Ammonium ions (NH4+) are emerging non‐metallic charge carriers for advanced electrochemical energy storage devices, due to their low cost, elemental abundance, and environmental benignity. However, finding suitable electrode materials to achieve rapid diffusion kinetics for NH4+ storage remains a great challenge. Herein, a 2D conjugated metal–organic framework (2D c‐MOF) for immobilizing iodine, as a high‐performance cathode material for NH4+ hybrid supercapacitors, is reported. Cu‐HHB (HHB = hexahydroxybenzene) MOF embedded with iodine (Cu‐HHB/I2) features excellent electrical conductivity, highly porous structure, and rich accessible active sites of copper‐bis(dihydroxy) (Cu─O4) and iodide species, resulting in a remarkable areal capacitance of 111.7 mF cm−2 at 0.4 mA cm−2. Experimental results and theoretical calculations indicate that the Cu─O4 species in Cu‐HHB play a critical role in binding polyiodide and suppressing its dissolution, as well as contributing to a large pseudocapacitance with adsorbed iodide. In combination with a porous MXene anode, the full NH4+ hybrid supercapacitors deliver an excellent energy density of 31.5 mWh cm−2 and long‐term cycling stability with 89.5% capacitance retention after 10 000 cycles, superior to those of the state‐of‐the‐art NH4+ hybrid supercapacitors. This study sheds light on the material design for NH4+ storage, enabling the development of novel high‐performance energy storage devices.
The rapid growth of sensor data in the artificial intelligence often causes significant reductions in processing speed and power efficiency. Addressing this challenge, in‐sensor computing is introduced as an advanced sensor architecture that simultaneously senses, memorizes, and processes images at the sensor level. However, this is rarely reported for organic semiconductors that possess inherent flexibility and tunable bandgap. Herein, an organic heterostructure that exhibits a robust photoresponse to near‐infrared (NIR) light is introduced, making it ideal for in‐sensor computing applications. This heterostructure, consisting of partially overlapping p‐type and n‐type organic thin films, is compatible with conventional photolithography techniques, allowing for high integration density of up to 520 devices cm−2 with a 5 µm channel length. Importantly, by modulating gate voltage, both positive and negative photoresponses to NIR light (1050 nm) are attained, which establishes a linear correlation between responsivity and gate voltage and consequently enables real‐time matrix multiplication within the sensor. As a result, this organic heterostructure facilitates efficient and precise NIR in‐sensor computing, including image processing and nondestructive reading and classification, achieving a recognition accuracy of 97.06%. This work serves as a foundation for the development of reconfigurable and multifunctional NIR neuromorphic vision systems.
17 February 2021 in ACS Sustainable Chemistry & Engineering
In this work, a triangle arrayed triple-screw extruder (TTSE) was used to prepare in situ polypropylene/polyamide 6,6 (PP/PA66) microfibrillar composites (MFCs) by direct extrusion at a processing temperature between the melting points of the two phases. The dispersed phase, PA66 particles, deformed, merged and was stretched into fibrils under the alternating shearing and extensional flow field in the TTSE. The fibrillar morphology was controlled through adjusting the PA66 content and processing parameters (temperature and screw speed). Dynamic oscillatory shear rheological properties and extensional viscosity of PP/PA66 microfibrils with different aspect ratio were studied. The obtained results showed that the storage modulus and complex viscosity of PP/PA66 MFCs were improved with increasing fibrillar aspect ratio. Meanwhile, the loss tangent tan δ value decreased and the radius of the Cole–Cole plot circle increased with an increase in fibrillar aspect ratio. The PP/PA66 MFCs exhibited a pseudo-solid or gel-like behavior. The gel point concentration, which was determined by the Winter–Chambon criterion, decreased with the increasing fibrillar aspect ratio due to the increased interfacial area and enhanced entangled network structure. Additionally, high-aspect-ratio PA66 fibrils have dramatically improved PP's melting temperature, crystallization kinetics, and mechanical properties.
The sodiation/de-sodiation mechanism of metallic NbSe2 anodes is corrected to involve an initial irreversible conversion from NbSe2 to Na2Se/Nb composites and the subsequent reversible selenide conversion reaction.