SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Kudakwashe Meki,Zhuowen Wang,Baojian Jing,Shan Qiu,Fengxia Deng
In the face of challenges presented by rapid urbanization and industrialization, the surge in dye wastewater has emerged as a prominent concern. This study introduces a pioneering novel approach aimed at augmenting the electrocatalytic efficiency of O 2 reduction to H 2 O 2 through the modification of a hybrid catalyst with dimethyl sulfoxide (DMSO) to construct gas diffusion electrodes (GDEs). The hybrid catalyst, consisting of carbon black and DMSO, was meticulously fabricated, and its electrocatalytic activity was thoroughly investigated using various characterization techniques. Within 180 min, the 3 %DM cathode showcased efficient H 2 O 2 generation, reaching 850 μM, and remarkable oxygen utilization, achieving 60.49 %. Intriguingly, the fabricated 3 %DM hybrid catalyst maintained a three-phase interfacial (TPI) due to its super-hydrophilic property. This study elucidates the pivotal role of DMSO in enhancing the performance of hybrid catalysts for O 2 reduction to H 2 O 2 . The insights provide valuable perspectives into the development of efficient and resilient electrochemical systems for sustainable energy conversion and environmental applications.
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高影响因子
TALANTA
·
2024
·
IF 5.6
Yucheng Zhou,Chaoyan Zhang,Jiyang Liu,Yiping Mou
Sensitive detection of tumor biomarkers is of great significance for early cancer diagnosis, treatment evaluation, and recurrence monitoring. Development of convenient electrochemiluminescence (ECL) immunosensor using dissolved oxygen (O 2 ) as an endogenous co-reactant of luminol combined with efficient nanocatalysts to boost ECL signal in neutral media is highly desirable. Herein, sensitive detection of tumor biomarker using ECL of luminal-O 2 enhanced by confinement of nitrogen-doped graphene quantum dots (N-GQDs) and platinum nanoparticles (PtNPs) on nanochannel array was demonstrated. A high-density nanochannel array-modified electrode was achieved by rapidly growing an amino-functionalized vertically-ordered mesoporous silica film (NH 2 -VMSF) on the inexpensive and readily available indium tin oxide (ITO) electrode. Through simple electrodeposition, N-GQDs were confined and PtNPs were in-situ synthesized in nanochannels of NH 2 -VMSF. These confined nanocomposites catalyzed the electroreduction of O 2 at negative potentials to generate a large amount of reactive oxygen species (ROS) and facilitated luminol oxidation, enhancing the ECL signal of luminol by 25 times. Two immunosensors were fabricated after covalent immobilization of the recognition antibody of carbohydrate antigen 199 (CA199) or carbohydrate antigen 125 (CA125) on the outer surface of the NH 2 -VMSF and blocking of non-specific sites. When tumor biomarkers bind to the corresponding antibodies on the recognition interface, the formed immunocomplex hindered the diffusion of luminol to the underlying electrode, resulting in a decrease in the ECL signal and sensitive detection of tumor biomarker. The constructed CA199 immunosensor exhibited a linear detection range for CA199 from 0.5 mU mL −1 to 50 U mL −1 , with a detection limit (DL) of 0.03 mU mL −1 . For CA125 detection, linear detection ranged from 0.5 mU mL −1 to 500 U mL −1 , with a DL of 0.005 mU mL −1 . The fabricated immunosensors demonstrated good selectivity and high reproducibility. This study provides great potential for the development of efficient luminol ECL systems in neutral media and expands the biological application in sensitive detection of tumor biomarker.
