ENVIRONMENTAL RESEARCH
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2024
·
IF 7.7
Min Zhang,Jin Wang,Xinyuan Zhan,Wusong Xu,Maolin He,Ding Ma,Zhengbo Yue
Thiocyanate (SCN − ), a non-volatile inorganic pollutant, is commonly found in various types of industrial wastewater, which is resistant to hydrolysis and has the potential to be toxic to organisms. Premagnetized iron-copper-carbon ternary micro-electrolytic filler (pre-Fe/Cu/C) was prepared to degrade SCN − . Pre-Fe/Cu/C exhibited the most significant enhancement effect on SCN − removal when magnetized for 5 min with an intensity of 100 mT, and the SCN − removal rate was the highest at an initial pH of 3.0 and an aeration rate of 1.6 L/min. The electrochemical corrosion and electron transfer in the pre-Fe/Cu/C system were confirmed through SEM, XPS , FTIR , XRD , and electrochemical tests. This resulted in the formation of more corrosion products and multiple cycles of Fe 2+ /Fe 3+ and Cu 0 /Cu + /Cu 2+ . Additionally, density functional theory (DFT) calculations and electron paramagnetic resonance (EPR) were utilized to illustrate the oxygen adsorption properties of the materials and the participation of reactive oxygen species ( 1 O 2 , ·O 2 − , and ·OH) in SCN − removal. The degradation products of SCN − were identified as SO 4 2− , HCO 3 − , NH 4 + , and N 2 . This study introduced the use of permanent magnets for the first time to enhance Fe/Cu/C ternary micro-electrolytic fillers, offering a cost-effective, versatile, and stable approach that effectively effectively enhanced the degradation of SCN − .
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高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Xiaonan Huang,Yulian Chen,He Jiang,Jiajun Hu,Xi Guo,Yanjuan Zhang,Jianzhang Li,Weisheng Sun,Yi Zhang
The development of melamine-formaldehyde (MF) resin-impregnated paper has great significance in the decoration and construction industries. However, the MF-impregnated paper is prone to cracking and burning due to the inherent brittleness and poor flame retardancy of MF resin, restricting its wide application. Herein, we report a hyperbranched polysiloxane (HBPSi@EP) containing a flexible Si–O–C skeleton and tailored terminal epoxy using a simple, low-cost, and easily controlled ester exchange strategy to modify MF resin for fabricating high-performance and multifunctional impregnated paper. The break elongation of MF/HBPSi@EP impregnated paper increased by 186.5% since the energy dissipation of the hyperbranched structure and lubrication of the Si–O–C skeleton enhance its toughness. The tough MF/HBPSi@EP impregnated paper displayed outstanding cracking resistance during the thermal–cooling cycle. Meanwhile, the tensile strength of MF/HBPSi@EP impregnated paper reached 10 MPa, owing to the formation of a dense cross-linked structure by the hyperbranched epoxy in the HBPSi@EP. Notably, this impregnated paper exhibited good flame retardancy (B1-level in GB 8624-2012), cigarette burn resistance (Level 4 in GB/T 17657-2013), and wear resistance (1305.5 r). This facile and effective strategy can promote the development of tough, strong, and versatile coatings, film materials, and multifunctional composites.
