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1.
COMPARAÇÃO ENTRE MÉTODOS PARA DETERMINAÇÃO DE CARGAS ATÔMICAS EM SISTEMAS MOLECULARES: A MOLÉCULA N-{N-(PTERINA-7-IL)CARBONILGLICIL}-L-TIROSINA (NNPT)
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Botelho, Fernanda Diniz
; Oliveira, Roberta Siqueira Soldaini de
; Almeida, Joyce S. F. D. de
; França, Tanos C. C.
; Borges Jr., Itamar
.
Selecting a method to compute partial atomic charges is not trivial because different methods usually provide different charge values and there is no consensus on the most useful approach. In this work, Mulliken, MBS, Chelp, Chelpg, MK, Hirshfeld, NPA, DMA and AIM methods were selected to compute atomic charges and electric dipole moment vector of N-{N-(Pterin-7-yl)carbonylglycyl}-L-tyrosine molecule, a ricin inhibitor which has different types of bonds and chemical environments. While MBS and DMA methods provided the most chemically consistent charges according to atomic electronegativity and electron resonance effects criteria, Chelp, Chelpg and MK had the worst performances. Atomic charges and dipole moment calculated by the Hirshfeld method had the smallest magnitudes, a well-known behavior. Despite the differences among atomic charges predicted by all methods, the direction of the dipole moment vector was essentially the same. Further charge calculations using different basis sets and quantum methods indicated that the dependency on this aspect was the highest for Mulliken and Chelp and the lowest for MBS, Hirshfeld and DMA methods. Thus, results point to MBS and DMA as the most suitable methods for computing chemically consistent atomic charges and dipole moment vectors of similar systems for different applications; e.g., molecular dynamics.
https://doi.org/10.21577/0100-4042.20170683
137 downloads
2.
Molecular Electronic Topology and Fragmentation Onset via Charge Partition Methods and Nuclear Fukui Functions: 1,1-Diamino-2,2-dinitroethylene
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We investigated theoretically the ground state electronic structure and the onset of molecular fragmentation of 1,1-diamino-2,2-dinitroethylene (FOX-7) using density functional theory. The molecular charge density was analyzed via two partition methods: the distributed multipole analysis (DMA) and the deformed atoms in molecules (DAM). In this framework, the push-pull effect, hydrogen intra-molecular bonding and site acid-base properties of the molecule were discussed. Our analysis indicates that the molecular origin of the low measured impact sensitivity of FOX-7 is due to the magnitude of multipole values of the C-N bonds in the NO2 groups, the delocalized electrons over the central C-C bond and the hydrogen bonds. The onset of FOX-7 decomposition and acid-base properties were examined with the nuclear Fukui functions. The results support nitro to nitrite rearrangement and direct release of a NO2 as a possible initial step in FOX-7 decomposition process. The approach suggested is general and can be especially useful for very large molecules to examine in detail their electronic structure and to guide the search for the decomposition mechanisms.
https://doi.org/10.5935/0103-5053.20150044
1047 downloads
3.
Growing knowledge: an overview of Seed Plant diversity in Brazil
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Zappi, Daniela C.
; Filardi, Fabiana L. Ranzato
; Leitman, Paula
; Souza, Vinícius C.
; Walter, Bruno M.T.
; Pirani, José R.
; Morim, Marli P.
; Queiroz, Luciano P.
; Cavalcanti, Taciana B.
; Mansano, Vidal F.
; Forzza, Rafaela C.
; Abreu, Maria C.
; Acevedo-Rodríguez, Pedro
; Agra, Maria F.
; Almeida Jr., Eduardo B.
; Almeida, Gracineide S.S.
; Almeida, Rafael F.
; Alves, Flávio M.
; Alves, Marccus
; Alves-Araujo, Anderson
; Amaral, Maria C.E.
; Amorim, André M.
; Amorim, Bruno
; Andrade, Ivanilza M.
; Andreata, Regina H.P.
; Andrino, Caroline O.
; Anunciação, Elisete A.
