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Nanosized energy storage, energy-harvesting, and functional devices are the three key components for integrated self-power systems. Here, we report on nanoscale electrochemical devices with a nearly three-fold enhanced stored charge under the field effect. We demonstrated the field-effect transistor can not only work as a functional component in nanodevices but also serve as an amplifier for the nanosized energy storage blocks. This unusual increase in energy storage is attributed to having a wide range of accessible electronic density of states (EDOS), hence redox reactions are occurring within the nanowire and not being confined to the surface. Initial results with MoS2 suggest that this field effect modulated energy storage mechanism may also apply to many other redox-active materials. Our work demonstrates the novel application of the field-effect in energy storage devices as a universal strategy to improve ion diffusion and the surface-active ion concentration of the active material, which can greatly enhance the charge storage ability of nanoscale devices. The fabrication process of the field-effect energy storage device is also compatible with microtechnology and can be integrated into other microdevices and nanodevices., Comment: 18 pages, 4 figures

Marine macroalgae are considered renewable natural resources due to their high carbohydrate content, which gives better utilization value in biorefineries and higher value conversion than first- and second-generation biomass. However, due to the diverse composition, complex structure, and rare metabolic pathways of macroalgae polysaccharides, their bioavailability needs to be improved. In recent years, enzymes and pathways related to the degradation and metabolism of macroalgae polysaccharides have been continuously developed, and new microbial fermentation platforms have emerged. Aiming at the bioutilization and transformation of macroalgae resources, this review describes the latest research results from the direction of green degradation, biorefining, and metabolic pathway design, including summarizing the the latest biorefining technology and the fermentation platform design of agarose, alginate, and other polysaccharides. This information will provide new research directions and solutions for the biotransformation and utilization of marine macroalgae.

MoS2/Ni3S2@C shows excellent sodium/potassium storage performance, which is due to carbon layer-confined heterostructure, creating more sodium/potassium storage sites, shortening ions diffusion path and relieving the volume change of the material.

To increase the specific capacitance of supercapacitors, polyaniline (PANI) has been chosen as additive electrode material for the pseudocapacitive performance. Here, we synthesize a molecular-level uniform reduced graphene oxide/PANI (rGO/PANI) composite film with high flexibility and conductivity via self-assembly and specific thermal reduction, which performs great potential in flexible supercapacitors with high areal capacitance. Particularly, the electrode of rGO/PANI-42.9% exhibits a high specific areal capacitance (1826 mF cm−2 at 0.2 mA cm−2), and it also presents a good cycling stability (it remains 76% of its initial capacitance after 10 500 cycles). Moreover, the specific gravimetric capacitance of rGO/PANI-33.3% reaches up to 256.4 F g−1 at 0.2 A g−1, showing greatly enhanced performance compared with the pure rGO electrode (183 F g−1). The results of various characteristic analysis demonstrate that electrochemical performance of the as-prepared rGO/PANI film is closely associated with the uniform distribution of PANI in rGO/PANI composite. Overall, our reported method is convenient and environmental-friendly, and could be beneficial for the development of high-performance capacitive energy storage materials.

Single-atom catalysts (SACs) have attracted widespread interest for many catalytic applications because of their distinguishing properties. However, general and scalable synthesis of efficient SACs remains significantly challenging, which limits their applications. Here we report an efficient and universal approach to fabricating a series of high-content metal atoms anchored into hollow nitrogen-doped graphene frameworks (M-N-Grs; M represents Fe, Co, Ni, Cu, etc.) at gram-scale. The highly compatible doped ZnO templates, acting as the dispersants of targeted metal heteroatoms, can react with the incoming gaseous organic ligands to form doped metal–organic framework thin shells, whose composition determines the heteroatom species and contents in M-N-Grs. We achieved over 1.2 atom % (5.85 wt %) metal loading content, superior oxygen reduction activity over commercial Pt/C catalyst, and a very high diffusion-limiting current (6.82 mA cm–2). Both experimental analyses and theoretical calculations reveal the oxygen reduction activity sequence of M-N-Grs. Additionally, the superior performance in Fe-N-Gr is mainly attributed to its unique electron structure, rich exposed active sites, and robust hollow framework. This synthesis strategy will stimulate the rapid development of SACs for diverse energy-related fields., An efficient and universal approach to fabricating a series of high-content metal atoms anchored into hollow nitrogen-doped graphene frameworks is developed via a nicely designed process.

