Electrocatalytic Metal-Mediated Nitrogen Fixation

电催化金属介导的固氮

基本信息

批准号：
1665421
负责人：
Lawrence Sita
金额：
$ 45万
依托单位：
University of Maryland, College Park
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-07-15 至 2020-06-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1665421&HistoricalAwards=false
关键词：
Electrocatalytic Metal Mediated Nitrogen Fixation

项目摘要

Electrocatalytic Metal-Mediated Nitrogen FixationAs the world's population is expected to increase from 7 billion to nearly 10 billion people within the next 35 years, there is the need to develop and commercialize new energy-efficient and environmentally-benign industrial processes that can provide chemicals that are required to support and advance civilization. In this regard, the century-old Haber-Bosch (HB) process, which converts nitrogen (N2) and hydrogen (H2) into over 140 million metric tons of ammonia (NH3) to be used as fertilizer each year, is critical for our survival, however, as practiced, it currently consumes up to 5% of the world's energy production and a substantial amount of chemical waste is generated to provide the required amount of hydrogen. More importantly, at the molecular level, scientists do not know how 'nitrogen fixation' by the HB process works. In this project, Dr. Sita and his research group are pursuing a new design for the development of chemistry that uses electricity as the source of power and water (H20) rather than hydrogen for achieving the ultimate goal of inexpensive, energy- and chemically-efficient nitrogen fixation that will not have an enormous future impact on natural resources and the environment. With funding from the Chemical Catalysis Program of the Chemistry Division, Dr. Sita of the University of Maryland is seeking to develop an electrochemically-driven catalytic process for the energy efficient and atom-economical conversion of N2 into NH3. Research activities include the design and optimization of molecularly-discrete mononuclear and dinuclear molybdenum (Mo) complexes that can coordinate N2 in a manner that leads to low temperature N-N bond cleavage, N-atom functionalization, and release of a nitrogen-containing product in a fashion that recycles the Mo complex back to the initial starting state. Bulk electrolysis, using optimized metal electrodes and trialkylsilyl halides, is being employed to establish a chemical process that is catalytic in the amount of Mo complex that is required for the production of trialkylsilylated amines from N2. Acid hydrolysis of the trialkylsilylated amines is providing NH3 and enabling recycling the trialkylsilyl halide. Validation of the new proposed paradigm for achieving electrocatalytic nitrogen fixation is providing an important scientific foundation that can contribute to the further advancement of chemical technologies that are beneficial to global civilization and the world economy. This project is also training a diverse new generation of scientists in interdisciplinary areas of electrochemistry, inorganic and industrial chemistry, catalysis, and reaction mechanisms. Dr. Sita is engaging in outreach activities with the general public to promote a better understanding of chemistry and its critical role in supporting civilization and a better quality of life. In particular, Dr. Sita is providing STEM education at the K-12 level and especially through involvement with groups of students from underrepresented groups.

电催化金属介导的氮固定预计在未来35年内，全球人口将从70亿人口增加到近100亿人口，需要开发和商业化新的节能和环保工业过程，这些工业可以提供支持和推动文明和推动文明所需的化学物质。在这方面，将氮（N2）和氢（H2）转换为超过1.4亿吨的氨（NH3）的百年历史的Haber-Bosch（HB）过程，每年用作肥料，这对于我们的生存至关重要，但是，由于实践，它的生存至关重要。更重要的是，在分子水平上，科学家不知道HB过程如何“固定氮”。在这个项目中，SITA博士和他的研究小组正在为化学发展开发新的设计，该设计将电力用作电力和水的来源（H20），而不是实现廉价，能量和化学效率高效的氮固定的最终目标，这将不会对自然资源和环境产生巨大影响。在化学部化学催化计划的资助下，马里兰大学的SITA博士正在寻求开发一种电化学驱动的催化过程，以将N2的能源效率和原子经济转化为NH3。研究活动包括设计和优化分子二异构的单核和双核钼（MO）络合物，可以以低温N-N键裂解，N原子官能化以及释放含氮气的产品的方式以低温N-N键裂解，以将MO恢复到MO综合体的方式，从而恢复到最初的起步状态。使用优化的金属电极和试验甲硅烷基卤化物的散装电解被用于建立一种化学过程，该化学过程是在Mo复合物量中催化的，这是从N2产生trykylsilyate的胺所需的。试验二烯丙基胺的酸水解提供了NH3，并可以回收试验性甲硅烷基卤化物。验证新提出的用于实现电催化氮固定的范式提供了一个重要的科学基础，该基础可以有助于进一步发展对全球文明和世界经济有益的化学技术。该项目还在培训电化学，无机和工业化学，催化和反应机制的跨学科领域的新一代科学家。 SITA博士正在与公众进行外展活动，以更好地了解化学及其在支持文明和更好的生活质量中的关键作用。特别是，SITA博士在K-12级提供STEM教育，尤其是通过参与来自代表性不足的群体的学生。