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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Development of a novel sensor based on Bi2O3 and carbonized UIO-66-NH2 nanocomposite for efficient detection of Pb(Ⅱ) ion in water environment

Chunwen Chang,Qiang Xue,Rong Wang,Zeyu Liu,Yao Liu,Lin He,Fei Liu,Haijiao Xie

Development of an efficient monitoring technology for rapid detection of toxic Pb(Ⅱ) ion in water environments is extremely important. Here, a novel and highly sensitive sensor was prepared using one-step calcination technique, based on Bi 2 O 3 nanoparticles and carbonized metal–organic framework (MOF) nanocomposite. Scanning electron microscopy, transmission electron microscopy, contact angle and X-ray photoelectron spectroscopy characterization methods were used to analyze the morphology and structure of the prepared materials. Based on the electrical double-layer capacitance theory and Raman spectroscopy, changes to the active sites of different modified materials were investigated. Besides, differential charge densities and adsorption energies of the different modified materials in Zr-O clusters were calculated using density functional theory (DFT). A Bi 2 O 3 and carbonized UIO-66-NH 2 (Bi 2 O 3 /C-UIO-66-NH 2 ) -modified glassy carbon electrode was used to detect Pb(Ⅱ) by differential pulse anodic stripping voltammetry. Under optimal experimental parameters, the developed electrochemical sensor has a wide linear range (2–130 μg/L) and a low detection limit (0.05 μg/L). Meanwhile, the sensor has excellent stability, repeatability, and anti-interference properties and has been successfully applied to detect Pb(Ⅱ) in actual water samples. The results of this paper show that our developed sensor an efficient and rapid sensor technology for monitoring lead in water environment.

研究领域: 材料科学 · 环境科学 · 分析化学
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Cleaner Engineering and Technology · 2021 · IF 0

Efficient, selective, and reusable metal–organic framework-based adsorbent for the removal of Pb(II) and Cr(VI) heavy-metal pollutants from wastewater

Yanjin Zheng,Feng Rao,Meilli Zhang,Jing Li,Wenxuan Huang

Water containing excess heavy metals poses a health risk to humans but can be purified effectively using adsorbents. As such, identifying novel and efficient adsorbents to remove heavy metals such as Pb(II) and Cr(VI) is vital. We report a new metal-organic framework (MOF), {[Cd 1.5 (btc)(bibp)·2H 2 O]·H 2 O}n, capable of capturing Pb(II) and Cr(VI) from water. The adsorbent has a high density of exposed active sites, with maximum adsorption capacities of 537.634 mg/g for Pb(II) (pH = 7) and 787.402 mg/g for Cr(VI) (pH = 6). Adsorption equilibrium was reached after 60 and 120 min with Pb(II) and Cr(VI), respectively, and the adsorbent was regenerated effectively using an ethanol-acetic acid eluent. Analysis of the adsorption kinetics using Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy showed that the abundant –OH groups (hard base) and the Pb(II)/Cr(VI) (soft acid) behave according to the hard-soft acid-base principle. In addition, electron pairs are shared between the imidazole N atoms and Pb(II)/Cr(VI). This study provides new insights into the design of three-dimensional MOFs for removing pollutants from industrial wastewaters, with the potential to mitigate health risks to humans and natural ecosystems.

研究领域: 环境科学 · 材料科学
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2021 ·Vol. 22 ·期 12 ·6540 · IF 5.924

Efficient Activation of Coal Fly Ash for Silica and Alumina Leaches and the Dependence of Pb(II) Removal Capacity on the Crystallization Conditions of Al-MCM-41

