共轭聚酰亚胺修饰的自支撑碳电极用于将二氧化碳电化学转化为二氧化碳

Daming Feng, Zuo Li, Huifang Guo, Xiaodong Sun, Peng Huang, Ying Sun, Hui Li, Tianyi Ma
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摘要

电化学还原二氧化碳(CO2RR)为解决能源短缺和环境恶化的双重挑战提供了一种前景广阔的方法。本研究提出了一种新型、经济、可扩展的电催化剂:用多孔共轭聚酰亚胺修饰的自支撑碳纸。这种创新材料有助于在水介质中高效转化二氧化碳,无需热解步骤。这种电催化剂的设计采用了一种非金属有机聚合物,具有高密度的氮原子,可作为催化的活性位点。其独特的介孔微球结构由随机堆叠的纳米片组成,这些纳米片在原位生成,并沿着碳纸基底的碳纤维排列。这种结构既能增强二氧化碳吸附能力,又能在聚合物共轭结构的促进下确保适当的电子传输。此外,共轭聚酰亚胺固有的疏水性也有助于其在选择性还原 CO2 方面发挥强大的催化性能,以高达 88.7% 的法拉第效率和 82.0 mmol g-1 h-1 的产率生成 CO 作为主要气态产物。因此,所提出的电催化剂为非金属有机材料催化的电化学 CO2RR 提供了一种可持续的解决方案,兼具高效率和制备工艺简单、无需昂贵材料或步骤等优点。这项研究有助于推动 CO2RR 技术的发展,有可能带来更环保、更节能的解决方案。
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Conjugated polyimides modified self-supported carbon electrodes for electrochemical conversion of CO2 to CO
The electrochemical reduction of carbon dioxide (CO2RR) offers a promising approach to address the dual challenges of energy scarcity and environmental degradation. This study presents a new, cost-effective, and scalable electrocatalyst: self-supporting carbon paper modified with porous conjugated polyimides. This innovative material facilitates efficient CO2 conversion in aqueous media, eliminating the need for a pyrolysis step. The electrocatalyst’s design utilizes a non-metallic organic polymer with a high density of nitrogen atoms, serving as active sites for catalysis. Its unique mesoporous microsphere structure comprises randomly stacked nanosheets that are generated in situ and aligned along the carbon fibers of carbon paper substrate. This architecture enhances both CO2 adsorption and ensures proper electron transportation, facilitated by the conjugated structure of the polymer. Additionally, the inherent hydrophobicity of conjugated polyimides contributes to its robust catalytic performance in selectively reducing CO2, yielding CO as the primary gaseous product with up to 88.7% Faradaic efficiency and 82.0 mmol g-1 h-1 yield rate. Therefore, the proposed electrocatalyst provides a sustainable solution for electrochemical CO2RR catalyzed by non-metal organic materials, combining high efficiency with the advantages of a simple preparation process and the absence of costly materials or steps. This research contributes to the advancement of CO2RR technologies, potentially leading to more environmentally friendly and energy-efficient solutions.
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