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Environmental Science-Nano · 2020 ·Vol. 7 ·期 12 ·3814-3823 · IF 7.683

In situ controlled synthesis of porous Fe–N–C materials from oily sludge by chlorinating calcination and their novel application in supercapacitors

Hanfeng Zhou,Zhibo Deng,Tianbao Liu,Tao Liu,Lijuan Zhang,Xintai Su,Zhang Lin

The science linking thermochemical conversion of large-scale industry oily sludge with applied materials has been improved in the last ten years. However, with the traditional converting methods it is hard to precisely control the composition and structure of oily sludge-based products during pyrolysis due to the complexity of the composition of the oily sludge. Here, a chlorinating calcination method using sodium chloride (NaCl) as a chlorinating salt and template was first developed to prepare porous Fe–N–C materials (FCN-500) through pyrolysis of oily sludge containing iron-bearing minerals and pyridine. The formation mechanism of FCN-500 was proposed, where iron ions (Fe3+) from the inorganic component (anorthite) in the sludge were rapidly dissociated with the assistance of NaCl, followed by coordination with the organic component (pyridine nitrogen) in the oily sludge to form the pyridine nitrogen–iron ((C5H6N)n–Fe) complex, and then carbonization. As-obtained FCN-500 exhibited higher specific capacitance (286.3 F g−1 at a current density of 0.5 A g−1), enhanced energy density (33.5 W h kg−1 at a power density of 606.1 W kg−1) and more excellent stability and durability (more than 80.1% capacitance retention after 10 000 cycles) compared with two other electrodes. The reasonably better performance of the obtained FCN-500 in supercapacitors (SCs) is attributed to its large surface area, hierarchically porous channels, high conductivity, and unique Fe–N–C structure. Therefore, this work not only provides a feasible way to solve the bottleneck problem in sludge pyrolysis, but also provides a method to design large scale porous Fe–N–C materials for practical applications.

研究领域: 环境科学 · 材料科学 · 能源科学
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Journal of the Taiwan Institute of Chemical Engineers · 2019 · IF 3.834

Fabrication of Fe3O4 quantum dots modified BiOCl/BiVO4 p-n heterojunction to enhance photocatalytic activity for removing broad-spectrum antibiotics under visible light

Runren Jiang,Donghai Wu,Guanghua Lu,Zhenhua Yan,Jianchao Liu,Ranran Zhou,Matthew Nkoom

Herein, Fe 3 O 4 quantum dots modified BiOCl/BiVO 4 p-n heterojunction was successfully synthesized by a facile strategy. Multiple techniques were carried out to characterize the as-prepared samples. Results show that the photocatalysts possess regular crystal structure and consisted of BiOCl/BiVO 4 nanosheet structure with Fe 3 O 4 QDs on its surface. Particularly, 20% Fe 3 O 4 QDs@BiOCl/BiVO 4 p-n heterojunction shows universal outstanding photocatalytic activity for removing four different broad-spectrum antibiotics under visible light. Meanwhile, the mineralization degree and degradation pathways of antibiotic were further studied by 3D-EEMs and LC-MS/MS. The improved photocatalytic performance for degradation of broad-spectrum antibiotics mainly attributes to the effective charge carrier mobility, large specific surface areas, and strong visible light absorption. The photocatalytic reaction mechanism was also revealed by the electron spin resonance (ESR) technique and the active species trapping experiments. The photocatalyst stays stable crystal structures after four reaction cycles and it can be easily separated from the solution by an external magnetic field both demonstrate that the Fe 3 O 4 QDs@BiOCl/BiVO 4 p-n heterojunction has unlimited potential for practical usage. This work is expected to be widely applicable to the removal of broad-spectrum antibiotics.

