Latest ArticlesStructural and functional biomimicking of the active site of [NiFe]-hydrogenases can provide helpful hints for designing bioinspired catalysts to replace the expensive noble metal catalysts for H2 generation and uptake. Treatment of dianion [Ni(phma)]2- [H4phma = N, N'-1, 2-phenylenebis(2-mercaptoacetamide)] with [NiCl2(dppp)] (dppp = bis(diphenylphosphino)propane) yielded a dinickel product [Ni(phma)(μ-S, S')Ni(dppp)] (1) as the model complex relevant to the active site of [NiFe]-H2ases. The structure of complex 1 has been characterized by single-crystal X-ray analysis. From cyclic voltammetry and controlled potential electrolysis studies, complex 1 was found to be a moderate electrocatalyst for the H2-evoluting reaction using ClCH2COOH as the proton source.
Alloy and small size nanostructures are favorable to catalytical performance, but not to surface-enhanced Raman spectroscopy (SERS) applications. Integrating SERS and catalytic activity into the nanocrystals with both alloy and small size structures is of great interest in fabrication of SERS platform to in situ monitor catalytical reaction. Herein, we report a facile method to synthesize Au@AgPd trimetallic nanoflowers (Au@AgPd NFs) with both SERS and catalytic activities, through simultaneous selective growth of Ag and Pd on Au core to form highly-branched alloy shell. These nanocrystals have the properties of small sizes, defects abundance, and highly-dispersed alloy shell which offer superior catalytic activity, while the merits of monodisperse, excellent stability, and highly-branched shell and core/alloy-shell structure promise the enhanced SERS activity. We further studied their growth mechanisms, and found that the ratio of Ag to Pd, sizes of Au core, and surfactant cetyltrimethylammonium bromide together determine this special structure. Using this as-synthesized nanocrystals, a monolayer bifunctional platform with both SERS and catalytical activity was fabricated through selfassembly at air/water interface, and applied to in situ SERS monitoring the reaction process of Pd-catalyzed hydrogenation of 4-nitrothiophenol to 4-aminothiophenol.
Metal-organic frameworks (MOFs), as an emerging family of porous inorganic-organic crystal materials, exhibit widely applications in gas storage and separation, drug release, sensing, and catalysis, owing to easily adjustable pore sizes, uniformly distributed metal centers, high surface areas, and tunable functionalities. However, MOF crystal powders are usually difficult to be directly applied into specific devices because of their brittleness, insolubility and low compatibility. Therefore, to expand versatile MOF membranes with robustness and operational flexibility is urgent to satisfy practical applications. Although numerous reports have reviewed the synthesis and applications of MOF membranes, relatively few reports the electrocatalytic properties based on MOF membranes. Herein, this mini-review provides an overview of preparation of MOF membranes, including directed synthesis, secondary growth and electrochemical deposition method. Meanwhile, fabrication of ultrathin 2D MOF nanosheets those can be also defined as a kind of nanoscale MOF membranes is also mentioned. Electrocatalytic performance of oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER) and CO2 reduction reaction (CO2RR) for diverse MOF membranes/nanosheets and their derivatives are introduced.
Tailored design and synthesis of high-quality electrocatalysts is vital for the advancement of oxygen evolution reaction (OER). Herein, we report a powerful puffing method to fabricate hierarchical porous N-doped carbon with numerous embedded Ni nanoparticles. Interestingly, during the puffing and annealing process, rice precursor with N and Ni sources can be in-situ converted into Niembedded N-doped porous carbon (N-PC/Ni) composite. The obtained N-PC/Ni composite possesses a cross-linked porous architecture containing conductive carbon backbone and active Ni nanoparticles electrocatalysts for OER. The pore formation in N-PC/Ni composite is also proposed because of carbothermic reduction. The N-PC/Ni composite is fully studied as electrocatalysts for OER. Due to increased active surface area, enhanced electronic conductivity and reactivity, the designed N-PC/Ni composite exhibits superior OER performance with a low Tafel slope (~88 mV/dec) and a low overpotential as well as excellent long-term stability in alkaline solution. Our proposed rational design strategy may provide a new way to construct other advanced metal/heteroatom-doped composites for widespread application in electrocatalysis.
