Latest ArticlesRegulation of chemical composition and nanostructure, such as the introduction of dopant into two-dimensional nanomaterials, is a general and valid strategy for the efficient electrocatalyst design. In this work, Co4S3/Co9S8 nanosheets, with an ultrathin layer structure, were successfully synthesized via an efficient solvothermal process combined with ultrasonic exfoliation. Different metal ions (M = Fe3+, Cr3+, Mn2+ and Ni2+) were then doped by a simple cation exchange method and the effects of different dopants on the OER activities of Co4S3/Co9S8 NS were further investigated in alkaline media. The corresponding results implied that M-doped Co4S3/Co9S8 NS (M = Fe3+, Cr3+, Mn2+ and Ni2+) exhibited different electrocatalytic properties. Evidenced by XPS spectra, the different OER activities were mainly aroused by the redistribution of charge at the interface due to an electronic interaction between the doped metal ions and Co4S3/Co9S8 NS.
Formic acid (FA), which can be produced via CO2 reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen content (4.4 wt%), and convenient storage/transportation. Designing highly efficient catalysts is the main challenge to realize the hydrogen production from FA. In this work, well-dispersed and electron-rich PdIr alloy nanoparticles with a size of 1.8 nm are confined in amino-modified 3D mesoporous silica KIT-6 and applied as a highly efficient catalyst for robust hydrogen production from FA at ambient temperature. Small PdIr alloy nanoparticles confined by amino-modified KIT-6 (PdIr/KIT-6-NH2) lead to better catalytic activity compared to that of Pd/KIT-6-NH2 and PdIr confined by bare KIT-6, achieving a high turnover frequency (TOF) value of 3533 h−1 at ambient temperature (303 K), 100% H2 selectivity and conversion toward the dehydrogenation of FA, which is comparable to the best heterogeneous catalysts ever reported. The high catalytic activity of PdIr/KIT-6-NH2 can be attributed to the synergistic effect between Pd and Ir, strong interaction between PdIr and KIT-6-NH2, as well as the amino-groups of KIT-6-NH2 which can act as a proton scavenger to promote the breaking of O-H bond of formic acid.
Developing all-solid-state polymer electrolytes (SPEs) with high electrochemical performances and stability is of great importance for exploiting of high energy density and safe batteries. Herein, ether linkage and imidazolium ionic liquid (ILs) are incorporated into the multi-armed polymer backbone though the series and parallel way. The parallel polymeric ionic liquid (P-P (PEGMA-IM)) maximizes the synergistic effect of ILs and ether linkage, which endowed the material with low crystallinity and high flame retardancy. The P-P (PEGMA-IM) based P-SPE presents a high ionic conductivity of 0.489 mS/cm at 60 ℃, an excellent lithium-ion transference number of 0.46 and a wide electrochemical window of 4.87 V. The assembled lithium metal battery using P-SPE can deliver a capacity of 151 mAh/g at 0.2 C, and the capacity retention ratio reaches 82% with a columbic efficiency beyond 99%. The overpotential of P-SPE based symmetric battery is 0.08 V, and there is no apparent magnifying even after 130 h cycling. This new design provides a new avenue for exploitation of advanced SPEs for the next-generation batteries.
Increasing active metal sites is a valid approach to improve the catalytic activity of the catalyst. Co3+ is the main active metal site of Co-based catalysts. In this research work, through the partial transformation of CoFePBA (CFP) via low-temperature heat treatment, the effective control of the Co3+/Co2+ ratio has been achieved. The partial transformation strategy of low-temperature heat treatment can not only maintain the original framework structure of CFP, but also increase more active sites. The characterization results show that the CFP-200 sample obtained via heat treatment at 200 ℃ for 2 h under N2 atmosphere has the highest Co3+/Co2+ ratio. As an oxygen evolution reaction electrocatalyst, CFP-200 shows the best electrocatalytic activity among all samples. In 1.0 mol/L KOH electrolyte, the overpotential is 312 mV at a current density of 10 mA/cm2. Therefore, low-temperature heat treatment provides an effective method for preparing low-cost and high-efficiency electrocatalysts.
Molecules with multifunctional properties are of immense interest in hybrid materials, while challenges still existed because of the limited compatibility of multiple functionalities in a single system. In this work, a series of metal-organic complexes were synthesized and characterized under the assembly of electron donor phosphonate, electron acceptor polypyridine ligand and spin carrier rare earth ions. All the compounds exhibited remarkable and reversible responses with photochromism and photomodulated fluorescence, originated from photogenerated radicals via electron transfer from phosphonates to polypyridine ligands. For the Dy analog, slow magnetic relaxation was observed at cryogenic temperature, indicating the single-molecule magnetic behavior. Furthermore, photogenerated radicals could enhance the proton conductive behavior, with about 2 times larger in magnitude after light irradiation for Dy and Y compounds. The introduction of photoluminescence, magnetism and proton conduction into metallic phosphonates can provide potential applications for photochromic materials.
