Mechanistic study of N8- polynitrogen synthesis and its oxygen reduction reaction

N8-多氮合成及其氧还原反应机理研究

• 批准号: 1804949
• 负责人: Xianqin Wang
• 金额: $ 33万
• 依托单位: New Jersey Institute of Technology
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1804949&HistoricalAwards=false
• 关键词: Mechanistic; study; N8; polynitrogen; synthesis

Fuel cells are devices for direct conversion of the chemical energy of a fuel into electricity through electrochemical reactions. However, widespread implementation of fuel cells has been hampered by the high cost of the platinum catalyst. Despite many decades of research, few non-precious metal fuel cell catalysts have been found that can rival the performance and stability of platinum. The project will investigate low-cost alternatives to platinum as fuel cell catalysts, thus helping to achieve higher penetration of fuel cell technology into the energy sector and increasing our Nation's energy security. The project will also include educational and outreach programs that will enhance energy awareness at all educational levels and build a future workforce highly trained in energy technology.The project under Dr. Xianqin Wang from New Jersey Institute of Technology, Newark, NJ, involves exploring polymeric nitrogen (PN) supported on multi-walled carbon nanotubes as the cathode catalyst for potential use in proton exchange membrane (PEM) fuel cells. The project seeks to advance fundamental understanding of PN synthesis and the role of the carbon-supported polymeric nitrogen species to promote the oxygen reduction reaction (ORR). The active sites associated with the anionic polynitrogen species will be linked to enhanced O=O bond reduction and more detailed understanding of the electrochemical reduction mechanism as obtained from both advanced characterization tools and density functional theory (DFT). In particular, the O2 chemisorption mode will be probed under reaction conditions by in situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), which when combined with kinetic experiments and theoretical calculations, can shed deeper insight regarding the ORR mechanism and its relationship to catalyst structure. The results will provide the basis for metal-free, green catalytic materials as oxygen reduction catalysts for hydrogen, methanol, and glucose or biomass powered fuel cells. Successful results from this effort will lead to use of non-metallic polymeric nitrogen in other applications, such as mild and selective oxidation reactions, hydrogenation reactions and multipurpose applications in biomass conversion and sustainable chemistry. Dr. Wang is actively involved in inspiring young students, especially female and underrepresented minorities, to develop their interests in science through research. She will provide opportunities for a diverse group of graduate, undergraduate, and K-12 students to collaborate in this interdisciplinary research project and work with scientists from different fields.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.

燃料电池是通过电化学反应将燃料的化学能直接转化为电能的装置。然而，铂催化剂的高成本阻碍了燃料电池的广泛应用。尽管经过几十年的研究，很少有非贵金属燃料电池催化剂能与铂的性能和稳定性相媲美。 该项目将研究铂作为燃料电池催化剂的低成本替代品，从而有助于实现燃料电池技术在能源领域的更高渗透率，并提高我国的能源安全。 该项目还将包括教育和推广计划，以提高所有教育水平的能源意识，并建立一个未来的劳动力在能源技术方面训练有素。该项目由来自新泽西理工学院，纽瓦克，新泽西州的王贤琴博士领导，涉及探索多壁碳纳米管支撑的聚合氮（PN）作为阴极催化剂，用于质子交换膜（PEM）燃料电池的潜在用途。 该项目旨在促进对PN合成的基本理解以及碳支撑的聚合氮物种在促进氧还原反应（ORR）中的作用。 与阴离子多氮物种相关的活性位点将被链接到增强的O=O键还原和更详细的了解的电化学还原机制，从先进的表征工具和密度泛函理论（DFT）。特别是，O2的化学吸附模式将探测反应条件下的原位壳隔离纳米粒子增强拉曼光谱（SHINERS），结合动力学实验和理论计算，可以更深入地了解ORR机制及其与催化剂结构的关系。 研究结果将为无金属、绿色催化材料作为氢、甲醇、葡萄糖或生物质燃料电池的氧还原催化剂提供基础。 这一努力的成功结果将导致非金属聚合氮在其他应用中的使用，例如温和和选择性氧化反应，氢化反应以及生物质转化和可持续化学中的多用途应用。 王博士积极鼓励年轻学生，特别是女性和少数民族学生，通过研究培养他们对科学的兴趣。 她将为不同的研究生、本科生和K-12学生提供机会，在这个跨学科的研究项目中与来自不同领域的科学家合作。该奖项反映了NSF的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

N8 stabilized single-atom Pd for highly selective hydrogenation of acetylene

• DOI: 10.1016/j.jcat.2020.12.009
• 发表时间: 2021-03
• 期刊: Journal of Catalysis
• 影响因子: 7.3
• 作者: Maocong Hu;Zhiyi Wu;Z. Yao;Joshua Young;L. Luo;Yingge Du;Chongmin Wang;Z. Iqbal;Xianqin Wang-Xianqin

Synthesis and Stabilization of Cubic Gauche Polynitrogen under Radio-Frequency Plasma

• DOI: 10.1021/acs.chemmater.2c00689
• 发表时间: 2022-05
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: Haizheng Zhuang;Safa Alzaim;Skywalker Li;El Mostafa Benchafia;Joshua Young;N. Ravindra;Z. Iqbal

Synthesis of polymeric nitrogen with non-thermal radio frequency plasma

• DOI: 10.1016/j.cattod.2022.04.009
• 发表时间: 2022-12-01
• 期刊: CATALYSIS TODAY
• 影响因子: 5.3
• 作者: Zhuang，Haizheng;Huo，Siming;Wang，Xianqin
• 通讯作者: Wang，Xianqin