Dimension Evolution of Self-Assembled Organic Microcrystal for Laser and Polarization-Rotation Function.

Multidimensional integrated micro/nanostructures are vitally important for the implementation of versatile photonic functionalities, whereas current material structures still suffer undesired surface defects and contaminations in either multistep micro/nanofabrications or extreme synthetic conditions. Herein, the dimension evolution of organic self-assembled structures 2D microrings and 3D microhelixes for multidimensional photonic devices is realized via a protic/aprotic solvent-directed molecular assembly method based on a multiaxial confined-assisted growth mechanism. The 2D microrings with consummate circle boundaries and molecular-smooth surfaces function as high-quality whispering-gallery-mode microcavities for dual-wavelength energy-influence-dependent switchable lasing. Moreover, the 3D microhelixes with smooth surfaces and natural twistable characteristics act as active photon-transport materials and polarization rotators. These results will broaden the horizon of constructing multidimensional microstructures for integrated photonic circuits.

Multiple physical crosslinked highly adhesive and conductive hydrogels for human motion and electrophysiological signal monitoring.

Hydrogel-based flexible electronic devices serve as a next-generation bridge for human-machine interaction and find extensive applications in clinical therapy, military equipment, and wearable devices. However, the mechanical mismatch between hydrogels and human tissues, coupled with the failure of conformal interfaces, hinders the transmission of information between living organisms and flexible devices, which resulted in the instability and low fidelity of signals, especially in the acquisition of electromyographic (EMG) and electrocardiographic (ECG) signals. In this study, we designed an ion-conductive hydrogel (ICHgel) utilizing multiple physical interactions, successfully applied for human motion monitoring and the collection of epidermal physiological signals. By incorporating fumed silica (F-SiO2) nanoparticles and calcium chloride into an interpenetrating network (IPN) composed of polyvinyl alcohol (PVA) and polyacrylamide (AAm)/acrylic acid (AA) chains, the ICHgel exhibited exceptional tunable stretchability (>1450% strain) and conductivity (10.58 ± 0.85 S m-1). Additionally, the outstanding adhesion of the ICHgel proved to be a critical factor for effective communication between epidermal tissues and flexible devices. Demonstrating its capability to acquire stable electromechanical signals, the ICHgel was attached to different parts of the human body. More importantly, as a flexible electrode, the ICHgel outperformed commercial Ag/AgCl electrodes in the collection of ECG and EMG signals. In summary, the synthesized ICHgel with its outstanding conformal interface capabilities and mechanical adaptability paves the way for enhanced human-machine interaction, fostering the development of flexible electronic devices.

Dense-Packed RuO2 Nanorods with In Situ Generated Metal Vacancies Loaded on SnO2 Nanocubes for Proton Exchange Membrane Water Electrolyzer with Ultra-Low Noble Metal Loading.

Proton exchange membrane water electrolyzer (PEMWE) is a green hydrogen production technology that can be coupled with intermittent power sources such as wind and photoelectric power. To achieve cost-effective operations, low noble metal loading on the anode catalyst layer is desired. In this study, a catalyst with RuO2 nanorods coated outside SnO2 nanocubes is designed, which forms continuous networks and provides high conductivity. This allows for the reduction of Ru contents in catalysts. Furthermore, the structure evolutions on the RuO2 surface are carefully investigated. The etched RuO2 surfaces are seen as the consequence of Co leaching, and theoretical calculations demonstrate that it is more effective in driving oxygen evolution. For electrochemical tests, the catalysts with 23 wt% Ru exhibit an overpotential of 178 mV at 10 mA cm-2 , which is much higher than most state-of-art oxygen evolution catalysts. In a practical PEMWE, the noble metal Ru loading on the anode side is only 0.3 mg cm-2 . The cell achieves 1.61 V at 1 A cm-2 and proper stability at 500 mA cm-2 , demonstrating the effectiveness of the designed catalyst.

