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http://elar.urfu.ru/handle/10995/111768
Название: | Lead(ii) Coordination Polymers Driven by Pyridine-Hydrazine Donors: From Anion-Guided Self-Assembly to Structural Features |
Авторы: | Mahmoudi, G. Afkhami, F. A. Kennedy, A. R. Zubkov, F. I. Zangrando, E. Kirillov, A. M. Molins, E. Mitoraj, M. P. Safin, D. A. |
Дата публикации: | 2020 |
Издатель: | Royal Society of Chemistry Royal Society of Chemistry (RSC) |
Библиографическое описание: | Lead(ii) Coordination Polymers Driven by Pyridine-Hydrazine Donors: From Anion-Guided Self-Assembly to Structural Features / G. Mahmoudi, F. A. Afkhami, A. R. Kennedy et al. // Dalton Transactions. — 2020. — Vol. 49. — Iss. 32. — P. 11238-11248. |
Аннотация: | In this work, we report extensive experimental and theoretical investigations on a new series of PbII coordination polymers exhibiting extended supramolecular architectures, namely [Pb2(LI)(NCS)4]n (1), [Pb(HLII)I2]n (2), [Pb(LIII)I]n (3) and [Pb(HLIV)(NO3)2]n·nMeOH (4), which were self-assembled from different PbII salts and various pyridine-hydrazine based linkers, namely 1,2-bis(pyridin-3-ylmethylene)hydrazine (LI), (pyridin-4-ylmethylene)isonicotinohydrazide (HLII), 1-(pyridin-2-yl)ethylidenenicotinohydrazide (HLIII) and phenyl(pyridin-2-yl)methylenenicotinohydrazide (HLIV), respectively. It is recognized that the origin of self-assembling is fundamentally rooted in a dual donor (6s2/6p0 hybridized lone electron pair) and electrophilic behaviour of PbII. This allows production of extended topologies from a 1D polymeric chain in 4 through a 2D layer in 2 to the 3D frameworks in 1 and 3, predominantly due to the cooperative action of both covalent and non-covalent tetrel interactions of the overall type Pb-X (X = O, N, S, I). Counterintuitively, the latter, seemingly weak interactions, have appeared to be even stronger than the typical covalent bonds due to the presence of a bunch of supportive London dispersion dominated contacts: π⋯π, Lp⋯π, C-H⋯O, C-H⋯I, C-H⋯H-C as well as more typical mainly electrostatically driven N-H⋯O or N/O-H⋯O hydrogen bonds. It is revealed that the constituting generally strong tetrel type Pb-X (X = O, N, S, I) bonds, though dominated by a classic Coulomb term, are therefore characterized by a very important London dispersion constituent, extremely strong relativistic effects and the two way dative-covalent Pb ↔ X electron charge delocalization contribution as revealed by the Extended Transition State Natural Orbital for Chemical Valence (ETS-NOCV) charge and energy decomposition scheme. It unravels that the pyridine-hydrazine linkers are also excellent London dispersion donors, and that together with the donor-acceptor properties of the heavy (relativistic) PbII atoms and nucleophilic counterions lead to extended self-assembling of 1-4. © 2020 The Royal Society of Chemistry. |
Ключевые слова: | ATOMS D REGION DISPERSIONS HYDRAZINE HYDROGEN BONDS NEGATIVE IONS POLYMERS PYRIDINE SELF ASSEMBLY COORDINATION POLYMERS DONOR-ACCEPTOR PROPERTIES ELECTROSTATICALLY DRIVEN ENERGY DECOMPOSITION GUIDED SELF-ASSEMBLY NUCLEOPHILIC COUNTERIONS SUPRAMOLECULAR ARCHITECTURES THEORETICAL INVESTIGATIONS LEAD COMPOUNDS |
URI: | http://elar.urfu.ru/handle/10995/111768 |
Условия доступа: | info:eu-repo/semantics/openAccess |
Идентификатор SCOPUS: | 85089710097 |
Идентификатор WOS: | 000561080600018 |
Идентификатор PURE: | 13659213 |
ISSN: | 1477-9226 |
DOI: | 10.1039/d0dt01704c |
Сведения о поддержке: | We are grateful to the University of Maragheh for the financial support of this research. The publication has been prepared with the support from the “RUDN University Program 5-100” (recipient F. I. Zubkov, synthesis of the ligands). DFT calculations were partially performed using the PL-Grid Infrastructure and resources provided by the ACC Cyfronet AGH (Cracow, Poland). A. M. Kirillov acknowledges the FCT and Portugal 2020 (LISBOA-01-0145-FEDER-029697 and UIDB/ 00100/2020). ICMAB acknowledges the Severo Ochoa Program (MINECO, SEV-2015-0496). M. P. Mitoraj acknowledges the financial support from the Polish National Science Center within the Sonata Bis Project 2017/26/E/ST4/00104. |
Располагается в коллекциях: | Научные публикации ученых УрФУ, проиндексированные в SCOPUS и WoS CC |
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