Probing Framework-Restricted Metal Axial Ligation and Spin State Patterns in a Post-Synthetically Reduced Iron-Porphyrin-Based Metal-Organic Framework

被引:28
作者
Kucheryavy, Pavel [1 ]
Lahanas, Nicole [1 ]
Velasco, Ever [1 ]
Sun, Cheng-Jun [2 ]
Lockard, Jenny V. [1 ]
机构
[1] Rutgers State Univ, Dept Chem, Newark, NJ 07102 USA
[2] Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA
基金
美国国家科学基金会;
关键词
X-RAY-ABSORPTION; ELECTRONIC-STRUCTURE; EMISSION-SPECTROSCOPY; RESONANCE RAMAN; SPECTRA; COMPLEXES; TRANSITION; BETA; EDGE; STEREOCHEMISTRY;
D O I
10.1021/acs.jpclett.6b00302
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
An iron-porphyrin-based metal organic framework PCN-222(Fe) is investigated upon postsynthetic reduction with piperidine. Fe K-edge X-ray absorption and K beta mainline emission spectroscopy measurements reveal the local coordination geometry, oxidation, and spin state changes experienced by the Fe sites upon reaction with this axially coordinating reducing agent. Analysis and fitting of these data confirm the binding pattern predicted by a space-filling model of the structurally constrained pore environments. These results are further supported by UV vis diffuse reflectance, IR, and resonance Raman spectroscopy data.
引用
收藏
页码:1109 / 1115
页数:7
相关论文
共 46 条
[1]   FLUORESCENCE, RESONANCE RAMAN, AND RADIATIONLESS DECAY IN SEVERAL HEMOPROTEINS [J].
ADAR, F ;
GOUTERMAN, M ;
ARONOWITZ, S .
JOURNAL OF PHYSICAL CHEMISTRY, 1976, 80 (20) :2184-2191
[2]   Electronic transitions in perovskite:: Possible nonconvecting layers in the lower mantle [J].
Badro, J ;
Rueff, JP ;
Vankó, G ;
Monaco, G ;
Fiquet, G ;
Guyot, F .
SCIENCE, 2004, 305 (5682) :383-386
[3]   Magnetism in FeO at megabar pressures from X-ray emission spectroscopy [J].
Badro, J ;
Struzhkin, VV ;
Shu, JF ;
Hemley, RJ ;
Mao, HK ;
Kao, CC ;
Rueff, JP ;
Shen, GY .
PHYSICAL REVIEW LETTERS, 1999, 83 (20) :4101-4104
[4]   X-RAY ABSORPTION-SPECTROSCOPY OF IRON-(II) AND IRON-(III) BASKET-HANDLE PORPHYRINS [J].
CARTIER, C ;
MOMENTEAU, M ;
DARTYGE, E ;
FONTAINE, A ;
TOURILLON, G ;
MICHALOWICZ, A ;
VERDAGUER, M .
JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, 1992, (04) :609-618
[5]   LIGATION AND REDUCTION OF IRON(III) PORPHYRINS BY AMINES - A MODEL FOR CYTOCHROME-P-450 MONOAMINE-OXIDASE [J].
CASTRO, CE ;
JAMIN, M ;
YOKOYAMA, W ;
WADE, R .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1986, 108 (14) :4179-4187
[6]   Biomimetic Catalysis of a Porous Iron-Based Metal-Metalloporphyrin Framework [J].
Chen, Yao ;
Tran Hoang ;
Ma, Shengqian .
INORGANIC CHEMISTRY, 2012, 51 (23) :12600-12602
[7]   RESONANCE RAMAN-SPECTRA OF IRON TETRAPHENYLPORPHYRIN COMPLEXES - CHARACTERIZATION OF STRUCTURE AND BONDING SENSITIVE BANDS [J].
CHOTTARD, G ;
BATTIONI, P ;
BATTIONI, JP ;
LANGE, M ;
MANSUY, D .
INORGANIC CHEMISTRY, 1981, 20 (06) :1718-1722
[8]  
Chou J.-H., 2000, Porphyrin Handb, V6, P43
[9]   SYNTHESIS, STEREOCHEMISTRY, AND STRUCTURE-RELATED PROPERTIES OF ALPHA, BETA, GAMMA, "DELTA-TETRAPHENYLPORPHINATOIRON(II) [J].
COLLMAN, JP ;
HOARD, JL ;
KIM, N ;
LANG, G ;
REED, CA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1975, 97 (10) :2676-2681
[10]   High resolution X-ray emission and X-ray absorption spectroscopy [J].
de Groot, F .
CHEMICAL REVIEWS, 2001, 101 (06) :1779-1808