Latest ArticlesDeveloping transition metal oxides (TMOs) with high energy, power, and long cycle lifetime for electric energy storage devices remains a critical challenge to date. Herein, we demonstrate a facile method that enables in-situ transformation of nickel cobalt oxide nanowire arrays (NiCoO NWA) into hierarchical nanowire-nanosheet arrays (ac-NiCoO NWSA) for enhanced energy storage properties. More specifically, the method leads to formation of atomically thin nanosheets (only 2.0 nm) and creates abundant antisite defects and oxygen vacancies. Owing to these merits, the as-prepared ac-NiCoO NWSA electrode exhibits over five-fold higher specific capacity, superior rate capability (up to 100 A/g), and excellent cycling stability of 10, 000 cycles at 50 A/g in alkaline electrolyte compared to pristine NiCoO NWA. Density functional theory (DFT) simulations elucidate the electrochemical activity enhancement mechanism of the TMOs. Moreover, our method triggers similar structural reconstruction phenomenon on other TMOs including ZnCo-, CoMn- and ZnNiCo-oxides, proving the universality of the method. Our findings provide a general method towards simultaneously manipulating the micro-morphologies and defects of TMOs for advanced energy storage devices.
A new relay C–H functionalization of di([1, 1′-biphenyl]-2-yl)phosphine oxide to obtain esterified and hydroxylated products with different hypervalent iodines as oxidants under palladium catalysis is disclosed. This reaction provides a more effective and concise strategy for the synthesis of novel structural hybrid-arylcyclophosphorus ligand precursors with a wide range of substrates and good functional group tolerance.
Aqueous zinc anodes have attracted the attention of many researchers owing to their high safety, low cost, and high theoretical specific capacity. However, its practical application is severely limited by the dendrite growth on zinc anode. Herein, we develop an intrinsically zincophobic barium-titanate protective layer with a porous structure to suppress the zinc dendrite formation by homogenizing the ion distribution on the anode surface, increasing the nucleation sites, and limiting the irregular zinc growth. Based on these synergistic effects, the coated zinc anode can exhibit long cycle life (840 h at 0.5 mA/cm2 for 0.5 mAh/cm2) and low voltage hysteresis (36 mV). This work can provide a feasible direction for the design of intrinsically zincophobic coating materials to uniformize the zinc stripping and plating.
Electrochemical carbon dioxide reduction (CO2RR) plays an important role in solving the problem of high concentration of CO2 in the atmosphere and realizing carbon cycle. Core-shell structure has many unique features including tandem catalysis, lattice strain effect, defect engineering, which exhibit great potential in electrocatalysis. In this review, we focus on the advanced core-shell metal-based catalysts (CMCs) for electrochemical CO2RR. The recent progress of CMCs in electrocatalytic CO2RR is described as the following aspects: (1) The mechanism of electrochemical CO2RR and evaluation parameters of electrocatalyst performance, (2) preparation methods of core-shell metal catalysts and core-shell structural advantages and (3) advanced CMCs towards electrochemical CO2RR. Finally, we make a brief conclusion and propose the opportunities and challenges in the field of electrochemical CO2RR.
Catalytic potential of carbon nanomaterials in peroxydisulfate (PDS) advanced oxidation systems for degradation of antibiotics remains poorly understood. This study revealed ordered mesoporous carbon (type CMK) acted as a superior catalyst for heterogeneous degradation of sulfadiazine (SDZ) in PDS system, with a first-order reaction kinetic constant (k) and total organic carbon (TOC) mineralization efficiency of 0.06 min-1 and 59.67% ± 3.4% within 60 min, respectively. CMK catalyzed PDS system exhibited high degradation efficiencies of five other sulfonamides and three other types of antibiotics, verifying the broad-degradation capacity of antibiotics. Under neutral pH conditions, the optimal catalytic parameters were an initial SDZ concentration of 44.0 mg/L, CMK dosage of 0.07 g/L, and PDS dosage of 5.44 mmol/L, respectively. X-ray photoelectron spectroscopy and Raman spectrum analysis confirmed that the defect structure at edge of CMK and oxygen-containing functional groups on surface of CMK were major active sites, contributing to the high catalytic activity. Free radical quenching analysis revealed that both SO4·- and ·OH were generated and participated in catalytic reaction. In addition, direct electron transfer by CMK to activate PDS also occurred, further promoting catalytic performance. Configuration of SDZ molecule was optimized using density functional theory, and the possible reaction sites in SDZ molecule were calculated using Fukui function. Combining ultra-high-performance liquid chromatography (UPLC)–mass spectrometry (MS)/MS analysis, three potential degradation pathways were proposed, including the direct removal of SO2 molecules, the 14S-17 N fracture, and the 19C-20 N and 19C-27 N cleavage of the SDZ molecule. The study demonstrated that ordered mesoporous carbon could work as a feasible catalytic material for PDS advanced oxidation during removal of antibiotics from wastewater.
