Kuang Tairong, Deng Linbing, Liu Mingjin, Ding Yutong, Guo Wei, Cai Zhao, Liu Wenxian, Huang Zhao-Xia
Functional Polymers & Advanced Materials (FPAM) Lab, State Key Laboratory of Advanced Separation Membrane Materials, College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, 310014, China.
National Engineering Research Center of Novel Equipment for Polymer Processing, Key Laboratory of Polymer Processing Engineering, Ministry of Education, Guangdong Provincial Key Laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing, Department of Mechanical and Automotive Engineering, South China University of Technology, Guangzhou, 510641, China.
Adv Mater. 2025 May;37(20):e2415616. doi: 10.1002/adma.202415616. Epub 2025 Mar 31.
Metal-organic frameworks (MOFs) are highly versatile materials with tunable chemical and structural properties, making them promising for triboelectric nanogenerators (TENGs) and electrocatalysis. However, achieving precise control over MOF coordination structures to optimize facet-dependent properties remains challenging. Here, a facile and scalable dual-solvent synthesis strategy is presented to fabricate dendrite Co-2-methylimidazole MOF (ZIF-67-D), enabling tailored preferred facet and coordination environments. Using density functional theory (DFT) calculations and synchrotron-based X-ray absorption spectroscopy, it is demonstrated that ZIF-67-D, enriched with (112) facets, features a reduced Co coordination number and enhanced electron-donating ability compared to the conventionally (011) facet-dominated rhombic dodecahedron ZIF-67 (ZIF-67-R). This facet engineering boosts TENG charge density by 2.4-fold, OER current density by 9.9-fold (@1.65 V), and HER current density by 1.9-fold (@-0.3 V). The (112)/(011) facet ratio can be also tuned to precisely alter TENG output. Moreover, the optimized ZIF-67-D shows excellent stability, maintaining electrolyzer performance for 72 h and enabling TENG devices even in high humidity. Consequently, ZIF-67-D-based TENG (D-TENG) devices exhibit robust energy generation and power ZIF-67-D||ZIF-67-D electrolyzers for continuous hydrogen (H) production. These findings introduce a new paradigm for converting mechanical energy into sustainable chemical energy, offering insights into facet engineering for high-performance energy harvesting systems.
金属有机框架材料（MOFs）是具有可调化学和结构性质的高度通用的材料，使其在摩擦电纳米发电机（TENGs）和电催化方面具有广阔前景。然而，实现对MOF配位结构的精确控制以优化面依赖性质仍然具有挑战性。在此，提出了一种简便且可扩展的双溶剂合成策略来制备树枝状Co-2-甲基咪唑MOF（ZIF-67-D），从而实现定制的择优面和配位环境。使用密度泛函理论（DFT）计算和基于同步加速器的X射线吸收光谱表明，与传统的以（011）面为主的菱形十二面体ZIF-67（ZIF-67-R）相比，富含（112）面的ZIF-67-D具有降低的Co配位数和增强的给电子能力。这种面工程使TENG电荷密度提高了2.4倍，OER电流密度提高了9.9倍（@1.65 V），HER电流密度提高了1.9倍（@ -0.3 V）。（112）/（011）面比率也可以调节以精确改变TENG输出。此外，优化后的ZIF-67-D表现出优异的稳定性，在72小时内保持电解槽性能，甚至在高湿度环境下也能使TENG器件正常工作。因此，基于ZIF-67-D的TENG（D-TENG）器件展现出强大的能量产生能力，并为ZIF-67-D||ZIF-67-D电解槽提供动力以实现连续制氢（H）。这些发现引入了一种将机械能转化为可持续化学能的新范例，为高性能能量收集系统的面工程提供了见解。
