Metal–organic frameworks (MOFs), which consist of central metal nodes and organic linkers, constitute a fast growing class of crystalline porous materials with excellent application potential. Herein, a series of Mn‐based multimetallic MOF (bimetallic and trimetallic MIL‐100) nano‐octahedra are prepared by a facile one‐pot synthetic strategy. The types and proportions of the incorporated elements can be tuned while retaining the original topological structure. The introduction of other metal ions is verified at the atomic level by combining X‐ray absorption fine structure experiments and theoretical calculations. Furthermore, these multimetallic Mn‐based MIL‐100 nano‐octahedra are utilized as sulfur hosts to prepare cathodes for Li–S batteries. The MnNi‐MIL‐100@S cathode exhibits the best Li–S battery performance among all reported MIL‐100@S composite cathode materials, with a reversible capacity of ≈708.8 mAh g−1 after 200 cycles. The synthetic strategy described herein is utilized to incorporate metal ions into the MOF architecture, of which the parent monometallic MOF nano‐octahedra cannot be prepared directly, thus rationally generating novel multimetallic MOFs. Importantly, the strategy also allows for the general synthesis and study of various micro‐/nanoscale MOFs in the energy storage field.

based on connecting central metal atoms/ clusters and organic ligands, have attracted considerable attention. [3][4][5] MOFs can be rationally designed by modifying their constituting metal atoms/clusters and organic ligands, allowing a control of their shapes and sizes. [6] Shapes are typically controlled by introducing modulators (cosolvents or surfactants) that preferentially adsorb onto specific crystal planes, consequently hampering their growth. Furthermore, the size can be adjusted by changing the solvent ratio or reaction time. For these reasons, MOFs are endowed with outstanding properties and potential applications, such as in sensors, [7] electrocatalysis, [8,9] and energy-storage devices. [10,11] The porous structure of MOFs makes them promising host materials to anchor sulfur in Li-S batteries, and this has attracted considerable attention because of their high theoretical capacity (1675 mAh g −1 ). [12,13] The main obstacle to impede commercialization of Li-S batteries is the shuttle effect, leading to an irreversible loss of sulfur during the discharge process. [14] At present, a variety of carbonaceous materials have been adopted as host materials to enable uniform dispersion of sulfur. [15] However, the physical confinement of lithium polysulfides (LPS, chemical formula: Li 2 S x , 4 ≤ x ≤ 8) in nonpolar carbonaceous materials is not sufficient to prevent Metal-organic frameworks (MOFs) with controllable shapes and sizes show a great potential in Li-S batteries. However, neither the relationship between shape and specific capacity nor the influence of MOF particle size on cyclic stability have been fully established yet. Herein, MIL-96-Al with various shapes, forming hexagonal platelet crystals (HPC), hexagonal bipyramidal crystals (HBC), and hexagonal prismatic bipyramidal crystals (HPBC) are successfully prepared via cosolvent methods. Density functional theory (DFT) calculations demonstrate that the HBC shape with highly exposed (101) planes can effectively adsorb lithium polysulfides (LPS) during the charge/discharge process. By changing the relative proportion of the cosolvents, HBC samples with different particle sizes are prepared. When these MIL-96-Al crystals are used as sulfur host materials, it is found that those with a smaller size of the HBC shape deliver higher initial capacity. These investigations establish that different crystal planes have different adsorption abilities for LPS, and that the MOF particle size should be considered for a suitable sulfur host. More broadly, this work provides a strategy for designing sulfur hosts in Li-S batteries.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202107836.

A direct electrochemical DNA sensor was constructed based on gold nanoparticles/graphene film. A precursor graphene film was fabricated on glassy carbon electrode (GCE) using both electrochemically reduced graphene oxide (ERGNO) and chemically reduced graphene oxide (CRGNO). The electrochemical approach was green and fast, and unlike chemical reduction, does not result in contamination of the reduced material, and at highly negative potential could reduce the oxygen functionalities (-OH, C-O-C and -COOH) of the graphene oxide more efficiently. ERGNO exhibited better electrochemical and electrocatalytic performances than CRGNO. Gold nanoparticles (AuNPs) were electrodeposited on the ERGNO/GCE to amplify the electrochemical signals. The resulting AuNPs/ERGNO composite film was characterized by scanning electron microscopy, energy dispersive spectroscopy and Raman spectroscopy. The electrochemical responses of guanine (G), adenine (A), thymine (T) and cytosine (C) were investigated at AuNPs/ERGNO/GCE, which showed more favorable electron transfer kinetics than at ERGNO/GCE, demonstrating the significantly synergistic electrocatalytic effect of ERGNO and AuNPs. Synthetic sequence-specific DNA oligonucleotides was successfully detected and the established immobilization-free biosensor had the ability to discriminate single-or double-base mismatched DNA.

The introduction of high-entropy into Prussian blue analogues (PBAs) has yet to attract attention in the field of lithium-sulfur battery materials. Herein, we systematically synthesize a library of PBAs from binary to high-entropy by a facile coprecipitation method. The coordination environment in PBAs is explored by X-ray absorption fine structure spectroscopy, which together with elemental mapping confirm the successful introduction of all metals. Importantly, electrochemical tests demonstrate that high-entropy PBA can serve as polysulfide immobilizer to inhibit shuttle effect and as catalyst to promote polysulfides conversion, thereby boosting its outstanding performance. Additionally, a variety of nanocubic metal oxides from binary to senary are fabricated by using PBAs as sacrificial precursors. We believe that a wide range of new materials obtained from our coprecipitation and pyrolysis methodology can promote further developments in research on PBA systems and sulfur hosts.

A novel one-step electrochemical synthesis of the reduced graphene oxide and poly(m-aminobenzenesulfonic acid, ABSA) nanocomposite (PABSA-rGNO) via pulse potentiostatic method (PPM) for direct and freely switchable detection of target genes is presented. Unlike most electrochemical preparation of hybrids based on rGNO and polymer, electrochemical synthesis of PABSA (during the pulse electropolymerization period of PPM) and electrochemical reduction of rGNO (during the resting period of PPM), in this paper, were alternately performed. The total progress synchronously resulted in PABSA-rGNO nanocomposite. This nanocomposite was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray powder diffraction (XRD), Fourier Transform infrared spectroscopy (FT-IR), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). The PABSA-rGNO nanocomposite integrated graphene (a single-atom thick, two-dimensional sheet of sp(2) bonded conjugated carbon) with PABSA (owning rich-conjugated structures, functional groups, and excellent electrochemical activity), which could serve as an ideal electrode material for biosensing and electrochemical cell, etc. As an example, the immobilization of the specific probe DNA was successfully conducted via the noncovalent method due to the π-π* interaction between conjugated nanocomposite and DNA bases. The hybridization between the probe DNA and target DNA induced the product dsDNA to be released from conjugated nanocomposite, accompanied with the self-signal regeneration of nanocomposite ("signal-on"). The self-signal changes served as a powerful tool for direct and freely switchable detection of different target genes, and the synergistic effect of PABSA-rGNO nanocomposite effectively improved the sensitivity for the target DNA detection.