This paper presents the first implementation of electrically conductive metal–organic framework (MOF) Ni₃(2,3,6,7,10,11-hexaiminotriphenylene)₂ (Ni₃(HITP)₂) integrated with nickel bis(diimine) (Ni-BDI) units for efficient solid-state electrochemical carbon dioxide (CO₂) capture. The electrochemical cell assembled using Ni₃(HITP)₂ as working electrodes can reversibly capture and release CO₂ through potential control. A high-capacity utilization of 96% and a Faraday efficiency of 98% have been achieved. The material also exhibits excellent electrochemical stability with its capacity maintained during 50 capture–release cycles and resistance to general interferences, including O₂, H₂O, NO₂, and SO₂. Capacity utilization of up to 35% is obtained at CO₂ concentrations as low as 1%. The capture of CO₂ at concentrations ranging from 1% to 100% requires exceptionally low energy consumption of only 30.5–72.4 kJ mol^–1. Studies combining spectroscopic experiments and computational approaches reveal that the CO₂ capture and release mechanism involves reversible carbamate formation on the N atom of the Ni-BDI unit in the MOF upon its one-electron redox reaction.

中文翻译：

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通过包含镍双（二亚胺）单元的导电金属-有机框架进行固态电化学二氧化碳捕获


本文首次实现了导电金属有机框架 （MOF） Ni₃（2,3,6,7,10,11-己氨基三苯乙烯）₂ （Ni₃（HITP）₂） 与镍双（二亚胺） （Ni-BDI） 单元集成，用于高效的固态电化学二氧化碳 （CO₂） 捕获。使用 Ni₃（HITP）₂ 作为工作电极组装的电化学电池可以通过电位控制可逆地捕获和释放 CO₂。实现了 96% 的高容量利用率和 98% 的法拉第效率。该材料还表现出优异的电化学稳定性，其容量可在 50 次捕获-释放循环中保持，并且耐一般干扰，包括 O₂、H₂O、NO₂ 和 SO₂。当_CO2 浓度低至 1% 时，产能利用率高达 35%。捕获浓度为 1% 至 100% 的 CO₂ 所需的能耗极低，仅为 30.5–72.4 kJ mol^–1。结合光谱实验和计算方法的研究表明，CO₂ 捕获和释放机制涉及 MOF 中 Ni-BDI 单元的 N 原子在其单电子氧化还原反应中形成可逆的氨基甲酸酯。