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.

工业规模合成氨的哈伯博世工艺的开发是 20 世纪的重大成就之一。通过提供获取合成肥料的便捷途径，它可以直接归功于维持全球人口的发展。该工艺基于纯 N2 和 H2 原料流在促进的铁基催化剂上的反应。它在高压（>100 个大气压）和中等温度下运行，整个过程目前占全球能源需求的很大一部分（>1%）。在这项研究中，我们正在尝试开发替代催化剂，通过在较低的反应温度下促进反应（具有热力学优势），从而有助于节省能源。所采取的方法将涉及计算设计和实验测试的结合，基于先前对金属氮化物催化剂的研究，该催化剂对氨合成表现出有趣的活性。金属氮化物的结构中可能含有“活化”氮，这种晶格氮的反应性可能是其高活性的关键。使用计算模型，将获得对实验结果的理解，并将其扩展到识别具有潜在高催化活性的氮化物材料。在平行实验室实验中，将合成和测试已识别的材料，并将结果反馈到计算模型中以提供更好的理解。通过这种方式，将确定最佳的催化剂配方，并在工业相关的氨合成条件下制备和测试这些配方，并将结果与传统工业应用的铁基催化剂的结果进行比较。

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