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Small
·
2024
·Vol. 20
·期 50
·2406489
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IF 13
Yijun Gao,Shanshan Song,Fei He,Xianglong Kong,Zhong Xiao,Xianchang Cui,Linbo Cao,Yumeng Zhang,Zhiliang Liu,Piaoping Yang
Silicon (Si) has attracted considerable attention as a promising alternative to graphite in lithium-ion batteries (LIBs) because of its high theoretical capacity and voltage. However, the durability and cycling stability of Si-based composites have emerged as major obstacles to their widespread adoption as LIBs anode materials. To tackle these challenges, a hollow core–shell dodecahedra structure of a Si-based composite (HD-Si@C) is developed through a novel double-layer in situ growth approach. This innovative design ensures that the nano-sized Si particles are evenly distributed within a hollow carbon shell, effectively addressing issues like Si fragmentation, volume expansion, and detachment from the carbon layer during cycles. The HD-Si@C composite demonstrates remarkable structural integrity as a LIBs anode, resulting in exceptional electrochemical performance and promising practical applications, as evidenced by tests in pouch-type full cells. Notably, the composite shows outstanding cycling stability, retaining 85% of its initial capacity (713 mAh g −1 ) even after 3000 cycles at a high current rate of 5000 mA g −1 . Additionally, the material achieves a gravimetric energy density of 369 W h kg −1 , showcasing its potential for efficient energy storage solutions. This research signifies a significant step toward realizing the practical utilization of Si-based materials in the next generation of LIBs.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yao Shen,Ke Wang,Lu Li,Jingkai Zhao,Jiexu Ye,Ping Chen,Xiang Gao,Shihan Zhang
Catalyst-aided CO 2 desorption offers a promising reduction in the energy penalty of amine scrubbing, but faces the challenges of slow mass transfer, sluggish desorption kinetics, and susceptibility to deactivation. In this work, a hollow composite catalyst C@ZrO 2 was developed to simultaneously realize rapid electron, proton and mass transfer for CO 2 desorption via facilitating proton-coupled electron transfer (PCET) effect. The CO 2 desorption rate of benchmark MEA solution increased by 126% and relative heat duty decreased by 69.9% in presence of C@ZrO 2 , and its catalytic performance didn’t noticeably decline after 10 cycles. Additionally, the desorption rate of biphasic solvents with a high viscosity increased by 112% and relative heat duty decreased by 57.3% with C@ZrO 2 . Based on theoretical calculation, the facilitated PCET efficiency of carbon layer increased the binding energy of carbamate to enhance its mass transfer rate from the liquid phase to the C@ZrO 2 surface, and stretched the C-N bond to reduce the proton transfer energy barrier by 66.8%. This work provided a novel insight to design catalysts for energy-efficient and stable CO 2 capture.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Jiangtao Ma,Yujun Zhu,Kai Huang,Peng Wang,Dinghua Liu,Yupei Zhao
In recent years, high-entropy alloy materials have garnered widespread attention in the field of water electrolysis catalysts, owing to their exceptional electrochemical performance . However, synthesizing efficient and highly stable catalysts remains a formidable challenge. This study presents the preparation of a highly stable FeCoNiCuMo/C high-entropy alloy catalyst , exhibiting an overpotential of 324 mV at a current density of 10 mA·cm −2 in a 1.0 M KOH solution, comparable to commercial RuO 2 . The Tafel slope reaches 70.5 mV·dec −1 , and the charge transfer resistance is only 3.6Ω, demonstrating outstanding electrochemical performance. Furthermore, stability tests conducted over 72 h indicate the excellent stability of the prepared high-entropy alloy catalyst, with only a slight deviation observed after 5000 cycles of accelerated durability experiments. Theoretical calculations show that due to lattice distortion and cocktail effect, the d-band center of FeCoNiCuMo/C moves away from the Fermi surface compared to the pure component, which attenuates the adsorption of the reaction intermediates and leads to a significant decrease in the oxygen evolution reaction overpotential. This study validates the potential for long-term, efficient, and stable operation of high-entropy alloys as water electrolysis catalysts, providing experimental support for expanding the application scope of HEA.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Ling-Xia Yun,Xin-Ran Shi,Tian-Bao Chen,Yu-Hang Gu,Meng Qiao,Hang-Tian Zhang,Jie-Xin Wang
