The merits of intrinsic electrical conductivity, high specific surface area, tunable chemical composition and tailor-made properties enable two-dimensional conductive metal-organic frameworks (2D c-MOFs) as promising ...The merits of intrinsic electrical conductivity, high specific surface area, tunable chemical composition and tailor-made properties enable two-dimensional conductive metal-organic frameworks (2D c-MOFs) as promising next-generation electrode materials in the field of energy storage and conversion. Herein, we have designed and synthesized a novel pyrazine-based 2D c-MOF (TPQG-Cu-MOF) bearing extended π-conjugated structure and abundant redox active sites. Thanks to the excellent redox reversibility of pyrazine units and CuO2 units, as well as the insolubility of the rigid framework skeleton, TPQG-Cu-MOF as the cathode material of lithium-ion battery exhibits a reversible specific capacity (150.2 mAh·g–1 at 20 mAh·g–1), good cycling stability (capacity retention of 82.6% after 500 cycles at 1 A·g–1) and excellent rate performance. Comprehensive ex-situ spectroscopic studies revealed the reversible redox activity of pyrazine units and CuO2 units of TPQG-Cu-MOF during the Li+ insertion/extraction process. The deepening fundamental understanding of the structure-property relationship was proposed, which might pave the way for further development of efficient MOF-based energy storage devices.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.51973153,22105144).
文摘The merits of intrinsic electrical conductivity, high specific surface area, tunable chemical composition and tailor-made properties enable two-dimensional conductive metal-organic frameworks (2D c-MOFs) as promising next-generation electrode materials in the field of energy storage and conversion. Herein, we have designed and synthesized a novel pyrazine-based 2D c-MOF (TPQG-Cu-MOF) bearing extended π-conjugated structure and abundant redox active sites. Thanks to the excellent redox reversibility of pyrazine units and CuO2 units, as well as the insolubility of the rigid framework skeleton, TPQG-Cu-MOF as the cathode material of lithium-ion battery exhibits a reversible specific capacity (150.2 mAh·g–1 at 20 mAh·g–1), good cycling stability (capacity retention of 82.6% after 500 cycles at 1 A·g–1) and excellent rate performance. Comprehensive ex-situ spectroscopic studies revealed the reversible redox activity of pyrazine units and CuO2 units of TPQG-Cu-MOF during the Li+ insertion/extraction process. The deepening fundamental understanding of the structure-property relationship was proposed, which might pave the way for further development of efficient MOF-based energy storage devices.