Capacitive deionization using carbon derived from an array of zeolitic-imidazolate frameworks

Abstract

Abstract Capacitive deionization (CDI) represents one of the most thermodynamically efficient technologies for brackish water desalination. Its performance is highly reliant on the surface properties of carbon-based electrodes. Zeolitic-imidazolate framework (ZIF)-derived carbon materials have emerged among the most promising candidates owing to their high structural and compositional tuneability. However, the impacts of the precursory ZIF structure on the properties of the final carbon, and therefore, CDI capacity and efficiency remain to be further explored. In this work, four Zn-based ZIFs with different side-chain substitutions on the imidazolates were synthesized on a gram scale with high yields to produce N-doped carbons by pyrolysis. The resulting carbons along with four commercial carbon blacks were characterized physically and electrochemically to explore the structure-performance relationship. We demonstrated that the imidazole side-chain substitution alters the ZIF's decomposition during pyrolysis, influencing the elemental compositions, surface properties, wettability and graphitization levels. The diverse carbon properties result in variable double layer capacitance and charge-transfer resistance, ultimately impacting the CDI performance. Among these carbons, Zn (4abIm)2-C afforded the greatest salt adsorption capacity of 14.19 mgNaCl·gC−1, while Zn (mIm)2-C showed the highest overall salt adsorption capacity and rate; both exceeded the performance of the commercial carbon blacks.