; Aona, Lidyanne Y.S.
; Aranguren, Yani
; Aranha Filho, João L.M.
; Araújo, Andrea O.
; Araújo, Ariclenes A.M.
; Araújo, Diogo
; Arbo, María M.
; Assis, Leandro
; Assis, Marta C.
; Assunção, Vivian A.
; Athiê-Souza, Sarah M.
; Azevedo, Cecilia O.
; Baitello, João B.
; Barberena, Felipe F.V.A.
; Barbosa, Maria R.V.
; Barros, Fábio
; Barros, Lucas A.V.
; Barros, Michel J.F.
; Baumgratz, José F.A.
; Bernacci, Luis C.
; Berry, Paul E.
; Bigio, Narcísio C.
; Biral, Leonardo
; Bittrich, Volker
; Borges, Rafael A.X.
; Bortoluzzi, Roseli L.C.
; Bove, Cláudia P.
; Bovini, Massimo G.
; Braga, João M.A.
; Braz, Denise M.
; Bringel Jr., João B.A.
; Bruniera, Carla P.
; Buturi, Camila V.
; Cabral, Elza
; Cabral, Fernanda N.
; Caddah, Mayara K.
; Caires, Claudenir S.
; Calazans, Luana S.B.
; Calió, Maria F.
; Camargo, Rodrigo A.
; Campbell, Lisa
; Canto-Dorow, Thais S.
; Carauta, Jorge P.P.
; Cardiel, José M.
; Cardoso, Domingos B.O.S.
; Cardoso, Leandro J.T.
; Carneiro, Camila R.
; Carneiro, Cláudia E.
; Carneiro-Torres, Daniela S.
; Carrijo, Tatiana T.
; Caruzo, Maria B.R.
; Carvalho, Maria L.S.
; Carvalho-Silva, Micheline
; Castello, Ana C.D.
; Cavalheiro, Larissa
; Cervi, Armando C.
; Chacon, Roberta G.
; Chautems, Alain
; Chiavegatto, Berenice
; Chukr, Nádia S.
; Coelho, Alexa A.O.P.
; Coelho, Marcus A.N.
; Coelho, Rubens L.G.
; Cordeiro, Inês
; Cordula, Elizabeth
; Cornejo, Xavier
; Côrtes, Ana L.A.
; Costa, Andrea F.
; Costa, Fabiane N.
; Costa, Jorge A.S.
; Costa, Leila C.
; Costa-e-Silva, Maria B.
; Costa-Lima, James L.
; Cota, Maria R.C.
; Couto, Ricardo S.
; Daly, Douglas C.
; De Stefano, Rodrigo D.
; De Toni, Karen
; Dematteis, Massimiliano
; Dettke, Greta A.
; Di Maio, Fernando R.
; Dórea, Marcos C.
; Duarte, Marília C.
; Dutilh, Julie H.A.
; Dutra, Valquíria F.
; Echternacht, Lívia
; Eggers, Lilian
; Esteves, Gerleni
; Ezcurra, Cecilia
; Falcão Junior, Marcus J.A.
; Feres, Fabíola
; Fernandes, José M.
; Ferreira, D.M.C.
; Ferreira, Fabrício M.
; Ferreira, Gabriel E.
; Ferreira, Priscila P.A.
; Ferreira, Silvana C.
; Ferrucci, Maria S.
; Fiaschi, Pedro
; Filgueiras, Tarciso S.
; Firens, Marcela
; Flores, Andreia S.
; Forero, Enrique
; Forster, Wellington
; Fortuna-Perez, Ana P.
; Fortunato, Reneé H.
; Fraga, Cléudio N.
; França, Flávio
; Francener, Augusto
; Freitas, Joelcio
; Freitas, Maria F.
; Fritsch, Peter W.
; Furtado, Samyra G.
; Gaglioti, André L.
; Garcia, Flávia C.P.
; Germano Filho, Pedro
; Giacomin, Leandro
; Gil, André S.B.
; Giulietti, Ana M.
