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Instruments / Technical Area	Publication Details	Published	Actions
B18-Core EXAFS	Largely pseudocapacitive two-dimensional conjugated metal–organic framework anodes with lowest unoccupied molecular orbital localized in nickel-bis(dithiolene) linkages Panpan Zhang , Mingchao Wang , Yannan Liu , Yubin Fu , Mingming Gao , Gang Wang , Faxing Wang , Zhiyong Wang , Guangbo Chen , Sheng Yang , Youwen Liu , Renhao Dong , Minghao Yu , Xing Lu , Xinliang Feng Journal Of The American Chemical Society 15 DOI: 10.1021/jacs.2c12684 Show Abstract ▼ Abstract: Although two-dimensional conjugated metal–organic frameworks (2D c-MOFs) provide an ideal platform for precise tailoring of capacitive electrode materials, high-capacitance 2D c-MOFs for non-aqueous supercapacitors remain to be further explored. Herein, we report a novel phthalocyanine-based nickel-bis(dithiolene) (NiS4)-linked 2D c-MOF (denoted as Ni2[CuPcS8]) with outstanding pseudocapacitive properties in 1 M TEABF4/acetonitrile. Each NiS4 linkage is disclosed to reversibly accommodate two electrons, conferring the Ni2[CuPcS8] electrode a two-step Faradic reaction with a record-high specific capacitance among the reported 2D c-MOFs in non-aqueous electrolytes (312 F g–1) and remarkable cycling stability (93.5% after 10,000 cycles). Multiple analyses unveil that the unique electron-storage capability of Ni2[CuPcS8] originates from its localized lowest unoccupied molecular orbital (LUMO) over the nickel-bis(dithiolene) linkage, which allows the efficient delocalization of the injected electrons throughout the conjugated linkage units without inducing apparent bonding stress. The Ni2[CuPcS8] anode is used to demonstrate an asymmetric supercapacitor device that delivers a high operating voltage of 2.3 V, a maximum energy density of 57.4 Wh kg–1, and ultralong stability over 5000 cycles.	Mar 2023
I07-Surface & interface diffraction	A two‐dimensional polyimide‐graphene heterostructure with ultra‐fast interlayer charge transfer Kejun Liu , Jiang Li , Haoyuan Qi , Mike Hambsch , Jonathan Rawle , Adrián Romaní Vázquez , Ali Shaygan Nia , Alexej Pashkin , Harald Schneider , Mirosllav Polozij , Thomas Heine , Manfred Helm , Stefan C. B. Mannsfeld , Ute Kaiser , Renhao Dong , Xinliang Feng Angewandte Chemie International Edition DOI: 10.1002/anie.202102984 Diamond Proposal Number(s): [25070] Open Access Show Abstract ▼ Abstract: Two‐dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic‐inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on‐water surface synthesis of large‐area (cm 2 ), monolayer 2D polyimide (2DPI) with 3.1‐nm lattice. Such 2DPI comprises metal‐free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI‐graphene (2DPI‐G) vdWHs via a face‐to‐face co‐assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra‐fast interlayer charge transfer (~60 fs) in the resultant 2DPI‐G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation‐π interaction between 2DP and graphene. Our work opens opportunities to develop 2DP‐based vdWHs via the on‐water surface synthesis strategy and highlights the unique interface‐induced optoelectronic properties.	Apr 2021

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