Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 11
·5699-5708
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IF 11.301
Xin Qian,Dongyang Wang,Yang Zhang,Haijun Wu,Stephen J. Pennycook,Lei Zheng,Pierre F. P. Poudeu,Li-Dong Zhao
The metallic elements with a small atomic radius can not only compensate for the intrinsic vacancies to improve the carrier mobility, but also can form interstitials to reduce lattice thermal conductivity. In this work, we investigate the contrasting roles of three different metallic elements with small atomic radius on the thermoelectric properties of n-type PbM0.01Se (M = Cu, Zn, Ni). We find that all the metallic elements can increase the carrier concentration as electron donors and improve the electrical transport properties. In addition, the lattice thermal conductivity of PbSe can be significantly decreased through the formation of interstitials by the incorporated extra metallic elements. We also find that the PbCu0.01Se sample exhibits a unique and complex behavior compared with the other samples due to the diffusion and the thermally activated oxidation of Cu+ ions. When the temperature increased to 673 K, the carrier concentration of PbCu0.01Se sample increases suddenly and continues to increase by nearly two folds, which we ascribe to the release of 3d orbital electrons in Cu+ ions. This results in a strong decoupling of the charge and heat transport in the material, which can be manifested by the overestimation of the electronic thermal conductivity when assuming strong electron–phonon coupling in Wiedemann–Franz law. A maximum ZT of ∼1.6 can be reached at 773 K and the average ZT of ∼0.96 can be achieved in PbCu0.01Se. Our results demonstrate the exceptional contrasting behavior of Cu in PbSe by comparing with Zn and Ni, and the thermoelectric performance of n-type PbSe can be enhanced through the introduction of extra metallic elements with small radius.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Miao Fu,Zhiying Feng,Jing Wang,Ying Zhu,Lanlan Gan,Xiaoming Yang
Room-temperature phosphorescence (RTP) materials have harvested enormous attention owing to their advanced optical properties, providing their possibility of the wider applications. Here, we designed a facile strategy to synthesize phosphorus and nitrogen co-doped carbon dots, while creatine provided the carbon and nitrogen source (CDs@creatine). Meanwhile, the as-prepared CDs@creatine exhibited the bright blue fluorescence in aqueous suspension, and showed the green RTP while being fixed on the filter paper. Significantly, the fluorescence of CDs@creatine was quenched by the introduction of warfarin, whereas their RTP was simultaneously enhanced. Specifically, their fluorescence reduction was mainly ascribed to static quenching effect (SQE) and inner filter effect (IFE). In addition, the abundant hydroxyl groups on the surface of CDs@creatine interacted with the carbonyl groups of warfarin to form hydrogen bonds which rigidified the excited triplet against the non-radiative transition, and thus leading to their enhanced phosphorescence. Therefore, a dual-channel detecting strategy of warfarin has been successfully proposed with the fluorescent linear range from 8 × 10 −3 to 8 × 10 −7 M and phosphorescent linear range of 2 × 10 −5 to 1 × 10 −8 M, which established a new way of assaying warfarin. Besides, CDs@creatine served as both fluorescent and phosphorescent ink, and were applied for painting and information encryption.