Surface oxidation of commercial activated carbon with enriching carboxyl groups for high-yield electrocatalytic H2O2production.

Two-electron oxygen reduction reaction (2e-ORR) for H2O2production is regarded as a more ecologically friendly substitute to the anthraquinone method. However, the search of selective and cheap catalysts is still challenging. Herein, we developed a neutral-selective and efficient nonprecious electrocatalyst that was prepared from a commercial activated carbon (AC) by simply microwave-assisted ash impurity elimination and hydrogen peroxide oxidation for surface functional sites optimization. The oxygen configuration can be tuned with enriching carboxyl group up to 6.65 at.% by the dosage of hydrogen peroxide (mass ratio of H2O2/C = ∼0-8.3). Chemical titration experiments identified the carbonyl groups as the most potential active sites, with selectivity boosted by the additional carboxyl groups. The microwave-assisted moderate-oxidized activated carbon (MW-AC5.0) demonstrated optimal 2e-ORR activity and selectivity in neutral electrolyte (0.1 M K2SO4), with H2O2selectivity reaching ∼75%-97%, a maximum H2O2production rate (1.90 mol·gcatal-1·h-1@0.1 V) and satisfying faradaic efficiency (∼85%) in gas-diffusion-electrode. When coupled with Fenton reaction, it can degrade a model organic pollutant (methylene blue [MB], 50 ppm) to colorless in a short time of 20 min, indicating the potential applications in the environmental remediation.

Mn-N-C catalysts derived from metal triazole framework with hierarchical porosity for efficient oxygen reduction.

Manganese and nitrogen co-doped porous carbon (Mn-N-C) are proposed as one of the most up-and-coming non-precious metal electrocatalysts to substitute Pt-based in the oxygen reduction reaction (ORR). Herein, we chose metal triazole frameworks as carbon substrate with hierarchical porosity for trapping and anchoring Mn-containing gaseous species by a mild one-step pyrolysis method. The optimized Mn-N-C electrocatalyst with a large metal content of 1.71 wt% and a volume ratio of 0.86 mesopores pore delivers a superior ORR activity with a half-wave potential (E1/2) of 0.92 V in 0.1 M KOH and 0.78 V in 0.1 M HClO4. Moreover, the modified Mn-N-C catalyst showed superior potential cyclic stability. TheE1/2remained unchanged in 0.1 M KOH and only lost 6 mV in 0.1 M HClO4after 5000 cycles. When applied as the cathode catalyst in Zn-air battery, it exhibited a maximum peak power density of 176 mW cm-2, demonstrating great potential as a usable ORR catalyst in practical devices.

Nitrogen-doped hollow mesoporous carbon spheres for efficient oxygen reduction.

Extensive investigations have been devoted to nitrogen-doped carbon materials as catalysts for the oxygen reduction reaction (ORR) in various conversion technologies. In this study, we introduce nitrogen-doped carbon materials with hollow spherical structures. These materials demonstrate significant potential in ORR activity within alkaline media, showing a half-wave potential of 0.87 V versus the reversible hydrogen electrode (RHE). Nitrogen-doped hollow carbon spheres (N-CHS) exhibit unique characteristics such as a thin carbon shell layer, hollow structure, large surface area, and distinct pore features. These features collectively create an optimal environment for facilitating the diffusion of reactants, thereby enhancing the exposure of active sites and improving catalytic performance. Building upon the promising qualities of N-CHS as a catalyst support, we employ heme chloride (1 wt%) as the source of iron for Fe doping. Through the carbonization process, Fe-N active sites are effectively formed, displaying a half-wave potential of 0.9 V versus RHE. Notably, when implemented as a cathode catalyst in zinc-air batteries, this catalyst exhibits an impressive power density of 162.6 mW cm-2.

High-performance manganese and nitrogen codoped carbon (Mn-N-C) oxygen reduction electrocatalyst from Mn2+coordinated sodium alginate.

