Latest ArticlesVersatile module design of precursor networks enables flexible functionalization of nano-carbon electrode materials to meet the adaptable energy-storage demand. Functionalized heterogeneous networks are more likely to decompose by swift temperature programming together with predesign module removal, so high functionality/network transfer from precursor to carbon is still a work in progress. A pre-stabilization route is proposed here to enhance the network strength at early pyrolysis and pin up precursor-level functionalities on the final carbon. Such strategy successfully fixes more electroactive N (4.28−8.86 wt%) into the resultant carbon microspheres compared with non-pretreated carbon (2.89 wt%), as well as achieves broad ion-accessible platforms of 1575–2269 m2/g with preset structural superiorities. As a result, a typical acidic device reveals an outstanding specific capacitance of 383 F/g at 10 mV/s. Taking advantage of a novel LiNO3-PAM polymer electrolyte, the upgraded symmetric device displays the maximum specific capacitance of 229 F/g, along with a boosted energy density of 41.1 Wh/kg at 643.4 W/kg. This work opens up a feasible insight into realizing highly efficient precursor/electrode design toward superior system with outstanding energy/power feature and temperature applicability.
Although SiO2-based anode is a strong competitor to supersede graphite anode for lithium-ion batteries, it still has problems such as low electrochemical activity, enormous loss of active lithium, and serious volume expansion. In order to solve these problems, we used a graphene network loaded with cobalt metal nanoparticles (rGO–Co) to coat SiO2 porous hollow spheres (SiO2@rGO–Co). The construction of porous hollow structure and graphene network can shorten the lithium-ion (Li+) diffusion distance and enhance the conductivity of the composite, which improves the electrochemical activity of SiO2 effectively. They also alleviate the volume expansion of the anode in the cycling process. Moreover, nano-scale cobalt metal particles dispersed on graphene catalyze the conversion reaction of SiO2 and activate the locked Li+ in Li2O through a reversible reaction, which improves the charge and discharge capacity of the anode. The capacity of SiO2@rGO–Co reaches 370.4 mAh/g after 100 cycles at 0.1 A/g, which is 6.19 times the capacity of pure SiO2 (59.8 mAh/g) under the same circumstance. What is more, its structure also exhibits excellent cycle stability, with a volume expansion rate of only 13.0% after 100 cycles at a current density of 0.1 A/g.
In the field of organic phototransistor, achieving both broad-spectral and high photosensitivity has always been a big challenge. The innovation of device structure has previously proven to be a possible solution to this problem. Here in this study, a novel organic phototransistor based on a high mobility n-type small molecule as the conducting layer and an isolated bulk heterojunction light-absorbing layer as the floating gate has been demonstrated in this study. With the special designed device structure, the phototransistor shows extremely high sensitivity to broad spectral and weak light irradiation, and the photoresponsivity and photocurrent/dark-current ratio of the device can reach up to 4840 mA/W and 1.8 × 105 respectively. For conclusion, this study suggests a potential way to obtain high-performance phototransistors at room temperature, which will further promote the commercial application of organic phototransistors.
Understanding phase transitions in multi-component crystals is of importance for regulating specified functional materials. Herein, we present two new organic-inorganic hybrid crystals, (Me3NCH2CH2X)4[Ni(NCS)6] (X = Cl and Br), revealing distinct phase transitions. Specifically, the Cl-substituted cations weakly interact with discrete inorganic part hence reveal step-wise dynamic changes upon heating, which result in multi-step solid-solid phase transitions (P1-P21/n–A2/a–Cmce) including a ferroelastic one with a spontaneous strain of 0.0475. Whereas the Br-substituted cations with larger steric effect prevent the solid-solid phase transition but give a solid-liquid phase transition at above 419 K. The present instances well demonstrate the complicity for multi-component crystals arising from the delicate balance established by abundant weak intermolecular interactions, and inspire the design of novel phase-transition materials by judiciously assembling multi-component crystals.
Utilizing metal-organic frameworks (MOFs) to design photocatalysts for CO2 reduction catalysts is an excellent idea but currently restricted by the relatively low activity. Enhancing CO2 affinity and tuning the oxidation state of metal clusters in MOFs might be a solution to improve the catalytic performance. Herein, the Cl-bridge atoms in the metal clusters of a cobalt MOF were easily exchanged with OH−, which simultaneously oxidized a portion of Co(Ⅱ) to Co(Ⅲ) and resulted in a much enhanced photocatalytic activity for CO2 reduction. In contrast, the original framework does not exhibit such superior activity. Comprehensive characterizations on their physicochemical properties revealed that the introduction of hydroxyl group not only greatly increases the CO2 affinity but also alters the oxidation state of metal clusters, resulting in significantly improved photocatalytic activities for CO2 reduction. This work provides important insight into the design of efficient photocatalysts.
