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Graphene oxide (GO) is an excellent chemical tunable optical platform for imaging and sensing. The photoluminescence (PL) quantum yield of GO is relatively low, which limited the application of the intrinsic and tunable fluorescence from GO. Here, we report the first case of metal-enhanced fluorescence (MEF) of GO. A significant enhancement (~10-fold) in fluorescence intensity is observed from GO on the Ag substrate as compared to that on the glass. FL, Raman, and SEM images are used to investigate the MEF behavior and are coincident with each other. The influence of the metal particle size of Ag substrate is investigated. The fluorescence is also found to be responsive when adding different metal ions into GO solution. GO contacting directly with metal substrate exhibits strong MEF without quenching, which makes it possible to use GO sheets for three-dimension optical imaging and sensing.

Ultrasmall metal nanoparticles (MNPs) and atomically dispersed metal sites (ADMSs) exhibit excellent catalytic activity and selectivity. However, they tend to aggregate into large particles during synthesis and catalysis due to high surface free energy. Aiming to break out of this dilemma, zeolite imidazolate frameworks (ZIFs) have proved to be ideal substrates for stabilizing the ultrafine metal nanostructures. The stabilizing mode includes confining MNPs inside their pore structures and converting intrinsic metal nodes into coordinately unsaturated metal sites (i.e., ZIF‐confined metal catalysts). Furthermore, various MNPs and ADMSs can also be immobilized into ZIF‐derived porous carbon through high‐temperature pyrolysis (i.e., ZIF‐derived carbon‐supported metal catalysts). In brief, ZIFs and their derivatives have gradually emerged as good platforms for designing metal catalysts at nanoscale and even atomic level. In this review, recent progress in the structural analysis and synthetic strategies of metal catalysts supported by ZIFs and their derivatives is presented. Besides, current challenges and future directions of atomically dispersed metal catalysts are discussed. This article will provide valuable insights into rational design of metal catalysts with exquisite nanostructure and high catalytic performance to meet further material requirements in the catalytic field.

Due to a lack of focus on China’s financial decentralization system, the existing research does not pay attention to the beneficial contribution of Chinese local governments to carbon emission reduction through their actions in the financial field. In this study, we collected 16 years of data from 30 provinces in China and utilized a two-way fixed-effects model to empirically test the impact of China’s financial decentralization on carbon emission reduction. The regression results show that China’s financial decentralization system has a significant carbon-emission reduction effect. A heterogeneity analysis shows that this effect is common in different regions of China and that fiscal decentralization will negatively moderate it. A mechanism analysis shows that under China’s financial decentralization system, the active intervention of local governments in local finance will significantly upgrade the energy consumption structure and ease the financing constraints of enterprises. The regression results of the spatial econometric model show that the carbon emission reduction effect of China’s financial decentralization still has a spatial spillover effect. Finally, we put forward corresponding policy recommendations.

Radioactive ions with high-heat release or long half-life could cause long-term influence on environment and they might enter the food chain to damage human body for their toxicity and radioactivity. It is of great importance to develop methods and materials to detect and remove radioactive ions. Carbon dots and their composite materials has been applied widely in many fields due to their plentiful raw materials, facile synthesis and functional process, unique optical property and abundant functional groups. This comprehensive review focuses on the preparation of CDs and composite materials for the detection and adsorption of radioactive ions. Firstly, the recent-developed synthetic methods for CDs were summarized briefly, including hydrothermal/solvothermal, microwave, electrochemistry, microplasma, chemical oxidation methods, focusing on the influence of CDs properties. Secondly, the synthetic methods for CDs composite materials were classified to four categories and summarized generally. Thirdly, the application of CDs for radioactive ions detection and adsorption were explored and concluded including uranium, iodine, europium, strontium, samarium et al. Finally, the detection and adsorption mechanism for radioactive ions were searched and the perspective and outlook of CDs for detection and adsorption radioactive ions have been proposed based on our understanding.

