Role of nanominerals on photochemical derived atmospheric NH3 and N2O

纳米矿物对光化学产生的大气 NH3 和 N2O 的作用

• 批准号: 1933646
• 负责人: Marta Hatzell
• 金额: $ 49.87万
• 依托单位: Georgia Tech Research Corporation
• 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: 2020-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1933646&HistoricalAwards=false
• 关键词: Role; nanominerals; photochemical; derived; atmospheric

Significant evidence suggests that the global nitrogen cycle is not balanced. The intensification of agriculture and rising emissions from the burning of fossil fuels are largely responsible for this imbalance, as both of these anthropogenic activities have enhanced reactive nitrogen emissions by a factor of three over the last century. Furthermore, these harmful environmental pollutants are responsible for the formation of certain aerosols, which have negative implications for both natural ecosystems and human health. A chief challenge in engineering solutions to this imbalance lies in quantifying and identifying all global nitrogen fluxes in the atmosphere and pedosphere. This requires high-resolution measurements of both natural and anthropogenic sources and sinks. This research will aim to quantify the rate of natural nitrogen-based atmospheric emissions that arise due to nanoscale interactions between soil nanominerals and sunlight. Currently, anthropogenic sources are generally more accurately mapped than emissions from natural or semi-natural sources. Therefore, further efforts to identify which nanoscale phenomena aid the formation and nitrogen-based emission in soils is important to advance our understanding of the global nitrogen cycle. The work will also support undergraduate education, serving as the basis of a capstone project through Georgia Tech's Food-Energy-Water initiatives, which is enabled through the Serve-Learn-Sustain program. This capstone project will engage undergraduate seniors from a range of academic disciplines including engineering and social sciences. In addition, this work seeks to engage the non-scientific community through a collaboration with the Atlanta wide initiative Science-Art-Wonder. Through this program, researchers will collaborate with artist to transform key scientific findings into art pieces that will be displayed at the Atlanta science festival. The main research objective of this project is to understand how photocatalytic earth-abundant nanominerals in soils and sands contribute to reactive nitrogen emissions. Specifically, the PI will investigate the role mineral, soil and atmospheric properties play in increasing the activity of nanominerals for ammonia and nitrous oxide production. The nanoscale structure-property relationships of common nanominerals will be probed through photo(electro)catalytic testing to discern the impact mineral size and surface nanostructure have on catalytic activity. In depth first-principles calculations and atmospheric testing will also elucidate which nanoscale chemical mechanisms and physical phenomena promote sunlight driven reactive nitrogen production and emission from soils and sands. This fundamental understanding will provide insight into the role terrestrial nanominerals play in mediating the natural nitrogen cycle, providing a foundation for more accurate models of nutrient fluxes in terrestrial and atmospheric settings. The project will seek to establish a holistic view of the role soils and agriculture play on atmospheric pollution. The impact of the work will be enhanced by outreach and educational efforts. The findings will be highlighted through a publicly accessible website and YouTube videos that demonstrate key findings and suggest simple experiments that can be performed with household items.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.

有重要证据表明，全球氮循环并不平衡。农业集约化和化石燃料燃烧排放的增加是造成这种不平衡的主要原因，因为在过去一个世纪里，这两种人为活动都使活性氮排放增加了三倍。此外，这些有害的环境污染物是某些气溶胶形成的原因，对自然生态系统和人类健康都有负面影响。解决这种不平衡的工程解决方案的一个主要挑战是量化和确定大气和土壤圈中的所有全球氮通量。这需要对自然和人为来源和汇进行高分辨率测量。这项研究的目的是量化由于土壤纳米矿物和阳光之间的纳米级相互作用而产生的自然氮基大气排放的速率。目前，人为来源的测绘通常比自然或半自然来源的排放更准确。因此，进一步努力确定哪些纳米尺度现象有助于土壤中氮素的形成和排放，对于促进我们对全球氮循环的理解是重要的。这项工作还将支持本科教育，作为佐治亚理工学院通过服务-学习-支持计划实现的食物-能源-水倡议的顶峰项目的基础。这个顶峰项目将吸引来自包括工程学和社会科学在内的一系列学术学科的本科生。此外，这项工作寻求通过与亚特兰大范围内的科学-艺术-奇迹倡议合作，吸引非科学社区的参与。通过这个项目，研究人员将与艺术家合作，将关键的科学发现转化为艺术作品，并在亚特兰大科学节上展出。该项目的主要研究目标是了解土壤和沙子中富含稀土的光催化纳米矿物是如何促进活性氮排放的。具体地说，PI将调查矿物、土壤和大气性质在增加纳米矿物对氨和一氧化二氮生产的活性方面所起的作用。通过光(电)催化测试来探索常见纳米矿物的纳米尺度结构-性质关系，以辨别矿物尺寸和表面纳米结构对催化活性的影响。深入的第一性原理计算和大气测试还将阐明哪些纳米尺度的化学机制和物理现象促进了阳光驱动的活性氮的产生和从土壤和沙子中排放。这一基本认识将有助于深入了解陆地纳米矿物在调节自然氮循环中所起的作用，为更准确地建立陆地和大气环境下的营养通量模型奠定基础。该项目将寻求建立土壤和农业在大气污染中所起作用的整体观点。这项工作的影响将通过外联和教育努力得到加强。这些发现将通过一个可公开访问的网站和YouTube视频突出显示，这些视频展示了关键发现，并提出了可以用家用物品进行的简单实验。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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

PdCu Electrocatalysts for Selective Nitrate and Nitrite Reduction to Nitrogen

• DOI: 10.1021/acscatal.2c04841
• 发表时间: 2023-01-06
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Lim, Jeonghoon;Chen, Yu;Hatzell, Marta C.
• 通讯作者: Hatzell, Marta C.

Energy Demand of Nitrogen and Phosphorus Based Fertilizers and Approaches to Circularity

• DOI: 10.1021/acsenergylett.2c02627
• 发表时间: 2023-02-17
• 期刊: ACS ENERGY LETTERS
• 影响因子: 22
• 作者: Daramola, Damilola A.;Hatzell, Marta C.
• 通讯作者: Hatzell, Marta C.

Impact of Local Microenvironments on the Selectivity of Electrocatalytic Nitrate Reduction in a BPM‐MEA System

• DOI: 10.1002/aenm.202304202
• 发表时间: 2024-02
• 期刊: Advanced Energy Materials
• 影响因子: 27.8
• 作者: Po-Wei Huang;Hakhyeon Song;Jaeyoung Yoo;Danae A. Chipoco Haro;Hyuck Mo Lee;Andrew J. Medford;Marta C. Hatzell

Ammonia and Nitric Acid Demands for Fertilizer Use in 2050

• DOI: 10.1021/acsenergylett.1c01614
• 发表时间: 2021-09-24
• 期刊: ACS ENERGY LETTERS
• 影响因子: 22
• 作者: Lim, Jeonghoon;Fernandez, Carlos A.;Hatzell, Marta C.
• 通讯作者: Hatzell, Marta C.

Prospects for Aerobic Photocatalytic Nitrogen Fixation

• DOI: 10.1021/acsenergylett.1c02260
• 发表时间: 2022-01-14
• 期刊: ACS ENERGY LETTERS
• 影响因子: 22
• 作者: Liu, Yu-Hsuan;Fernandez, Carlos A.;Hatzell, Marta C.
• 通讯作者: Hatzell, Marta C.