; A.P.Godoy, Silvana
; Goldenberg, Renato
; Gomes da Costa, Géssica A.
; Gomes, Mário
; Gomes-Klein, Vera L.
; Gonçalves, Eduardo Gomes
; Graham, Shirley
; Groppo, Milton
; Guedes, Juliana S.
; Guimarães, Leonardo R.S.
; Guimarães, Paulo J.F.
; Guimarães, Elsie F.
; Gutierrez, Raul
; Harley, Raymond
; Hassemer, Gustavo
; Hattori, Eric K.O.
; Hefler, Sonia M.
; Heiden, Gustavo
; Henderson, Andrew
; Hensold, Nancy
; Hiepko, Paul
; Holanda, Ana S.S.
; Iganci, João R.V.
; Imig, Daniela C.
; Indriunas, Alexandre
; Jacques, Eliane L.
; Jardim, Jomar G.
; Kamer, Hiltje M.
; Kameyama, Cíntia
; Kinoshita, Luiza S.
; Kirizawa, Mizué
; Klitgaard, Bente B.
; Koch, Ingrid
; Koschnitzke, Cristiana
; Krauss, Nathália P.
; Kriebel, Ricardo
; Kuntz, Juliana
; Larocca, João
; Leal, Eduardo S.
; Lewis, Gwilym P.
; Lima, Carla T.
; Lima, Haroldo C.
; Lima, Itamar B.
; Lima, Laíce F.G.
; Lima, Laura C.P.
; Lima, Leticia R.
; Lima, Luís F.P.
; Lima, Rita B.
; Lírio, Elton J.
; Liro, Renata M.
; Lleras, Eduardo
; Lobão, Adriana
; Loeuille, Benoit
; Lohmann, Lúcia G.
; Loiola, Maria I.B.
; Lombardi, Julio A.
; Longhi-Wagner, Hilda M.
; Lopes, Rosana C.
; Lorencini, Tiago S.
; Louzada, Rafael B.
; Lovo, Juliana
; Lozano, Eduardo D.
; Lucas, Eve
; Ludtke, Raquel
; Luz, Christian L.
; Maas, Paul
; Machado, Anderson F.P.
; Macias, Leila
; Maciel, Jefferson R.
; Magenta, Mara A.G.
; Mamede, Maria C.H.
; Manoel, Evelin A.
; Marchioretto, Maria S.
; Marques, Juliana S.
; Marquete, Nilda
; Marquete, Ronaldo
; Martinelli, Gustavo
; Martins da Silva, Regina C.V.
; Martins, Ângela B.
; Martins, Erika R.
; Martins, Márcio L.L.
; Martins, Milena V.
; Martins, Renata C.
; Matias, Ligia Q.
; Maya-L., Carlos A.
; Mayo, Simon
; Mazine, Fiorella
; Medeiros, Debora
; Medeiros, Erika S.
; Medeiros, Herison
; Medeiros, João D.
; Meireles, José E.
; Mello-Silva, Renato
; Melo, Aline
; Melo, André L.
; Melo, Efigênia
; Melo, José I.M.
; Menezes, Cristine G.
; Menini Neto, Luiz
; Mentz, Lilian A.
; Mezzonato, A.C.
; Michelangeli, Fabián A.
; Milward-de-Azevedo, Michaele A.
; Miotto, Silvia T.S.
; Miranda, Vitor F.O.
; Mondin, Cláudio A.
; Monge, Marcelo
; Monteiro, Daniele
; Monteiro, Raquel F.
; Moraes, Marta D.
; Moraes, Pedro L.R.
; Mori, Scott A.
; Mota, Aline C.
; Mota, Nara F.O.
; Moura, Tania M.
; Mulgura, Maria
; Nakajima, Jimi N.
; Nardy, Camila
; Nascimento Júnior, José E.
; Noblick, Larry
; Nunes, Teonildes S.
; O'Leary, Nataly
; Oliveira, Arline S.
; Oliveira, Caetano T.