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
shuailong Song,Zhinan Wu,Tong Zhou,Yunxia Wen,Wei Cao,Han Lin,Xiaohua Lu,Tuo Ji,Jiahua Zhu
The major challenge that solid amine sorbents face in practical large-scale applications is their susceptibility to degradation under humid and oxygen-containing conditions. This study developed a superhydrophobic alkyl-silica by co-hydrolyzing alkyl-silane and tetraethyl orthosilicate and then immobilizing polyethyleneimine as a CO2 sorbent. By adjusting the chain length and density, the surface of the alkyl-silica has abundant alkyl chains, and the PEI molecules are intercalated into the surface alkyl layer. These alkyl chains effectively block the contact of O2 and H2O with the amine group, thereby selectively allowing the adsorption/desorption of CO2 molecules through the alkyl layer. The results showed that the working capacity of PEI/alkyl-silica was maintained at 86% by oxidation treatment and 85% by rinsing treatment, respectively, exhibiting excellent stability compared to unprotected PEI/SiO2. Meanwhile, the alkyl chain due to the steric hindrance effect weakens the interaction between CO2 and amine and does not reduce its original working capacity. The energy consumption of PEI/alkyl-silica during regeneration was lowered to 1.24 GJ·t-1-CO2. This interfacial building concept provides a new path for designing a long-term stable amine sorbent for cost-effective CO2 capture by avoiding the contact of O2 and H2O with the amine.
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ChemSusChem
·
2024
·
IF 7.5
Dan Li,Qian Chen,Rui Li,Yaolin Hou,Yulong Liu,Haiming Xie,Jia Liu,Jiefang Zhu
Graphical The incorporation of the polyionic liquid additive [PBVIm]-TFSI in LiI-mediated Li-O 2 batteries enables the in situ formation of a protective layer on the Li anode. [PBVIm] + cations migrate to the Li anode, forming a cationic shield that promotes uniform Li + deposition. A [PBVIm][TFSI]-containing cell demonstrates a considerable reversibility and cycling stability. Redox mediators (RMs) have shown promise in enhancing Li-O 2 battery cycling stability by reducing overpotential. However, their application is hindered by the shuttle effect, leading to RM loss and Li anode corrosion. Here, we introduce a polyionic liquid, poly (1-Butyl-3-vinylimidazolium bis(trifluoromethanesulfonylimine)) ([PBVIm]-TFSI) as an additive, showcasing a novel Li anode protection strategy for LiI-mediated Li-O 2 batteries. [PBVIm] + cations migrate to the Li anode, forming a protective cationic shield that promotes uniform Li + deposition. The addition of [PBVIm]-TFSI enhances the cycling stability, achieving 105 cycles at 200 mA⋅g −1 , compared to the cell with LiI which exhibited 38 cycles under the same conditions. Synchrotron X-ray tomography reveals the evolution of this protective layer, providing insights into its formation mechanism, in conjunction with XPS analysis. Our findings offer a new approach to Li anode protection in Li-O 2 batteries, emphasizing the critical role of interfacial engineering for battery performance.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Shuang Zhou,Da Wen,Wei Zhong,Jianjun Zhang,Yaorong Su,Aiyun Meng
The effective adsorption of oxygen (O 2 ) molecules over photocatalysts is a critical step in promoting the performance of photocatalytic H 2 O 2 production. However, g-C 3 N 4 usually features a Yeager-type (side-on) adsorption configuration of O 2 molecules, which causes the breaking of O–O bonds and severely hinders the H 2 O 2 production activity. Herein, we synthesized an oxygen-vacancy-rich TiO 2– x /g-C 3 N 4 step-scheme (S-scheme) heterojunction to regulate the oxygen adsorption configuration and improve the 2e – ORR selectivity of H 2 O 2 production. In-situ X-ray photoelectron spectroscopy (in-situ XPS) and density functional theory (DFT) calculations reveal that the S-scheme heterojunction is formed between TiO 2– x and g-C 3 N 4 . The difference between their Fermi levels leads to the electron flow from g-C 3 N 4 to TiO 2– x , which