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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(43):13669-13673
A stable 5,10‐bis(9‐fluorenylidene)porphyrin (Por‐Fl) diradicaloid was synthesized. It shows a quinoidal, saddle‐shaped geometry in the single crystal but can be thermally populated to a triplet diradical both in solution and in the solid state. Coordination with the Ni2+ ion (Por‐Fl‐Ni) does not significantly change the contorted conformation but reduces the singlet–triplet gap. Heat‐induced geometric change can explain the observed paramagnetic properties as well as unusual hysteresis in SQUID measurements. On the other hand, protonation (Por‐Fl‐2H+) dramatically changes the conformation while maintains the closed‐shell electronic structure. Our studies demonstrate how heat, coordination, and protonation affect the geometry, diradical character, and physical properties of conformationally flexible open‐shell singlet diradicaloids. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(32):9504-9508
Mechanical anisotropy is ubiquitous in biological tissues but is hard to reproduce in synthetic biomaterials. Developing molecular building blocks with anisotropic mechanical response is the key towards engineering anisotropic biomaterials. The three‐way‐junction (3WJ) pRNA, derived from ϕ 29 DNA packaging motor, shows strong mechanical anisotropy upon Mg2+ binding. In the absence of Mg2+, 3WJ‐pRNA is mechanically weak without noticeable mechanical anisotropy. In the presence of Mg2+, the unfolding forces can differ by more than 4‐fold along different pulling directions, ranging from about 47 pN to about 219 pN. Mechanical anisotropy of 3WJ‐pRNA stems from pulling direction dependent cooperativity for the rupture of two Mg2+ binding sites, which is a novel mechanism for the mechanical anisotropy of biomacromolecules. It is anticipated that 3WJ‐pRNA can be used as a key element for the construction of biomaterials with controllable mechanical anisotropy. 相似文献
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Keigo Kobayashi Prof. Hirokazu Kobayashi Prof. Mitsuhiko Maesato Dr. Mikihiro Hayashi Tomokazu Yamamoto Dr. Satoru Yoshioka Prof. Syo Matsumura Prof. Takeharu Sugiyama Dr. Shogo Kawaguchi Prof. Yoshiki Kubota Prof. Hiroshi Nakanishi Prof. Hiroshi Kitagawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(23):6678-6682
We report on hexagonal close-packed (hcp) palladium (Pd)–boron (B) nanocrystals (NCs) by heavy B doping into face-centered cubic (fcc) Pd NCs. Scanning transmission electron microscopy–electron energy loss spectroscopy and synchrotron powder X-ray diffraction measurements demonstrated that the B atoms are homogeneously distributed inside the hcp Pd lattice. The large paramagnetic susceptibility of Pd is significantly suppressed in Pd–B NCs in good agreement with the reduction of density of states at Fermi energy suggested by X-ray absorption near-edge structure and theoretical calculations. 相似文献
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