The development of efficient method to prepare poly(silyl ether)s (PSEs) is highly desirable. Herein, an environmentally sustainable copper-catalyzed dehydrocoupling polymerization was developed with good yields and high molecular weight (up to 48, 400 of Mn and up to 97% yield). Monomers of different types (AB type or AA and BB type) are suitable to afford PSEs. The PSEs show good thermal stability and low glass-transition temperature.
A copper-catalyzed three-component reaction of alkenes, cycloketone oximes and DABCO·(SO2)2 is developed, which provides a convenient route for the synthesis of diverse (E)-cyanoalkylsulfonyl alkenes in moderate to good yields with excellent regio- and stereoselectivity. A broad substrate scope with excellent functional group tolerance is observed. A plausible radical pathway is proposed, which involves copper-catalyzed ring-opening CC bond cleavage of O-acyl oxime and insertion of sulfur dioxide. During the reaction process, cyanoalkyl radical and cyanoalkylsulfonyl radical are the key intermediates.
The increase of atmospheric CO2 concentration has caused many environmental issues. Electrochemical CO2 reduction reaction (CO2RR) has been considered as a promising strategy to mitigate these challenges. The electrocatalysts with a low overpotential, high Faradaic efficiency, and excellent selectivity are of great significance for the CO2RR. Carbon-based materials including metal-free carbon catalysts and metal-based carbon catalysts have shown great potential in the CO2RR, owing to the tailorable porous structures, abundant natural resources, resistance to acids and bases, high-temperature stability, and environmental friendliness. In this review, various carbon materials including graphene, carbon nanotubes, quantum dots, porous carbon, and MOF-derived catalysts, etc., for the CO2RR have been summarized. Particularly, recent progress in terms of the mechanism and pathway of CO2 conversion has been comprehensively reviewed. Finally, the opportunities and challenges of carbon-based electrocatalysts for the CO2RR are proposed.
Biomedicine is one of the fastest growing areas of additive manufacturing. Especially, in the field of in vitro diagnostics (IVD), contributions of 3D printing include ⅰ) rapid prototyping and iterative IVD proof-of-concept designing ranging from materials, devices to system integration; ⅱ) conceptual design simplification and improved practicality of IVD products; ⅲ) shifting the IVD applications from centralized labs to point-of-care testing (POCT). In this review, the latest developments of 3D printing and its advantages in IVD applications are summarized. A series of 3D-printed objects for IVD applications, including single-function modules, multi-function devices which integrate several single-function modules for specific analytical applications such as sample pre-treatment and chemo-/bio-sensing, and all-in-one systems which integrate multi-function devices and the instrument operating them, are analyzed from the perspective of functional integration. The current and potential commercial applications of 3D-printed objects in the IVD field are highlighted. The features of 3D printing, especially rapid prototyping and low start-up, enable the easy fabrication of bespoke modules, devices and systems for a range of analytical applications, and broadens the commercial IVD prospects.
Monovalent cation perm-selective membrane (MCPMs) allow fast and selective transport of monovalent cations, and they are promisingly required for extraction of special ions, such as lithium extraction, acid recovery and sea salt production. Herein, we report a novel strategy to design the critical functional layers of MCPMs with both space charge repulsion and cross-linked dense screenability. The in-situ deposition polymerization of pyrrole was carried out on the surface of sulfonated polyphenyl sulfone (SPPSU) substrate membrane followed by cross-linking quaternization of the polypyrrole (PPy) layer with diiodinated functional molecules, thus, the membrane obtained more excellent selective permeability and stable transport properties of monovalent cations. It confirms that the designed PPy layers with charged surface and cross-linking structure improved the hydrophilicity, facilitated cation transport and increased ion flux. Meanwhile, for the dense PPy layer, the charged cross-linked structure endowed the functional layer with the synergistic characteristics of Donnan exclusion and pore size sieving for positively charged ions, which improved the monovalent cation perm-selectivity of the membranes. At a constant current density of 5.1 mA/cm2, the optimal membrane exhibited superior perm-selectivity (PMgNa) and monovalent cation flux (JNa+ = 2.80×10 -8 mol cm-2 s-1) during electrodialysis.
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