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ANALYTICA CHIMICA ACTA
·
2019
·
IF 5.256
Zhongtang Wang,Zhaoya Huang,Yun Xie,Zhaoyi Tan
Plutonium has been extensively studied in the environment, for the purpose of radiological assessment, environmental behavior study and nuclear emergency response. To determine Pu isotopes in environmental soil and sediment, a novel analytical method was established in this study using a new type of extraction resin, TK200 resin. Firstly an investigation was performed to study the extraction behaviors of Pu, U, Th, Hg, Tl, Pb, Bi and Hf on TK200 resin. On the basis of the results, a new chromatographic procedure was then proposed to separate Pu from the elements that interfere the accurate determination of Pu isotopes by mass spectrometry. Owing to the excellent separation efficiency between Pu and interfering elements (IEs) of the developed procedure, high decontamination factors (DFs) were obtained for IEs, e.g. the DF(U) (>7.5 × 10 7 ) was the highest reported value. The separation procedure was finally combined with HNO 3 leaching, CaF 2 /LaF 3 coprecipitation and sector field-inductively coupled plasma mass spectrometry (SF-ICPMS) measurement to establish a complete method. The established method was evaluated by analyzing four standard reference materials (soil, sediment), and the results showed that both 239+240 Pu activity and 240 Pu/ 239 Pu isotopic ratio were accurately determined, with stable and high Pu chemical recoveries (81–91%). The whole analytical method only took about 15 h, and the limits of detection were calculated to be 0.13–0.24 fg g −1 for Pu isotopes (for 2 g soil or sediment), guaranteeing the rapid determination of ultra-trace level Pu in soil and sediment samples.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 40
·23084-23090
·
IF 10.733
Yucen Li,Qi Dang,Chunjing Shi,Wei Zhang,Chengbin Jing,Xin Li,Ming Hu
Auto-switchable power supply systems on the basis of Prussian blue (PB) coordination polymers can smartly tackle both high energy and high power electricity requirements in seawater. To adapt to the complex underwater conditions, it is very important to make the coordination polymer electrode flexible. In this study, we succesfully grew a PB film on a carbon felt. Scanning electron microscopy (SEM) and X-ray diffraction (XRD) confirmed that the PB layer was about 500 ± 50 nm in thickness. The electrochemical modification of the carbon felt guaranteed a strong coating of the PB layer. The obtained electrode worked effectively under bending and in vigorously flowing water. This PB coating was not detached during working under mechanical deformation. Both high-energy and high-power modes were realized in this system even when the PB electrode was deformed, permitting this seawater energy extraction system to support several electronic devices.
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ACS Omega
·
2019
·
IF 2.584
Wei Sun,Qi Sun,Qiang Zhao,Luminita Marin,Xinjian Cheng
In this work, SiO2 microspheres were first prepared by a conventional Stöber method and then etched by NaOH solution to obtain porous ones. By tuning the degree of etching, specific surface area of SiO2 microspheres could be controlled. Then, small fluorescent molecules are synthesized and incorporated onto the surface and/or pores of the SiO2 via layer-by-layer reaction to obtain fluorescent microspheres, namely, SiO2–NH2–BODIPY (SiNBB), SiO2–NH2–BODIPY–indole–benzothiazole (SiNBIT), and SiO2–NH2–BODIPY–indole–benzoxazole (SiNBIO). The as-prepared microspheres SiNBB exhibit highly sensitive and selective recognition ability for Hg2+ and Pb2+. When SiNBB encounters Hg2+ and Pb2+, the fluorescence intensity of SiNBB is increased up to fivefold. SiNBIT and SiNBIO are solely sensitive to Hg2+, and both have a single high sensitivity to recognize Hg2+. The adsorption efficiency of Hg2+ by the three fluorescent microspheres SiNBB, SiNBIT, and SiNBIO reached 2.91, 0.99, and 0.98 g/g of microspheres, respectively. Experimental results of A549 cells and zebrafish indicate that the fluorescent microspheres are permeable to cell membranes and organisms. The distribution of Hg2+ in the brain of zebrafish was obtained by the fluorescence confocal imaging technique, and Hg2+ was successfully detected in A549 cells and zebrafish.
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CHEMICAL PAPERS
·
2019
·Vol. 74
·期 2
·485-497
·
IF 1.246
Quan Cong,Liu Jiayu,Sun Wei,Cheng Xinjian
It is extremely necessary to detect heavy metals sensitively and selectively, especially the ions that will cause great harm to humans and the environment. This work deals with two fluorescent chemosensors and their outstanding role when detecting Zn 2+ and Cd 2+ ions. First, a small molecular chemosensor (TPB) has been designed and synthesized via Suzuki reaction using one part of benzene-1,3,5-triyltriboronic acid and three parts of 2-bromo-1, 10-phenanthroline as starting materials. And then, its corresponding macromolecular fluorescent chemosensor (PTPB) was synthesized. The infrared spectra, mass spectrometry (MS), and 1 H-NMR were used to study the structures of TPB and PTPB. From what has been studied, the TPB and PTPB were stable in a relative wide pH range. As soon as the Cd 2+ and Zn 2+ ions added, fluorescence of the two sensors TPB and PTPB was changed obviously. In addition, PTPB was found have better performance to both Cd 2+ and Zn 2+ than TPB through the ‘‘molecular wire’’ mechanism. Job’s plots were also be tested, showing that the combination ratio of TPB and PTPB to Cd 2+ and Zn 2+ were both 3:1 (ion/sensor). In addition, the minimum detection limits of the macromolecular chemosensor PTPB for Cd 2+ and Zn 2+ reached 0.424 μM and 1.27 μM, respectively.