研究领域: 环境科学 · 材料科学
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Desalination and Water Treatment · 2024 · IF 1

Complexation flotation of boron from the salt lake brine using a novel flotation agent prepared by N-methyl-D-glucamine and 1,2-epoxyoctadecane

Chun Bai,Kexin Li,Yanping Wang,Haining Liu,Huifang Zhang,Quan Li,Jun Li,Xiushen Ye,Zhijian Wu

ABSTRACT A novel boron flotation agent (N-2-hydroxyoctadecyl-N-Methylglucamine, NHO-NMDG) was fabricated using 1,2-epoxyoctadecane and N-methyl-D-glucamine. The obtained collector possesses both collecting and foaming properties and it was characterized by nuclear magnetic resonance, mass spectrometry, Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy methods. The flotation performance for boron removal from the salt lake brine has been studied. The flotation experiments indicated a highly effective removal of boron from the salt lake brine. The boron removal rate in the Da Qaidam brine could reach 67.08% by NHO-NMDG. The mechanism analysis shows that the meglumine group in the bifunctional flotation agent can be complexed with boron, and the long-chain alkyl group can attach to the surface of the bubble and enter into the bubble layer, so as to separate boron from the aqueous solution.

研究领域: 化学工程 · 环境科学
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Industrial Chemistry & Materials · 2024 · IF 0

Elongated Fe–N–C containing trace atomic Co dopants for high power density PEMFCs

Jiayao Cui,Junyong Min,Hao Wang,Jianglan Shui,Lishan Peng,Zhenye Kang,Jieyuan Liu,Qingjun Chen,Shuo Bai,Yanrong Liu

Developing single-atom Fe–N4/C catalysts is crucial for the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). While Fe–N4/C catalysts are inherently active in accelerating the slow ORR process, their performance is still inferior to that of Pt/C. Herein, a trace Co-doped Fe single-atom catalyst (Fe(tCo)–N–C) containing more active Fe2N8 sites has been synthesized. Interestingly, compared with typical FeN4 sites in an Fe–N–C electrocatalyst, the Fe2N8 sites generate a larger Fe–N bond length due to Co-doping. The elongated Fe–N bond in Fe2N8 lowers the d-band center and charge density of iron sites, enhancing the ORR process by facilitating the formation of *OOH and generation and desorption of *OH. Fe(tCo)–N–C manifested excellent acidic and alkaline ORR activity, with a half-wave potential (E1/2) of 0.80 V in HClO4 solution and 0.89 V in KOH medium. More importantly, high peak power densities (Pmax) were realized by applying Fe(tCo)–N–C in PEMFCs, with the Pmax reaching 890 mW cm−2 in H2–O2 and 380 mW cm−2 in H2–air. Additionally, trace Co dopants in the catalyst improved carbon graphitization and provided high ORR catalytic stability. This research introduces an innovative approach to engineering highly active Fe2N8 sites, providing valuable insights for the sustainable progress of PEMFC technology.

研究领域: 电化学 · 催化 · 能源材料 · 燃料电池 · 纳米技术
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LANGMUIR · 2021 · IF 3.882

Mesoporous N–P Codoped Carbon Nanosheets as Superior Cathodic Catalysts of Neutral Metal–Air Batteries

Aling Chen,Qingfeng Yi,Kuang Sheng,Yuebing Wang,Jiangchuan Chen,Qiaoli Zhang,Kaiwen Xiang,Guanghua Tan

Development of high-efficiency oxygen reduction reaction (ORR) catalysts under neutral conditions has made little research progress. In this work, we synthesized a three-dimensional porous N/P codoped carbon nanosheet composites (CNP@PNS) by high-temperature thermal treatment of dicyandiamide, starch, and triphenylphosphine and subsequent porous structure-making treatment using the NaCl molten salt template. In the neutral solution, the electrocatalytic performance of the CNP@PNS-4 catalyst exhibits an onset potential of 0.98 V (vs reversible hydrogen electrode) and a half-wave potential of 0.91 V for ORR, which greatly surpasses commercial Pt/C (40%). Three kinds of neutral metal–air batteries (Zn–air, Al–air, and Fe–air) using the prepared samples as cathodic catalysts were constructed, corresponding to the maximum power density of 120.2, 78.3, and 18.9 mW·cm–2, respectively. Also, they reveal outstanding discharge stability under different current densities. The density functional theory calculation depicts the reduction of the free energy of the determining step and subsequent decline of the overpotential for ORR.