A key challenge of photoregulated living radical polymerization is developing efficient and robust photocatalysts. Now carbon dots (CDs) have been exploited for the first time as metal-free photocatalysts for visible-light-regulated reversible addition-fragmentation chain-transfer (RAFT) polymerization. Screening of diverse heteroatom-doped CDs suggested that the P- and S-doped CDs were effective photocatalysts for RAFT polymerization under mild visible light following a photoinduced electron transfer (PET) involved oxidative quenching mechanism. PET-RAFT polymerization of various monomers with temporal control, narrow dispersity (Đ≈1.04), and chain-end fidelity was achieved. Besides, it was demonstrated that the CD-catalyzed PET-RAFT polymerization was effectively performed under natural solar irradiation.

Fluorescent polydopamine nanoparticles (FPD) are a kind of promising fluorescent nanoparticles for biosensing and imaging, while the rapid and controllable synthesis of FPD is still challenging. In this paper, we developed a microplasma electrochemistry strategy to regulate the oxidative polymerization process of dopamine, resulting in a controlled formation of FPD. Treating the dopamine solution with microplasma anode could not only generate oxidative species to trigger the nucleation of polydopamine nanoparticles at the plasma-liquid interface, but also provide an acidic environment to inhibit their further growing up during the diffusion process. Thus, uniform FPD with a diameter of 3.1 nm could be prepared within minutes. And, continuous generation of FPD could be achieved without the formation of aggregates when prolonging the reaction time. The obtained FPD had abundant functional groups on the surfaces, showing tunable fluorescent emission properties. These luminescent nanoparticles were demonstrated for highly selective detection of uranium with a detection limit of 2.1 mg/L. The novel microplasma electrochemistry strategy established in this work provided better opportunity for controllable synthesis of FPD, as well as other luminescent nanoparticles, and broadened their application in chemical sensing area.

An extensible multidimensional colorimetric sensor array for the detection of protein is developed based on DNA functionalized gold nanoparticles (DNA-AuNPs) as receptors. In the presence of different proteins, the aggregation behavior of DNA-AuNPs was regulated by the high concentrations of salt and caused different color change; while DNA-AuNPs grew induced by the reduction of HAuCl4 and NH2OH as a reductant on the surface of nanoparticles exhibited different morphologies and color appearance for different proteins. The transducers based on AuNPs modified by specific and nonspecific DNA enables naked-eye discrimination of the target analytes. This extensible sensing platform with only two receptors could simultaneously discriminate ten native proteins and their thermally denatured conformations using hierarchical cluster analysis (HCA) at the concentration of 50nM with 100% accuracy. This opens up the possibility of the sensor array to investigate the different conformational changes of biomacromolecules, and it gives a new direction of developing multidimensional transduction principles based on plasmonic nanoparticle conjugates. Furthermore, the sensing system could discriminate proteins at the concentration of 500nM in the presence of 50% human urine, which indicated this sensor array has great potential ability in analyzing real biological fluids. In addition, the multidimensional colorimetric sensor array is suitable for analysis of target analytes in the resource-restricted regions because of rapid, simple, low cost, and in-field detection with the naked eye.

The photophysical process of localized surface plasmon resonance (LSPR) is, for the first time, exploited for broadband photon harvesting in photo-regulated controlled/living radical polymerization. Efficient macromolecular synthesis was achieved under illumination with light wavelengths extending from the visible to the near-infrared regions. Plasmonic Ag nanostructures were in situ generated on Ag3 PO4 photocatalysts in a reversible addition-fragmentation chain transfer (RAFT) system, thereby promoting polymerization of various monomers following a LSPR-mediated electron transfer mechanism. Owing to the LSPR-enhanced broadband photon harvesting, high monomer conversion (>99 %) was achieved under natural sunlight within 0.8 h. The deep penetration of NIR light enabled successful polymerization with reaction vessels screened by opaque barriers. Moreover, by trapping active oxygen species generated in the photocatalytic process, polymerization could be implemented without pre-deoxygenation.

Molten salt electrolysis is normally conducted with solid anode, such as noble metal or graphite, which has defects such as high cost or emission of carbon oxide. Herein, we report that a microplasma based on atmospheric-pressure glow discharge could act as a kind of gaseous anode for electrolysis in molten salt. When the Ag/Ag+ redox couple was chosen as the research object, the microplasma anode could initiate charge-transfer reactions in the molten salt and Ag could be electrodeposited with current efficiency of above 90%. The microplasma anode has also shown excellent anticorrosive performance in both chloride and carbonate molten salt. Furthermore, the microplasma anode could potentially serve as an excitation source of atomic emission spectrometry (AES), making it possible to determine the concentration of Ag ions in the molten salt in situ and in real-time. With properties such as being carbon-free and having corrosion resistance and extensive utilization for analysis, the microplasma anode has ope...