The recent emergence of electrically conductive nanoporous membranes based on graphene and other 2D materials opens up new opportunities to revisit some longstanding nanoconfined ion transport problems under electrification. This work probes the ionic resistance in electrified multilayered graphene membranes with electrochemical impedance spectroscopy. This study demonstrates that the combination of additive-free feature and tunable slit pore sizes in the sub-10 nm range in graphene-based membranes has made it possible to deconvolute the different ionic processes from the impedance obtained and examine the exclusive influence of pore size on the ionic resistance in a quantitative manner. The trends revealed for the ionic resistance at the pore entrance and inside the pores under severe nanoconfinement (2 nm) are found to be generally consistent with the microscale theoretical simulations previously reported. It also allows a quantitative analysis of the relative effects of the external polarization potential and ion identity under nanoconfinement. The results suggest that the classic electrochemical impedance spectroscopy technique, when applied to appropriate nanoporous electrode materials, can provide rich information about nanoconfined ion transport phenomena under electrification for fundamental understanding and application development.

Biological fluoride ion channels are sub-1-nanometer protein pores with ultrahigh F− conductivity and selectivity over other halogen ions. Developing synthetic F− channels with biological-level selectivity is highly desirable for ion separations such as water defluoridation, but it remains a great challenge. Here we report synthetic F− channels fabricated from zirconium-based metal-organic frameworks (MOFs), UiO-66-X (X = H, NH2, and N+(CH3)3). These MOFs are comprised of nanometer-sized cavities connected by sub-1-nanometer-sized windows and have specific F− binding sites along the channels, sharing some features of biological F− channels. UiO-66-X channels consistently show ultrahigh F− conductivity up to ~10 S m−1, and ultrahigh F−/Cl− selectivity, from ~13 to ~240. Molecular dynamics simulations reveal that the ultrahigh F− conductivity and selectivity can be ascribed mainly to the high F− concentration in the UiO-66 channels, arising from specific interactions between F− ions and F− binding sites in the MOF channels., While biological fluoride ion channels display excellent F− conductivity and selectivity, designing synthetic analogues remains highly challenging. Here the authors show that zirconium-based metal–organic frameworks with F− binding sites and sub-1-nanometer channels exhibit ultrahigh F− conductivity and selectivity.

Transition metal nitrides are of great interest for lithium storage application due to their high electrical conductivity and low voltage plateau. However, the relative cycling stability restricts their practical application. Herein, a stable bimetal nitride NiCo2N hollow sphere material with interconnected nanosheets shell was successfully synthesized via a facial solvothermal route. When used as anodes for lithium-ion batteries, the unique structure can effectively relieve the volume change of the electrode material, and shorten the diffusion distance of lithium ions during the repeated cycling processes. As a result, the NiCo2N electrode exhibits an excellent electrochemical performance. It delivers high discharge capacity of 1244.5 mAh g−1 at a current density of 1 A g−1 after 400 cycles, the capacity can maintain 529.4 mAh g−1 at high current density of 5 A g−1. Furthermore, the electrochemical reaction mechanism of the electrodes is revealed by ex situ XRD, ex situ EIS, and ex situ HRTEM characterization.

The oxygen evolution reaction involves complex interplay among electrolyte, solid catalyst, and gas-phase and liquid-phase reactants and products. Monitoring catalysis interfaces between catalyst and electrolyte can provide valuable insights into catalytic ability. But it is a challenging task due to the additive solid supports in traditional measurement. Here we design a nanodevice platform and combine on-chip electrochemical impedance spectroscopy measurement, temporary I-V measurement of an individual nanosheet, and molecular dynamic calculations to provide a direct way for nanoscale catalytic diagnosis. By removing O2 in electrolyte, a dramatic decrease in Tafel slope of over 20% and early onset potential of 1.344 V vs. reversible hydrogen electrode are achieved. Our studies reveal that O2 reduces hydroxyl ion density at catalyst interface, resulting in poor kinetics and negative catalytic performance. The obtained in-depth understanding could provide valuable clues for catalysis system design. Our method could also be useful to analyze other catalytic processes., Electrocatalysis offers important opportunities for clean fuel production, but uncovering the chemistry at the electrode surface remains a challenge. Here, the authors exploit a single-nanosheet electrode to perform in-situ measurements of water oxidation electrocatalysis and reveal a crucial interaction with oxygen.

Transition metal dichalcogenides, such as MoS2 and VSe2 have emerged as promising catalysts for the hydrogen evolution reaction (HER). Substantial work has been devoted to optimizing the catalytic performance by constructing materials with specific phases and morphologies. However, the optimization of adsorption/desorption process in HER is rare. Herein, we concentrate on tuning the dynamics of the adsorption process in HER by applying a back gate voltage to the pristine VSe2 nanosheet. The back gate voltage induces the redistribution of the ions at the electrolyte–VSe2 nanosheet interface, which realizes the enhanced electron transport process and facilitates the rate-limiting step (discharge process) under HER conditions. A considerable low onset overpotential of 70 mV is achieved in VSe2 nanosheets without any chemical treatment. Such unexpected improvement is attributed to the field tuned adsorption-dynamics of VSe2 nanosheet, which is demonstrated by the greatly optimized charge transfer resistance (...