研究领域: 材料科学 · 电化学 · 能源科学
✓ 已验证 DOI 高影响因子
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CHEMOSPHERE · 2022 · IF 8.943

Degradation mechanisms of cyanobacteria neurotoxin β-N-methylamino-l-alanine (BMAA) during UV254/H2O2 process: Kinetics and pathways

Boyin Yan,Songxue Wang,Zhiquan Liu,Da Wang,Wenxin Shi,Fuyi Cui

In this work, the UV 254 /H 2 O 2 process was utilized to remove β-N-methylamino- l -alanine (BMAA), a kind of cyanobacteria neurotoxin, and the influence of reaction parameters and environmental factors on the degradation of BMAA has been systematically investigated. The results showed that BMAA could be effectively removed in the UV 254 /H 2 O 2 system compared to UV or H 2 O 2 alone and OH was confirmed as the main ROS to degrade BMAA. The degradation rate of BMAA increased first and then decreased with the increase of pH and the maximum k obs was 0.1545 min −1 obtained at pH 9. The removal of BMAA in the UV 254 /H 2 O 2 system was inhibited in actual water, while the degradation rate of BMAA in actual water could still exceed 90% by appropriately extending the reaction time. The decrease in the degradation efficiency of BMAA in actual water was primarily due to the ultraviolet light absorption and competition effects of NOM, and anions (Cl − and HCO 3 − ) would also inhibit the degradation of BMAA. Five by-products ([M − H] -  = 118, 103, 88, 87 and 59) were identified in this study and the degradation pathways of BMAA were proposed. The production of by-products was attributed to the fracture of the C–N bond and hydroxylation reaction. This study is worthwhile to deepen the understanding of the degradation mechanism of BMAA in the UV 254 /H 2 O 2 system.

研究领域: 环境科学 · 毒理学
✓ 已验证 DOI 高影响因子
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ACS Applied Engineering Materials · 2023 · IF 0

Fe/N Codoped Paper Carbon Fiber Foam Promoted Extracellular Electron Transfer for a High-Performance Microbial Fuel Cell

Demin Jiang,Kai Cheng,Liang Li,Kun Xie,Haijun Tao,Yuqiao Wang

Anodes are considered an important component of microbial fuel cells (MFCs) to recover electric energy from organic wastewater. Herein, Fe/N codoped paper carbon fiber foam was developed as an anode for MFCs to enhance electricity generation and wastewater treatment. The interconnected microporous network was beneficial for bacteria colonization and biofilm formation. The N doping enhanced the hydrophilicity to facilitate bacterial proximity. The Fe doping modulation adhered to the microorganisms due to the positive charge of iron ions. The codoped anode promoted the organic matter degradation efficiency and intrinsic electricity generation property based on the optimized thick biofilm. The high electricity output of MFCs was increased by the decreased internal resistance. The assembled MFCs possessed a short start-up time of 29.1 h, high maximum power density of 2270 ± 118 mW·m–2, desirable chemical oxygen demand removal efficiency of 71.7 ± 1.9%, and high decolorization efficiency of 90.3 ± 2.5% at 44 h. Fe/N codoped strategy is proposed to construct anodes for improving the electricity generation property and wastewater treatment efficiency of MFCs.

研究领域: 环境科学 · 生物电化学 · 材料科学 · 微生物学
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RSC Advances · 2020 ·Vol. 10 ·期 33 ·19169-19177 · IF 3.119

Design of a p–n heterojunction in 0D/3D MoS2/g-C3N4 composite for boosting the efficient separation of photogenerated carriers with enhanced visible-light-driven H2 evolution