The research on low-cost, high-performance non platinum group metal (PGM) oxygen reduction reaction (ORR) catalysts is of great significance for the rapid promotion of fuel cells' practical applications. In this work, Mn-N-C catalyst with outstanding activity was prepared through using hydrogel formed by coordination of sodium alginate (SA) and Mn2+as the precursor. During the preparation process, g-C3N4was added to improve the surface area enrich the pore structure of catalysts, as well as to function as the nitrogen source. Compare with commercial Pt/C catalyst, the optimum Mn-N-C catalyst possesses extraordinary ORR activity in alkaline electrolytes, with a half-wave potential (E1/2) of 0.90 V. In addition, the Mn-N-C catalyst also displays exceptional stability in alkaline and acidic electrolytes, much superior to Pt/C catalyst.

Bead-like carbon fibers consisting of abundantly exposed active sites for the oxygen reduction reaction.

Rational design is essential in the synthesis of electrocatalysts for the oxygen reduction reaction (ORR). Herein, we introduced zeolitic imidazolate framework-8 (ZIF-8) and polyvinyl pyrrolidone (PVP) into the electrospinning process of the polyacrylonitrile (PAN) and hemin to increase the active site loading and exposed active area of the final product with empty bead-like structures. In this method, ZIF-8 acts as a carbon skeleton to provide a rich microporous structure that can support active sites, and as a nitrogen dopant to improve nitrogen contents. PVP changes the properties of the spinning solution, adjusts the fiber morphology, and to increase the exposed area of active sites as a pore former. The obtained Fe-N-C ORR catalyst delivered a half-wave potential (E1/2) of 0.924 V in a 0.1 M KOH solution and 0.77 V in a 0.1 M HClO4solution. A homemade zinc air battery with power density of 236 mW cm-2demonstrated the excellent performance of the catalyst under working conditions.

Surface-confinement assisted synthesis of nitrogen-rich single atom Fe-N/C electrocatalyst with dual nitrogen sources for enhanced oxygen reduction reaction.

The utilization of earth abundant iron and nitrogen doped carbon as a precious-metal-free electrocatalyst for oxygen reduction reaction (ORR) significantly depends on the rational design and construction of desired Fe-Nxmoieties on carbon substrates, which however remains an enormous challenge. Herein a typical nanoporous nitrogen-rich single atom Fe-N/C electrocatalyst on carbon nanotube (NR-CNT@FeN-PC) was successfully prepared by using CNT as carbon substrate, polyaniline (PANI) and dicyandiamine (DCD) as binary nitrogen sources and silica-confinement-assisted pyrolysis, which not only facilitate rich N-doping for the inhibition of the Fe agglomeration and the formation of single atom Fe-Nxsites in carbon matrix, but also generate more micropores for enlarging BET specific surface area (up to 1500 m2·g-1). Benefiting from the advanced composition, nanoporous structure and surface hydrophilicity to guarantee the sufficient accessible active sites for ORR, the NR-CNT@FeN-PC catalyst under optimized conditions delivers prominent ORR performance with a half-wave potential (0.88 V versus RHE) surpass commercial Pt/C catalyst by 20 mV in alkaline electrolyte. When assembled in a home-made Zn-air battery device as cathodic catalyst, it achieved a maximum output power density of 246 mW·cm-2and a specific capacity of 719 mA·h·g-1Znoutperformed commercial Pt/C catalyst, holding encouraging promise for the application in metal-air batteries.

Boosting the lithium and sodium storage performance of graphene-based composite via pore engineering and surface protection.