Xu Zhang,Tao Du,He Jia

In this study, four different coal fly ashes (CFAs) were used as raw materials of silica and alumina for the preparation of the alumina-containing Mobil Composition of Matter No. 41 (Al-MCM-41) and the exploration of an activation strategy that is efficient and universal for various CFAs. Alkaline hydrothermal and alkaline fusion activations proceeded at different temperatures to determine the best treatment parameters. We controlled the pore structure and surface hydroxyl density of the CFA-derived Al-MCM-41 by changing the crystallization temperature and aging time. The products were characterized by small-angle X-ray diffraction, nitrogen isotherms, Fourier-transform infrared spectroscopy,29Si silica magic-angle spinning nuclear magnetic resonance, and transmission electron microscopy, and they were then grafted with thiol groups to remove Pb(II) from aqueous solutions. This paper innovatively evaluates the CFA activation strategies using energy consumption analysis and determines the optimal activation methodology and parameters. This paper also unveils the effect of the crystallization condition of Al-MCM-41 on its subsequent Pb(II) removal capacity. The results show that the appropriate selection of crystallization parameters can considerably increase the removal capacity over Pb(II), providing a new path to tackle the ever-increasing concern of aquic heavy-metal pollution.Keywords:coal fly ash;CFA activation;Al-MCM-41;crystallization parameters;Pb(II) removal capacity

研究领域: 环境科学 · 材料科学
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CRYSTENGCOMM · 2022 ·Vol. 24 ·期 14 ·2567-2574 · IF 3.756

Efficient charge migration in TiO2@PB nanorod arrays with core–shell structure for photoelectrochemical water splitting

Guobing Mao,Chunxiao Li,Zhengdao Li,Miao Xu,Heng Wu,Qi Liu

Herein, TiO2@Prussian-blue (PB) core–shell nanorod arrays for photoelectrochemical (PEC) applications were designed and prepared via a facile hydrothermal and electrodeposition process. Due to the combined merits of the anti-reflection structure of TiO2 nanorod arrays and broad light response of PB, the TiO2@PB film shows high light absorption efficiency. Additionally, the appropriate gradient energy gap of the core–shell heterostructure can promote photogenerated carrier separation and low electron–hole recombination rate. As a result, compared with TiO2 and PB films, the as-prepared TiO2@PB photoanode effectuates enhanced photocatalytic activity and the photocurrent density of TiO2@PB photoanode reaches 1.5 mA cm−2 at 1.23 V vs. RHE, which is approximately twice that of pristine TiO2 (0.75 mA cm−2). The introduction of the PB shell layer does not only improve light absorption ability but also enhances the photogenerated charge carrier's transfer and separation.

研究领域: 材料科学 · 能源转换与储存 · 光催化
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Journal of Materials Chemistry C · 2024 ·Vol. 12 ·期 45 ·18391-18400 · IF 5.7

Dual-anchored configuration involving Pb(NO3)2 for effective and stable FAPbI3 quantum dot solar cells

Meidan Que,Shenghui He,Lili Gao,Boyue Zhang,Yabo Wang,Jin Chen,Bo Li,Wei Huang,Peng Zhong

The dynamic nature of formamidine lead iodide quantum dots (FAPbI3 QDs) limits their practical application by causing the appearance of ionic vacancy defects on the surface of QDs, which would then allow for significant trap-assisted non-radiative recombination of charge carriers. Herein, we explore a feasible surface modification strategy for passivating vacancy defects. Different lead salts are employed in the post-treatment procedure of quantum dot films. Based on both experimental and theoretical findings, Pb(NO3)2 passivation comprises Pb2+ and FA+. On the quantum dot surface, the O atoms from NO−3 form strong chemical bonds with FA+, and the O–C⋯O–N structure, defined by a dual-anchored configuration, contributes to the establishment of a stable crystal structure by exhibiting optimal bond lengths (3.486 Å and 3.775 Å, respectively) and a higher binding energy (10.51 eV). Finally, FAPbI3 quantum dot solar cells simultaneously achieve both exceptional environmental stability and a champion photoelectric conversion efficiency of 12.11%. This work provides valuable insights into surface chemical engineering of quantum dots, paving the way for high-performing photovoltaic devices.

