Collaborative Research: New Roles for Reactive Oxygen Species in Mediating Carbon Fluxes at the Terrestrial-Aquatic Interface

合作研究：活性氧在调节陆地-水生界面碳通量中的新作用

• 批准号: 2029665
• 负责人: Yu-Ping Chin
• 金额: $ 23.64万
• 依托单位: University of Delaware
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-07-01 至 2025-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2029665&HistoricalAwards=false
• 关键词: Collaborative; Research; New; Roles; Reactive

Wetlands in the north central region of the United States are important ecosystems that play critical roles in the regional carbon cycle and are likely to be dramatically affected by climate change. Rates of greenhouse gas release from these wetlands may increase with warming and offset their ability to sequester carbon. By studying the chemical and microbiological processes in wetland sediments over space and time, predictions of the effects of climate change on these critical habitats will be possible. Documentation of the ecological importance of this region via photography will demonstrate the value of wetlands to a broad audience.The drivers of biogeochemical activity that dictate the emissions of carbon dioxide and methane in small, inland waters are poorly constrained, yet processes in these water bodies play an oversized role in understanding climate change. One process that is poorly understood is the role of chemical reactions in mediating carbon dioxide and methane formation in small lakes and wetlands, especially the abiotic production of reactive oxygen species (ROS) at the sediment-water interface (SWI). The hypothesis for this project is that the reaction of reduced soluble and particulate forms of iron, sulfur, and carbon with trace level oxygen to form ROS at the SWI is an under-appreciated, yet critical, control on microbiological activity and the cycling of carbon in small inland water bodies. Using a combination of field work in the prairie pothole region of North Dakota, controlled laboratory experiments, and mesocosm studies, this work will 1) identify the geochemical drivers of ROS generation at the SWI, 2) determine spatiotemporal patterns of linked pore water chemistry and ROS at the SWI, and 3) track the generation of specific labile carbon substrates produced through ROS-DOM reactions that affect rates of carbon mineralization and methane production in small lake and wetland sediments. A combination of in situ voltammetry measurements, detailed characterization of dissolved and particulate organic matter, iron, and sulfur species, and microbial -omics analyses will be used to understand the coupled biogeochemical processes. A key component of this work is understanding how abiotic ROS driven reactions at the sediment-water interface lead to turnover of terminal electron acceptors and generation of labile microbial substrates. Establishing a baseline understanding of these processes is needed to predict changes in carbon dioxide and methane fluxes under different climate scenarios. The collected data will enable understanding of how biogeochemical cycles are maintained through coupled abiotic/biotic pathways, and how these processes impact carbon cycling in aquatic environments. This approach is also applicable to other systems and the cycling of other elements, such as nitrogen, which may be especially important in urban wetland regions. The societal benefit will be improved understanding of processes that influence, and are influenced by, climate change. To reach as broad an audience as possible regarding the importance of this region, a photographer will document the landscape and its ecological function during field sampling trips.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.

美国中北部地区的湿地是重要的生态系统，在区域碳循环中发挥着关键作用，很可能受到气候变化的巨大影响。这些湿地的温室气体释放速率可能会随着气候变暖而增加，并抵消它们固碳的能力。通过研究湿地沉积物在空间和时间上的化学和微生物过程，可以预测气候变化对这些关键栖息地的影响。通过摄影记录该地区的生态重要性将向广大观众展示湿地的价值。决定小型内陆水域二氧化碳和甲烷排放的生物地球化学活动的驱动因素很少受到限制，但这些水体的过程在理解气候变化方面发挥了过大的作用。一个鲜为人知的过程是化学反应在小湖泊和湿地中调节二氧化碳和甲烷形成的作用，特别是在沉积物-水界面(SWI)非生物产生活性氧物种(ROS)的过程。该项目的假设是，在SWI，还原的可溶性和颗粒态的铁、硫和碳与微量氧反应形成ROS，这是对内陆小水体中微生物活动和碳循环的一种被低估但关键的控制。利用北达科他州草原坑洼地区的实地工作、对照实验室实验和中观研究相结合，这项工作将1)确定SWI产生ROS的地球化学驱动因素，2)确定相互关联的孔隙水化学和SWI ROS的时空模式，3)追踪通过ROS-DOM反应产生的特定不稳定碳底物的产生，这些反应影响小湖泊和湿地沉积物中的碳矿化和甲烷产生的速率。将结合现场伏安测量、溶解和颗粒有机物、铁和硫物种的详细表征以及微生物组学分析来了解耦合的生物地球化学过程。这项工作的一个关键组成部分是了解非生物ROS如何驱动沉积物-水界面的反应导致末端电子受体的周转和不稳定微生物底物的产生。需要建立对这些过程的基线理解，以预测不同气候情景下二氧化碳和甲烷通量的变化。收集到的数据将有助于理解生物地球化学循环是如何通过耦合的非生物/生物途径维持的，以及这些过程如何影响水生环境中的碳循环。这种方法也适用于其他系统和其他元素的循环，如氮，这在城市湿地地区可能特别重要。社会利益将是更好地理解影响气候变化及其影响的过程。为了让尽可能广泛的观众了解这一地区的重要性，摄影师将在实地采样旅行期间记录该景观及其生态功能。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

Influence of Organic Ligands on the Redox Properties of Fe(II) as Determined by Mediated Electrochemical Oxidation

• DOI: 10.1021/acs.est.2c01782
• 发表时间: 2022-06-08
• 期刊: ENVIRONMENTAL SCIENCE & TECHNOLOGY
• 影响因子: 11.4
• 作者: Hudson, Jeffrey M.;Luther, George W., III;Chin, Yu-Ping
• 通讯作者: Chin, Yu-Ping