Biao Zhou,Bo Yang,Muhammad Waqas,Ke Xiao,Caizhen Zhu,Ling Wu

Constructing a 0D/3D p–n heterojunction is a feasible strategy for accelerating photo-induced charge separation and promoting photocatalytic H2 production. In this study, a 0D/3D MoS2/g-C3N4 (0D/3D-MCN) photocatalyst with a p–n heterojunction was prepared via a facile light-assisted deposition procedure, and the 3D spongy-like g-C3N4 (3D-CN) was synthesized through simple thermolysis of NH4Cl and melamine mixture. For comparison, 2D-MoS2 nanosheets were also embedded in 3D-CN by a solution impregnation method to synthesize a 2D/3D-MCN photocatalyst. As a result, the as-prepared 0D/3D-MCN-3.5% composite containing 3.5 wt% 0D-MoS2 QDs exhibited the highest photocatalytic H2 evolution rate of 817.1 μmol h−1 g−1, which was 1.9 and 19.4 times higher than that of 2D/3D-MCN-5% (containing 5 wt% 2D-MoS2 nanosheets) and 3D-CN, respectively. The results of XPS and electrochemical tests confirmed that a p–n heterojunction was formed in the 0D/3D-MCN-3.5% composite, which could accelerate the electron and hole movement in the opposite direction and retard their recombination; however, it was not found in 2D/3D-MCN-5%. This study revealed the relationship among the morphologies of MoS2 using g-C3N4 as a substrate, the formation of a p–n heterojunction, and the H2 evolution activity; and provided further insights into fabricating a 3D g-C3N4-based photocatalyst with a p–n heterojunction for photocatalytic H2 evolution.

研究领域: 材料科学 · 能源化学
✓ 已验证 DOI PubMed 高影响因子
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ACS Applied Bio Materials · 2019 · IF 0

Promoting Nanozyme Cascade Bioplatform by ZIF-Derived N-Doped Porous Carbon Nanosheet-based Protein/Bimetallic Nanoparticles for Tandem Catalysis

Junsong Mou,Xianzhen Xu,Feifei Zhang,Jianfei Xia,Zonghua Wang

Nanozymes are a class of nanomaterials with enzyme-like activities that have been extensively studied for their possibilities and superiorities over natural enzymes. Intelligent design and fabrication of a nanozyme platform with highly efficient and stable tandem enzyme characteristics is necessary. Herein, a nanozyme cascade promoting bioplatform based on protein/bimetallic nanoparticles attached to ZIF-derived multilayer N-doped carbon nanosheets is proposed. Due to the carbon-based large surface area and solitary pairs of nitrogen electrons, the metal could be riveted to the carbon-based surface and reduced in situ to nanoparticles. Simultaneously, the addition of BSA has made it possible to establish a biological platform. The obtained BSA-PtAu@CNS has a linear range of 2 × 10–6 to 2 × 10–3 M for H2O2 and apparent dynamic Km of 0.005 × 10–3 M, which shows stronger affinity with H2O2 than HRP. The nanohybrid could adapt to severe reaction environment and enable prominent tandem dual-enzyme activity for glucose sensing. As a result, the cascade nanozyme bioplatform based on BSA-PtAu@CNS is accomplished and provides insights for subsequent biocompatible nanomaterials for use in medical and diagnostic applications.

研究领域: 生物材料学 · 医学诊断 · 纳米生物学
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Petroleum Science · 2021 · IF 4.09

N-hydroxyphthalimide anchored on hexagonal boron nitride as a metal-free heterogeneous catalyst for deep oxidative desulfurization

Lin-Jie Lu,Pei-Wen Wu,Jing He,Ming-Qing Hua,Yan-Hong Chao,Ning Yang,Lin-Lin Chen,Wei Jiang,Lei Fan,Hong-Bing Ji,Wen-Shuai Zhu

A metal-free N-hydroxyphthalimide/hexagonal boron nitride (NHPI/h-BN) catalytic system was developed for deep oxidative desulfurization (ODS) of fuel oils. Detailed experiments find that the heterogenization process of loading NHPI on h-BN not only benefits to the dispersion and utilization of NHPI, but also can significantly promote the catalytic performance. By employing NHPI/h-BN as the catalyst, azodiisobutyronitrile (AIBN) as the metal-free initiator, a 95% conversion of dibenzothiophene (DBT) can be acquired under the reaction conditions of 120 °C and atmospheric pressure with molecular oxygen (O 2 ) as oxidant. Moreover, the heterogenization is convenient for the regeneration of the catalyst with >94% DBT conversion after being recycled seven times. Characterizations illustrate that the promoted catalytic activity along with the regenerability originate from the interactions between NHPI and h-BN. The catalytic mechanism study shows that molecular oxygen is readily activated by the NHPI/h-BN to form a superoxide radical (O 2 •− ), which oxidize DBT to DBTO 2 for desulfurization.

