羟基化石墨烯使Haber过程高效化
The Haber Process Made Efficient by Hydroxylated Graphene
摘要：
Haber-Bosch工艺是由双原子氮和氢生产氨的主要工业方法。它对能量要求很高，使用铁催化剂，需要高温和高压。哈伯法的任何改进都将产生极大的科学和经济影响。我们报告了使用羟基化石墨烯的氨产量的显着增加。利用N2/H2和NH3之间的极性差异，以及NH3的普遍质子受体行为，我们证明了哈伯-博世过程的平衡向氨的强烈转变。羟基化石墨烯提供了有利于正向反应的极性环境，并且在所研究的热力学条件下保持稳定。约50 kJ mol ~（-1）焓增益和ca.在298-1300 K和1-1000 bar下获得60-70 kJ mol-1自由能增益，强烈地使反应平衡向产物移动。使用电子结构计算和实时反应模拟给出了一个清晰的微观解释所观察到的现象。所证明的原理可以应用于许多极性基团，使具有高表面积的基材官能化，条件是该体系对H2、N2和NH3是化学惰性的。改进的Haber-Bosch方法对化学工业具有重要意义，因为它在降低温度和压力的同时显著提高了反应产率，从而降低了成本。
英文摘要：
The Haber-Bosch process is the main industrial method for producing ammonia from diatomic nitrogen and hydrogen. Very demanding energetically, it uses an iron catalyst, and requires high temperature and pressure. Any improvement of the Haber process will have an extreme scientific and economic impact. We report a significant increase of ammonia production using hydroxylated graphene. Exploiting the polarity difference between N2/H2 and NH3, as well as the universal proton acceptor behavior of NH3, we demonstrate a strong shift of the equilibrium of the Haber-Bosch process towards ammonia. Hydroxylated graphene provides the polar environment favoring the forward reaction, and remain stable under the investigated thermodynamic conditions. Ca. 50 kJ mol-1 enthalpy gain and ca. 60-70 kJ mol-1 free energy gain are achieved at 298-1300 K and 1-1000 bar, strongly shifting the reaction equilibrium towards the product. A clear microscopic interpretation of the observed phenomenon is given using electronic structure calculations and real-time reactive simulations. The demonstrated principle can be applied with many polar groups functionalizing a substrate with a high surface area, provided that the system is chemically inert to H2, N2 and NH3. The modified Haber-Bosch process is of significant importance to the chemical industry, since it provides a substantial increase of the reaction yield while decreasing the temperature and pressure, thereby, reducing the cost.
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