Regarding the environmental and ecological hazards of waste plastics, the unexploited polyester resources promise to produce valuable chemicals and fuels by electrocatalytic upcycling in combination with alkaline hydrolysis. Herein, we propose a universal approach to synthesize carbon supported NiCo 2 O 4 nanoparticles (NPs) utilizing high gravity technology combined with heat treatment for electrocatalytic valorization of polyethylene terephthalate (PET). This route enables instantaneous and continuous precipitation of the composites including Co-NH 3 complex and Ni hydroxide on carbon in a rotating packed bed (RPB) reactor, and achieves ultrasmall and ligand-free NiCo 2 O 4 NPs (6 nm) with significantly improved dispersity after heat treatment. The as-prepared NiCo 2 O 4 NPs/C converts PET-derived EG to formate with a promising faradaic efficiency (FE) of over 90 % and a high productivity of about 4.5 mmol·cm −2 ·h −1 at 1.5 V (vs RHE). Furthermore, this strategy can also be extended to the preparation of other supported ternary oxide NPs for efficient electro-oxidation of PET hydrolysate.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2024
·
IF 4.1
Haiping Lei,Tianwei Wei,Jiguo Tu,Yiwa Luo,Suqin Li,Shuqiang Jiao
NiO possesses a high theoretical capacity, but its poor conductivity and significant volume changes during the redox process lead to severe electrochemical performance degradation, limiting its applications. In this study, flower-like structure NiO@C composite materials were synthesized via a hydrothermal method. The particle size of the material is approximately 10–16 μm, with a well-defined morphology of carbon material composite. Al-NiO@C batteries were constructed using NiO@C cathode and subjected to electrochemical performance testing. The initial discharge capacity of NiO@C composite material at a current density of 200 mA g −1 is 126 mA h/g, and even after 150 cycles, it retains a discharge specific capacity of 54 mA h/g. In contrast, the pure NiO exhibits an initial capacity of only 49 mA h/g, which decreases to 23 mA h/g after 150 cycles. The cycling stability of NiO@C material is significantly better than that of NiO alone. This improvement is attributed to the enhanced conductivity of NiO material by the addition of carbon material, which provides improved electron/ion transport properties. Additionally, the inclusion of carbon material helps alleviate the volume changes of NiO during the reaction process, thereby enhancing the overall electrochemical performance of Al-NiO batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaomei Li,Linfeng Fu,Lin Cao,Lihui Lei,Xinxing Zhan,Changgang Hu,Xin Tong,Juan Tian
Ordered platinum intermetallic alloys, due to their structured chemical composition and high activity, have been considered as one of the ideal electrocatalysts for fuel cells. Ensuring the controlled structure of alloy nanoparticles (NPs) is a prerequisite for obtaining highly active platinum-based alloy catalysts. In this study, we employed different pH adjusters to modulate the crystallization of Pt alloy NPs in catalysts. By balancing the competition between precipitation and complexation reactions in the solution, the size and structure of platinum alloy particles can be effectively adjusted. Utilizing NH 3 ·H 2 O as a pH adjuster, we synthesized an ordered PtCu 3 alloy catalyst with a particle size of 3.3 nm. This catalyst exhibits a half-wave potential of 0.945 V and a mass activity of 1.061 mA µg Pt –1 , which is 11.7 times higher than that of commercial 20 % Pt/C (TKK). This enhancement in catalytic activity is attributed to the introduction of transition metal copper atoms into the catalyst, forming an ordered intermetallic structure that induces compressive strain. This strain lowers the d-band center, weakens the adsorption of oxygen-containing intermediates, which strengthen catalytic activity. Therefore, by adjusting the morphology of metal precursors to improve the microstructural form and state of the catalyst, the oxygen reduction activity can be significantly enhanced.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Qiang Zhong,Yan Xue,Zihao Qi,Yue Sun,Leliang Wu,Dunyu Sun,Chenmin Xu,Kwangchol Ri,Shaogui Yang,Jiandong Zhu,Qiuyi Ji,Yazi Liu,Shiyin Li,Huan He
Two-dimensional cage-in-cage carbon-coated FeSeS superlattices with varying degrees of sulfidation (FeSeS@C) are developed for activating peroxymonosulfate (PMS) to effectively degrade diatrizoic acid (DTZ), and the intrinsic origin that govern the activity of FeSeS@C are deeply elucidated. Experimental and theoretical analyses manifested that proper sulfidation led to increased surface acidity of FeSeS@C. The high surface acidity can optimize the exposure and spin state of Fe sites for FeSeS@C-4, a high spin state of Fe (6.27 μ B ) not only regulating PMS adsorption for enhancing the charge density, but also expediting interfacial charge deliver to trigger the efficient PMS activation. Therefore, among FeSeS@C, FeSeS@C-4 exhibited the best degradation performance for DTZ, with first-order kinetic rate constants (k obs ) of 0.232 min −1 and degradation rate of 100 %. This study demonstrates a novel application of cage-in-cage superlattices in environmental remediation and offers new insights into the mechanism of PMS activation by sulfur modification Fe-based catalysts.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 17