Transition metal oxides with high theoretical capacities are widely investigated as potential anodes for alkali-metal ion batteries. However, the intrinsic conductivity deficiency and large volume changes during cycles result in poor cycling stability and low rate capabilities. Graphene has been widely used to support metal oxide for enhanced performance, but the cycling life is limited by the aggregation/collapse of active materials on graphene surface. Herein, we significantly improve the battery performance of graphene-metal oxide composite via pore engineering and surface protection. In this architecture, the mesoporous NiFe2O4 is designed for fast ion diffusion and volume accommodation, and the outer graphene protection can further enhance the electrical conductivity and prevent the aggregation during cycle. Thus, as-prepared G@p-NiFe2O4@G composite for lithium storage delivers high capacity (1244 mA h g-1 after 300 cycles at 0.2 A g-1), excellent rate performance (563 mA h g-1 at 4 A g-1), and outstanding cycling life up to 1200 cycles at 1.5 A g-1. For sodium storage, it also displays good cycling stability and superior rate performance. Moreover, the effects of various microstructures on the battery performance, the reaction kinetics of various electrodes, and the reaction mechanism of NiFe2O4 have been systematically investigated in this work.

Vibration monitoring based on flexible multi-walled carbon nanotube/polydimethylsiloxane film sensor and the application on motion signal acquisition.

Flexible sensors at small scales have potential applications in many fields. Until now, the research on high-performance vibration sensors based on soft materials with high sensitivity and precision, fast response and high stability are still in its infancy. In this work, a flexible, wearable and high precision film sensor based on multi-walled carbon nanotube (MWCNT) was prepared via a vacuum filtration process and then encapsulated within polydimethylsiloxane (PDMS). The sensor exhibits an ultrahigh sensitivity with gauge factor of 214.3 at flexural strain of 0.4%. When used to monitor the vibration responses of a carbon-fiber beam induced by the base excitation and impact hammer, the time and frequency responses were comparable with the results obtained by the accelerometer, with difference less than 1\!%. In addition, when the MWCNT/PDMS thin film was employed as an electronic skin sensor attached on the human body to detect human activities, the high sensitivity and repeatability demonstrate a great potential application in monitoring human motion.

High-efficient and environmentally friendly enrichment of semiconducting single-walled carbon nanotubes by combining short-time electrochemical pre-oxidation and combustion.

High purity semiconducting single-walled carbon nanotubes (s-SWCNTs) have bright prospects in the field of microelectronics, but their enrichment processes are usually very complicated and cost time and energy, which represent a major impediment for their future applications. Here, we report on a new efficient covalent modification enrichment approach that tackles this problem. Our method is to first selectively functionalize the surface of arc-discharge metallic single-walled carbon nanotubes (m-SWCNTs) rapidly by electrochemical pre-oxidation at 7.0 V in 0.1 M KCl aqueous solution, and subsequently followed up by removing the m-SWCNTs with a short-time combustion process at 600 °C for 30 s to enrich high purity s-SWCNTs. Although the surface of the s-SWCNTs was functionalized and heat-treated, the intrinsic tubular structure and electronic characteristics were well maintained. Besides, our approach, without any complex equipment or toxic reagents, is energy and time saving and can be easily scaled up. Milligrams of high-quality s-SWCNTs with high purity of more than 95 wt% can be easily obtained in only several minutes. The retention rate of s-SWCNTs after combustion is as high as 61 wt%.

Enrichment of semiconducting single-walled carbon nanotubes by simple equipment and solar radiation.

High-purity semiconducting (s-) single-walled carbon nanotubes (SWCNTs) have great potential to replace silicon-based materials for microelectronic devices. However, the enrichment methods of s-SWCNTs usually required complex devices and non-renewable energy. In this study, instead of a traditional heating method, renewable solar was employed to dramatically increase the heating rate and improve the reaction to be simple and more controllable, thereby water was successfully used to selectively etch metallic (m-) SWCNTs. In this work, purified SWCNTs films were wetted by water and then exposed to focused solar radiation, causing the surface temperature of the SWCNT films to reach about 800 °C within 2 s. In this case, the m-SWCNTs could be selectively etched by water rapidly. Finally, s-SWCNTs with a purity of about 95 wt% were obtained in several minutes without any complex devices or non-renewable energy.