研究领域: 材料科学 · 光伏技术 · 化学工程 · 表面化学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Synthesis of amino-functionalized magnetic aerobic granular sludge-biochar for Pb(II) removal: Adsorption performance and mechanism studies

Xin Huang,Dong Wei,Xinwen Zhang,Dawei Fan,Xu Sun,Bin Du,Qin Wei

In the present study, a novel amino-functionalized magnetic aerobic granular sludge-biochar (NH 2 -M-AGS) was successfully fabricated through magnetization and functional modification and applied for Pb(II) sorption . The composite was characterized by using scanning electron microscopy (SEM), energy dispersive spectrum (EDS), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), Zeta potential analysis, vibrating sample magnetometer (VSM) and X-ray photoelectron spectroscopy (XPS). The effects of adsorbent dosage, pH value, contact time and initial metal concentration on the adsorption of Pb(II) were investigated by using batch equilibrium experiments. It was concluded that the pseudo-second-order model was better to describe adsorption kinetic of Pb(II) onto NH 2 -M-AGS. The Langmuir model was more accorded with the experimental data, and the maximum adsorption capacity of Pb(II) was 127.0 mg/g. A possible adsorption mechanism could be mainly caused by surface complexation, electrostatic attraction and precipitation. In five adsorption-desorption cycles, the desorption efficiency of Pb(II) exhibited a slight decline and still reached at 88.14%. Furthermore, the good reproducibility indicated that NH 2 -M-AGS could be used a desirable, economic and recyclable adsorbent in practical metal-contaminated wastewater treatment .

研究领域: 环境科学 · 材料科学
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 27 ·16161-16175 · IF 10.733

Tailored Janus silica nanosheets integrating bispecific artificial receptors for simultaneous adsorption of 2,6-dichlorophenol and Pb(II)

Jinxin Liu,Pan Wang,Mengdie Zhou,Yue Ma,Xiangheng Niu,Guoqing Pan,Jianming Pan

Potentially toxic dichlorophenols and heavy metal ions commonly coexist in industrial sewage, posing a serious threat to public health and the environment and making the treatment more challenging. Inspired by Suzhou bifacial embroidery, whereby the Janus-like planar structure allows different compositions to be compartmentalized onto two distinct surfaces, Janus silica nanosheets partitioning bispecific artificial receptors (i.e., molecularly imprinted sites and thiol groups) onto distinct recognition surfaces (J-MIPs/cys) were designed to independently take up 2,6-dichlorophenol (DCP) and Pb(II). For J-MIPs/cys, the thiol groups are expected to capture Pb(II) via chelating action and molecularly imprinted cavities act as highly specific recognition sites for DCP. J-MIPs/cys possessed uniform cross-sectional dimensions and thickness (∼25.3 nm), and a particle-like surface imprinted layer (∼21.8 nm). In the monocomponent system, J-MIPs/cys displayed fast binding kinetics (60 min and 45 min), large monolayer adsorption capacity (129.4 mg g−1 and 82.95 mg g−1), high affinity, and excellent regeneration after five reuse cycles (9.134% and 12.16% loss in adsorption amounts) for DCP and Pb(II), respectively. Additionally, a spontaneous and endothermic adsorption process was also confirmed. In a binary system, the presence of Pb(II) produced a prominent increase in DCP adsorption at high initial concentrations and a decrease at low initial concentrations, owing to the partial complexation of Pb(II) with excess DCP and occupation of imprinted sites by Pb(II). However, the uptake of Pb(II) was inhibited over the whole range of concentration in the presence of DCP due to the competitive adsorption onto thiol groups. In summary, J-MIPs/cys integrating novel bispecific receptors open wide possibilities for efficient and specific treatment of coexisting toxic pollutants.

研究领域: 环境科学 · 材料科学 · 化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Three dimensional flower-like magnetic polyethyleneimine@MoS2 composites for highly efficient removal of Cr(VI) and Pb(II) ions