·7639-7645
·
IF 2.7
Qianxi Wang,Yuyu Dai,Xueli Hong,Yunyang Hong,Rui Zhang,Xinhuan Yan
Non-precious metal catalysts play a significant role in the field of hydrogenation. This study synthesized Co-BTC from cobalt nitrate hexahydrate and 1,3,5-tricarboxylic acid benzene. By changing the calcination temperature of Co-BTC in an inert atmosphere, a series of novel non-precious metal Co/C microsphere catalysts were successfully prepared. The composition and structure of the Co/C-n catalysts were characterised by FESEM, TEM, XRD, IR, XPS and BET. These results confirm that 1,3,5-benzenetricarboxylic acid provides a rich carbon matrix and metallic Co nanoparticles are generated by self-reduction on the carbon matrix. The graphite matrix formed during the calcination process has a rich pore structure and good dispersion of active components on the catalyst surface, which is very favourable for the catalytic reaction. In the hydrogenation of o-chloronitrobenzene (o-CNB) to o-chloroaniline (o-CAN), the Co/C-500 catalyst showed the best catalytic performance. At 80 °C and 2 MPa H2 for 60 minutes, the conversion rate of o-CNB reached 99% and the selectivity reached 99%. When the reaction takes 5 minutes, the conversion rate reaches 10.5%, and the TOF value reaches 36.3 h−1. The Co/C-500 catalyst can be easily recycled and reused after reaction with the help of a magnetic field. Moreover, this catalyst is also effective in the selective hydrogenation of other nitroaromatic hydrocarbons containing halogen or unsaturated groups to corresponding aniline. This simple and direct synthesis method may lead to the economic production of large-scale Co/C catalysts, which is an attractive prospect for the industrial trial production of corresponding aniline.
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RSC Advances
·
2024
·Vol. 14
·期 12
·8100-8107
·
IF 3.9
Yu Hua,Xiaomeng Zhang,Fulin Chen,Yuantao Sun,Xinyu Wang,Ziliang Wen,Qinghao Tan,Chenxi Sun,Buhe Bateer
In this study, we utilized a simple calcination method to prepare a Ni/TiO2/C composite, which was synchronously grown from magnetic, semiconductor, and conductive materials. XRD, SEM, Raman, and XPS characterization methods were used to analyze the crystal structure, graphitization degree, morphology size, and valence state of Ni/TiO2/C, and its electromagnetic wave absorption performance was tested. It was revealed that rod-like Ni/TiO2/C had good electromagnetic wave absorption performance at a thickness of 1–5.5 mm; in particular, its reflectance reached −40 dB at 3.5 mm and its absorption bandwidth (reflectivity < −10 dB) reached 4.4 GHz (6.0–10.4 GHz) at a thickness of 4.0 mm. It was thus revealed that its electromagnetic wave absorption rate and absorption bandwidth can be regulated by its thickness. Compared with Ni/TiO2, it was proven that the conductive materials (carbon), magnetic materials (Ni), and semiconductor materials (TiO2) in the rod-like Ni/TiO2/C composite can synergistically absorb electromagnetic wave energy through dielectric and magnetic losses.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Nan Wang,Zhiwei Zhou,Chunjiao Liu,Yongwang Liu,Xing Li,Yanling Yang,Li Zhao
Algae-derived organic matter (AOM) limits the effectiveness of conventional water treatment processes, affects the normal operation of water treatment plants, and causes water quality deterioration. Efficient elimination of AOM is an urgent issue in the advanced treatment of drinking water. In this study, A heterogeneous interface for AOM removal was established based on BT/C, which can be driven by visible light. The removal efficiencies of extracellular organic matter (EOM), intracellular organic matter (IOM), and AOM by BT/C reached the optimal levels at 30 min, 60 min, and 90 min, respectively, reaching 48.5 %, 81.8 %, and 74.0 %. BT/C can oxidize and break down a large amount of high-molecular-weight organic matter in EOM into medium- and low-molecular-weight organic substances, and effectively remove the low-molecular-weight organic matter in EOM. In addition, BT/C can efficiently remove humic acids(HS) and aromatic protein organic matter in IOM, directly mineralize or decompose high-molecular-weight biopolymers into small-molecular-weight acidic and neutral organic matter; electron paramagnetic resonance spectroscopy and reactive oxygen species trapping experiments verified that hydroxyl radical (·OH) have play most important role on the degradation of various molecular weight organic matters. Superoxide radical (·O 2 – ) plays a dominant role in the oxidation process of soluble microbial metabolites and HS, and ·OH plays a significant role in the oxidation process of amino acid-like proteins. This study provides new ideas and technical support for the complete removal of algae-derived organic matter and the protection of drinking water safety.
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