptotique pour tout a dans c*#n. Ceci constitue une sorte d'analogue a la theorie de nevanlinna en plusieurs variables

Els complexos organometàl·lics de coure, plata i or juguen un paper fonamental com espècies reactives en diverses transformacions químiques. Aquesta tesi aporta coneixement sobre el comportament d’aquests complexos en la formació d’enllaços C-C i/o C-N. En concret, estudiem: i) el mecanisme de reacció a través del qual els complexos de coure co-catalitzen un acoblament oxidant en el context de sistemes bimetàl·lics de rodi i coure; ii) el potencial de nucleòfils de plata com a agents transmetal·lants en reaccions de trifluorometilació catalitzades per pal·ladi; iii) el mecanisme de reacció de sistemes bimetàl·lics de Pd/Ag emprant un sistema model; i iv) el comportament de complexos bis(trifluorometil) cuprat, argentat i aurat com a nucleòfils. En aquesta tesi, on s´han combinat estudis experimentals i computacionals, s’ha adquirit nou coneixement sobre els processos estudiats, i s’ha contribuït al camp de la recerca química basada en el coneixement.
Los complejos organometálicos de cobre, plata y oro juegan un papel fundamental como especies reactivas en diversas transformaciones químicas. Esta tesis aporta conocimiento sobre el comportamiento de estos complejos en la formación de enlaces C-C y/o C-N. En concreto, estudiamos: i) el mecanismo de reacción por el cual complejos de cobre co-catalizan un acoplamiento oxidante en el contexto de sistemas bimetálicos de rodio y cobre; ii) el potencial de nucleófilos de plata como agentes transmetalantes en reacciones de trifluorometilación catalizadas por paladio; iii) el mecanismo de reacción de sistemas bimetálicos de Pd/Ag usando un sistema modelo; y iv) el comportamiento de complejos bis(trifluorometil) cuprato, argentato y aurato como nucleófilos. En esta tesis, donde se han combinado estudios experimentales y computacionales, se ha adquirido nuevo conocimiento sobre los procesos estudiados, y se ha contribuido al campo de la investigación química basada en el conocimiento.
Organometallic coinage metal complexes are be key reactive species for promoting a wide variety of chemical transformations. This thesis improves the understanding the behavior of these complexes in relevant C-C and/or C-N bond-forming reactions. Specifically, we have explored: i) the mechanistic intricacies of copper species as co-catalyst in the context of rhodium/copper-catalyzed oxidative coupling reactions; ii) the capability of silver nucleophiles as transmetalating agents in palladium-catalyzed trifluoromethylation reactions; iii) the reaction mechanism of Pd/Ag bimetallic reactions using a model system as probe; and, iv) the study of bis(trifluoromethyl) coinage metallates as nucleophiles. The fundamental insights gathered in this Thesis, encompassing both experimental and computational approaches, improve our understanding of the processes under study and make a contribution to the general field of knowledge-driven research in Chemistry.