Chengwei Sun,Gang Song,Lili Chen,Xuemei Ren,Changlun Chen

Magnetic Fe 3 O 4 nanoparticles were coated by polyethyleneimine (PEI), and then Fe 3 O 4 @PEI was further modified with MoS 2 by the hydrothermal method to fabricate 3D flower-like structured magnetic polyethyleneimine@MoS 2 (MP@MoS 2 ) composites, and the composites were served as efficient adsorbents to capture Cr(VI) and Pb(II) from aqueous solution. The effects of temperature, pH, shaking time and environmental conditions on adsorption performance of MP@MoS 2 towards Cr(VI) and Pb(II) have been conducted by batch adsorption experiments. The prepared MP@MoS 2 exhibited high adsorption capacities (192.30 mg/g for Cr(VI) at pH 3.0 and 256.41 mg/g for Pb(II) at pH 6.0) and the adsorption equilibrium could be achieved in a short time. Moreover, MP@MoS 2 composites with high saturation magnetization could be simply separated under an external magnet. Combined experiments and spectral analysis, the underlying adsorption mechanism for Cr(VI) on MP@MoS 2 was mainly attributed to the reduction of Cr(VI) to Cr(III), and the removal of Pb(II) was due to the complexation with sulfur groups and amino-groups. Consequently, the prepared 3D flower-like structured MP@MoS 2 has a great potential for the practical application in removing Cr(VI) and Pb(II) from the aquatic environment.

研究领域: 環境科學 · 材料科學
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2020 ·Vol. 22 ·期 13 ·7012-7020 · IF 3.43

Charge compensation weakening ionized impurity scattering and assessing the minority carrier contribution to the Seebeck coefficient in Pb-doped Mg3Sb2 compounds

Qiang Zhang,Jichong Hou,Jianfeng Fan,Shaoping Chen,Wenhao Fan,Hua Zhang,Wenxian Wang,Yucheng Wu,Bingshe Xu

This work reports the electrical and thermal transport processes in p-type Pb-doped Mg3(1+x)Sb2−yPby (0.02 ≤ x ≤ 0.08; 0 ≤ y ≤ 0.02) compounds. Low-energy electron acceptor defects Mg vacancies are easy to form, which can provide holes and make p-type transport in the Mg3Sb2 matrix. However, with an increase in excess Mg, the transport behavior changes from p type to n type as manifested synergistically by both the Hall coefficient and Seebeck coefficient. This indicates the effective role of Mg in tuning carrier type and concentration for a pristine Mg3Sb2 compound. Upon substitution of Sb by Pb, the hole concentration slightly increases, and mobility is greatly improved by 133% at room temperature. The significant increase in mobility is attributed to the weakening ionized impurity scattering, stemming from the decreasing concentration induced by Pb doping. Thus, the power factor is enhanced with a 146% improvement at room temperature. Consequently, the figure of merit ZT of the Pb-doped sample is 1.8 times larger than the pristine one at around 300 K. Moreover, the non-degenerate transport behavior revealed by electrical properties is simply analyzed regarding the effects of minority carriers on the overall Seebeck coefficient. This study proposes a new strategy of charge compensation for improving mobility and a simple way to guide the prediction about the onset of bipolar conduction for Mg3Sb2-based compounds and other potential thermoelectric materials.

研究领域: 材料科学 · 热电学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Constructing Pb-O bonds to trigger efficient cross-scale charge transfer for high-performance electromagnetic wave absorption and multicolor conversion

Jie Huang,Lingjie Hu,Liuying Wang,Weichao Wang,Chaoqun Ge,Long Wang,Mengzhou Chen,Renbing Wu,Gu Liu,Bin Wang

The simultaneous achievement of controllable electromagnetic wave absorption and electrochromism through micro-nanostructure design holds significant importance for radar stealth and visible light compatibility in complex surveillance environments. However, the synergistic design of anion insertion/intercalation and dielectric loss coordination still face significant challenges. Herein, CPBs-VO NWs composites with excellent electromagnetic wave absorption and electrochromic performance are prepared by in situ growth of CsPbBr 3 quantum dots on the surface of V 2 O 5 nanowires leveraged by the chelation effect of Pb-O bonds. The loading concentration of CsPbBr 3 quantum dots on the surface of V 2 O 5 nanowires is designed to regulate the formation and breakdown of Pb-O bonds, facilitating the investigation of the energy transfer process at the interface. The analysis reveals that the formation of Pb-O bonds enhances electron transfer across multiscale heterogeneous interfaces, resulting in increased local charge density differences, polarization, and conductivity. Additionally, it aids in the valence state change of vanadium ions through bridging, thereby achieving efficient electromagnetic wave absorption and compatibility with electrochromic performance. This study provides an insight at the atomic-level into performance enhancement and compatibility of visible light and radar stealth by precisely controlling the interface sites.

