Direct Transformation of Molecular Dinitrogen into Ammonia Catalyzed by Cobalt Dinitrogen Complexes Bearing Anionic PNP Pincer Ligands

被引:183
作者
Kuriyama, Shogo [1 ]
Arashiba, Kazuya [1 ]
Tanaka, Hiromasa [2 ,3 ]
Matsuo, Yuki [2 ,3 ]
Nakajima, Kazunari [1 ]
Yoshizawa, Kazunari [2 ,3 ]
Nishibayashi, Yoshiaki [1 ]
机构
[1] Univ Tokyo, Sch Engn, Dept Syst Innovat, Bunkyo Ku, Hongo, Tokyo 1138656, Japan
[2] Kyushu Univ, Inst Mat Chem & Engn, Nishi Ku, Fukuoka 8190395, Japan
[3] Kyoto Univ, Elements Strategy Initiat Catalysts & Batteries, Nishikyo Ku, Kyoto 6158520, Japan
关键词
ammonia; catalysis; cobalt; dinitrogen; pincer ligands; AMBIENT REACTION CONDITIONS; SINGLE MOLYBDENUM CENTER; BOND ORDER; UNIQUE BEHAVIOR; PENDANT AMINES; N-2; ACTIVATION; ALKALI-METAL; REDUCTION; CLEAVAGE; NITROGEN;
D O I
10.1002/anie.201606090
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The direct formation of ammonia from molecular dinitrogen under mild reaction conditions was achieved by using new cobalt dinitrogen complexes bearing an anionic PNP-type pincer ligand. Up to 15.9 equivalents of ammonia were produced based on the amount of catalyst together with 1.0 equivalent of hydrazine (17.9 equiv of fixed nitrogen atoms).
引用
收藏
页码:14289 / 14293
页数:5
相关论文
共 74 条
[1]   Characterization of an FeN-NH2 Intermediate Relevant to Catalytic N2 Reduction to NH3 [J].
Anderson, John S. ;
Cutsail, George E., III ;
Rittle, Jonathan ;
Connor, Bridget A. ;
Gunderson, William A. ;
Zhang, Limei ;
Hoffman, Brian M. ;
Peters, Jonas C. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (24) :7803-7809
[2]   Catalytic conversion of nitrogen to ammonia by an iron model complex [J].
Anderson, John S. ;
Rittle, Jonathan ;
Peters, Jonas C. .
NATURE, 2013, 501 (7465) :84-+
[3]   A molybdenum complex bearing PNP-type pincer ligands leads to the catalytic reduction of dinitrogen into ammonia [J].
Arashiba, Kazuya ;
Miyake, Yoshihiro ;
Nishibayashi, Yoshiaki .
NATURE CHEMISTRY, 2011, 3 (02) :120-125
[4]   TRANSITION METAL COMPLEXES OF DITHIOACETYLACETONE AND DISELENOACETYLACETONE - SYNTHESES PROPERTIES AND INFRARED SPECTRA [J].
BARRACLOUGH, CG ;
MARTIN, RL ;
STEWART, IM .
AUSTRALIAN JOURNAL OF CHEMISTRY, 1969, 22 (05) :891-+
[5]   The Mayer bond order as a tool in inorganic chemistry [J].
Bridgeman, AJ ;
Cavigliasso, G ;
Ireland, LR ;
Rothery, J .
JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, 2001, Royal Society of Chemistry (14) :2095-2108
[6]   Reversible Carbon-Carbon Bond Formation Induced by Oxidation and Reduction at a Redox-Active Cobalt Complex [J].
Carmen, Crisita ;
Atienza, Hojilla ;
Milsmann, Carsten ;
Semproni, Scott P. ;
Turner, Zoe R. ;
Chirik, Paul J. .
INORGANIC CHEMISTRY, 2013, 52 (09) :5403-5417
[7]   ISOLATION AND CHARACTERIZATION OF (PNP)2CO(CN)4, AN UNUSUAL SQUARE-PLANAR COBALT(II) COMPLEX [J].
CARTER, SJ ;
FOXMAN, BM ;
STUHL, LS .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1984, 106 (15) :4265-4266
[8]   Bimetallic Cobalt-Dinitrogen Complexes: Impact of the Supporting Metal on N2 Activation [J].
Clouston, Laura J. ;
Bernales, Varinia ;
Carlson, Rebecca K. ;
Gagliardi, Laura ;
Lu, Connie C. .
INORGANIC CHEMISTRY, 2015, 54 (19) :9263-9270
[9]   Binding of dinitrogen to an iron-sulfur-carbon site [J].
Coric, Ilija ;
Mercado, Brandon Q. ;
Bill, Eckhard ;
Vinyard, David J. ;
Holland, Patrick L. .
NATURE, 2015, 526 (7571) :96-99
[10]   Diiron Bridged-Thiolate Complexes That Bind N2 at the FeIIFeII, FeIIFeI, and FeIFeI Redox States [J].
Creutz, Sidney E. ;
Peters, Jonas C. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (23) :7310-7313