文献类型：期刊文献

英文题名：Delocalized-electron engineered 2D mesoporous COFs boosting interfacial desolvation toward low-temperature zinc metal batteries

作者：Duan, Yidan[1];Zhang, Yongzheng[2];Wang, Zhiyan[2];Liu, Yue[1];Han, Rui[1];Ma, Cheng[3];Bin, Duan[4];Lu, Hongbin[2];Qiao, Wenming[1];Wang, Jitong[1,5];Ling, Licheng[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[2]Nantong Univ, Sch Text & Clothing, Nantong 226019, Peoples R China;[3]East China Univ Sci & Technol, Minist Educ, Key Lab Specially Funct Polymer Mat & Related Tec, Shanghai 200237, Peoples R China;[4]Nantong Univ, Sch Chem & Chem Engn, Nantong 226019, Peoples R China;[5]Guangxi Univ, Univ Engn Res Ctr Green Chem New Mat, Sch Chem & Chem Engn, Nanning 530004, Guangxi, Peoples R China

年份：2026

卷号：537

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20261620537493);WOS:【SCI-EXPANDED(收录号:WOS:001751598800001)】；

基金：This work is financially supported by the National Natural Science Foundation of China (Nos.U21A2060, 22178116 and 52571082) and the Fundamental Research Funds for the Central Universities (No. JKD01251701) and the funded by Basic Research Program of Jiangsu Province (BK20251840) and Guangxi Science and Technology Program under grant (JF2503980007) .

语种：英文

外文关键词：Covalent organic frameworks; Delocalized electrons; Catalytic desolvation; Zinc metal batteries; Low-temperature performance

摘要：Aqueous zinc-metal batteries offer significant advantages in terms of safety and cost, yet they remain constrained by large desolvation energy barrier of the bulky [Zn(H2O)6]2+ solvation clusters, leading to issues such as dendrite growth and side reactions. To overcome these challenges, a two-dimensional ordered-mesoporous covalent organic framework with electron-delocalized characteristics (2D mCOF) is developed as an interfacial catalyst layer to inhibit undesirable parasitic reactions and modulate Zn2+ flux. Serving as an interfacial kinetic accelerator, the 2D mCOF promotes Zn2+ dissociation through the size-screening effect of their intrinsic microporous structure and the strong Zn2+ affinity of surface functional groups. Simultaneously, the mesoporous structure enables rapid Zn2+ transport under high current densities. The incorporation of electron-withdrawing cyano groups (-CN) within the framework further enhances local electron delocalization, boosting the electrocatalytic activity of the COF and accelerating desolvation kinetics, as supported by theoretical simulations, Raman spectroscopic analyses, and detailed electrochemical tests. Remarkably, under extreme low-temperature conditions, Zn symmetric cell with the 2D mCOF promoter demonstrates an exceptional long-term cycling stability, operating reliably for over 4500 h at 0.5 mA cm-2. Moreover, when assembled into a full cell, an impressive capacity retention of 97.1% is maintained after 4000 cycles at 20 A g-1, highlighting the strong potential of 2D mCOF for enabling high-performance low-temperature aqueous zinc-metal batteries.