热-电共驱胺捕集CO2的流动传热传质机理及其小温差循环能量耗散特性

Substantial amount of CO2 emission from industry produces great pressure on emission mitigation in society. Amine absorption method with effective mass transfer is suitable for mitigating industrial CO2 emission, which however consumes much energy. By employing amine, cell method captures CO2 with low energy consumption, which however shows low desorption efficiency. Considering the simultaneous utilizations of amines and complementary traits of the energy and desorption efficiency in two processes, this proposal is to develop a novel amine capture CO2 process co-driven by heat and cell (cell method). This novel process aims to reduce the temperature difference during absorption and desorption cycles and simultaneously utilize reaction heat and cell energy, which finally achieves the highly efficient CO2 mitigation with low energy consumption. Based on the theoretical and experimental analysis of the novel process, this work will study coupled mechanisms between fluid flow, thermodynamic and cell effects, which also identifies interactive effects of flow pattern formation and transformation, liquid film break-up, interface characteristic and heat and mass transfer influenced by these coupled mechanisms. This work will determine the key parameters (cell structure and operating conditions) of influencing the process performance and develop multi-parameters and non-linear fluid flow and heat and mass transfer model. According to the model, phenomenological theory is extended to study the energy dissipation characteristic of small temperature difference during CO2 absorption and desorption cycles. Strategies of adjusting cycle temperature differences are obtained by optimizing fluid flow and heat and mass transfer with operating conditions (pressure and column structure, etc.) and cell structure (electrode geometry and surface area, etc.), which finally offers theoretical guide for efficient CO2 capture with low energy consumption.

工业大量排放CO2产生了巨大的社会减排压力。高效传质的胺吸收法虽然适合工业减排CO2，但能耗较高；胺的电池法捕集CO2能耗低，但CO2解吸效率亦低。基于两种方法均采用胺，且能量和解吸效率互补的特点，本申请提出热-电（电池）共驱胺捕集CO2新过程，其目的是降低吸收和解吸CO2循环温差，高效利用反应热和电池能，实现高效低能耗减排CO2的目标。在该过程的理论和实验分析基础上，本申请重点研究流动、热力和电池作用的耦合规律，揭示其对流型形成及其转换、液膜破碎、界面特性和传热传质机制的影响规律，确定影响该过程性能的关键参数（电池结构和工况条件），建立该过程多参数非线性流动传热传质模型。从该模型出发，拓展唯象理论，探索该过程吸收和解吸CO2的小温差循环能量耗散特性，获得以工况条件（压力、塔结构等）和电池结构（电极形状和表面积等）优化流动传热传质的调控循环温差的策略，为实现高效低能耗捕集CO2提供理论指导。

为了解决减排工业二氧化碳（CO2）高能耗问题，项目提出了热力学和电化学耦合驱动CO2捕集的思路，解决了传统胺法捕集CO2工业应用的瓶颈问题，对于控制温室效应具有重要意义。..项目开发了热-电共驱胺捕集CO2、热-电共驱产氢耦合CO2捕集过程。针对这些过程，搭建了热-电共驱胺捕集CO2过程的实验系统，开展了这些过程的反应动力学分析，建立了这些过程的传热传质模型和密度泛函理论模型，完成了数值计算分析，研究了反应传热传质机理。同时，针对能量耗散分析，基于改进的场协同模型（唯象理论），开发了介尺度、高阶多场协同和动态全场协同等方法，并成功应用于胺法捕集CO2多离子系统、煤浮选耦合CO2捕集和煤粉炉掺烧废水等过程中。..研究过程中获得的热-电共驱胺捕集CO2的循环伏安特性、CO2浓度分布、气液两相流场、温度场和电势分布规律、动量/能量传递机制、二次产氢和二次氢放的基本产氢反应机制、多离子体系流动传热传质机理、介尺度过程强化方法和掺烧的动态全场特性等科学本质，为指导工业生产实际提供了强有力的理论支撑，具有重要的科学价值。.项目实现了343K-373K温度范围解吸CO2，将胺法捕集CO2的能耗从传统3.5GJ/t左右降低至了1.3GJ/t，热-电共驱产氢耦合CO2捕集能耗可降低至1GJ/t，大幅降低了胺法捕集CO2成本，为CO2捕集的高效工业应用提供了新的技术支撑。开发的能量耗散分析方法解决了220t/h煤粉炉掺烧废水的动态特性分析的工业实际问题，具有重要的工程应用价值。.项目发表了SCI论文13篇，其中第一作者和通讯作者8篇，影响因子大于5的SCI论文4篇，获批国家发明专利1件，申请国家发明专利1件，培养毕业硕士研究生2名（即将毕业1名），出版英文专著1章。此外，参加国内外会议6次，并邀请英国、澳大利亚的国外专家来访交流2次，参与教育部教改项目1项。