Rational design of multi-walled carbon nanotube@hollow Fe3O4@C coaxial nanotubes as long-cycle-life lithium ion battery anodes.

In this work, we report a high-performance anode material created by rationally encapsulating multi-walled carbon nanotubes (MWNTs) within hollow Fe3O4 nanotubes followed by applying a carbon coating. When tested for lithium storage, as-prepared MWNT@hollow Fe3O4@C coaxial nanotubes present high specific capacity, superior rate performance, and outstanding cycling stability. It is capable of delivering high capacities of 758 mA h g-1 at 500th cycle at 0.2 A g-1, and 409 mA h g-1 after 1000 cycles at a high rate of 1.5 A g-1. This excellent performance can be attributed to its unique architecture, which provides high electrical conductivity, offers enough void space for volume accommodation, and mitigates the pulverization of Fe3O4 during cycles.

An Fe-N co-doped tube-in-tube carbon nanostructure used as an efficient catalyst for the electrochemical oxygen reduction reaction.

An Fe-N co-doped tube-in-tube carbon nanostructure is synthesized for an efficient oxygen reduction reaction. Thanks to its hollow nature, the mesoporous structure is enriched while defects are not prominent, allowing excellent activity (E 1/2 = 0.851 V) and durability together with methanol tolerance in an electrochemistry test under alkaline conditions. Furthermore, when the material is used as the cathode catalyst of a Zn-air battery, the battery exhibits a peak power density of 181.5 mW cm-2.

Diode-pumped tape casting planar waveguide YAG/Nd:YAG/YAG ceramic laser.

We demonstrated the efficient guided laser action in a diode-pumped YAG/Nd:YAG/YAG ceramic planar waveguide produced by tape casting and vacuum sintering technology for the first time to the best of our knowledge. In the regime of continuous wave operation, a maximum output power of 840 mW corresponding to the slope efficiency of 65% was achieved. During passively Q-switched operation, by replacing the dichroic mirror with graphene-oxide based output coupler, we obtained the stable pulse trains with the shortest pulse duration of 179 ns at a pulse repetition rate of 930 kHz which resulted in the single pulse energy of 221 nJ.

Universal and Energy-Efficient Approach to Synthesize Pt-Rare Earth Metal Alloys for Proton Exchange Membrane Fuel Cell.

Traditional synthesis methods of platinum-rare earth metal (Pt-RE) alloys usually involve harsh conditions and high energy consumption because of the low standard reduction potentials and high oxophilicity of RE metals. In this work, a one-step strategy is developed by rapid Joule thermal-shock (RJTS) to synthesize Pt-RE alloys within tens of seconds. The method can not only realize the regulation of alloy size, but also a universal method for the preparation of a family of Pt-RE alloys (RE = Ce, La, Gd, Sm, Tb, Y). In addition, the energy consumption of the Pt-RE alloy preparation is only 0.052 kW h, which is 2-3 orders of magnitude lower than other reported methods. This method allows individual Pt-RE alloy to be embedded in the carbon substrate, endowing the alloy catalyst excellent durability for oxygen reduction reaction (ORR). The performance of alloy catalyst shows negligible decay after 20k accelerated durability testing (ADT) cycles. This strategy offers a new route to synthesize noble/non-noble metal alloys with diversified applications besides ORR.

Highly coordinative molecular cobalt-phthalocyanine electrocatalyst on an oxidized single-walled carbon nanotube for efficient hydrogen peroxide production.

