Wang Yanzhi, He Hangjuan, Lv Hao, Jia Fengrui, Liu Ben
Key Laboratory of Green Chemistry and Technology of Ministry of Education, College of Chemistry, Sichuan University, 610064, Chengdu, China.
School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, 200240, Shanghai, China.
Nat Commun. 2024 Aug 8;15(1):6761. doi: 10.1038/s41467-024-50721-2.
Mesoporous single crystals have received more attention than ever in catalysis-related applications due to their unique structural functions. Despite great efforts, their progress in engineering crystallinity and composition has been remarkably slower than expected. In this manuscript, a template-free strategy is developed to prepare two-dimensional high-entropy oxide (HEO) nanoplates with single-crystallinity and penetrated mesoporosity, which further ensures precise control over high-entropy compositions and crystalline phases. Single-crystalline mesoporous HEOs (SC-MHEOs) disclose high electrocatalytic performance in 5-hydroxymethylfurfural oxidation reaction (HMFOR) for efficient biomass upgrading, with remarkable HMF conversion of 99.3% and superior 2,5-furandicarboxylic acid (FDCA) selectivity of 97.7%. Moreover, with nitrate reduction as coupling cathode reaction, SC-MHEO realizes concurrent electrosynthesis of value-added FDCA and ammonia in the two-electrode cell. Our study provides a powerful paradigm for producing a library of novel mesoporous single crystals for important catalysis-related applications, especially in the two-electrode cell.
介孔单晶因其独特的结构功能，在催化相关应用中受到了前所未有的关注。尽管付出了巨大努力，但其在结晶度和组成工程方面的进展明显比预期要慢。在本论文中，我们开发了一种无模板策略，用于制备具有单晶性和贯穿介孔的二维高熵氧化物（HEO）纳米片，这进一步确保了对高熵组成和晶相的精确控制。单晶介孔HEO（SC-MHEO）在5-羟甲基糠醛氧化反应（HMFOR）中展现出高效生物质升级的高电催化性能，HMF转化率高达99.3%，2,5-呋喃二甲酸（FDCA）选择性高达97.7%。此外，以硝酸盐还原作为耦合阴极反应，SC-MHEO在两电极电池中实现了增值FDCA和氨的同时电合成。我们的研究为制备用于重要催化相关应用的新型介孔单晶库提供了一个有力的范例，特别是在两电极电池中。