研究领域: 化学工程 · 催化材料 · 环境科学
✓ 已验证 DOI 高影响因子
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Advanced Electronic Materials · 2023 ·Vol. 9 ·期 11 ·2300392 · IF 6.2

N-Type Doping and Passivation of Black Phosphorus Using Pentacene for Infrared Polarization-Sensitive Photodetection and Imaging

Guangliang Li,Lingxian Kong,Qi Su,Xianhua Tan,Xuning Zhang,Zhiyong Liu,Tielin Shi,Guanglan Liao,Bo Sun

Few-layer black phosphorus (FL-BP) shows great potential in infrared polarization-sensitive photodetection due to its narrow bandgap and strong in-plane anisotropy. However, FL-BP is easy to be oxidized and degraded, which severely restricts its applications. Herein, a simple and scalable in situ interfacial passivation method based on pentacene film is reported to enhance the ambient stability of FL-BP as well as achieve n-type doping for improved polarization-sensitive photoimaging. High crystal quality FL-BP flakes with intrinsic anisotropy are prepared by electrochemical exfoliation. The morphology and Raman spectra of FL-BP/pentacene exhibit excellent stability 28 days after passivation. In addition, the hole mobility is significantly enhanced and dark current is substantially suppressed due to the interfacial passivation and n-type doping effect. The FL-BP/Pentacene based photodetector shows a broadband response from visible to near-infrared with good stability. The photoresponsivity under 915 nm illumination is calculated as 2.2 mA W −1 with an anisotropy ratio of 1.29. Furthermore, the polarization imaging under the irradiation at zigzag and armchair directions directly reveals the strong infrared polarization-sensitive imaging capability of FL-BP/pentacene. This work also opens up new avenues to enhance the photoresponse and stability of various optoelectronics based on similarly unstable 2D materials.

研究领域: 纳米材料学 · 光电子学 · 二维材料 · 半导体物理 · 红外成像 · 表面科学
✓ 已验证 DOI 高影响因子
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INORGANIC CHEMISTRY · 2025 · IF 4.7

Structural Chemistry of AlCl3–N-Methylformamide Deep Eutectic Solvent: Study on Spectroscopy Techniques and Quantum Chemical Calculations

Qingling Meng,Xianwei Hu,Ruidong Guo,Aimin Liu,Jiangyu Yu,Zhongning Shi,Zhaowen Wang

The application of AlCl3-amide deep eutectic solvent (DES) prompted research into its physicochemical properties and ionic structures. In the present study, first, the viscosity, density, conductivity, and electrochemical behavior of AlCl3–N-methylformamide (AlCl3–NMF) DES were determined at 303–363 K. Then, types of complex ions and the bonding form in AlCl3–NMF were elucidated by Raman spectroscopy, nuclear magnetic resonance spectroscopy, and quantum chemical calculations. Finally, four chemical reactions between Al species and their thermodynamic data were clarified at 303–373 K. The results indicated that AlCl3–NMF exhibited satisfactory physical properties. Thus, AlCl3–NMF DES could be applied in various fields. The electrochemical study showed the reduction or oxidation behavior of Al (III) or Al. The complex species existing in AlCl3–NMF were identified as AlCl4–, Al2Cl7–, AlCl3L, and Al2Cl6L (“L” stood for NMF). Especially, Al species coordinated with NMF through carboxyl oxygen to generate AlCl2L2+, with an energy of −6.16 eV. Furthermore, [AlCl2NMF2]+[Al2Cl7]− exhibited weaker hydrogen bonding compared with [AlCl2NMF2]+[AlCl4]− in the system. Finally, thermodynamic calculations showed that the formation of the above Al species in AlCl3–NMF was exothermic within the temperature range of 303–373 K.

CAS / MDL: 123-39-7
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