increases the electron-deficient sites in g-C 3 N 4 . As a result, the cleavage of O–O bonds on the surface of g-C 3 N 4 is avoided and the oxygen adsorption configuration is tuned from Yeager-type to Pauling-type (end-on). Consequently, the photocatalytic H 2 O 2 production rate is dramatically improved to 1780.3 μmol h –1 , which is about 5 times higher than that of pristine g-C 3 N 4 . This work paves a new way to tailor the oxygen adsorption configuration by rationally designing S-scheme heterojunction photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jiaming Wang,Feifei Kang,Yifei Chen,Xiujuan Zhang,Xiaobin Jiang,Gaohong He,Xuehua Ruan
Artificial lung membranes are the heart for extracorporeal oxygenation. Hereinto, the nonporous PDMS-based membranes have excellent biocompatibility, and also isolation ability to both blood and harmful matters. Nevertheless, their CO 2 /O 2 selectivity, in the conventional cases using pure-oxygen sweeping stream, is not enough to accomplish sufficient CO 2 removal in balance with O 2 addition. In this work, the oxygenation mode using oxygen-enriched stream, faithfully based on the permeation mechanism, is established to overcome this bottleneck. To neutralize the negative impacts caused by lowering oxygen content and its partial pressure, PDMS-based composite membranes with ultra-thin selective layer to enhance mass transfer have been fabricated successfully. The experiments manifest that the selective layer, on the basic condition that the composite structure is stable enough to make surface modification and realistic utilization, is decreased to 376 nm on the porous substrates. O 2 and CO 2 permeation rates through the ultimate membrane samples have been enhanced to 502 GPU and 4117 GPU, respectively. In this instance, the essential oxygenation could be sustained with O 2 partial pressure less than 446 mmHg in the sweeping stream. The minimum membrane area for a common treatment case is 0.05 square meters. Once the membrane area is increased to 0.18 square meters, the sterile air after purification could be directly used for oxygenation. In comparison to the oxygenation devices being used currently, membrane area can be saved by about 90 %, which is highly significant to reduce the injuring influence on blood cells. All in all, the artificial lung membranes with ultra-thin PDMS coating layer have promising future in realistic utilization.
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高影响因子
RSC Advances
·
2018
·Vol. 8
·期 56
·32325-32332
·
IF 2.936
Yuhan Zhu,Yu Pan,Wenjun Wang,Haibing Xu,Liqun Zhou,Xiaoguang Liu,Ling Li
The local crystal sites occupied by Eu3+ in Ca5(BO3)3F:1% Eu3+ phosphor were investigated experimentally and theoretically. Ca5(BO3)3F:1% Eu3+ was synthesized by high-temperature solid-state method in air. The crystal structure and optical properties of the phosphor were studied by X-ray powder diffraction and photoluminescence, respectively. Two different O2− → Eu3+ CT broad bands with the peaks at 266 and 283 nm in Ca5(BO3)3F:1% Eu3+ were detected, indicating the Eu3+ sites occupied Ca2 and Ca1, respectively. The different sharp f–f emission spectra under the excitation of 283 and 266 nm proved that there are two different local lattice environments around Eu3+ existing in Ca5(BO3)3F:1% Eu3+. Environmental factor he, the standard deviation of environmental factor (EFSD) and the bond energy were used to illustrate and explain the site occupancy mechanism of Eu3+ into the host lattice. By comparing the intensity ratios of 5D0 → 7F2 transition to the 5D0 → 7F1 transition, I(5D0/7F2)/I(5D0/7F1) of Eu3+ at Ca2 (7.381) was found to be 2.5 times stronger than that of Eu3+ at Ca1 site (2.933). was calculated to analyze the I(5D0/7F2)/I(5D0/7F1) value. On the basis of the bond valence model, a bond-energy method was used to study the occupancy of the Eu ion, which indicated that the preferential sites of Eu ion occupancy in the Ca5(BO3)3F are the Ca2 and Ca1 sites. All three theoretical calculation results are consistent with each other.
