Latest ArticlesA dual-readout sensing platform based on two signal transduction channels can integrate the unique advantages of each sensing pattern, compensate for the deficiency in the adaptive capacity, and enable a more convincing performance in analytical applications. Here, we introduce a responsive molecule dye, xylenol orange (XO), to combine with lanthanide terbium ions (Tb3+). The resultant Tb3+-XO complex exhibited tunable optical properties and was used as a novel colorimetric and luminometric dual-readout sensing platform for assaying the anthrax biomarker, dipicolinic acid (DPA). In the presence of Tb3+, the XO solution underwent a color change from yellow to magenta; however, upon adding DPA, the color changed back to yellow immediately, accompanied by the characteristic luminescence emission of Tb3+. Considering the strong affinity between DPA/XO and metal ions, the proposed sensing platform was further employed for the determination and differentiation of certain metal ions using linear discriminant analysis. This convenient dual-readout sensing platform offers several notable features and significantly promotes the application and development of lanthanide-based materials.
Sluggish kinetics of lithium/sulfur (Li/S) conversion chemistry and the ion channels formation in the cathode is still a bottleneck for developing future Li/S batteries with high-rate, long-cycling and high-energy. Here, a rational cathode structure design of an oxygen (O) and nitrogen (N) tailoring carbon fiber aerogel (OCNF) as a host material integrated with platinum (Pt) electrocatalysis interface is employed to regulate Li/S conversion chemistry and ion channel. The Pt nanoparticles were uniformly sprayed onto the S surface to construct the electrocatalysis interface (Pt/S/OCNF) for generating ion channels to promote the effective penetration of electrolyte into the cathode. This Pt/S/OCNF gives the cathode a high sulfur utilization of 77.5%, an excellent rate capacity of 813.2 mAh/g (2 C), and an outstanding long-cycling performance with a capacitance retention of 82.6% and a decay of 0.086% per cycle after 200 cycles at 0.5 C. Density functional theory (DFT) calculations reveal that the Pt electrocatalysis interface makes the cathode a high density of state (DOS) at Fermi level to facilitate the electrical conductivity, charge transfer kinetics and electrocatalysis to accelerate the lithium polysulfides (LiPSs) electrochemical conversion. Furthermore, the unique chemisorption structure and adsorption ability of Li2Sn (n = 1, 2, 4, 6, 8) and S8 on OCNF are attributed to the bridging effects of interfacial Pt and the bonding of N-Li. The Pt electrocatalysis interface combined with the unique 3D hierarchical porous structure and abundant functional active sites at OCNF guarantee strong adsorption confinement, fast Li/S electrocatalytic conversion and unblocked ion channels for electrolyte permeation in cathode.
In this study, through direct pyrolysis of a nitrogen-rich metal-organic framework of Fe-BTT at different temperatures and followed by acid treatment, we prepared a series of Fe–N–CT (T = 800–1000 ℃) composite catalysts with uniform cubic morphology and homogeneously distributed active sites. Acid leaching leads to the removal of excess Fe NPs and the exposure of more pyridinic N and porphyrin-like Fe–Nx sites and creates a higher specific surface area. Structural and electrochemical performance test results showed that Fe–N–C900 catalyst exhibited the highest selectivity for CO product at –1.2 V vs. Ag/AgCl, with 496 mV of overpotential and 86.8% of Faraday efficiency, as well as excellent long-term stability, due to the good inheritance from rich-N Fe–BTT precursor.
Nickel cobalt bimetallic heterogeneous sulfides are attractive battery-type materials for electrochemical energy storage. However, the precise synthesis of electrode materials that integrate highly efficient ions/electrons diffusion with abundant charge transfer channels has always been challenging. Herein, an effective and concise controllable hydrothermal approach is reported for tuning the crystalline and integrated structures of MOF-derived bimetallic sulfides to accelerate the charge transfer kinetics, and thus enabling rich Faradaic redox reaction. The as-obtained low-crystalline heterogeneous NiCo2S4/Co3S4 nanocages exhibit a high specific capacity (1023 C/g at 1 A/g), remarkable rate performance (560 C/g at 10 A/g), and outstanding cycling stability (89.6% retention after 5000 cycles). Furthermore, hybrid supercapacitors fabricated with NiCo2S4/Co3S4 and nitrogen-doped reduced graphene oxide display an outstanding energy density of 40.8 Wh/kg at a power density of 806.3 W/kg, with an excellent capacity retention of 88.3% after 10000 charge-discharge cycles.
Supramolecular chemistry has received considerable attention in host-guest recognition. The structure-response relationship of host-guest recognition system is a meaningful issue. Herein, a series of tripodal nitrogen mustard derivatives (TMs) have been developed in this paper. By rationally design the intramolecular alkyl chain lengths of host, the host-guest binding model have been successfully tuned, which underwent a transformation from π-π to multiple hydrogen bonds. This process enhances the host-guest binding force and recognition efficiency.
The production of CH3COOH from CO2 and CH4 has stimulated much interest due to the high energy density of C2 species. Various kinds of catalysts have been developed while the high dissociation barrier of CH4 and low selectivity still hinders the efficiency of the reaction. We have herein proposed a novel catalyst with single metals loaded on 2D BC3N2 substrate (M@2D-BC3N2) based on density functional theory. Among numerous candidates, Pt@2D-BC3N2 possesses the most favorable reactivity with an ultralow barrier of CH4 splitting (0.26 eV), which is due to the efficient capture ability of CH4 on Pt site. Besides, the selectivity for CH3COOH is also very high, which mainly stems from the unique electronic properties of molecules and substrate: The degenerated states, including s, px, py and pz, in CO2 reflects the existence of delocalized π bonds between C and O. This can interact with states of Pt(s), Pt(pz), Pt(dxz), Pt(dyz), and Pt(z2) in Pt@2D-BC3N2. The kinetics model also proves that our system can promote CH3COOH production via simply increasing the temperature or the coverage of CH4 and CO2. Our results provide a reasonable illustration in clarifying mechanism and propose promising candidates with high reactivity for further study.
