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leiws

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[交流] [Nature]催化合成氨获研究进展 已有6人参与

Title: Catalytic conversion of nitrogen to ammonia by an iron model complex
Abstract:
The reduction of nitrogen (N2) to ammonia (NH3) is a requisite transformation for life1. Although it is widely appreciated that the iron-rich cofactors of nitrogenase enzymes facilitate this transformation, how they do so remains poorly understood. A central element of debate has been the exact site or sites of N2 coordination and reduction. In synthetic inorganic chemistry, an early emphasis was placed on molybdenum8 because it was thought to be an essential element of nitrogenases3 and because it had been established that well-defined molybdenum model complexes could mediate the stoichiometric conversion of N2 to NH3 (ref. 9). This chemical transformation can be performed in a catalytic fashion by two well-defined molecular systems that feature molybdenum centres. However, it is now thought that iron is the only transition metal essential to all nitrogenases3, and recent biochemical and spectroscopic data have implicated iron instead of molybdenum as the site of N2 binding in the FeMo-cofactor. Here we describe a tris(phosphine)borane-supported iron complex that catalyses the reduction of N2 to NH3 under mild conditions, and in which more than 40 per cent of the proton and reducing equivalents are delivered to N2. Our results indicate that a single iron site may be capable of stabilizing the various NxHy intermediates generated during catalytic NH3 formation. Geometric tunability at iron imparted by a flexible iron–boron interaction in our model system seems to be important for efficient catalysis. We propose that the interstitial carbon atom recently assigned in the nitrogenase cofactor may have a similar role, perhaps by enabling a single iron site to mediate the enzymatic catalysis through a flexible iron–carbon interaction.
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http://www.nature.com/nature/jou ... ll/nature12435.html[Nature]催化合成氨获研究进展
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人的烦恼就是记性太好，如果可以把所有事都忘掉，以后每一日都是个新开始，你说多好。
1楼 2013-09-05 10:03:28
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学习一下！
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2楼2013-09-05 10:19:04
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豆豆要科研

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谢谢分享！好厉害！
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3楼2013-09-06 20:46:10
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jiangyun2

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一天到晚游泳的鱼啊，鱼不停游~
4楼2013-09-06 21:37:09
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林夕08

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值得学习下
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jaej_hero

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太好了
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做一个有贡献的人
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