复杂氧化物载氧体的调变策略及在过程强化中的应用

doi:10.11949/0438-1157.20211333

摘要/Abstract

摘要：

CO₂减排已经成为各国发展的重要议题之一。化工产业的传统分离过程由于?效率过低，往往会导致大量的能源浪费及CO₂排放。作为一种典型的、耦合分离与反应的过程强化策略，化学链技术有利于实现产物分离、能量梯级利用，从而显著提升系统?效率。高通量计算与化学链技术的结合，可以针对不同化学反应，指导相应的化学链载氧体热力学性质的调变策略。以化学链空气分离、氧化脱氢和热化学储能三个典型过程为例，简述化学链过程中复杂载氧体热力学性质的调变策略。热力学分析表明，不同化学链流程中载氧体性质的优化方向和最优区间均存在显著差异。因此，未来化学链技术发展的重要方向之一，是针对不同的化工流程进行载氧体的精确调变，从而实现化工流程的最优化。

关键词: 化学链, 复杂氧化物, 氧化还原, 钙钛矿, ?, 过程强化

Abstract:

Carbon dioxide emission reduction has become one of the important issues for the development of various countries. Conventional separation steps in chemical manufacturing usually come with a low second law efficiency, leading to large amounts of energy consumption as well as CO₂ emissions. By coupling separation with chemical reactions using an oxygen storage material, the chemical looping technology represents a promising approach to intensify chemical manufacturing via simplified product separation and cascade energy utilization. As a result, a significant increase in exergy efficiency can be realized. A combination of the chemical looping strategy and high throughput computation based on ab-initio materials simulation has the potential to rationalize the design of complex oxides for various applications. In this paper, three representative chemical looping processes, i.e., chemical looping air separation (CLAS), chemical looping oxidative dehydrogenation (CL-ODH), and chemical looping thermochemical energy storage (CL-TES), are used to exemplify the strategy to tailor the thermodynamic properties of complex oxides. Thermodynamic analysis showed that the desired thermodynamic properties for the oxides vary considerably depending on the target application. Therefore, a key direction for the development of the chemical looping strategy is application-specific and precision-engineering of complex oxides to push the existing boundaries for process efficiency and emission reduction.

Key words: chemical looping, complex oxides, redox, perovskites, exergy, process intensification

中图分类号:

TQ 511

蔡润夏, 李凡星. 复杂氧化物载氧体的调变策略及在过程强化中的应用[J]. 化工学报, 2021, 72(12): 6122-6130.

Runxia CAI, Fanxing LI. Tailoring the thermodynamic properties of complex oxides for thermochemical air separation and beyond[J]. CIESC Journal, 2021, 72(12): 6122-6130.

图/表 3

图1 化学链反应系统与载氧体热力学性质的计算预测示意图(右上图引自文献[35])

Fig.1 Schematics of a chemical looping reaction system and computationally predicted redox properties of complex oxides (the upper right figure was cited from Ref.[35])

图2 针对不同化学链流程，载氧体热力学性质合适的分布区间:（a）全局视图；（b）低熵、低焓区域放大视图（部分数据点引自文献[5,45,48-51],Ca2MnAlO5数据源于本课题组正在进行的实验工作）

Fig.2 Desired thermodynamic properties of complex oxides for different chemical looping process: (a) Overview; (b) Callout view of the low entropy and enthalpy region (Some data points were cited from Refs.[5,45,48-51], data for Ca2MnAlO5 were collected from an on-going experimental study in the authors’ research group)

图3 DFT 指导和优化CLAS流程中SrxA1-xFeyB1-yO3-δ载氧体性质：(a)载氧体ΔEv和Δe存在线性关系；(b)实验测得700°C、1%~20%氧分压变压运行得到的氧容量与ΔEv和Δe有很强的关联性;（c）氧气传递能垒也与Δe相关[32]

Fig.3 DFT was used for the design and optimization of SrxA1-xFeyB1-yO3-δoxygen sorbents in the CLAS process: (a) Linear relationship between ΔEv and Δe was observed; (b) Experimental oxygen capacity at 700 °C within 1%-20% PO2 swing as functions of ΔEv and Δe; (c) Oxygen migration barrier as a function of Δe per O atom[32]

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