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Harvesting renewable mechanical energy is envisioned as a promising and sustainable way for power generation. Many recent mechanical energy harvesters are able to produce instantaneous (pulsed) electricity with a high peak voltage of over 100 V. However, directly storing such irregular high-voltage pulse electricity remains a great challenge. The use of extra power management components can boost storage efficiency but increase system complexity. Here utilizing the conducting polymer PEDOT:PSS, high-rate metal-free micro-supercapacitor (MSC) arrays are successfully fabricated for direct high-efficiency storage of high-voltage pulse electricity. Within an area of 2.4 × 3.4 cm2 on various paper substrates, large-scale MSC arrays (comprising up to 100 cells) can be printed to deliver a working voltage window of 160 V at an ultrahigh scan rate up to 30 V s−1. The ultrahigh rate capability enables the MSC arrays to quickly capture and efficiently store the high-voltage (≈150 V) pulse electricity produced by a droplet-based electricity generator at a high efficiency of 62%, significantly higher than that (<2%) of the batteries or capacitors demonstrated in the literature. Moreover, the compact and metal-free features make these MSC arrays excellent candidates for sustainable high-performance energy storage in self-charging power systems., QC 20231122

Synchrotron radiation X-ray diffraction (XRD) with nanoscale beam size was used here for in situ and in operando study of micro-supercapacitors (MSC) with gel electrolyte and MXene Ti3C2Tx electrodes. The electrode structure was characterized as a function of applied voltage and distance from the gap separating electrodes using microscopic cells with cylindrical shape designed for transmission mode XRD. The devices with gel electrolytes based on H2SO4 (with H2O/PVA and DMSO/PVA) showed stable performance with no changes in MXene structure under voltage swaps between positive and negative values. Experiments with KI-based electrolytes demonstrated changes of MXene structure correlated with decrease of energy storage parameters under conditions of increased operation voltage starting from 0.8 V. The optimal performance of the MSCs was observed when the MXene structure remained unchanged upon switching the applied voltage polarity. The changes of inter-layer distance of MXene upon swap of applied voltage correlate with decrease of device performance and are undesirable for stable operation of MSC's. We also tested feasibility of X-ray fluorescence (XRF) for characterization of electrolyte ion migration in MSCs using 2D element mapping. Irreversible sorption of iodine by MXene was found using XRF mapping of charged electrodes using standard in-plane MSC device and KI electrolyte.

The rapid development of emerging electronics requires power sources with the advantages of lightweight, high efficiency, and portability. Considering the use of critical raw materials (such as Li, Co, etc.) and the increasing global concern of battery waste, self-charging power systems (SCPSs) integrating energy harvesting, power management, and energy storage devices have been envisioned as promising solutions to replace traditional batteries to avoid the use of toxic materials and the need of frequent recharging/replacement. Up to date, the reported SCPSs still hold the problem of large form factor, unscalable fabrication, noble materials, and material complexity. In our work, a highly stable and eco-friendly organic conductive ink based on poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) has been developed for monolithic fabrication on-paper SCPSs almost fully through a simple direct ink writing (DIW) process. The ink possesses multiple functions and enables to directly print almost all the key components in the SCPSs, including electrodes for triboelectric nanogenerators (TENGs, mechanical energy harvesters), electrodes for micro-supercapacitors (MSCs, energy storage devices), and interconnects, on the same paper substrate in a monolithic manner without the need for “post-integration”. The monolithic printing process exhibits excellent upscaling capability for manufacturing. In particular, the direct patterning merit of the DIW process offers great flexibility in optimizing the system performance through adjusting the cell number, electrode dimension, and thickness of the MSC arrays. By adjusting the cell numbers, the MSC arrays attain high-rate capability up to 50 V/s to match the pulsing electricity produced from the TENGs. For small-size printed SCPSs (~ 2 cm × 3 cm ×1 mm), after continuous press and release of the TENGs for ~79000 cycles, the 3-cell series-connected MSC array can be charged to 1.6 V while 6-cell array to 3.0 V. For a lar, Part of ISBN 9789189896925QC 20240719

Self-charging power systems (SCPSs) are envisioned as promising solutions for emerging electronics to mitigate the increasing global concern about battery waste. However, present SCPSs suffer from large form factors, unscalable fabrication, and material complexity. Herein, a type of highly stable, eco-friendly conductive inks based on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) are developed for direct ink writing of multiple components in the SCPSs, including electrodes for miniaturized spacer-free triboelectric nanogenerators (TENGs) and microsupercapacitors (MSCs), and interconnects. The principle of “one ink, multiple functions” enables to almost fully print the entire SCPSs on the same paper substrate in a monolithic manner without post-integration. The monolithic fabrication significantly improves the upscaling capability for manufacturing and reduces the form factor of the entire SCPSs (a small footprint area of ≈2 cm × 3 cm and thickness of ≈1 mm). After pressing/releasing the TENGs for ≈79000 cycles, the 3-cell series-connected MSC array can be charged to 1.6 V while the 6-cell array to 3.0 V. On-paper SCPSs are promising to serve as lightweight, thin, sustainable, and low-cost power supplies., QC 20240514

The raised demand for portable electronics in high-temperature environments (> 150 degrees C) stimulates the search for solutions to release the temperature constraints of power supply. All-solid-state microsupercapacitors (MSCs) are envisioned as promising on-chip power supply components, but at present, nearly none of them can work at temperature over 200 degrees C, mainly restricted by the electrolytes which possess either low thermal stability or incompatible fabrication process with on-chip integration. In this work, we have developed a novel process to fabricate highly thermally stable ionic liquid/ceramic composite electrolytes for on-chip integrated MSCs. Remarkably, the electrolytes enable MSCs with graphene-based electrodes to operate at temperatures as high as 250 degrees C with a high areal capacitance (similar to 72 mFcm(-2) at 5 mVs(-1)) and good cycling stability (70% capacitance retention after 1000 cycles at 1.4 mAcm(-2)).