In recent decades, the properties and behaviors of nanofluidic devices have been widely explored in varied subjects such as engineering, physics, chemistry, and biology. Among the rich properties of nanofluidics, ionic current rectification (ICR) is a unique phenomenon arising from asymmetric nanofluidic devices with electric double layer (EDL) overlapped. The ICR property is especially useful in applications including energy conversion, mass separation, sea water purification and bioanalysis. In this review, the ICR property in nanofluidics as well as the underlying mechanism is demonstrated. The influencing factors concerning to the ICR property are systematically summarized. The asymmetric geometry as well as the charge distribution is in charge of the ICR behavior occurring in nanofluidic devices. This review is aimed at readers who are interested in the fundamentals of mass transport in nanofluidics in general, as well as those who are willing to apply nanofluidics in various research fields.
In the past few years, the increasing energy consumption of traditional fossil fuels has posed a huge threat to human health. It is very imperious to develop the sustainable and renewable energy storage and conversion devices with low cost and environment friendly features. Hybrid supercapacitors are emerging as one of the promising energy devices with high power density, fast charge-discharge process and excellent cycle stability. However, morphology and structure of the electrode materials exert serious effect on their electrochemical performances. In this review, we summarized recent progresses in transition metal oxide based electrode materials for supercapacitors. Different synthesis routes and electrochemical performances of electrode materials and storage mechanisms of supercapacitor devices have been presented in details. The future developing trends of supercapacitor based on metal oxide electrode materials are also proposed.
Access to safe drinking water has become an extremely urgent research topic worldwide. In recent years, the technology of solar vapor generation has been extensively explored as a potential and effective strategy of transforming elements content in seawater. In this review, the basic concepts and theories of metal-based photothermal vapor generation device (PVGD) with excellent optical and thermal regulatory are introduced. In the view of optical regulation, how to achieve high-efficiency localized evaporation in different evaporation system (i.e., volumetric solar heating and interface solar heating) is discussed; from the aspect of thermal regulation, the importance of selective absorption surface for interfacial PVGD is analyzed. Based on the above discussion and analysis, we summarize the challenges of metal-based desalination device.
Dual ion batteries (DIBs) exhibit broad application prospects in the field of electrical energy storage (EES) devices with excellent properties, such as high voltage, high energy density, and low cost. In the graphitebased DIBs, high voltage is needed to store enough anions with the formation of anion intercalation compound XCn (X = AlCl4-, PF6-, TFSI-, etc.). Hence, it is difficult for graphite-based DIBs to match proper anodes and electrolytes. Here, an Se/graphene composite is prepared via a convenient method, and assembled into a dual-ion full battery (DIFB) as anode with graphite cathode and 1 mol/L NaPF6 in EC: EMC (1:1, v:v). This DIFB has achieved a high discharge capacity of 75.9 mAh/g and high medium output voltage of 3.5 V at 0.1 A/g. Actually, the suitable anode materials, such as the present Se/graphene composite, are extremely important for the development and application of graphite-based DIBs. This study is enlightening for the design of future low-cost EES devices including graphite-based DIBs.
Facile achievement of gold nanorods (AuNRs) with controllable longitudinal surface plasmon resonance (LSPR) is of great importance for their applications in various fields. The LSPR of AuNRs is sensitive to their aspect ratio, which is still hard to be precisely tuned by direct synthesis. In this work, we report a simple approach for end-selective etching of AuNRs by a rapid oxidation process with Au(Ⅲ) in cetyltrimethylammonium bromide (CTAB) solution at a mild temperature. The LSPR wavelength and the length of AuNRs blue shifted linearly as a function of the amount of Au(Ⅲ), while the diameter of AuNRs remained nearly constant. The oxidative rate is temperature dependent, and the oxidative process for a desired LSPR can be accomplished within 15 min at 60 ℃. Further investigations indicated that Br- determine the occurrence of the oxidation between AuNRs and Au(Ⅲ), and a small amount of surfactant chain (CTA+) is crucial for stabilizing AuNRs. This method presents a quick but robust strategy for acquiring AuNRs with an arbitrary intermediate LSPR wavelength using the same starting AuNRs, and can be a powerful tool for subsequent applications.
Potassium-ion capacitors (KICs) emerge as a promising substitute for the well-developed lithium-ion capacitors (LICs), however, the energy density of KICs is below expectations because of lacking a suitable electrical double-layer positive electrode. Using chemical activation of the Aldol reaction product of acetone with KOH, we synthesized a porous carbon with a Brunauer-Emmett-Teller surface area of up to 2947 m2/g and a narrow pore size distribution ranging from 1 nm to 3 nm. Half-cell (versus potassium metal) test demonstrates that this porous carbon has high capacitive performance in K+ based organic electrolytes. Furthermore, a novel KIC fabricated by this porous carbon as the cathode, yields high values of energy density and power density. The processes used to make this porous carbon are readily low-cost to fabricate metal-ion capacitors.
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