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Analytical Methods
·
2019
·Vol. 11
·期 34
·4382-4389
·
IF 2.378
Fanglin Ming,Jingzhou Hou,Danqun Huo,Jun Zhou,Mei Yang,Caihong Shen,Suyi Zhang,Changjun Hou
A luminescent amino-functionalized metal–organic framework (Cu–MOFs) was synthesized from 2-aminoterephthalic acid and Cu(II) ions by a solvothermal method. Cu–MOFs displayed blue fluorescence with a peak at 430 nm under 330 nm excitation. Its structure was characterized by FTIR, TEM, XRD, and XPS. The fluorescence of the Cu–MOFs was quenched by Fe3+ in aqueous solutions. The limit of detection was 0.5 μM, and the linear working range extended from 2 μM to 35 μM. Additionally, a good logarithmic relationship between relative fluorescence intensity (F/F0) and Fe3+ concentrations ranging from 2 to 180 μM was obtained with a detection limit of 1.56 μM (R2 = 0.9975). No clear interference was observed when challenged with a wide variety of cations and anions. The recoveries from spiked real water samples were in the range of 91.7–107.7%, and the detection results were consistent with inductively coupled plasma mass spectrometry (ICP-MS) results. Therefore, the fluorescent sensor has great potential in environmental monitoring.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Xuechao Xu,Linjie Wang,Xiaobo Zou,Shuwen Wu,Jianming Pan,Xin Li,Xiangheng Niu
Given that hypertoxic arsenite (As 3+ ) poses a serious threat to the environment and global health, developing high-performance, low-cost and easy-to-use approaches to specifically monitor As 3+ in environmental matrices turns to be of great importance. In the present work, we reported a novel colorimetric assay of As 3+ based on the reassembly-induced oxidase-like activity inhibition of dithiothreitol-capped Pd nanoparticles (Pd-DTT). The Pd-DTT nanozyme exhibits good oxidase-like catalytic activity to trigger the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of O 2 , forming a blue product TMBox. When As 3+ exists, it can chelate the sulfydryl groups in DTT more strongly, leading to a reassembly of Pd-DTT. Compared with the original nanozyme, the reassembled one has much less oxidase-like activity, resulting in the significantly suppressed TMB reaction. Based on this principle, highly sensitive detection of As 3+ was achieved, providing a wide linear range from 33 ng L −1 to 333.3 μg L −1 and an ultralow detection limit of 35 ng L −1 . With the help of EDTA as a chelating agent, the method could also offer excellent selectivity for the determination of As 3+ against other metal ions. Besides, our colorimetric assay was employed to accurately measure the analyte in spiked drinking and river water, revealing its great promise in environmental analysis application.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 37
·21386-21403
·
IF 10.733
Xin Song,Jiangle An,Chao He,Jukai Zhou,Yuanting Xu,Haifeng Ji,Li Yang,Jiarui Yin,Weifeng Zhao,Changsheng Zhao
Super adsorbents with ultrahigh adsorption capabilities are highly desired for efficient wastewater remediation. However, most of the adsorbents with high adsorption capabilities are powdery adsorbents, showing inescapable limitations in practical adsorption column application. It is practically urgent to develop a simple and effective method for preparing adsorbents with ultrahigh adsorption capability and convenient column operation ability. Herein, inspired by oviparity, we fabricate super-adsorbent hydrogel spheres (SAHSs) based on self-sacrificing micro-reactors, which achieve the interior cross-linking polymerization of the hydrogel network and subsequent self-disintegration within only 150 seconds. The as-prepared poly(2-acrylamido-2-methyl-propanesulfonic acid-co-acrylic acid) hydrogel spheres show outstanding adsorption capabilities toward organic dyes (4625 ± 231 mg g−1 for methylene blue) and heavy metallic ions (4312 ± 185 mg g−1 for Pb(II)). Remarkably, the adsorption column packed with the SAHSs exhibits splendid removal abilities for organic dyes, which can purify 6280 mL of dye-containing wastewater (150 μmol L−1) thoroughly using only 7 mL SAHSs. This is the first time that a maximum dynamic removal capacity over 50 g L−1 spheres has been obtained using an adsorption column. In addition, the hydrogel spheres also show good recyclability, dynamic filtration–regeneration, selective adsorption and smart separation–regeneration. Thus, the oviparity-inspired method to fabricate super-adsorbent hydrogel spheres has great potential to be used in efficient, economical and environmental wastewater treatment.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Fukun Li,Zhangmin Li,Liam John France,Jiali Mu,Changhua Song,Yuan Chen,Lilong Jiang,Jinxing Long,Xuehui Li