Deuteration of hydrogen-bonded phase transition crystals can increase the transition temperatures due to the isotope effect. But rare examples show the opposite trend that originates from the structural changes of the hydrogen bond, known as the geometric H/D isotope effect. Herein, we report an organic crystal, diethylammonium hydrogen 1,4-terephthalate, exhibits a reversible structural phase transition and dielectric switching. Structural study shows the cations reside in channels formed by one-dimensional hydrogen-bonded anionic chains and undergo an order-disorder transition at around 206 K. The deuterated counterpart shows an elongation of the O···O hydrogen bond by about 0.005 Å. This geometric isotope effect releases the internal pressure of the anionic host on the cation guests and results in a downward shift of the phase transition temperature by 10 K.
All-inorganic CsPbI2Br perovskite with suitable bandgap and excellent thermal stability has been reported as the most promising candidate for efficient perovskite solar cells (PSCs). However, the high annealing temperature (> 250 ℃) and poor stability of α-CsPbI2Br greatly limit the future application in photovoltaic field. Herein, a facile method is reported to prepare α-CsPbI2Br perovskite film with high stability at low temperature (70 ℃) by incorporating a small amount of γ-aminobutyric acid (GABA) in the precursor solutions. The devices exhibit reproducible photovoltaic performance with a champion efficiency up to 15.16%, along with the excellent stability, maintaining more than 80% of its initial efficiency after stored in ambient condition for 600 h without any encapsulation. Most importantly, the method enables fabrication of semitransparent CsPbI2Br PSCs with a PCE of 6.76%, as well as an average visible transparency (AVT) of 25.38%. To the best of our knowledge, this is the first attempt to apply CsPbI2Br to the semitransparent solar cells.
In recent years, especially when there is increasing concern about the safety issue of lithium-ion batteries (LIBs), aqueous Zn-ion batteries (ZIBs) have been getting a lot of attention because of their cost-effectiveness, materials abundance, high safety, and ecological friendliness. Their working voltage and specific capacity are mainly determined by their cathode materials. Vanadium oxides are promising cathode materials for aqueous ZIBs owing to their low cost, abundant resources, and multivalence. However, vanadium oxide cathodes still suffer from unsatisfactory capacity, poor stability, and low electrical conductivity. In this work, cascading V2O3/nitrogen doped carbon (V2O3/NC) hybrid nanosheets are prepared for high-performance aqueous ZIBs by pyrolyzing pentyl viologen dibromide (PV) intercalated V2O5 nanosheets. The unique structure features of V2O3/NC nanosheets, including thin sheet-like morphology, small crystalline V2O3 nanoparticles, and conductive NC layers, endow V2O3/NC with superior performance compared to most of the reported vanadium oxide cathode materials for aqueous ZIBs. The V2O3/NC cathode exhibits the discharge capacity of 405 mAh/g at 0.5 A/g, excellent rate capability (159 mAh/g at 20 A/g), and outstanding cycling stability with 90% capacity retention over 4000 cycles at 20 A/g.
Sodium-ion batteries (SIBs) are promising alternatives to lithium-ion batteries (LIBs) for large-scale energy storage considering the abundance and low cost of Na-containing resources. However, the energy density of SIBs has been limited by the typically low specific capacities of traditional intercalation-based cathodes. Metal fluorides, in contrast, can deliver much higher capacities based on multi-electron conversion reactions. Among metal fluorides, CuF2 presents a theoretical specific capacity as high as 528 mAh/g while its Na-ion storage mechanism has been rarely reported. Here, we report CuF2 as a SIB cathode, which delivers a high capacity of 502 mAh/g but suffers from poor electrochemical reversibility. As a solution, we adjust the cell configuration by inserting a carbon-coated separator, which hinders the transportation of dissolved Cu ions and improves the reversibility of the CuF2 cathode. By using in-situ XRD measurements and theoretical calculation, we propose that a one-step conversion reaction occurs during the discharge process, and a reconversion reaction competes with the oxidization of Cu to dissolved Cu ion during the charge process.
Morphology-controlled electrocatalysts with the ability of CO2 adsorption/activation, mass transfer, high stability and porosity are much desired in electrochemical CO2 reduction reaction (CO2RR). Here, three kinds of multi-dimensional nanostructures (i.e., hollow sphere, nanosheets and nanofibers) have been successfully produced through the modulation of porphyrin-based covalent organic frameworks (COFs) with various modulators. The obtained nanostructures with high-stability, large surface-area, and single metal sites enable efficient CO2RR into CH4. Notably, they all exhibit higher FE (hollow sphere, 68.2%; nanosheet, 64.2% and nanofiber, 71.0%, −0.9 V) than COF-366-Cu (43.0%, −0.9 V) after morphology control. Noteworthy, the FE of COF-366-Cu (HS) keeps higher than 52.4% over a wide potential range from −0.9 V to −1.1 V and the achieved FECH4+C2H4 (82.8%, −0.9 V) is superior to most of reported COFs and copper-based electrocatalysts. This work paves a new way in the exploration of COF-based multi-dimensional nanostructures applicable in efficient CO2RR to CH4.
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