CAREER: Confinement Induced Structural Evolution of Calcium- and Magnesium- Carbonates in Architected Siliceous Nanochannels

职业：限制诱导的硅质纳米通道中碳酸钙和碳酸镁的结构演化

• 批准号: 2144373
• 负责人: Greeshma Gadikota
• 金额: $ 53.5万
• 依托单位: Cornell University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-08-01 至 2027-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2144373&HistoricalAwards=false
• 关键词: CAREER; Confinement; Induced; Structural; Evolution

Advancing gigaton-scale solutions to capture, convert, store, and remove carbon dioxide (CO2) from gas emissions and air is crucial to limit the detrimental environmental impacts of climate change. Carbon mineralization is a scalable and thermodynamically favorable approach for converting anthropogenic CO2 into calcium or magnesium carbonates using earth-abundant nanoporous silicates. The carbonate products are stable, water-insoluble inorganic compounds, ideal for CO2 storage applications. However, our limited understanding of the pore-scale interfacial mechanisms that influence the carbon mineralization process challenges our ability to predictively control carbonate formation. To address this scientific challenge, this research project will develop architected siliceous nanochannels with ordered porosity to investigate carbonate crystallization mechanisms in confinement. The fundamental knowledge gained from these studies will inform the design of new technologies that harness carbonate crystallization mechanisms for the reactive separation of gases, recovery of high-value metals, and predicting the fate of CO2 injected into geological reservoirs. The research program is closely integrated with educational and outreach activities focused on training the future STEM workforce and co-creating community-level carbon removal solutions by engaging members of underrepresented groups in STEM and members of underserved rural communities. This project will investigate the crystallization mechanisms of calcium and magnesium carbonate crystallization in confined fluids within architected siliceous nanochannels with sizes ranging from 2 to 20 nm. Carbonate crystallization mechanisms in confined fluids will be investigated in less reactive silica interfaces and more reactive calcium and magnesium silicate surfaces. Morphological and compositional controls on siliceous pores will be achieved via sol-gel synthesis in anodic alumina membranes with ordered pores. Non-invasive and dynamic characterization of carbonate crystallization will be realized through operando X-ray scattering and advanced spectroscopy measurements. The experimental results will be used to investigate the validity of classical and non-classical mechanisms of carbonate formation and propose new mechanisms if needed. These research activities will serve as an educational and outreach platform for engaging underrepresented K-12 students in science education and communication through illustrative workbooks, mentoring videos in collaboration with PBS, and hands-on experimental modules supported by Expanding Your Horizons and Sciencenter. Undergraduate students will be recruited and mentored through the NSF Louis Stokes Alliances for Minority Participation program using research activities related to carbon transformations as a platform. Topics related to decarbonization in the context of science and engineering for climate, energy, and environmental technologies will be made more accessible through blended learning formats for undergraduate and graduate students. Insights from research activities will be used to co-create carbon removal solutions through mineral weathering with local farmers. The closely integrated research, outreach, and educational activities are designed to foster enthusiasm for and engagement in sustainable climate, environment, and energy solutions.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.

推进千兆吨规模的解决方案，从气体排放和空气中捕获、转换、储存和去除二氧化碳（CO2），对于限制气候变化对环境的有害影响至关重要。碳矿化是利用地球上丰富的纳米多孔硅酸盐将人为二氧化碳转化为碳酸钙或碳酸镁的一种可扩展和热力学有利的方法。碳酸盐产品是稳定的，不溶于水的无机化合物，理想的二氧化碳储存应用。然而，我们对影响碳矿化过程的孔隙尺度界面机制的了解有限，挑战了我们预测控制碳酸盐岩形成的能力。为了解决这一科学挑战，该研究项目将开发具有有序孔隙度的硅质纳米通道，以研究限制条件下碳酸盐的结晶机制。从这些研究中获得的基础知识将为利用碳酸盐结晶机制进行气体活性分离、回收高价值金属和预测注入地质储层的二氧化碳命运的新技术的设计提供信息。该研究项目与教育和推广活动紧密结合，重点是培训未来的STEM劳动力，并通过让STEM中代表性不足的群体成员和服务不足的农村社区成员参与进来，共同创造社区层面的碳去除解决方案。该项目将研究碳酸钙和碳酸镁在受限流体中结晶的结晶机制，这些流体位于硅质纳米通道内，尺寸从2到20纳米不等。碳酸盐在受限流体中的结晶机制将在反应性较低的二氧化硅界面和反应性较强的硅酸钙和镁表面进行研究。硅质孔隙的形态和成分控制将通过溶胶-凝胶合成在有序孔隙的阳极氧化铝膜上实现。通过operando x射线散射和先进的光谱测量，将实现碳酸盐岩结晶的无创和动态表征。实验结果将用于研究碳酸盐岩形成的经典和非经典机制的有效性，并在必要时提出新的机制。这些研究活动将作为一个教育和推广平台，通过插图练习册、与PBS合作的指导视频以及由expand Your Horizons和Sciencenter支持的动手实验模块，吸引代表性不足的K-12学生参与科学教育和交流。本科生将通过美国国家科学基金会路易斯·斯托克斯少数民族参与联盟项目招募和指导，该项目利用与碳转化相关的研究活动作为平台。在气候、能源和环境技术的科学和工程背景下，与脱碳相关的主题将通过本科生和研究生的混合学习形式更容易获得。研究活动的见解将用于与当地农民共同创造通过矿物风化的碳去除解决方案。紧密结合的研究、推广和教育活动旨在培养对可持续气候、环境和能源解决方案的热情和参与。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识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

Confinement induces stable calcium carbonate formation in silica nanopores

限制诱导二氧化硅纳米孔中稳定碳酸钙的形成

• DOI: 10.1039/d2nr01834a
• 发表时间: 2022
• 期刊: Nanoscale
• 影响因子: 6.7
• 作者: Asgar, Hassnain;Mohammed, Sohaib;Gadikota, Greeshma
• 通讯作者: Gadikota, Greeshma