Novel and selective strategies for platform chemical production from renewable biomass are highly attractive in respect to value-added utilization of sustainable resources. In this study, a series of low-cost, commercially available, transition metal carbonates (Zr, Ni, Mg, Zn, and Pb) were investigated for catalytic transfer hydrogenation of levulinate esters to γ-valerolactone (GVL) via the cascade process of Meerwein–Ponndorf–-Verley (MPV) reduction and lactonization reaction. Among the selected catalysts, basic zirconium carbonate is the most active, with the highest turnover frequency (TOF) of 3.1 h–1 and a surface reaction rate of 0.21 mol m–2 h–1. At 453 K, 3.0 h, and 1.0 MPa N2, 100% ethyl levulinate conversion, 96.3% GVL yield, and 91.9% hydrogen donor utilization are observed due to the cooperative effect between acid (Mn+) and base (−OH) sites. Furthermore, this catalyst shows high recyclability under the optimized conditions, where a satisfactory catalytic activity is shown even after six consecutive runs.
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Energy & Environmental Science
·
2018
·Vol. 11
·期 7
·1848-1858
·
IF 30.067
Li You,Yefeng Liu,Xin Li,Pengfei Nan,Binghui Ge,Ying Jiang,Pengfei Luo,Shanshan Pan,Yanzhong Pei,Wenqing Zhang,G. Jeffrey Snyder,Jiong Yang,Jiye Zhang,Jun Luo
Here we find the peculiar behavior of Cu ions in the PbSe–Cu system increases its thermoelectric performance. For the electrical transport, a dynamic doping effect is achieved because more Cu ions enter into the PbSe lattice and provide extra charge carriers as the temperature increases, which guarantees an optimized carrier concentration over a wide temperature range. For the thermal transport, the presence of Cu2Se nanoprecipitates and dislocations at a low temperature range as well as the vibration of Cu atoms around the interstitial sites of PbSe at high temperatures result in hierarchical phonon scattering and a significantly reduced lattice thermal conductivity over the whole temperature range. As a result, a peak thermoelectric material figure of merit zT of up to 1.45 and a thermoelectric device figure of merit ZT close to unity are obtained for the sample with 0.375 at% Cu. Furthermore, enhanced thermoelectric properties are also realized for the Cu-intercalated PbS, implying that the temperature-driven dynamic behavior of Cu ions in a rigid lattice can serve as a general strategy to optimize the thermoelectric performance of IV–VI compounds.
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ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Yang Li,Qingfen Niu,Tao Wei,Tianduo Li
A novel bifunctional thiophene-based Schiff base TS as a colorimetric and fluorescent turn-on sensor for rapid and simultaneous detection of Al 3+ and Zn 2+ ions with high selectivity and sensitivity has been developed. The sensor shows remarkable fluorescence enhancement response for Al 3+ and Zn 2+ over a broad pH range with good anti-interference capability, which accompanied with an obvious color change easily detected by naked eyes. Sensor TS can detect as low as 3.7 × 10 −9 M for Al 3+ and 3.0 × 10 −8 M for Zn 2+ , whereas respective association constants are 1.16 × 10 4 M −1 and 2.08 × 10 4 M −1 . With the help of fluorescence titration and Job's plot, the stoichiometric ratio of TS with Al 3+ /Zn 2+ was determined to be 1:1. The sensing mechanism of sensor TS with Al 3+ /Zn 2+ based on the chelation-enhanced fluorescence (CHEF) was analyzed in detail through 1 H NMR titration, FTIR, HRMS and DFT studies . Moreover, sensor TS has been applied to the detection of Al 3+ and Zn 2+ in real environmental water and food samples as well as the filter paper-based test strips. Furthermore, sensor TS has good cell-permeability and can be used to selectively sense intracellular Al 3+ and Zn 2+ by bioimaging.
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