Plants are unable to metabolise atmospheric nitrogen it requires conversion into ammoniai

植物不能代谢大气中的氮，它需要转化为氨气。这一过程被称为生物固氮，由一组专门的生物纳米机器进行。土壤含氮量是影响土壤肥力和生产力的关键因素。在上个世纪初，唯一能使土壤肥沃的固体天然形态的氮是秘鲁的鸟粪和智利的硝酸盐。2015年，氨生产是农业的基础，支撑着人类食物摄入量的三分之一到一半；尽管技术有所改进，但它仍然需要高温(400-600摄氏度)和高压(20-40兆帕)，这些都消耗了全球能源生产的1%以上，并产生温室气体。此外，氨肥的使用也导致了世界性的生态问题：水体富营养化和氮气大气平衡的改变。最近的研究表明，钼和钨的酶非常古老，它们的酶作用和功能一直被保存下来。人们认为，在原始世界的还原环境中，钨酶受到青睐。在那个时代，氧原子转移反应比现代世界更具挑战性，人们更喜欢钼酶。可溶金属催化剂的使用为其他功能化有机氮分子提供了直接途径，并进一步深入了解了多相Haber-Bosch催化剂或直接制氨的低能固氮酶。通过加深我们对氮循环微生物种群的了解，我们可以找到提供更有效的生物工程解决方案的机会。到目前为止，还没有人系统地探索从这一新知识中产生的脱氮新生物技术，因为纯粹的经验探索需要大量的调查。不过，可以使用成本效益高的高级建模方法加快这一进程，正如本提案中所详述的那样。为了探索分子氮的功能化及其对分子氮的催化转化，我们需要结合以下方面的专业知识：a)无机化学，通过探索催化转化的第二块金属；b)计算化学，通过描述反应路径和寻找反应中间产物；c)代谢模型，描述氮循环中微生物种群之间的代谢活动和协同作用，确定为脱氮产生有效聚集体结构的工艺条件。伊科。APPL1997，7,737-750.iClark，B，Foster，J.B.Int.J.Comp.书名：Soc.2009,50311-334.iSchoepp-Cothenet B.代表：2012年，2263人。首页--期刊主要分类--期刊细介绍--期刊题录与文摘--期刊详细文摘内容化学。2，30-35(2010)。

Plants are unable to metabolise atmospheric nitrogen it requires conversion into ammoniai. This process, known as biological nitrogen fixation, is carried out by a specialized group of biological nano-machines. Nitrogen content of soils is a key factor regarding soil fertility and productivity. At the start of the last century, the only solid natural forms of nitrogen to enrich the soil were Peruvian guano and Chilean nitrate.ii In 1913, the Haber-Bosch process changed the course of the 20thcentury allowing mass production of ammonia. Ammonia production is the base of agriculture in 2015, supporting between a 3rd and half of human food intake; despite technical improvements it still requires both high temperature (400-600 C), high pressure (20-40 MPa) that consume more than 1% of world-wideenergy production and produces greenhouse gases. Also, use of ammonia fertilizers has led to worldwide ecological problems: water eutrophication and alteration of the nitrogen atmospheric balance. Recent work indicated that molybdenum and tungsten enzymes are incredibly ancient, and their enzymatic role and functionality has been preserved. iii It is thought that in the reducing environment of the primordial world Tungsten-enzymes were favored. In those days, oxygen atom transfer reactions were more challenging than in the modern world, with a preference for molybdenum-enzymes. ivThe use of soluble metal catalysts offers direct routes to other functionalized organonitrogen molecules and provides further insight into the heterogeneous Haber-Bosch catalyst or the low-energy nitrogenase enzymes that directly make ammonia. vBy deepening our understanding of the microbial populations that cycle nitrogen, we can find opportunities to deliver more efficient bioengineering solutions. To date, no one has systematically explored the new biotechnologies for nitrogen removal that can emerge from this new knowledge because a purely empirical exploration would require significant investigation. This, however, could be accelerated using a cost-effective advanced modelling approach, as the one detailed in this proposal. To explore the functionalization of molecular dinitrogen and its catalytic conversion of molecular dinitrogen we will need to combine expertise in: a) inorganic chemistryby exploring the catalytic conversiond-block metals; b) computational chemistryby describing the reaction pathway and finding the reaction intermediates; c) metabolic modelingto describe the metabolic activities and synergies between microbial populations in the nitrogen-cycle, identifying the process conditions that generate efficient aggregates architectures for nitrogen-removal.iVitousek P. M., et alD. Ecol. Appl. 1997,7, 737-750.iiClark, B, Foster, J. B. Int. J. Comp. Soc.2009, 50,311-334.iiiSchoepp-Cothenet B., et alSci. Rep. 2012, 2, 263. ivPushie J. M., Cotelesagea J. J., George G. N., Metallomics2014, 6, 15-24.vKnobloch, D. J., Lobkovsky, E. & Chirik, P. J. Nat. Chem. 2, 30-35 (2010).