N(2) -to-NH(3) Conversion by a triphos-Iron Catalyst and Enhanced Turnover under Photolysis.
N(2) -to-NH(3) Conversion by a triphos-Iron Catalyst and Enhanced Turnover under Photolysis.
复制标题
DOI：
10.1002/anie.201703244
复制
发表时间：
2017-06-06
期刊：
影响因子：
--
通讯作者：
Peters JC
中科院分区：
文献类型：
--
作者：
Buscagan TM;Oyala PH;Peters JC
桥连铁离子被提议在催化二氮还原成氨的过程中在MoFe-固氮酶的活性位点处形成，并且可能是通过还原消除H2来结合和活化N2的关键。这种可能性激发了研究定义明确的分子铁的前体催化N2-到-NH3转化。在此，我们描述了新的P2P′PhFe（N2）（H）x系统的合成和表征，该系统具有催化N2到NH3转化的活性。最有趣的是，我们表明，氨的产率可以显着增加，如果在汞灯照射的存在下进行催化。提供的证据表明，光消除的H2是一种手段，通过该增强的活动可能会出现。点亮它：报道了光增强的N2到NH3转化催化。新的三氧化二铁负载的Fe（N2）Hx催化剂提供更高的氨产率为1大气压N2，和多达180%的改进后，照射汞灯。
Bridging iron hydrides are proposed to form at the active site of MoFe-nitrogenase during catalytic dinitrogen reduction to ammonia and may be key in the binding and activation of N2 via reductive elimination of H2. This possibility inspires the investigation of well-defined molecular iron hydrides as precursors for catalytic N2-to-NH3 conversion. Herein, we describe the synthesis and characterization of new P2P′PhFe(N2)(H)x systems that are active for catalytic N2-to-NH3 conversion. Most interestingly, we show that the yields of ammonia can be significantly increased if the catalysis is performed in the presence of mercury lamp irradiation. Evidence is provided to suggest that photo-elimination of H2 is one means by which the enhanced activity may arise. Light it up: Light-enhanced N2-to-NH3 conversion catalysis is reported. New triphos-supported Fe(N2)Hx catalysts provide higher ammonia yields for 1 atm N2, and as much as 180% improvement upon irradiation by a mercury lamp.
登录
查看更多内容
影响因子：
4.6
作者：
Field, Leslie D.;Hazari, Nilay;Li, Hsiu L.
通讯作者：
Li, Hsiu L.
影响因子：
62.1
作者：
Hoffman, Brian M.;Lukoyanov, Dmitriy;Yang, Zhi-Yong;Dean, Dennis R.;Seefeldt, Lance C.
通讯作者：
Seefeldt, Lance C.
DOI：
10.1039/dt9840001349
发表时间：
1984-01-01
期刊：
JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS
影响因子：
--
作者：
ADDISON, AW;RAO, TN;VERSCHOOR, GC
通讯作者：
VERSCHOOR, GC
合成单位Fe氮酶：高离职率，冻结（57）feMössbauer数据和氢化物静止状态。
影响因子：
15
作者：
Del Castillo TJ;Thompson NB;Peters JC
通讯作者：
Peters JC
影响因子：
15
作者：
Betley, TA;Peters, JC
通讯作者：
Peters, JC