Graphene oxide (GO) membranes with unique nanolayer structure have demonstrated excellent separation capability based on their size‐selective effect, but there are few reports on achieving ion–ion separation, because it is difficult to inhibit the swelling effect of GO nano sheets as well as to precisely control the interlayer spacing d to a specific value between the sizes of different metal ions. Here, selective separation of uranium from acidic radioactive waste containing multication is achieved through a precise dual‐adjustment strategy on d. It is found that GO swelling is greatly restricted in highly acidic solution due to protonation effect. Then the interlayer spacing is further precisely reduced to below the diameter of uranyl ion by increasing the oxidation degree of GO. Sieving uranyl ions from other nuclide ions is successfully realized in pH =3–3 mol L−1 nitric acid solutions., Precisely controlling the interlayer spacing of graphene oxide (GO) membrane in a wide range (11.4–15.5 Å) is realized by using a dual‐adjustment strategy of combining acidity with oxidation degree. Such GO membranes can successfully sieve uranyl ions from other nuclide ions in pH =3–3 mol L−1 HNO3 aqueous, showing their potential application in the treatment of highly acidic radioactive waste.

Photocatalysis-assist transition of uranium from soluble ions to insoluble nanoparticles is benefit for the extraction of uranium but has been rarely realized under air atmosphere. Here we developed a novel graphene aerogel (GA), GA-200, for the photocatalytic removal of uranium from water under visible light and air atmosphere for the first time. By controlling the reduction degree, GA-200 remained numbers of functional groups for anchoring uranium and possessed high photocurrent response and narrow band gap to generate and transfer electrons/holes readily. Under visible light irradiation, neutral (UO2)O2·2H2O nanoparticles were formed and could evacuate from the surface of GA-200 to regenerate the active sites in-situ, resulting in a high removal capacity of 1050 mg/g. The mechanism was further studied. It was found that at the presence of O2 in air, the photochemistry property of uranyl itself played an essential role to generate H2O2 and (UO2)O2·2H2O was formed instead of UO2, which was different from that in oxygen-free atmosphere.

In this study, a new kind of short-channel SBA-15 mesoporous silica decorated with polyazamacrocyclic ligands was developed, showing selective binding ability to palladium ions based on host–guest interaction. The established synthesis protocol involved the co-condensation synthesis of an SBA-15 precursor with halogen atoms uniformly incorporated in the mesoporous silica matrix, followed by the anchoring of 1,4,7,10-teraazacyclododecane (Cyclen) ligands via post-grafting. Due to the short straight channels and large pore size facilitating the diffusion of the molecules and ions, the mesoporous silicas were found to possess a high density of the functional Cyclen ligands, as well as high adsorption capacity of Pd(II) in HNO3 solutions. The structure and morphology of the Cyclen functionalized mesoporous silicas were fully characterized. And, the adsorption behavior toward Pd(II) was investigated combined with the theoretical interpretation of the experimental data based on typical kinetic equations, isotherm models and thermodynamic equations. Furthermore, the detailed coordination mechanism between the Cyclen ligands and Pd(II) was examined by high resolution X-ray photoelectron spectroscopy (XPS). A suggested mechanism involving the synergistic effect of four cyclic amines in the Cyclen ligands was proposed to describe the coordination to Pd(II) in HNO3 solutions. Overall, this work provides a facile and effective pathway to build polyazamacrocycle ligand decorated mesoporous silicas with short-channels and large pores, which might be potentially used for molecule recognition and selective enrichment of precious metals.

Developing convenient and rapid method for eliminating uranium from massive contaminated water under emergency conditions is highly needed. Herein we developed a novel chemical precipitation strategy based on graphene aerogel capsulated with the degradation products of phytic acid (PAGA). With hydrothermal treatment, graphene oxide was twisted and reduced to generate aerogel, acting as an encapsulator. At the same time, phytic acid (PA) was degraded into various compounds and capsulated into graphene aerogel with a high loading capacity of 85 g/g. After adding PAGA into uranium contaminated water, the degradation products were released out of GA skeleton to combined with uranium and form sediments. The elimination capacity reached up to 3550 mg/g within 40 min and the obtained sediments possessed good stability in the following 72 h. PAGA capsule also presented high removal rate in various water systems, making it a kind of versatile material in the elimination of uranium under emergency conditions.

