We report a facile method to dope submicrometer carbon spheres with Ag nanoparticles (NPs) to fabricate Ag-NP/C composites via microwaving suspensions of nanoporous carbon spheres in aqueous Ag(NH3)2 + solutions with poly(N-vinylpyrrolidone) as reducer. The composite particles are synthesized in high yield within a short reaction time, and the size, number density, and to some extent even the locations of NPs in/on the carbon spheres can be controlled by adjusting reaction parameters. The controllability is discussed based on the experimental results from transmission electron microscopy, X-ray photoelectron spectroscopy depth profiling, and X-ray diffraction. By controlling the Ag doping, the composite spheres exhibit not only a tunable plasmon resonance shift but also an excellent catalytic activity toward the reduction of 4-nitrophenol by sodium borohydride.

To achieve high‐performance wearable supercapacitors (SCs), a new class of flexible electrodes with favorable architectures allowing large porosity, high conductivity, and good mechanical stability is strongly needed. Here, this study reports the rational design and fabrication of a novel flexible electrode with nanotube‐built multitripod architectures of ternary metal sulfides' composites (FeCo2S4–NiCo2S4) on a silver‐sputtered textile cloth. Silver sputtering is applicable to almost all kinds of textiles, and S2− concentration is optimized during sulfidation process to achieve such architectures and also a complete sulfidation assuring high conductivity. New insights into concentration‐dependent sulfidation mechanism are proposed. The additive‐free FeCo2S4–NiCo2S4 electrode shows a high specific capacitance of 1519 F g−1 at 5 mA cm−2 and superior rate capability (85.1% capacitance retention at 40 mA cm−2). All‐solid‐state SCs employing these advanced electrodes deliver high energy density of 46 W h kg−1 at 1070 W kg−1 as well as achieve remarkable cycling stability retaining 92% of initial capacitance after 3000 cycles at 10 mA cm−2, and outstanding reliability with no capacitance degradation under large twisting. These are attributed to the components' synergy assuring rich redox reactions, high conductivity as well as highly porous but robust architectures. An almost linear increase in capacitance with devices' area indicates possibility to meet various energy output requirements. This work provides a general, low‐cost route to wearable power sources.

Pd-Ag bimetallic dendrites have been synthesized via a galvanic replacement reaction of Ag dendrites in a Na 2 PdCl 4 solution. Scanning and transmission electron microscopy (SEM and TEM), energy dispersive X-ray spectrometry (EDX), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) analysis reveal that the resulting product is composed of partially depleted Ag dendrites covered with a rough surface with many Pd granules protruding by up to about 20 nm. High-solution TEM combined with EDX and selected area electron diffraction (SAED) confirms the formation of bimetallic interfaces between Pd and Ag. These Pd-Ag dendrites show up to four times higher catalytic activity toward the reduction of 4-nitrophenol (4-NP) by sodium borohydride (NaBH 4 ) than the best recently reported catalysts. This further enhancement over the already strong performance of similarly synthesized Au-Ag dendrites is explained by the presence of Pd, adding a hydrogen relay mechanism on top of the very effective electron relay capability of bimetallic dendrites.

Dendritic Ag/Au bimetallic nanostructures have been synthesized via a galvanic replacement reaction (GRR) of Ag dendrites in a chlorauric acid (HAuCl4) solution. After short periods of time, one obtains structures with protruding flakes; these will mature into very porous structures with little Ag left over. The morphological, compositional, and crystal structural changes involved with reaction time t were analyzed by using scanning and transmission electron microscopy (SEM and TEM, respectively), energy-dispersive X-ray spectrometry (EDX), and X-ray diffraction. High-resolution TEM combined with EDX and selected area electron diffraction confirmed the replacement of Ag with Au. A proposed formation mechanism of the original Ag dendrites developing pores while growing Au flakes cover this underlying structure at longer reaction times is confirmed by exploiting surface-enhanced Raman scattering (SERS). Catalytic reduction of 4-nitrophenol (4-NP) by sodium borohydride (NaBH4) is strongly enhanced, implying promising applications in catalysis.

A significant advance toward the design and fabrication of a novel hierarchical supercapacitor electrode consisting of FeCo2S4‐tubes with well‐defined square cross‐section and intersecting nanosheets built porous shells on a 3D porous Ni backbone via controlled sulfidation is reported. This general method allows template‐free synthesis of metal sulfides tubular structures with polygonal cross‐sections and also fine control over the nanostructure leading to both maximized porosity and saturation sulfidation. New insights into concentration and time dependent sulfidation reaction kinetics are proposed. The FeCo2S4 electrode achieves a specific capacitance reaching 2411 F g‐1 at 5 mA cm‐2 and good rate capability, which are superior over those for nanotube arrays of other ternary transition metal sulfides. This is attributed to rich redox reactions, the highly porous but robust architecture as well as high electrical conductivity. Especially such porous shells effectively avoid “dead volume”, thus improve the utilization ratio of the electrode material. Asymmetric solid‐state device applying the FeCo2S4 as positive electrode and N‐doped graphene hydrogel film as negative electrode has a high cell voltage of 1.6 V and thus delivers considerably higher energy density of 76.1 W h kg‐1 (at 755 W kg‐1) than those reported for similar devices.

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High energy density, fast recharging ability, and sustained cycle life are the primary requisite of supercapacitors (SCs); these necessities can be fulfilled by engineering a smart current collector with hierarchical combination of different active materials. This study reports a multicomponent design of hierarchical zinc cobalt sulfide (ZCS) hollow nanotube arrays wrapped with interlaced ultrathin Ni(OH)2 nanoflakes for high‐performance electrodes. The ZCS exhibits a unique pentagonal cross‐section and a rough surface that facilitates the deposition of Ni(OH)2 nanoflakes with a thickness of 7.5 nm. The ZCS/Ni(OH)2 hierarchical electrode exhibits a high specific capacitance of 2156 F g−1 and excellent cyclic stability with 94% retention over 3000 cycles. This is attributed to enhanced redox reactions, the direct growth of arrays on 3D porous foam acting as a “superhighway” for electron transport, and the increased availability of electrochemical active sites provided by the ultrathin Ni(OH)2 flakes that also sustain the stability of the electrode by sacrificing themselves during long charge/discharge cycles. Symmetric SCs are assembled to achieve high energy density of 74.93 W h kg−1 and exhibit superior cyclic stability of 78% retention with 81% coulombic efficiency over 10 000 cycles.

Hierarchically porous yet densely packed MnO2 microspheres doped with Fe3O4 nanoparticles are synthesized via a one-step and low-cost ultrasound assisted method. The scalable synthesis is based on Fe(2+) and ultrasound assisted nucleation and growth at a constant temperature in a range of 25-70 °C. Single-crystalline Fe3O4 particles of 3-5 nm in diameter are homogeneously distributed throughout the spheres and none are on the surface. A systematic optimization of reaction parameters results in isolated, porous, and uniform Fe3O4-MnO2 composite spheres. The spheres' average diameter is dependent on the temperature, and thus is controllable in a range of 0.7-1.28 μm. The involved growth mechanism is discussed. The specific capacitance is optimized at an Fe/Mn atomic ratio of r = 0.075 to be 448 F/g at a scan rate of 5 mV/s, which is nearly 1.5 times that of the extremely high reported value for MnO2 nanostructures (309 F/g). Especially, such a structure allows significantly improved stability at high charging rates. The composite has a capacitance of 367.4 F/g at a high scan rate of 100 mV/s, which is 82% of that at 5 mV/s. Also, it has an excellent cycling performance with a capacitance retention of 76% after 5000 charge/discharge cycles at 5 A/g.