Heterogeneous catalysis is a vivid branch of traditional catalysis field, with the advantage of high efficiency and being easily separated from reactants and products after reaction, and have received widespread attentions in large-scale industrial production, especially in the field of energy utilization. Boron has been found to be a key functional component for designing high-performance heterogeneous catalysts. In this review, we cover and categorize the past and recent progress in boron-containing materials and their applications in heterogeneous catalysis particularly in energy‐related fields. The fundamental roles of boron components in the emerging heterogeneous catalysis of construction, regulation and stabilization of active phases/sites are highlighted, with the emphasis on how they regulating structural and electronic properties of host materials. We then categorize boron-containing catalysts into six kinds mainly including intermetallic boride catalysts, metal boride-derived catalysts, boron-doped catalysts, metal boride-decorated catalysts, boron-containing compounds as catalyst supports, and single-boron-site catalysts, as well as try to establish structure-catalytic activity relationship. The catalytic applications of these six boron-containing catalysts are discussed separately, focusing on the energy-related reactions such as hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO2RR) and nitrogen reduction reaction (NRR). Finally, the opportunities and challenges related to boron-containing compounds in the field of catalysis are prospected.
The transformation of quantum dots (QDs) by organisms has attracted broad attention but remains unclear. Understanding of the metabolites helps to reveal the transformation pathway of QDs. Cd containing-metallothionein (MT) are the main species formed by Cd released from CdSe QDs in HepG2 cells, while speciation analysis of Cd containing MTs remains a challenge because MTs has several subisoforms and can bind with several metals. Herein, we built a hyphenated platform for speciation analysis of QDs in HepG2 cells after treatment with CdSe/ZnS QDs. The Cd-containing MTs were separated in reversed phase high performance liquid chromatography (RP-HPLC) and subsequently online detected by inductively coupled plasma mass spectrometry (ICP-MS) and electrospray ionization quadrupole time-of-flight mass spectrometry (ESI-Q-TOF-MS) parallelly. Four groups of Cd-containing metabolites were found by detecting Cd in ICP-MS. Their structures were identified in ESI-Q-TOF-MS and further confirmed with standards of four subisoforms of MT, including N-terminal acetylation MT2a, N-terminal acetylation MT1e, N-terminal acetylation MT1g and MT1m. Each group of them contains various stoichiometry of Cd/Zn. The metabolites of QDs remain same while the concentrations of each metabolite and its stoichiometry of Cd/Zn vary for different incubation concentration/time. This work provides a new parallel hyphenation technique of HPLC-ICP-MS/ESI-MS with high separation resolution and powerful detection ability, and the obtained results provide detailed metabolism information of QDs in HepG2 cells after treatment of CdSe/ZnS QDs, contributing to deep exploration of the functional mechanisms of QDs in organisms.
NH3 plays an essential role in human life since it is an important raw material for fertilizers, plastics and rubbers production. As an NH3 synthesis technology under ambient conditions, electrocatalytic N2 reduction reaction (NRR) has great potential to replace the energy-intensive Haber-Bosch process. The key of electrocatalytic NRR is the exploration of efficient catalysts. Transition metal Mo is promising since it exists naturally in nitrogenase due to the unique Mo-N2 interaction; particularly in the form of 2D material such as MoSe2, the surface area is maximized for more active sites. However, the NRR performance of MoSe2 is still unsatisfactory because Mo is only exposed at the semi-open edge, and the electronegative Se-mantled surface area remains inaccessible to N2. Herein, we propose a simple and effective strategy to create high-concentration Se vacancies in MoSe2 through heteroatom doping induced lattice strain, which effectively enhances the Mo-N2 interaction on the surface area. In result, high NH3 yield (3.04 × 10–10 mol s–1 cm–2) and Faraday efficiency (21.61%) are attained at –0.45 V vs. RHE in 0.1 mol/L Na2SO4.
Chemical fixation of CO2 into C1 source, as a general approach, can effectively alleviate the emission of greenhouse gasses. Whereas, the challenge posed by the need for efficient catalysts with high catalytic active sites still exists. In this work, we reported a series of new hexavanadate clusters, [(C6H6ON)2(C2H8N2)2(CH3O)6V6IVO8] (V6–1), [(C6H6ON)2(C3H10N2)2(CH3O)6V6IVO8] (V6–2), [(C6H6ON)2(C6H14N2)2(CH3O)6V6IVO8] (V6–3) and [(C6H6ON)2(C4H11N2O)2(CH3O)4V6IVO8] (V6–4), assembled by 2-aminophenol and four different kinds of Lewis bases (LB), ethanediamine (en), 1,2-diaminopropane, 1,2-cyclohexanediamine and N-(2-hydroxyethyl)ethylenediamine (ben) together. Among them, the basic unit {V6} cluster featured Z-shaped configuration represents a brand-new example of hexanuclear vanadium clusters. Remarkably, the catalytic tests demonstrated that V6–1 as catalyst displays high catalytic activity in the cycloaddition for the CO2 fixation into cyclic carbonates by virtue of open V sites. As expected, for oxidative desulfurization of sulfides, V6–1 also exhibits satisfied catalytic effectiveness. Furthermore, the recycling test confirmed that catalyst V6–1 may be a bifunctional heterogeneous catalyst with great promise for both CO2 cycloaddition and oxidative desulfurization reactions.
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