Redox Tuning in Crystalline and Electronic Structure of Bimetal-Organic Frameworks Derived Cobalt/Nickel Boride/Sulfide for Boosted Faradaic Capacitance.

The development of efficient electrode materials is a cutting-edge approach for high-performance energy storage devices. Herein, an effective chemical redox approach is reported for tuning the crystalline and electronic structures of bimetallic cobalt/nickel-organic frameworks (Co-Ni MOFs) to boost faradaic redox reaction for high energy density. The as-obtained cobalt/nickel boride/sulfide exhibits a high specific capacitance (1281 F g-1 at 1 A g-1 ), remarkable rate performance (802.9 F g-1 at 20 A g-1 ), and outstanding cycling stability (92.1% retention after 10 000 cycles). An energy storage device fabricated with a cobalt/nickel boride/sulfide electrode exhibits a high energy density of 50.0 Wh kg-1 at a power density of 857.7 W kg-1 , and capacity retention of 87.7% (up to 5000 cycles at 12 A g-1 ). Such an effective redox approach realizes the systematic electronic tuning that activates the fast faradaic reactions of the metal species in cobalt/nickel boride/sulfide which may shed substantial light on inspiring MOFs and their derivatives for energy storage devices.

Construction of Metal-Organic Framework/Conductive Polymer Hybrid for All-Solid-State Fabric Supercapacitor.

Metal-organic frameworks (MOFs) hold promising potential in energy storage but are limited by poor conductivity. In this work, a metal-organic framework/polypyrrole hybrid is constructed by a facile one-pot electrodeposition method in the presence of dopamine. An all-solid-state fabric supercapacitor based on this hybrid demonstrates excellent electrochemical energy-storage performance, which achieves a specific capacitance of 10 mF cm-1 (206 mF cm-2), a power density of 132 µW cm-1 (2102 µW cm-2), and an energy density of 0.8 µWh cm-1 (12.8 µWh cm-2). The stable cycling life and excellent mechanical flexibility over a wide range of working temperature are also achieved, which maintains a capacitance retention of 89% over 10 000 charging/discharging cycles, a capacitance decrease of only 4% after 1000 frizzy (360° bending) cycles, and no obvious capacitance loss under 100 repeated heating (100 °C)/cooling (-15 °C) cycles. This fibrous supercapacitor displays promising potential in wearable textile electronics as it can be easily woven into common cotton cloth. Our strategy may shed some valuable light on the construction of MOF-based hybrids for flexible energy-storage electronics.

Publisher Correction: Role of outer surface probes for regulating ion gating of nanochannels.

The original version of this Article contained an error in Fig. 3. The scale bars in Figs 3c and 3d were incorrectly labelled as 50 µA. In the correct version, the scale bars are labelled as 0.5 µA. This has now been corrected in both the PDF and HTML versions of the Article.

Role of outer surface probes for regulating ion gating of nanochannels.

Nanochannels with functional elements have shown promise for DNA sequencing, single-molecule sensing, and ion gating. Ionic current measurement is currently a benchmark, but is focused solely on the contribution from nanochannels' inner-wall functional elements (NIWFE); the attributes of functional elements at nanochannels' outer surface (NOSFE) are nearly ignored, and remain elusive. Here we show that the role of NOSFE and NIWFE for ion gating can be distinguished by constructing DNA architectures using dual-current readout. The established molecular switches have continuously tunable and reversible ion-gating ability. We find that NOSFE exhibits negligible ion-gating behavior, but it can produce a synergistic effect in alliance with NIWFE. Moreover, the high-efficiency gating systems display more noticeable synergistic effect than the low-efficiency ones. We also reveal that the probe amount of NOSFE and NIWFE is almost equally distributed in our biomimetic nanochannels, which is potentially a premise for the synergistic ion-gating phenomena.

Fabrication of "Plug and Play" Channels with Dual Responses by Host-Guest Interactions.

The "Plug and Play" template can be individually or successively grafted by dual-responsive molecules on the α-CD modified channels by host-guest interactions and can be peeled off by UV irradiation. The artificial channels present six kinds of responses cycling among four states responding to three environment stimuli, as light, pH, and temperature.

Sensitive Zn(2+) sensor based on biofunctionalized nanopores via combination of DNAzyme and DNA supersandwich structures.

The sensitivity of detection based on biofunctionalized nanopores is limited since the target-to-signal ratio is 1 : 1. Isothermal amplification is a promising amplification strategy at constant temperature due to its easy operation, quick results, PCR-like sensitivity, low cost and energy efficiency. In the present work, the isothermally amplified detection of Zn(2+) is achieved by using a DNA supersandwich structure and Zn(2+)-requiring DNAzymes. The DNA supersandwich structures, due to the multiple amplification of nucleic acids, heavily plug the nanopore. Simultaneously, the DNA supersandwich structures bond with the sessile probe (SP) of the substrate in the nanopore which partially hybridizes with DNAzymes. In the presence of Zn(2+), the Zn(2+)-requiring DNAzyme cleaves the SP into two fragments, while the DNA supersandwich structures are peeled off and the ionic pathway is unimpeded. A steep drop and a sequential complete recovery of the current occur in the I-V plot when the DNA supersandwich structures are decorated and peeled off. In the present system, the reliable detection limit of Zn(2+) is as low as 1 nM. Discrimination between different types of ions (Cu(2+), Hg(2+), Pb(2+)) is achieved.

Highly Robust Nanopore-Based Dual-Signal-Output Ion Detection System for Achieving Three Successive Calibration Curves.

In recent years, artificial stimuli-responsive bioinspired nanopores have attracted a lot of attention due to their unique property of confined spaces and flexibility in terms of shapes and sizes. Most of the nanopore systems demonstrated their transmembrane properties and applications in target detections. However, almost all of the nanopores can be used only once due to either the irreversible reactions between targets and probes or the plugged nanopores not easily being unplugged again. In this work, we propose a dual-signal-output nanopore system that could detect the cations (Hg(2+)) inducing the plugged nanopores. The detection system is highly recoverable by the anions (S(2-)) inducing the unplugged nanopores. More importantly, as far as we know, it is seldom reported for the same nanopores to achieve successive calibration curves for three times by subsequent reversible plug-unplug processes, which strongly demonstrates the high robustness of this novel nanopore-detection system. In addition, unlike monitoring the plug-unplug phenomena by only one type of signal, we combined the ionic current signal with the fluorescence output and could directly observe that the change of ionic current does in fact correspond to the plug-unplug of the nanopores by the target stimuli.

Nanopore-based DNA-probe sequence-evolution method unveiling characteristics of protein-DNA binding phenomena in a nanoscale confined space.

Almost all of the important functions of DNA are realized by proteins which interact with specific DNA, which actually happens in a limited space. However, most of the studies about the protein-DNA binding are in an unconfined space. Here, we propose a new method, nanopore-based DNA-probe sequence-evolution (NDPSE), which includes up to 6 different DNA-probe systems successively designed in a nanoscale confined space which unveil the more realistic characteristics of protein-DNA binding phenomena. There are several features; for example, first, the edge-hindrance and core-hindrance contribute differently for the binding events, and second, there is an equilibrium between protein-DNA binding and DNA-DNA hybridization.