研究领域: 材料科学 · 纳米技术 · 电子工程
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JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY · 2024 ·Vol. 39 ·期 12 ·2974-2981 · IF 3.1

A Pb-free Sn–Bi alloy mount preparation method for secondary ion mass spectrometry (SIMS) analyses

Wan-Feng Zhang,Qing Yang,Xiao-Ping Xia,De-Wen Zheng,Ze-Xian Cui,Yan-Qiang Zhang,Yi-Gang Xu

Sample preparation is a critical step to achieve reliable in situ chemical analysis. Sample mounting technique with a tin-based alloy was developed in recent years, which is particularly useful for high-precision volatile analyses by secondary ion mass spectrometry (SIMS). However, the success of this technique is hindered by challenges, such as complex alloy preparation and potential Pb contamination. Herein, we introduce a new Sn–Bi alloy preparation method that may overcome these hurdles and assess its potential as a standard preparation method for in situ volatile and isotope analyses. This new alloy can be manufactured with commercially available pure tin and bismuth metal (atomic Sn : Bi = 42 : 58), and its production requires only a heating plate and clean containers. This ensures its high accessibility to laboratories worldwide. The Pb content of the alloy is dependent on the tin and bismuth used. The material (Sn and Bi) from three different manufacturers were evaluated in this study, resulting in the virtually Pb-free MAC alloy (Pb <0.2 μg g−1). The SIMS U–Pb dating results of the zircon standards (Qinghu, Plešovice, and SA01) are consistent with the recommended values (within error). Furthermore, the mounted samples exhibit satisfactory relief on this alloy, suggesting that this alloy material is appropriate for the analysis of oxygen isotopes. The routine external precision of oxygen isotope ratios is better than 0.30‰ (2sd), on par with that obtained with epoxy mounts. The water background in the SIMS sample chamber can be recovered rapidly after sample transfer from the storage to the sample chamber. Hence, this tin-based alloy is suitable for sample mounting for SIMS volatile and isotope (incl. U–Pb) analyses.

研究领域: 材料科学 · 分析化学 · 地球化学
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MATERIALS CHEMISTRY AND PHYSICS · 2023 · IF 4.6

Detection of Pb(II) in water via a NH2-MIL-53(Fe)@ITO electrochemical sensor

Hangxi Liu,Haorong Sun,Ming Fang,Yifeng Zhang,Mingguang Kong,Zhimin Lv,Xiaoli Tan

The evaluation of the concentration of Pb(II) in solution has great significance in avoiding harm to ecology health. In this work, NH 2 -MIL-53(Fe) modified ITO glass (NH 2 -MIL-53(Fe)@ITO) was utilized as an electrochemical sensor for the detection of Pb(II) in solutions. FTIR and XPS investigation disclosed that the plentiful surface –NH group on the NH 2 -MIL-53(Fe) should be responsible for the highly efficient and selective detection abilities of Pb(II) due to the capture and conductivity abilities. The NH 2 -MIL-53(Fe) was prepared by a solvothermal technique and electrophoresed on the surface of ITO glass . A square wave voltammetry (SWV) method is employed for the sensitive determination of Pb(II). The factors of the detection condition such as the pH and ion interference are also studied. The sensitivity of 16.072 μA μM −1  cm −2 in the linear range of 2–4 μM and 54.143 μA μM −1  cm −2 in the linear range of 5–17 μM, and the limit of detection (LOD) of 0.1 μM are acquired. The repeatability and reproducibility are also studied. EIS and Tafel curves are utilized to investigate the effect of temperatures on the properties of the NH 2 -MIL-53. This work presents a facile strategy for the preparation of NH 2 -MIL-53(Fe)@ITO electrochemical sensor via electrolysis, which enhances the sensitivity toward Pb(II) and shows great application potential.

CAS / MDL: 68-12-2 10025-77-1
研究领域: 环境科学 · 分析化学 · 材料科学 · 电化学
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