研究领域:
材料科学
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固体化学
·
光学
·
晶体学
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DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2025
·
IF 1.6
Zhiqing Liang,Zhongying Liu,Xiuyuan Wei,Hui Wu,Chanjuan Liu,Xiaohua Huang
Bifunctionalized NH2-UiO-66-CF3 nanofillers were successfully prepared by grafting - CF3 on NH2-UiO-66 via aldehyde-amine condensation reaction and applied to the preparation of 6FDA-ODA/NH2-UiO-66-CF3 mixed matrix membranes (MMMs). The successful introduction of -NH2 and -CF3 groups was verified by FT-IR, XRD, and XPS characterization, and the integrity of the crystal structure was ensured. Due to the presence of hydrogen bonding, NH2-UiO-66-CF3 showed good interfacial compatibility with the polymer matrix. Due to the introduction of the - CF3 group, the MMMs exhibited excellent thermal stability (T10% > 500°C, Tg = 300°C–305°C), hydrophobicity (contact angle of 92.96–97.71), and mechanical properties (tensile strength of 74–85 MPa). The gas separation performance tests showed that the MMMs exhibited significantly improved gas permeability and selectivity compared to the pure 6FDA-ODA membranes, which was attributed to the fact that the -NH2 and -CF3 groups provided more adsorption sites for gases. In particular, the PI/NUF(10) MMMs showed the best performance, with permeabilities of 42.71, 9.22, and 92.79 Barrer for CO2, O2, and He, respectively, which were 248%, 213%, and 173% higher than those of the pure membranes. Meanwhile, the selectivities of CO2/N2, O2/N2 and He/N2 were improved by 37%, 24%, and 8%, respectively. Close to the Robeson upper limit, demonstrating excellent gas separation potential.
研究领域:
材料科学
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化学工程
·
膜技术
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气体分离
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纳米技术
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高影响因子
Communications Chemistry
·
2025
·Vol. 8
·期 1
·389
·
IF 6.2
Han Lei,Tan Jingying,Zhang Yucui
Given the promising prospect of nanozymes in colorimetric test strips, it is essential to eliminate the interferences of their multi-activities and various colors on the test strip. Here, white Mn-based metal-organic frameworks (Mn-MOFs) with ultrathin 2D morphology (3 nm thick) were successfully synthesized by a simple ultrasonic approach. The origin of the white optical property in Mn-MOFs was systematically investigated, revealing that it stems from specific metal-ligand coordination polymerization rather than morphological features or defect states. Mn-MOF nanozymes possessed exclusive peroxidase-mimicking activity rather than oxidase-like activity, effectively resisting O 2 interference during colorimetric assay. Moreover, Mn-MOF nanozymes displayed unique substrate selectivity without additional modification. Unlike other colored nanozymes, the whiteness of Mn-MOF nanozymes enhanced the paper’s whiteness, boosting contrast for colorimetric detection on test strip. This study pioneers a systematic investigation into the origin of whiteness in MOF nanozymes. The coordination-defined properties enable interference-free optical design and O 2 -resistant on-site detection.
研究领域:
材料科学
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纳米技术
·
分析化学
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生物传感器
·
酶模拟
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·Vol. 60
·期 48
·25148-25163
·
IF 3.9
Zhang Zhenyan,Chai Huan,Yu Zhengqian,Li Jinsheng,Li Pengfei,Wu Lei,Li Zhanshuai,Qi Xiwei
TiO 2 -based materials are widely used in high-temperature capacitors and aerospace electronics but face challenges such as high dielectric loss and limited thermal stability in conventional single-component systems. To address these issues, we propose a novel strategy integrating high-entropy doping design and oxygen vacancy engineering. In 2 O 3 -doped (GeMnTiSnMo)O 2 high-entropy ceramics (GMTSMO- x In, x = 0.1–1) were synthesized via solid-state reaction. Experimental results reveal that In 3+ doping generates high-density oxygen vacancies (V o ·· ) through charge compensation, forming [Ti 3+ - V o ·· -Ti 3+ ] and [Mn 3+ - V o ·· -Mn 3+ ] defect-dipole clusters. These clusters enhance electron localization and suppress carrier migration, reducing dielectric loss by threefold. Simultaneously, oxygen vacancy enrichment strengthens interfacial polarization, increasing the dielectric constant by fourfold. The optimal GMTSMO-0.5In exhibits a relative permittivity ( ε r ) of 4.0 × 10 6 and a low loss tangent of 15 at 650 ℃/100 Hz, outperforming traditional TiO 2 -based materials and existing high-entropy oxides. All compositions demonstrate excellent temperature stability (25–400 ℃) and frequency-independent behavior above 10 4 Hz. This work provides a high-entropy-driven approach for dynamic defect engineering, paving the way for advanced dielectric materials in extreme-condition energy storage systems.