; Oliveira, Juliana A.
; Oliveira, Luciana S.D.
; Oliveira, Maria L.A.A.
; Oliveira, Regina C.
; Oliveira, Renata S.
; Oliveira, Reyjane P.
; Paixão-Souza, Bruno
; Parra, Lara R.
; Pasini, Eduardo
; Pastore, José F.B.
; Pastore, Mayara
; Paula-Souza, Juliana
; Pederneiras, Leandro C.
; Peixoto, Ariane L.
; Pelissari, Gisela
; Pellegrini, Marco O.O.
; Pennington, Toby
; Perdiz, Ricardo O.
; Pereira, Anna C.M.
; Pereira, Maria S.
; Pereira, Rodrigo A.S.
; Pessoa, Clenia
; Pessoa, Edlley M.
; Pessoa, Maria C.R.
; Pinto, Luiz J.S.
; Pinto, Rafael B.
; Pontes, Tiago A.
; Prance, Ghillean T.
; Proença, Carolyn
; Profice, Sheila R.
; Pscheidt, Allan C.
; Queiroz, George A.
; Queiroz, Rubens T.
; Quinet, Alexandre
; Rainer, Heimo
; Ramos, Eliana
; Rando, Juliana G.
; Rapini, Alessandro
; Reginato, Marcelo
; Reis, Ilka P.
; Reis, Priscila A.
; Ribeiro, André R.O.
; Ribeiro, José E.L.S.
; Riina, Ricarda
; Ritter, Mara R.
; Rivadavia, Fernando
; Rocha, Antônio E.S.
; Rocha, Maria J.R.
; Rodrigues, Izabella M.C.
; Rodrigues, Karina F.
; Rodrigues, Rodrigo S.
; Rodrigues, Rodrigo S.
; Rodrigues, Vinícius T.
; Rodrigues, William
; Romaniuc Neto, Sérgio
; Romão, Gerson O.
; Romero, Rosana
; Roque, Nádia
; Rosa, Patrícia
; Rossi, Lúcia
; Sá, Cyl F.C.
; Saavedra, Mariana M.
; Saka, Mariana
; Sakuragui, Cássia M.
; Salas, Roberto M.
; Sales, Margareth F.
; Salimena, Fatima R.G.
; Sampaio, Daniela
; Sancho, Gisela
; Sano, Paulo T.
; Santos, Alessandra
; Santos, Élide P.
; Santos, Juliana S.
; Santos, Marianna R.
; Santos-Gonçalves, Ana P.
; Santos-Silva, Fernanda
; São-Mateus, Wallace
; Saraiva, Deisy P.
; Saridakis, Dennis P.
; Sartori, Ângela L.B.
; Scalon, Viviane R.
; Schneider, Ângelo
; Sebastiani, Renata
; Secco, Ricardo S.
; Senna, Luisa
; Senna-Valle, Luci
; Shirasuna, Regina T.
; Silva Filho, Pedro J.S.
; Silva, Anádria S.
; Silva, Christian
; Silva, Genilson A.R.
; Silva, Gisele O.
; Silva, Márcia C.R.
; Silva, Marcos J.
; Silva, Marcos J.
; Silva, Otávio L.M.
; Silva, Rafaela A.P.
; Silva, Saura R.
; Silva, Tania R.S.
; Silva-Gonçalves, Kelly C.
; Silva-Luz, Cíntia L.
; Simão-Bianchini, Rosângela
; Simões, André O.
; Simpson, Beryl
; Siniscalchi, Carolina M.
; Siqueira Filho, José A.
; Siqueira, Carlos E.
; Siqueira, Josafá C.
; Smith, Nathan P.
; Snak, Cristiane
; Soares Neto, Raimundo L.
; Soares, Kelen P.
; Soares, Marcos V.B.
; Soares, Maria L.
; Soares, Polyana N.
; Sobral, Marcos
; Sodré, Rodolfo C.
; Somner, Genise V.
; Sothers, Cynthia A.
; Sousa, Danilo J.L.
