First principles design of novel ammonia synthesis catalysts

新型氨合成催化剂的第一性原理设计

基本信息

批准号：
EP/L02537X/1
负责人：
Justin Hargreaves
金额：
$ 40.33万
依托单位：
University of Glasgow
依托单位国家：
英国
项目类别：
Research Grant
财政年份：
2014
资助国家：
英国
起止时间：
2014 至无数据
项目状态：
已结题

来源：
https://gtr.ukri.org/projects?ref=EP%2FL02537X%2F1
关键词：
First principles design novel ammonia

项目摘要

The development of the Haber Bosch Process for the synthesis of ammonia on an industrial scale was one of the major achievements of the 20th Century. It can be directly credited with sustaining the global population through the provision of an accessible route to synthetic fertilizers. The process is based upon the reaction of pure N2 and H2 feedstreams over a promoted iron based catalyst. It is operated at high pressure (>100 atmospheres) and moderate temperature and the process as a whole currently accounts for a significant proportion of global energy demand (>1%). In this research, we are attempting to develop alternative catalysts which will contribute to energy savings by facilitating the reaction at lower reaction temperatures (where there is a thermodynamic advantage.) The approach to be taken will involve a mixture of computational design and experimental testing and is based upon previous studies of metal nitride catalysts which exhibit interesting activity for ammonia synthesis. Metal nitrides potentially contain "activated" nitrogen within their structure and it is the reactivity of this lattice nitrogen which which could be the key to their high activity. Using computational modelling, understanding of experimental results will be obtained and will be extended to the identification of nitride materials of potential high catalytic activity. In parallel laboratory experiments, the identified materials will be synthesised and tested and the results fed back into the computational modelling to provide improved understanding. In this way, optimal catalyst formulations will be identified and these will be prepared and tested under industrially relevant ammonia synthesis conditions and the results will be compared to those from conventional industrially applied iron based catalysts.

哈伯·博世（Haber Bosch）在工业规模上合成氨的过程是20世纪的主要成就之一。通过提供合成肥料的可及途径，可以将其直接归功于维持全球人口。该过程基于纯N2和H2馈线在基于铁的催化剂上的反应。它在高压（> 100个大气）和中等温度下进行操作，整个过程目前占全球能源需求的很大比例（> 1％）。在这项研究中，我们正在尝试开发替代性催化剂，这些催化剂将通过促进较低反应温度下的反应（在具有热力学优势的情况下促进反应。）采用的方法将涉及计算设计和实验测试的混合，并基于先前对氮化金属催化剂的研究，这些氮化金属催化剂表现出有趣的ammonia nitride催化剂。金属氮化物可能在其结构内包含“活化”的氮，而这是该晶格氮的反应性，这可能是其高活性的关键。使用计算建模，将获得对实验结果的理解，并将扩展到潜在高催化活性的氮化物材料的鉴定。在平行实验室实验中，将合成和测试确定的材料，并将结果反馈到计算建模中以提供改进的理解。通过这种方式，将确定最佳的催化剂制剂，并将在工业相关的氨合成条件下制备和测试，并将结果与常规工业施用的铁基催化剂进行比较。

项目成果

期刊论文数量（10）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

The Role of Composition for Cobalt Molybdenum Carbide in Ammonia Synthesis

DOI：
10.1021/acssuschemeng.7b02168
发表时间：
2017-10-01
期刊：
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
影响因子：
8.4
作者：
AlShibane, Ihfaf;Daisley, Angela;Smith, Ronald I.
通讯作者：
Smith, Ronald I.

XAS investigation of silica aerogel supported cobalt rhenium catalysts for ammonia decomposition.

DOI：
10.1039/d0cp00558d
发表时间：
2020-06
期刊：
Physical chemistry chemical physics : PCCP
影响因子：
0
作者：
Karsten G Kirste;S. Laassiri;Zhigang Hu;D. Stoian;L. Torrente‐Murciano;J. Hargreaves;K. Mathisen
通讯作者：
Karsten G Kirste;S. Laassiri;Zhigang Hu;D. Stoian;L. Torrente‐Murciano;J. Hargreaves;K. Mathisen

DFT Study of the Mars - van Krevelen Mechanism for Ammonia Synthesis on Co3Mo3N (111)-surfaces

Co3Mo3N（111）表面合成氨的 Mars - van Krevelen 机理的 DFT 研究