Potassium-ion batteries (PIBs) have attracted tremendous attention for large-scale energy storage fields based on abundant potassium resources. Graphite is a promising anode material for PIBs due to its low potassium ion intercalation voltage and mature industrialized preparation technology. However, the inability of graphitic structures to endure large volume change during charge/discharge cycles is a major limitation in their advancement for practical PIBs. Herein, a soft carbon-coated bulk graphite composite is synthesized using PTCDA as a carbon precursor. The PTCDA-derived soft carbon coating layer with large interlayer distance facilities fast potassium ion intercalation/extraction in the BG@C composite and buffers severe volume change during the charge/discharge cycles. When tested as anode for PIBs, the composite realizes enhanced rate capability (131.3 mAh/g at 2 C, 1 C = 279 mA/g) and cycling performance (capacity retention of 76.1% after 150 cycles at 0.5 C). In general, the surface modification route to engineer graphite anode could inherently improve the electrochemical performance without any structural alteration.
The electricity-driven water splitting acts as a promising pathway for renewable energy conversion and storage, yet anodic oxygen evolution reaction (OER) largely hinders its efficiency. Seeking the alternatives to OER exhibits the competitive advance to address this predicament. In this work, we show a more thermodynamically and kinetically favorable reaction, electrochemical oxidative dehydrogenation (EODH) of benzylamine to replace the conventional OER, catalyzed by a cobalt cyclotetraphosphate (Co2P4O12) nanorods catalyst grown on nickel foam. This anodic reaction lowers the electricity input of 317 mV toward the desired current density of 100 mA/cm2, together with a highly selective benzonitrile product of more than 97%. More specifically, when coupling it with cathodic hydrogen evolution reaction (HER), the proposed HER||benzylamine-EODH configuration only requires a cell voltage of 1.47 V@100 mA/cm2, exhibiting an energy-saving up to 17% relative to conventional water splitting, as well as the near unit selectivity toward cathodic H2 and anodic benzonitrile products.
Ammonia is the feedstock chemical for most fertilizers and the alternative of renewable energy carriers. Environmentally benign electrochemical nitrogen reduction reaction (NRR) under mild conditions has been recognized as one of the most attractive strategies for N2 fixation. Herein, inspired by Mo-based nitrogenase, W/Mo-doping electrocatalysts were developed with mixed-metal polyoxometalate H3PW6Mo6O40 as the precursor for high performance electrocatalytic NRR. Trace amount of Pt was transplanted on the surface of W/Mo@rGO via in situ electroplating treatment to further improve the NRR performance. The resulting Pt-W/Mo@rGO-6 achieves excellent performance for NRR with a high NH3 yield of 79.2 µg h−1 mgcat−1 due to the multicomponent synergistic effect in the composite catalyst. The Pt-W/Mo@rGO-6 represents the first example of highly efficient NRR electraocatalyst derived from mixed-metal polyoxometalate, which exhibits outstanding stability confirmed by the constant catalytic performance over 24 h chronoamperometric test. This finding opens a new avenue to construct highly efficient NRR electrocatalyst by employing mixed metal polyoxometalate as the precursor under ambient conditions.
Stimulus-responsive vesicles have broad applications in a variety of areas. Herein, oxidation-responsive framboidal triblock copolymer vesicles are prepared by photoinitiated RAFT seeded emulsion polymerization of a thioether-functionalized monomer using diblock copolymer vesicles as seeds. The obtained framboidal vesicles can transform into worms or spheres in the presence of reactive oxygen species, which can be further used for controlled release of cargos (e.g., silica nanoparticles).
A cadmium tetracyanoplatinate host clathrate, (MV)[Cd2{Pt(CN)4}3]⋅2(H2O) (1), including a methylviologen dication (MV2+) was synthesized, and the crystal structures, photochromic and photoluminescence properties were investigated. In 1, the alternatively parallel stacking between the MV2+ dications as electron acceptors in the channels and the electron donors [Pt1(CN)4]2– units in the host frameworks give a unique donor-acceptor (DA) system. Under UV irradiation, the electron transfer between MV2+ and [Pt(CN)4]2– ions generates MV·+ radicals with a photochromic behavior from pale-yellow to blue. This process occurs through single-crystal-to-single-crystal (SCSC) transformation and obvious structure variation of viologen cations is successfully observed. Moreover, the spectral overlap between the emission bands of 1 and the absorption around 623 nm for the MV·+ radicals leads to a modulation of the photoluminescence.
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