H2O2 production via the two-electron oxygen reduction reaction (2e- ORR) offers a potential alternative to the current anthraquinone method owing to its efficiency and environmental friendliness. However, it is necessary to determine the structures of electrocatalysts with cost-effectiveness and high efficiency for future industrialization demand. Herein, a supramolecular catalyst composed of cobalt-phthalocyanine on a near-monodispersed and oxidized single-walled carbon nanotube (CoPc/o-SWCNT) was synthesized via a solution self-assembly method for catalyzing the 2e- ORR for H2O2 electrosynthesis. Benefiting from the enhanced intermolecular interaction by introducing oxygen functional groups on o-SWCNTs, the oxidation states of single-atom Co sites were tuned via the formation of two extra Co-O bonds. Coupled with structural characterizations, density-functional theory (DFT) calculations reveal that the depressed d-band center of the Co site regulated by two axially-bridged O atoms gives rise to a suitable binding strength of oxygen intermediates (*OOH) to favor the 2e- ORR. Thus, the CoPc-6wt%/o-SWCNT-2 catalyst with optimized synthetic parameters delivers competitive 2e- ORR performance for H2O2 electrosynthesis in a neutral electrolyte (pH = 7), including enhanced H2O2 generation, satisfactory molar selectivity of ∼83-95% and long-period stability (75 h) in H-cell measurement. Moreover, it could also be boosted to show a high current of 45 mA cm-2, recorded turnover frequency of 25.3 ± 0.5 s-1 and maximum H2O2 production rate of 5.85 mol g-1 h-1 with a continuous H2O2 accumulation of 1.2 wt% in a flow-cell device, which outperformed most of the reported neutral-selective nonprecious metal single-atom catalysts.

Physiological sensing system integrated with vibration sensor and frequency gel dampers inspired by spider.

Recent advances in bioelectronics in mechanical and electrophysiological signal detection are remarkable, but there are still limitations because they are inevitably affected by environmental noise and motion artifacts. Thus, we develop a gel damper-integrated crack sensor inspired by the vibration response of the viscoelastic cuticular pad and slit organs in a spider. Benefitting from the specific crack structure design, the sensor possesses excellent sensing behaviors, including a low detection limit (0.05% strain), ultrafast response ability (3.4 ms) and superior durability (>300 000 cycles). Such typical low-amplitude fast response properties allow the ability to accurately perceive vibration frequency and waveform. In addition, the gel damper exhibits frequency-dependent dynamic mechanical behavior that results in improved stability and reliability of signal acquisition by providing shock resistance and isolating external factors. They effectively attenuate external motion artifacts and low-frequency mechanical noise, resulting in cleaner and more reliable signal acquisition. When the gel damper is combined with the crack-based vibration sensor, the integrated sensor exhibits superior anti-interference capability and frequency selectivity, demonstrating its effectiveness in extracting genuine vocal vibration signals from raw voice recordings. The integration of damping materials with sensors offers an efficient approach to improving signal acquisition and signal quality in various applications.

Bimodal Intelligent Electronic Skin Based on Proximity and Tactile Interaction for Pressure and Configuration Perception.

The flexible bimodal e-skin exhibits significant promise for integration into the next iteration of human-computer interactions, owing to the integration of tactile and proximity perception. However, those challenges, such as low tactile sensitivity, complex fabrication processes, and incompatibility with bimodal interactions, have restricted the widespread adoption of bimodal e-skin. Herein, a bimodal capacitive e-skin capable of simultaneous tactile and proximity sensing has been developed. The entire process eliminates intricate fabrication techniques, employing DLP-3D printing for the electrode layers and sacrificial templating for the dielectric layers, conferring high tactile sensitivity (1.672 kPa-1) and rapid response capability (∼30 ms) to the bimodal e-skin. Moreover, exploiting the "fringing electric field" effect inherent in parallel-plate capacitors has facilitated touchless sensing, thereby enabling static distance recognition and dynamic gesture recognition of varying materials. Interestingly, an e-skin sensing array was created to identify the positions and pressure levels of various objects of different masses. Furthermore, with the aid of machine learning techniques, an artificial neural network has been established to possess intelligent object recognition capabilities, facilitating the identification, classification, and training of various object configurations. The advantages of the bimodal e-skin render it highly promising for extensive applications in the field of next-generation human-machine interaction.