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91.
Dr. Marek Łuczkowski Dr. Brian A. Zeider Alia V. H. Hinz Dr. Monika Stachura Dr. Saumen Chakraborty Prof. Lars Hemmingsen Dr. David L. Huffman Prof. Vincent L. Pecoraro 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(27):9042-9049
Although metal ion homeostasis in cells is often mediated through metallochaperones, there are opportunities for toxic metals to be sequestered through the existing transport apparatus. Proper trafficking of CuI in human cells is partially achieved through complexation by HAH1, the human metallochaperone responsible for copper delivery to the Wilson and Menkes ATPase located in the trans‐Golgi apparatus. In addition to binding copper, HAH1 strongly complexes HgII, with the X‐ray structure of this complex previously described. It is important to clarify the solution behavior of these systems and, therefore, the binding of HgII to HAH1 was probed over the pH range 7.5 to 9.4 using 199Hg NMR, 199mHg PAC and UV–visible spectroscopies. The metal‐dependent protein association over this pH range was examined using analytical gel‐filtration. It can be concluded that at pH 7.5, HgII is bound to a monomeric HAH1 as a two coordinate, linear complex (HgS2), like the HgII–Atx1 X‐ray structure (PDB ID: 1CC8). At pH 9.4, HgII promotes HAH1 association, leading to formation of HgS3 and HgS4 complexes, which are in exchange on the μs–ns time scale. Thus, structures that may represent central intermediates in the process of metal ion transfer, as well as their exchange kinetics have been characterized. 相似文献
92.
Fullmer BC Fan H Pink M Huffman JC Tsvetkov NP Caulton KG 《Journal of the American Chemical Society》2011,133(8):2571-2582
All attempts to synthesize (PNP)Ni(OTf) form instead ((t)Bu(2)PCH(2)SiMe(2)NSiMe(2)OTf)Ni(CH(2)P(t)Bu(2)). Abstraction of F(-) from (PNP)NiF by even a catalytic amount of BF(3) causes rearrangement of the (transient) (PNP)Ni(+) to analogous ring-opened [((t)Bu(2)PCH(2)SiMe(2)NSiMe(2)F)]Ni(CH(2)P(t)Bu(2)). Abstraction of Cl(-) from (PNP)NiCl with NaB(C(6)H(3)(CF(3))(2))(4) in CH(2)Cl(2) or C(6)H(5)F gives (PNP)NiB(C(6)H(3)(CF(3))(2))(4), the key intermediate in these reactions is (PNP)Ni(+), [(PNP)Ni](+), in which one Si-C bond (together with N and two P) donates to Ni. This makes this Si-C bond subject to nucleophilic attack by F(-), triflate, and alkoxide/ether (from THF). This σ(Si-C) complex binds CO in the time of mixing and also binds chloride, both at nickel. Evidence is offered of a "self-healing" process, where the broken Si-C bond can be reformed in an equilibrium process. (PNP)Ni(+) reacts rapidly with H(2) to give (PN(H)P)NiH(+), which can be deprotonated to form (PNP)NiH. A variety of nucleophilic attacks (and THF polymerization) on the coordinated Si-C bond are envisioned to occur perpendicular to the Si-C bond, based on the character of the LUMO of (PNP)Ni(+). 相似文献
93.
94.
Large-scale purification of single-wall carbon nanotubes: process, product, and characterization 总被引:13,自引:0,他引:13
A.G. Rinzler J. Liu H. Dai P. Nikolaev C.B. Huffman F.J. Rodríguez-Macías P.J. Boul A.H. Lu D. Heymann D.T. Colbert R.S. Lee J.E. Fischer A.M. Rao P.C. Eklund R.E. Smalley 《Applied Physics A: Materials Science & Processing》1998,67(1):29-37
Received: 13 February 1998 相似文献
95.
All Mendelsohn designs containing a Frobenius group with cyclic complement of orderv – 1 as a subgroup of the automorphism are found. Furthermore, the automorphism group of each of the designs is constructed. These designs generalize Mendelsohn's construction of Mendelsohn designs containing a certain doubly transitive automorphism group.The research on this paper was partially supported by North Texas State Faculty Research Grant #35524. 相似文献
96.
97.
We consider the real-time evolution of a strongly coupled system of lattice fermions whose dynamics is driven entirely by dissipative Lindblad processes, with linear or quadratic quantum jump operators. The fermion 2-point functions obey a closed set of differential equations, which can be solved with linear algebra methods. The staggered occupation order parameter of the t-V model decreases exponentially during the dissipative time evolution. The structure factor associated with the various Fourier modes shows the slowing down of low-momentum modes, which is due to particle number conservation. The processes with nearest-neighbor-dependent Lindblad operators have a decay rate that is proportional to the coordination number of the spatial lattice. 相似文献
98.
Adhikari D Mossin S Basuli F Huffman JC Szilagyi RK Meyer K Mindiola DJ 《Journal of the American Chemical Society》2008,130(11):3676-3682
Pincer-type ligands are believed to be very robust scaffolds that can support multifarious functionalities as well as highly reactive metal motifs applied in organometallic chemistry, especially in the realm of catalysis. In this paper, we describe the redox and, therefore, noninnocent behavior of a PNP (PNP- = N[2-P(CHMe2)2-4-methylphenyl]2) pincer ancillary bound to nickel. A combination of structural, spectroscopic, and theoretical techniques suggests that this type of framework can house an electron hole when coordinated to Ni(II). 相似文献
99.
100.
Incomplete N-atom transfer from Fe to P is observed when the ferrous amide complex (PNP)Fe(dbabh) (PNP-=N[2-P(iPr)2-4-methylphenyl]2, dbabh=2,3:5,6-dibenzo-7-azabicyclo[2.2.1]hepta-2,5-diene), prepared from salt metathesis of (PNP)FeCl and Li(dbabh), is thermolyzed at 70 degrees C over 48 h in C6D6. Several plausible reaction pathways resulting from the transformation of (PNP)Fe(dbabh) are discussed, including the possibility of an Fe(IV) nitride as an intermediate. 相似文献