; Souza, Elnatan B.
; Souza, Élvia R.
; Souza, Marcelo
; Souza, Maria L.D.R.
; Souza-Buturi, Fátima O.
; Spina, Andréa P.
; Stapf, María N.S.
; Stefano, Marina V.
; Stehmann, João R.
; Steinmann, Victor
; Takeuchi, Cátia
; Taylor, Charlotte M.
; Taylor, Nigel P.
; Teles, Aristônio M.
; Temponi, Lívia G.
; Terra-Araujo, Mário H.
; Thode, Veronica
; Thomas, W.Wayt
; Tissot-Squalli, Mara L.
; Torke, Benjamin M.
; Torres, Roseli B.
; Tozzi, Ana M.G.A.
; Trad, Rafaela J.
; Trevisan, Rafael
; Trovó, Marcelo
; Valls, José F.M.
; Vaz, Angela M.S.F.
; Versieux, Leonardo
; Viana, Pedro L.
; Vianna Filho, Marcelo D.M.
; Vieira, Ana O.S.
; Vieira, Diego D.
; Vignoli-Silva, Márcia
; Vilar, Thaisa
; Vinhos, Franklin
; Wallnöfer, Bruno
; Wanderley, Maria G.L.
; Wasshausen, Dieter
; Watanabe, Maurício T.C.
; Weigend, Maximilian
; Welker, Cassiano A.D.
; Woodgyer, Elizabeth
; Xifreda, Cecilia C.
; Yamamoto, Kikyo
; Zanin, Ana
; Zenni, Rafael D.
; Zickel, Carmem S
.
Resumo Um levantamento atualizado das plantas com sementes e análises relevantes acerca desta biodiversidade são apresentados. Este trabalho se iniciou em 2010 com a publicação do Catálogo de Plantas e Fungos e, desde então vem sendo atualizado por mais de 430 especialistas trabalhando online. O Brasil abriga atualmente 32.086 espécies nativas de Angiospermas e 23 espécies nativas de Gimnospermas e estes novos dados mostram um aumento de 3% da riqueza em relação a 2010. A Amazônia é o Domínio Fitogeográfico com o maior número de espécies de Gimnospermas, enquanto que a Floresta Atlântica possui a maior riqueza de Angiospermas. Houve um crescimento considerável no número de espécies e nas taxas de endemismo para a maioria dos Domínios (Caatinga, Cerrado, Floresta Atlântica, Pampa e Pantanal), com exceção da Amazônia que apresentou uma diminuição de 2,5% de endemicidade. Entretanto, a maior parte das plantas com sementes que ocorrem no Brasil (57,4%) é endêmica deste território. A proporção de formas de vida varia de acordo com os diferentes Domínios: árvores são mais expressivas na Amazônia e Floresta Atlântica do que nos outros biomas, ervas são dominantes no Pampa e as lianas apresentam riqueza expressiva na Amazônia, Floresta Atlântica e Pantanal. Este trabalho não só quantifica a biodiversidade brasileira, mas também indica as lacunas de conhecimento e o desafio a ser enfrentado para a conservação desta flora.
Abstract An updated inventory of Brazilian seed plants is presented and offers important insights into the country's biodiversity. This work started in 2010, with the publication of the Plants and Fungi Catalogue, and has been updated since by more than 430 specialists working online. Brazil is home to 32,086 native Angiosperms and 23 native Gymnosperms, showing an increase of 3% in its species richness in relation to 2010. The Amazon Rainforest is the richest Brazilian biome for Gymnosperms, while the Atlantic Rainforest is the richest one for Angiosperms. There was a considerable increment in the number of species and endemism rates for biomes, except for the Amazon that showed a decrease of 2.5% of recorded endemics. However, well over half of Brazillian seed plant species (57.4%) is endemic to this territory. The proportion of life-forms varies among different biomes: trees are more expressive in the Amazon and Atlantic Rainforest biomes while herbs predominate in the Pampa, and lianas are more expressive in the Amazon, Atlantic Rainforest, and Pantanal. This compilation serves not only to quantify Brazilian biodiversity, but also to highlight areas where there information is lacking and to provide a framework for the challenge faced in conserving Brazil's unique and diverse flora.
https://doi.org/10.1590/2175-7860201566411
33340 downloads
4.
