MOF-derived Co/Zn single-atom catalysts for reversible hydrogenation and dehydrogenation of quinoline hydrogen carrier

• Published in: Applied catalysis. B, Environmental Environmental, 2023-07, Vol.328, Article 122482
• Main Authors: Naveen, Kanagaraj, Mahvelati-Shamsabadi, Tahereh, Sharma, Pragyan, Lee, Seong-hun, Hur, Seung Hyun, Choi, Won Mook, Shin, Tae Joo, Chung, Jin Suk
• Format: Article
• Language: English
• Subjects: Liquid organic hydrogen carrier; Non-precious metal catalysts; Quinolines derivatives; Reversible hydrogenation/dehydrogenation; Single-atom catalysts
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2023.122482

Storage of hydrogen, particularly liquid organic hydrogen carrier (LOHC), has attracted much attention to address the problem of safe storage and transport of H2. N-heterocycles are promising hydrogen carriers for storing/releasing hydrogen through reversible catalytic hydrogenation/dehydrogenation cycles. Therefore, designing cost-effective, efficient, reusable single catalysts for both processes with high catalytic activity is currently of interest. Herein, we report the successful preparation of atomically dispersed Co/Zn single-atom catalysts on nitrogen-doped carbon by pyrolysis of bimetallic CoxZny-MOF-508@Melamine. The synthesized CoxZny-NC catalyst showed highly efficient catalytic activity for the reversible hydrogenation and dehydrogenation of quinoline derivatives in the same solvent. Catalytic reversible hydrogen storage/release was demonstrated for three consecutive cycles without losing efficiency. The main features of this work require low loading of catalysts compared to reported heterogeneous non-precious metal catalysts. A control experiment revealed that free N-H groups/N-atoms are essential for dehydrogenation/hydrogenation reactions, and a possible reaction mechanism was proposed. [Display omitted] •MOF-508 is a precursor to prepare Co/Zn single-atom catalysts for the first time.•Co/Zn-NC an efficient catalyst for hydrogenation/dehydrogenation of quinolines.•Low loading of catalyst used compared to reported non-noble metal catalysts.•No loss of catalytic activity observed for 3 cycles of hydrogen storage-release.•Solvent-free hydrogen storage-release of quinolines has been studied.