As a useful heavy metal ion, chromium has seen its applications in various fields. While it is also a toxic contaminant in water and may cause serious threats to the environment and human health. To develop a novel material with good adsorption capacity and easy solid-liquid separation strategy was necessary and significant. In this paper, the β-cyclodextrin (β-CD) functionalized three-dimensional structured graphene foam (CDGF) was successfully synthesized with the facile and one-step hydrothermal method. The SEM, BET, XRD, FT-IR and XPS analysis were carried out and the results confirmed the successfully grafting of β-CD onto GF. The batch adsorption of Cr(VI) was also taken out and the CDGF possessed good selectivity compared with other metal ions at pH = 3. The adsorption capacity reduced gradually as the initial pH of the Cr(VI) solution grew higher, which was because the anionic species of Cr(VI) were partial to the positively charged surface of CDGF. The easy separation strategy of the CDGF was also demonstrated and the CDGF could be taken out easily with a tweezer after the adsorption of Cr(VI), which significantly simplified the separation procedure and reduced time. By comparing the FT-IR and XPD analysis results, the adsorption mechanism was explored and the hydroxyl groups on CDGF played the main role in the adsorption process. This work brings a novel material for the adsorption of Cr(VI) from water and provides an innovative direction for the easy and fast solid-liquid separation strategy in the adsorption and other application fields.

There has been growing attention on plasma electrodes, as they are much cheaper than commonly used metal electrodes such as Pt and have renewable electrode interfaces. However, most research was mainly focused on plasma cathodes, while the research and application of plasma anodes has been rarely reported. In this paper, we applied an atmospheric-pressure microplasma as a gaseous anode for transferring positive charges and inducing electrochemical reactions in solution. Cu and Cu2O nanocrystals have been co-deposited on ITO cathodes in 100 mM CuSO4 solution at room temperature. By simply changing the precursor concentration and reaction temperatures, pure Cu and Cu2O product could be prepared. Our work will expend the application area of plasma electrodes in electrochemistry and nanomaterials synthesis, and it is also a new rapid and simple electrochemical method for preparing copper and cuprous oxide nanostructures.

Plasmon-enhanced fluorescence (PEF) generally requires the samples settled on a metal substrate and the effective enhancement distance is less than 100 nm, which limit its application in intracellular sensing. Herein, we report a nano endoscopy with PEF effect for sensing analytes inside the extremely small volume samples. The nano endoscopy was fabricated by assembling single nanoporous gold nanowire (PGNW) on the tip of a tungsten needle. It was accurately manipulated to insert into a micro droplet, and an effective sensing was realized at micrometre scale with submicrometer resolution. By taking lysozyme as a model sensing target, a 23-fold improvement of sensitivity was obtained, comparing with that of smooth gold nanowire (SGNW). These results indicated that the nano endoscopy can realize a high spatial resolution sensing, showing its potential application in intracellular sensing.

Single-crystalline Ag2Se complex nanostructures have been synthesized via a solvothermal route in which selenophene (C4H4Se) as a selenylation source reacts with AgNO3 at a temperature of 240 °C. An orthorhombic phase β-Ag2Se nanostructure was identified by X-ray diffraction (XRD), Raman spectroscopy, field emission scanning electron microscopy (FE-SEM), high resolution transmission electron microscopy (HRTEM), and photoluminescence (PL) spectroscopy. The wettability of the as-synthesized β-Ag2Se nanostructure was studied by measurement of the water contact angle (CA). Static water CA values of over 150° were obtained, which can be attributed to the β-Ag2Se complex nanostructure having a combination of micro- and nanostructures. The superhydrophobic Ag2Se nanostructure may find applications in self-cleaning. Additionally, the photocatalytic activity of the as-synthesized β-Ag2Se nanostructure was evaluated by photodegradation of rhodamine B (RhB) dye under ultraviolet (UV) light irradiation.

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