Probing topological electronic effects in catalysis: thiophene adsorption on NiMoS and CoMoS clusters
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Journal of the Brazilian Chemical Society
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Um método teórico geral em duas etapas para estudar redistribuições eletrônicas em processos catalíticos é apresentado. Na primeira etapa, teoria do funcional da densidade (DFT) é usada para otimizar completamente duas geometrias: o aglomerado que representa o catalisador e o sistema aglomerado mais molécula adsorvida. Na segunda etapa, a densidade eletrônica molecular convergida é dividida em multipolos centrados em sítios atômicos obtidos segundo uma análise de multipolos distribuídos, que fornece informação topológica detalhada da redistribuição de carga do catalisador e da molécula, antes e depois da adsorção. Esta abordagem é aplicada para a adsorção de tiofeno sobre a borda metálica 10-10 dos catalisadores Ni(Co)MoS e comparada com a mesma reação em MoS2 não-substituído. Energias de adsorção, geometrias e a análise de multipolos calculada indicam uma fraca adsorção do tiofeno em ambas as situações. Um modelo coulombiano para a ligação química mostra que a magnitude da ligação metal-enxofre na superfície dos catalisadores de Ni(Co)MoS promovidos é consideravelmente menor do que em MoS2 não substituído, desta forma confirmando a origem do aumento da atividade de hidrodessulfurização (HDS) nestes catalisadores.
A general two-step theoretical approach to study electronic redistributions in catalytic processes is presented. In the first step, density functional theory (DFT) is used to fully optimize two geometries: the cluster representing the catalyst and the cluster plus adsorbed molecule system. In the second step, the converged electron density is divided into multipoles centered on atomic sites according to a distributed multipole analysis which provides detailed topological information on the charge redistribution of catalyst and molecule before and after adsorption. This approach is applied to thiophene adsorption on the 10-10 metal edge of Ni(Co)MoS catalysts and compared to the same reaction on bare MoS2. Calculated adsorption energies, geometries and multipole analysis indicate weak thiophene chemisorption on both cases. A Coulombic bond model showed that surface metal-sulfur bond strengths in Ni(Co)MoS promoted catalysts are considerably smaller than in bare MoS2, thus confirming the origin of the enhancement of hydrodesulfurization (HDS) activity in these catalysts.
3222 downloads
5.
Defesa química: histórico, classificação dos agentes de guerra e ação dos neurotóxicos
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Silva, Gustavo Rocha
; Borges Jr., Itamar
; Figueroa-Villar, José Daniel
; Castro, Alexandre Taschetto de
.
Chemical agents are substances used for their toxic effects on humans, animals and plants. The main objective of chemical defense is to develop systems that reduce these effects while minimizing impact on the operational capacity of military troops. In this work, a report on the development of chemical warfare agents since the First World War and their classification is presented. Special attention is given to neurotoxic agents, the most lethal group of chemical agents known to date.
19878 downloads
6.
Theoretical investigations on valence vibronic transitions
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This article reviews previously employed methods to study several valence electronic transitions, optically forbidden or not, enhancing intensity through vibronic coupling. Electronic transition dipole moments were calculated using several ab initio methods including electron correlation. In this method the square of the electronic transition dipole moments are directly calculated along the normal coordinates of vibration and then expanded with a polynomial function. Afterwards, analytical vibrational integration using harmonic wave functions, of the square of the transition moments function, allows us to obtain partial (i.e. for each vibrational mode) and total optical oscillator strengths (OOS), for the vibronic transition of interest. We illustrate the accuracy of the method through valence transitions of benzene (C6H6), formaldehyde (H2CO), acetone (C3H6O) and formic acid (HCOOH).
1513 downloads
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