CAS: Molecular Catalysts to Control Dinitrogen Reduction and Ammonia Oxidation

CAS：控制氮还原和氨氧化的分子催化剂

• 批准号: 1956161
• 负责人: Michael Mock
• 金额: $ 47.57万
• 依托单位: Montana State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-07-01 至 2023-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1956161&HistoricalAwards=false
• 关键词: CAS; Molecular; Catalysts; Control; Dinitrogen

The Established Program to Stimulate Competitive Research (EPSCoR) and the Chemical Catalysis Program in the Chemistry Division, both of the National Science Foundation, support this project led by Professor Michael Mock of Montana State University. Professor Mock leads an effort to develop fuels that are derived from nitrogen in the air and ammonia that is produced from that nitrogen. The overarching goal is to explore new systems for energy storage. The focus is on the synthesis and analysis of new metal catalysts for the interconversion of nitrogen gas and ammonia. The new catalysts are based on ruthenium, nickel, iron, and chromium. Compounds consisting of these metals are proposed to exhibit novel behavior that facilitates the interconversion of nitrogen and ammonia. Of specific interest are strategies for the attachment and removal of hydrogen atoms. One approach involves creating chemical relays that carry the hydrogen from the metal to the nitrogen. The chemical synthesis of these relays is a specialty of Professor Mock. In addition to the research, Professor Mock is developing outreach activities to engage students at area schools, teaching them about energy technologies. He also is recruiting Native American undergraduate students from Montana Tribal Colleges to work in his laboratory. By providing hands-on experience in chemistry and catalysis to Native Americans, the project is strengthening the technical workforce in the United States. Professor Michael Mock of Montana State University is leading an effort to develop a nitrogen-based cycle to store energy in N-H bonds by synthesizing new molecular catalysts for the fundamental processes involved in the interconversion of dinitrogen (N2) and ammonia (NH3). The goal of this research is the development of molecular catalytic systems for N2 reduction and NH3 oxidation with a common strategy of delivery of H-atoms to N2 and and the removal of H-atoms from NH3 ligands. This project seeks to understand the reaction mechanisms of these processes by characterizing metal-NxHy intermediates, and measuring thermodynamic N-H bond strengths to advance catalyst design. The proposed work on catalytic N2 reduction schemes uses chemically robust chromium complexes. In the development of NH3 oxidation catalysts, the use of Ru and Ni-based platforms is advancing the goal of understanding homolytic N–H bond cleavage and N–N coupling steps en route to N2 formation. In addition to this research, Professor Mock is developing science outreach activities to engage students at area schools and Tribal Colleges about alternative forms of energy and new chemical technologies that have a positive impact on the environment and society. Professor Mock is recruiting Native American undergraduate students to his lab from Montana Tribal Colleges through summer internships to gain hands-on experience in chemistry and catalysis.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

国家科学基金会既支持竞争研究（EPSCOR）和化学部的化学催化计划的既定计划，支持由蒙大拿州立大学的迈克尔·莫克（Michael Mock）领导的该项目。 Mock教授领导了开发从空气和氨中衍生出的燃料，这些燃料是由该氮产生的。总体目标是探索新的能源存储系统。重点是对氮气和氨相互转化的新金属催化剂的合成和分析。新的催化剂基于氟树，镍，铁和铬。提出由这些金属组成的化合物表现出促进氮和氨相互转化的新型行为。特定感兴趣的是连接和去除氢原子的策略。一种方法涉及创建将氢从金属带到氮的化学继电器。这些继电器的化学合成是模拟教授的专长。除了研究外，模拟教授还正在开发外展活动，以吸引学生在地区学校中，向他们教会能源技术。他还正在招募来自蒙大拿州部落学院的美国原住民本科生在他的实验室工作。通过向美洲原住民提供化学和催化的动手经验，该项目正在加强美国的技术劳动力。蒙大拿州立大学的迈克尔·莫克（Michael Mock）教授正在努力开发基于氮的循环，通过合成新的分子催化剂来存储N-H键中的能量，以涉及参与二氧二抗（N2）和氨（NH3）的基本过程。这项研究的目的是开发用于N2降低和NH3氧化的分子催化系统，并通过将H原子传递到N2的共同策略以及从NH3配体中去除H原子。该项目旨在通过表征金属-NXHY中间体并测量热力学N-H键强度以推动催化剂设计来了解这些过程的反应机制。提出的关于催化N2还原方案的工作使用化学坚固的铬配合物。在NH3氧化催化剂的开发中，基于RU和NI的平台的使用正在促进理解均利性N – H键裂解和N – N耦合步骤的目标，以实现N2形成。除了这项研究外，模拟教授还正在开发科学外展活动，以使学生在地区学校和部落学院与替代形式的能源形式和新的化学技术，这些技术对环境和社会产生积极影响。 Mock教授正在通过暑期实习招募美国原住民的本科生从蒙大拿州部落学院招募实验室，以获得化学和催化方面的动手经验。该奖项反映了NSF的法定任务，并被认为是通过基金会的知识分子优点和更广泛的影响来评估的珍贵的支​​持。

项目成果

Synthesis, characterization, and liquid injection field desorption ionization mass spectrometry analysis of pincer ligated group 6 (Cr, Mo, W) carbonyl complexes

• DOI: 10.1177/14690667221149498
• 发表时间: 2023-01
• 期刊: European Journal of Mass Spectrometry
• 影响因子: 1.3
• 作者: Olivia L. Duletski;N. Arulsamy;Michael T. Mock

Catalytic Ammonia Oxidation to Dinitrogen by a Nickel Complex

镍络合物催化氨氧化制氮

• DOI: 10.1002/anie.202213462
• 发表时间: 2022
• 期刊: Angewandte Chemie International Edition
• 作者: Stephens, David N.;Szilagyi, Robert K.;Roehling, Paige N.;Arulsamy, Navamoney;Mock, Michael T.
• 通讯作者: Mock, Michael T.