Over or under: hydride attack at the metal versus the coordinated nitrosyl ligand in ferric nitrosyl porphyrins

被引：27

作者：

Abucayon, E. G. ^{[1
]}

Khade, R. L. ^{[2
]}

Powell, D. R. ^{[1
]}

Shaw, M. J. ^{[3
]}

Zhang, Y. ^{[2
]}

Richter-Addo, G. B. ^{[1
]}

机构：

[1] Univ Oklahoma, Dept Chem & Biochem, Norman, OK 73019 USA

[2] Stevens Inst Technol, Dept Biomed Engn Chem & Biol Sci, Castle Point Hudson, Hoboken, NJ 07030 USA

[3] Southern Illinois Univ Edwardsville, Dept Chem, Edwardsville, IL 62025 USA

来源：

DALTON TRANSACTIONS | 2016年 / 45卷 / 45期

基金：

美国国家科学基金会; 美国国家卫生研究院;

关键词：

ELECTRONIC-STRUCTURE; AB-INITIO; CYTOCHROME-C; NITROXYL HNO; HEME; MODEL; COMPLEXES; REDUCTION; PERCHLORATE; (FENO)(8);

D O I：

10.1039/c6dt03860c

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

Hydride attack at a ferric heme-NO to give an Fe-HNO intermediate is a key step in the global N-cycle. We demonstrate differential reactivity when six- and five-coordinate ferric heme-NO models react with hydride. Although Fe-HNO formation is thermodynamically favored from this reaction, Fe-H formation is kinetically favored for the 5C case.

引用

页码：18259 / 18266

页数：8

共 41 条

[1] Hydride Attack on a Coordinated Ferric Nitrosyl: Experimental and DFT Evidence for the Formation of a Heme Model-HNO Derivative [J].

Abucayon, Erwin G. ;

Khade, Rahul L. ;

Powell, Douglas R. ;

Zhang, Yong ;

Richter-Addo, George B. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (01) :104-107

[2] Exchange functionals with improved long-range behavior and adiabatic connection methods without adjustable parameters:: The mPW and mPW1PW models [J].

Adamo, C ;

Barone, V .

JOURNAL OF CHEMICAL PHYSICS, 1998, 108 (02) :664-675

[3] ELECTROCATALYTIC REDUCTION OF NITRITE TO AMMONIA BASED ON A WATER-SOLUBLE IRON PORPHYRIN [J].

BARLEY, MH ;

TAKEUCHI, KJ ;

MEYER, TJ .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1986, 108 (19) :5876-5885

[4] DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].

BECKE, AD .

JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652

[5] ATOMIC CHARGES DERIVED FROM SEMIEMPIRICAL METHODS [J].

BESLER, BH ;

MERZ, KM ;

KOLLMAN, PA .

JOURNAL OF COMPUTATIONAL CHEMISTRY, 1990, 11 (04) :431-439

[6]

BRANDSTROM A, 1972, TETRAHEDRON LETT, P3173

[7] Six-Electron Reduction of Nitrite to Ammonia by Cytochrome c Nitrite Reductase: Insights from Density Functional Theory Studies [J].

Bykov, Dmytro ;

Neese, Frank .

INORGANIC CHEMISTRY, 2015, 54 (19) :9303-9316

[8] ELECTROCHEMICAL AND SPECTROSCOPIC STUDIES OF IRON PORPHYRIN NITROSYLS AND THEIR REDUCTION PRODUCTS [J].

CHOI, IK ;

LIU, YM ;

FENG, D ;

PAENG, KJ ;

RYAN, MD .

INORGANIC CHEMISTRY, 1991, 30 (08) :1832-1839

[9] New developments in the polarizable continuum model for quantum mechanical and classical calculations on molecules in solution [J].

Cossi, M ;

Scalmani, G ;

Rega, N ;

Barone, V .

JOURNAL OF CHEMICAL PHYSICS, 2002, 117 (01) :43-54

[10] Ab initio study of solvated molecules: A new implementation of the polarizable continuum model [J].

Cossi, M ;

Barone, V ;

Cammi, R ;

Tomasi, J .

CHEMICAL PHYSICS LETTERS, 1996, 255 (4-6) :327-335

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