研究领域:
材料科学
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陶瓷与介电材料
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电子材料
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储能技术
·
缺陷化学
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高影响因子
CHEMISTRY OF MATERIALS
·
2025
·
IF 7
Jiale Han,Guofan Wang,Xu Hu,Jinlin Li,Zhaojun Xie,Zhen Zhou
Rechargeable lithium oxygen (Li–O2) batteries are regarded as promising candidates for future energy storage systems due to their exceptionally high theoretical energy density. However, their practical implementation faces major obstacles, including high charge and discharge overpotentials and a semiopen battery structure that is highly sensitive to humidity. These factors lead to reduced efficiency and poor stability in moist air, significantly limiting real-world application. To address these challenges, a composite photoelectrode was developed by directly growing tungsten trioxide (WO3) nanoribbons on carbon paper (CP), followed by the uniform deposition of platinum nanoparticles using atomic layer deposition. Compared to WO3 photoelectrode, the resulting Pt–WO3 photoelectrode enables stable operation of photoassisted Li–O2 batteries under humid oxygen atmosphere. The batteries sustain stable operation for over 100 cycles without failure at current densities of 0.05 and 0.2 mA cm–2. Advanced characterization and theoretical calculations confirm the formation of an ohmic contact between platinum and tungsten trioxide, which promotes the separation of photogenerated electrons and holes, improves charge transfer, and facilitates the reversible formation and decomposition of lithium hydroxide (LiOH). This strategy effectively overcomes critical barriers faced by conventional Li–O2 batteries in real-world environments and provides a promising direction for the design of environmentally tolerant and photoelectrochemically efficient energy storage systems.
研究领域:
能源材料
·
电化学
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纳米材料
·
光电化学系统
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Zhiwei Yang,Yiwen Luo,Jiapeng Yue,Xinyu Wang,Hao Xu,Qian Ye,Yujian Zhang,Xinyi Xing,Qingguo Wang,Jing Zhang
This study proposes a method to activate O 2 by accelerating the corrosion process for zero-valent zinc (ZVZ) with the assistance of Cu(II), promoting the consecutive production of reactive oxygen species . The mechanisms for reactive oxygen species generation are clarified with metronidazole (MTZ) as the targeted pollutant. The outcome suggests the association of Cu(Ⅱ) and ZVZ presents an apparent cooperative activity, an enhancement of 85% in MTZ removal is attained for the ZVZ/Cu(Ⅱ) system after 10 min compared to that for ZVZ. Analysis of the mechanisms involved indicates that this improvement is due to the addition of Cu(Ⅱ), which can accelerate the corrosion of ZVZ. In addition, quenching experiments and electron paramagnetic resonance (EPR) technology show that superoxide radicals (·O 2 − ) result in rapid MTZ degradation. The primary component that is liable for O 2 activation and a certain amount of H 2 O 2 generation is verified to be ZVZ. Moreover, Cu(I) is detected in the ZVZ/Cu(Ⅱ) system, which arises from a direct reduction pathway driven by ZVZ and an indirect reduction pathway driven by active hydrogen atoms .
研究领域:
环境科学
·
化学工程
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高影响因子
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