The development of highly efficient robust electrocatalysts with low overpotential and industrial-level current density is of great significance for CO2 electroreduction (CO2ER), however the low proton transport rate during the CO2ER remains a challenge. Herein, a porous N-doped carbon nanofiber confined with tin-nitrogen sites (Sn/NCNFs) catalyst is developed, which is prepared through an integrated electrospinning and pyrolysis strategy. The optimized Sn/NCNFs catalyst exhibits an outstanding CO2ER activity with the maximum CO FE of 96.5%, low onset potential of −0.3 V, and small Tafel slope of 68.8 mV dec−1. In a flow cell, an industrial-level CO partial current density of 100.6 mA cm−2 is achieved. In situ spectroscopic analysis unveil the isolated Sn-N site acted as active center for accelerating water dissociation and subsequent proton transport process, thus promoting the formation of intermediate *COOH in the rate-determining step for CO2ER. Theoretical calculations validate pyrrolic N atom adjacent to the Sn-N active species assisted reducing the energy barrier for *COOH formation, thus boosting the CO2ER kinetics. A Zn-CO2 battery is designed with the cathode of Sn/NCNFs, which delivers a maximum power density of 1.38 mW cm−2 and long-term stability., QC 20230614

Harvesting ocean wave energy through carbon-based materials, particularly graphene, is receiving increasing attention. However, the complicated fabrication process and the low output power of the present monolayer graphene-based wave energy generators limit their further application. Here, we demonstrate the facile fabrication of a new type of wave energy generator based on graphene/TiO2 nanoparticle composite films using the doctor-blading method. The developed wave energy harvesting device exhibits a high open-circuit voltage of up to 75 millivolts and a high output power up to 1.8 microwatts. A systematic study was conducted to explore the optimal conditions for the energy harvesting performance., QC 20221222

Toward next-generation electroluminescent quantum dot (QD) displays, inkjet printing technique has been convinced as one of the most promising low-cost and large-scale manufacturing of patterned quantum dot light-emitting diodes (QLEDs). The development of high-quality and stable QD inks is a key step to push this technology toward practical applications. Herein, a universal ternary-solvent-ink strategy is proposed for the cesium lead halides (CsPbX3) perovskite QDs and their corresponding inkjet-printed QLEDs. With this tailor-made ternary halogen-free solvent (naphthene, n-tridecane, and n-nonane) recipe, a highly dispersive and stable CsPbX3 QD ink is obtained, which exhibits much better printability and film-forming ability than that of the binary solvent (naphthene and n-tridecane) system, leading to a much better qualitied perovskite QD thin film. Consequently, a record peak external quantum efficiency (EQE) of 8.54% and maximum luminance of 43 883.39 cd m−2 is achieved in inkjet-printed green perovskite QLEDs, which is much higher than that of the binary-solvent-system-based devices (EQE = 2.26%). Moreover, the ternary-solvent-system exhibits a universal applicability in the inkjet-printed red and blue perovskite QLEDs as well as cadmium (Cd)-based QLEDs. This work demonstrates a new strategy for tailor-making a general ternary-solvent-QD-ink system for efficient inkjet-printed QLEDs as well as the other solution-processed electronic devices in the future., QC 20221019

Covalent triazine frameworks (CTFs) are among the most valuable frameworks owing to many fantastic properties. However, molten salt-involved preparation of CTFs at 400–600 °C causes debate on whether CTFs represent organic frameworks or carbon. Herein, new CTFs based on the 1,3-dicyanoazulene monomer (CTF-Azs) are synthesized using molten ZnCl2 at 400–600 °C. Chemical structure analysis reveals that the CTF-Az prepared at low temperature (400 °C) exhibits polymeric features, whereas those prepared at high temperatures (600 °C) exhibit typical carbon features. Even after being treated at even higher temperatures, the CTF-Azs retain their rich porosity, but the polymeric features vanish. Although structural de-conformation is a widely accepted outcome in polymer-to-carbon rearrangement processes, the study evaluates such processes in the context of CTF systems. A proof-of-concept study is performed, observing that the as-synthesized CTF-Azs exhibit promising performance as cathodes for Li- and K-ion batteries. Moreover, the as-prepared NPCs exhibit excellent catalytic oxygen reduction reaction (ORR) performance; hence, they can be used as air cathodes in Zn-air batteries. This study not only provides new building blocks for novel CTFs with controllable polymer/carbon features but also offers insights into the formation and structure transformation history of CTFs during thermal treatment., QC 20230327