固态电解质反应器驱动的大气环境CO2捕集与电催化转化
收稿日期: 2025-04-04
修回日期: 2025-05-05
录用日期: 2025-05-13
网络出版日期: 2025-05-13
Ambient CO2 Capture and Valorization Enabled by Tandem Electrolysis Using Solid-State Electrolyte Reactor
Received date: 2025-04-04
Revised date: 2025-05-05
Accepted date: 2025-05-13
Online published: 2025-05-13
电催化二氧化碳还原是一种有望解决全球能源和环境危机的变革性技术。然而，其实际应用面临着两大关键挑战：一是分离混合还原产物的过程复杂且能耗高，二是所使用碳源（反应物）的经济可行性。为了同时解决这些挑战，固态电解质（SSE）反应器的研究正在受到日益广泛的关注。在这篇综述中，我们着眼于探讨将SSE应用于电化学CO2捕获和转化串联系统的可行性。我们首先讨论了SSE反应器的结构和基本原理，随后介绍了其在上述两个领域及串联电解的应用实例。与传统的H型电解池、流动池及膜电极电解池相比，SSE的关键创新在于阴离子交换膜和阳离子交换膜之间部署的SSE层，它实现了高效的离子传输，且可通过去离子水或湿润的氮气流有效地分离离子传导和产物收集功能。目标产物可以在SSE中间层通过两极离子复合形成，并通过多孔的SSE层被流动介质高效地带走，产生纯净的液相产物。由于CO2还原反应可以生成一系列液体产物，过去几年中先进催化剂的开发也进一步推动了SSE反应器在高效化学品生产中的实践应用。值得注意的是，由于阴极还原反应常常消耗水中的质子并导致局部高碱性环境，SSE可应用于从不同气源（如烟道气）中捕获酸性CO2以形成碳酸根离子。在电场的驱动下，形成的CO32-可以通过阴离子交换膜，并被阳极半反应产生的质子所酸化，实现高浓度CO2的再生，进而被收集作为下游CO2电还原的低成本原料。基于这一原理，近年来已有多种SSE构型的反应器被报道用于高效捕获不同气源的CO2。通过两个SSE单元的协同作用，已经实现了串联电化学CO2捕获和电催化转化。最后，我们对SSE在未来面向碳中和领域的应用中提出了展望，并建议更多关注以下具体方面的优化：SSE层的基本物理化学性质、电化学工程视角下离子和物种通量及选择性，以及连续CO2捕获和转化单元之间的系统性匹配。这些努力旨在进一步推动固态电解质反应器在更广泛的电化学领域中的应用示范。
华炎波 , 倪宝鑫 , 蒋昆 . 固态电解质反应器驱动的大气环境CO2捕集与电催化转化[J]. 电化学, 2025 , 31(6) : 2504082 . DOI: 10.61558/2993-074X.3547
Electrocatalytic carbon dioxide reduction is a promising technology for addressing global energy and environmental crises. However, its practical application faces two critical challenges: the complex and energy-intensive process of separating mixed reduction products and the economic viability of the carbon sources (reactants) used. To tackle these challenges simultaneously, solid-state electrolyte (SSE) reactors are emerging as a promising solution. In this review, we focus on the feasibility of applying SSE for tandem electrochemical CO2 capture and conversion. The configurations and fundamental principles of SSE reactors are first discussed, followed by an introduction to its applications in these two specific areas, along with case studies on the implementation of tandem electrolysis. In comparison to conventional H-type cell, flow cell and membrane electrode assembly cell reactors, SSE reactors incorporate gas diffusion electrodes and utilize a solid electrolyte layer positioned between an anion exchange membrane (AEM) and a cation exchange membrane (CEM). A key innovation of this design is the sandwiched SSE layer, which enhances efficient ion transport and facilitates continuous product extraction through a stream of deionized water or humidified nitrogen, effectively separating ion conduction from product collection. During electrolysis, driven by an electric field and concentration gradient, electrochemically generated ions (e.g., HCOO- and CH3COO-) migrate through the AEM into the SSE layer, while protons produced from water oxidation at the anode traverse the CEM into the central chamber to maintain charge balance. Targeted products like HCOOH can form in the middle layer through ionic recombination and are efficiently carried away by the flowing medium through the porous SSE layer, in the absence of electrolyte salt impurities. As CO2RR can generate a series of liquid products, advancements in catalyst discovery over the past several years have facilitated the industrial application of SSE for more efficient chemicals production. Also noteworthy, the cathode reduction reaction can readily consume protons from water, creating a highly alkaline local environment. SSE reactors are thereby employed to capture acidic CO2, forming CO32- from various gas sources including flue gases. Driven by the electric field, the formed CO32- can traverse through the AEM and react with protons originating from the anode, thereby regenerating CO2. This CO2 can then be collected and utilized as a low-cost feedstock for downstream CO2 electrolysis. Based on this principle, several cell configurations have been proposed to enhance CO2 capture from diverse gas sources. Through the collaboration of two SSE units, tandem electrochemical CO2 capture and conversion has been successfully implemented. Finally, we offer insights into the future development of SSE reactors for practical applications aimed at achieving carbon neutrality. We recommend that greater attention be focused on specific aspects, including the fundamental physicochemical properties of the SSE layer, the electrochemical engineering perspective related to ion and species fluxes and selectivity, and the systematic pairing of consecutive CO2 capture and conversion units. These efforts aim to further enhance the practical application of SSE reactors within the broader electrochemistry community.
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