SusChEM: Carbon Capture and Utilization by Controlled Carbonate Mineralization

SusChEM：通过控制碳酸盐矿化进行碳捕获和利用

• 批准号: 1335694
• 负责人: Michael Doherty
• 金额: $ 54.75万
• 依托单位: University of California-Santa Barbara
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-08-01 至 2018-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1335694&HistoricalAwards=false
• 关键词: SusChEM; Carbon; Capture; Utilization; Controlled

1335694 (Doherty). One of the defining problems of our time is that levels of CO2 in the atmosphere have increased from 315 ppm in 1958 to 394 ppm in 2012, leading to concerns about changes in climate occurring at a rate that will be difficult to manage. The steady increase in CO2 emissions from stationary sources across a spectrum of industrial processes (e.g., electricity generation, manufacturing of cement, chemicals, plastics) has raised tremendous interest in the process of carbon capture and utilization, ideally without adversely affecting living standards world-wide. But, if CO2 capture is to be economically and environmentally sustainable in the long-term, it is crucial to find ways of turning CO2 from harmful waste into a useful product at an economical price. This project is a high-risk high-reward strategy toward achieving this goal. A novel holistic approach for CO2 capture underpinned by scientific and green engineering foundations that has the potential to transform CO2 into a useful solid product with net positive value will be explored. The current standard approach to dealing with this problem has been to separate CO2 from combustion gases in the form of a highly compressed and almost pure fluid that is then disposed of in one of several ways, most of which will require careful monitoring for re-emission. Instead, pn this project, the combustion gases will be reacted with reagents (Ca2+, OH-, silicates, or saccharides/phosphonates) to form a benign and potentially valuable solid carbonate material with applications in the construction industry. The proposers estimate that the energy penalty for carbonate mineralization technology is significantly less than that for current approaches. They propose to establish and optimize the governing molecular processes that underlie the use of subsurface geological brines or reactive minerals as feedstocks to capture and utilize CO2 in the form of solid carbonates and/or silicates. These feedstocks have high Ca2+ contents, as well as desirable alkalinities, which significantly increase the carbonation rates. The proposes hypothesize that deep molecular understanding of the metastable solid products formed, coupled with state-of-the-art conceptual process design and development (a systems approach), will lead to an effective combined capture and utilization technology for CO2 that will be transformative in its approach and potentially in its societal impact.The intellectual merit of the approach is the novel coupling of fundamental materials science at a molecular level to establish the molecular design rules for the formation and stabilization of reactive metastable carbonate/silicate solids with process design (systems) strategies for implementing these rules at macroscopic scale. This will be achieved by exploiting state-of-the-art techniques of NMR spectroscopy, which have only recently become available for key 43Ca, 25Mg, 13C, 31P and dipolar-coupled 29Si and 1H species in carbonates and cementious materials. The novel use of saccharides/phosphonates or other organic molecules to stabilize reactive carbonates is expected to promote their processability, storage stability, and conversion into valuable structural materials. Based on the molecular insights obtained, materials processing variables (e.g., temperature, pressure, pH, composition, and reactor/separator configurations) will be assessed and optimized to control precipitation and crystallization of carbonate solids with engineered structures, particle morphologies, and surface compositions, including techno-economic considerations. The broader impacts of this research include (1) educating graduate and undergraduate students broadly in state-of-the-art methods of molecular engineering of crystalline solids and process design strategies for their syntheses, (2) fostering broad awareness of greenhouse gas emissions, their impacts, candidate strategies for CO2 utilization, and associated energy and environmental ramifications, and (3) the specific possibility for developing a paradigm-changing approach by which CO2 is converted to a valuable structural material. The insights gained from the proposed project will be general, enabling students and the broader scientific community to develop novel approaches for converting waste products into potentially valuable materials, along with quantifying process design and economic factors through a systems approach to evaluate cost-effectiveness.

1335694（Doherty）。 我们这个时代的一个决定性问题是，大气中的二氧化碳含量从1958年的315 ppm增加到2012年的394 ppm，导致人们担心气候变化的速度将难以控制。在一系列工业过程中，来自固定源的二氧化碳排放量稳步增加（例如，发电、水泥制造、化学品、塑料）已经引起了人们对碳捕获和利用过程的极大兴趣，理想情况下不会对全世界的生活水平产生不利影响。但是，如果CO2捕集要在经济和环境上长期可持续，关键是要找到将CO2从有害废物转化为经济价格的有用产品的方法。这个项目是实现这一目标的高风险高回报战略。将探讨一种新的二氧化碳捕集整体方法，该方法以科学和绿色工程基础为基础，有可能将二氧化碳转化为具有净正价值的有用固体产品。目前处理这一问题的标准方法是以高度压缩且几乎纯净的流体形式将CO2从燃烧气体中分离出来，然后以几种方式之一进行处置，其中大多数需要仔细监测再排放。相反，在该项目中，燃烧气体将与试剂（Ca 2+，OH-，硅酸盐或碳酸盐/膦酸盐）反应，形成一种在建筑行业应用的良性和潜在有价值的固体碳酸盐材料。提议者估计，碳酸盐矿化技术的能源代价明显低于目前的方法。他们建议建立和优化控制分子过程，这些过程是使用地下地质盐水或活性矿物作为原料以固体碳酸盐和/或硅酸盐形式捕获和利用CO2的基础。这些原料具有高的Ca 2+含量，以及所需的碱性，这显著提高了碳酸化速率。该提议假设，对形成的亚稳固体产物的深入分子理解，加上最先进的概念过程设计和开发，（系统方法），将导致一种有效的CO2联合捕获和利用技术，这种技术将在其方法和潜在的社会影响方面具有变革性。这种方法的智力价值是将基础材料科学与在分子水平上建立用于反应性亚稳碳酸盐/硅酸盐固体的形成和稳定的分子设计规则，以及用于在宏观尺度上实施这些规则的工艺设计（系统）策略。这将通过利用最先进的NMR光谱技术来实现，该技术最近才可用于碳酸盐和碳酸盐材料中的关键43 Ca，25 Mg，13 C，31 P和偶极耦合29 Si和1H物质。预期使用双膦酸酯/膦酸酯或其它有机分子来稳定反应性碳酸酯的新用途将促进它们的可加工性、储存稳定性和转化成有价值的结构材料。基于获得的分子见解，材料加工变量（例如，温度、压力、pH、组成和反应器/分离器配置）将被评估和优化，以控制具有工程结构、颗粒形态和表面组成的碳酸盐固体的沉淀和结晶，包括技术经济考虑。这项研究的更广泛影响包括（1）对研究生和本科生进行广泛的教育，了解结晶固体分子工程的最先进方法及其合成工艺设计策略，（2）培养对温室气体排放及其影响的广泛认识，二氧化碳利用的候选策略，以及相关的能源和环境影响，以及（3）开发一种范式改变方法的具体可能性，通过该方法将CO2转化为有价值的结构材料。从拟议的项目中获得的见解将是一般性的，使学生和更广泛的科学界开发新的方法，将废物转化为潜在的有价值的材料，沿着量化过程设计和经济因素，通过系统的方法来评估成本效益。