ANALYTICAL CHEMISTRY
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2024
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IF 6.7
Jiamin Luo,Heng Lu,Bao-Ying Wen,Qiaowen Zheng,Junying Zhang,Yishan Li,Wenping Hong,Shanshan Zhao,Libo Shun,Feiming Li,Zhixiong Cai,Jin-Ming Lin,Qiang Chen,Maosheng Zhang,Jian-Feng Li
Methyl iodide (CH3I) gas as a toxic gas causes great harm to organisms due to its high volatility and high reactivity with biological nucleophiles. Unfortunately, the sensing and detection of CH3I gas are challenging because of the diffusive nature of the gases and its low concentrations in the environment. Herein, we have developed a fast, green, and sensitive CH3I gas visual sensing method based on the capture technology of toxic gases by natural deep eutectic solvents (NADESs) coupled to the halide rapid exchange capability of perovskite nanocrystals (PNCs). In this strategy, NADESs are used as an absorption solution to adsorb gaseous CH3I, while simultaneously exposing I– through the action of the nucleophilic reagent; then, CsPbBr3 PNCs were synthesized in NADESs and used as sensing material to achieve I– exchange. Benefiting from the capture and enrichment of CH3I gas, the sensitivity of the gas sensor was highly improved. The sensor exhibited the lowest detection limit (limits of detection) of 164.15 μmol/m3, below the minimum safe level for human inhalation, which is 200 μmol/m3. This breakthrough offers greater possibilities for the quantitative detection of CH3I gas.
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高影响因子
LANGMUIR
·
2024
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IF 3.7
Fajun Li,Huaizhu Wang,Guizhi Wang,Min Ding,Qihui Ma,Haifeng Xu,Zhong Jin
Advancements in cost-effective, high-performance alkaline water-splitting systems are crucial for the hydrogen industry. While the significance of electrode material design has been widely acknowledged, the practical implementation of these advancements remains challenging. In this study, we focused on the holistic design of the electrolysis system and successfully developed a novel alkaline water-splitting electrolyzer. The unique configuration of our electrolyzer allows the designed NiFe-LDH/carbon cloth gas diffusion anode to interact solely with the PVA-based gel membrane and air, enabling the direct discharge of oxygen into the gas phase. This innovative feature accelerates anode bubble overflow, reduces gas interference, and decreases the system impedance by minimizing electrode spacing. As a result, by utilizing the NiFeSn-alloy/nickel mesh cathode, our electrolyzer achieves a high current density of 308 mA cm–2 at a cell voltage of 2.0 V and demonstrates exceptional stability over 1000 h.
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ENERGY & FUELS
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2024
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IF 5.2
Yuan-Ming Cao,Xue-Lei Duan,Miao Bian,Hou-Yu Wang,Yi-Wen Shen,Chong Gao,Chun-Gang Yuan
The immobilization of Hg0 and detoxication of Hg-containing composites are enormous challenges for Hg pollution control, which provide a high requirement for the design and synthesis of materials. Herein, a new composite with halloysite, selenium, and transition metals as raw materials (FeCo-LDH/HNTs@Se) for a Hg0 trap was designed by precipitation with ion exchange and an in situ selenization method. Intrinsic features such as high affinity, microwave permittivity (109–1012), large surface area, abundant pores, and many active components favored Hg0 removal and immobilization. The removal performance, flue gas tolerance, and synergistic effect of active components were improved greatly when microwave was added. The study indicated that (1) the Hg0 removal efficiency of the composite could reach 99.4%; (2) the composite had excellent tolerance to different industries’ flue gases. The electron exchange of Co(II)/Co(III) and Fe(II)/Fe(III) and the existence of Se and SeO2 were important for Hg0 immobilization. HgSe was the main adsorption product based on both X-ray photoelectron spectroscopy (XPS) and an online lab-built thermal decomposition system (TPD-AFS) analysis, which made the used-materials possess low mercury leaching content (0.09 mg·L–1) lower than the US EPA regulatory value (0.2 mg·L–1). This work provides a sound way for mercury control, which is significant for environmental protection.
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CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Yanghai Gui,Shuaishuai Zhao,Kuan Tian,Jintao Wu,Huishi Guo,Xiaoyun Qin,Xiaomei Qin,Dongjie Guo,Guangwen Zheng,Yao Guo
N-methyl pyrrolidone (NMP) is an important organic compound that is widely used in many industrial fields. Due to its volatility and toxicity, the detection of NMP content becomes crucial. Plasma treatment is an efficient method that utilizes high-energy ions generated by plasma to change the surface properties of materials, which can dramatically improve the performance of gas sensors. In this paper, ZnO nanorods were in-situ grown on ceramic tubes via hydrothermal method, followed by oxygen plasma treatment for different time, and the gas-sensing performance of the treated ZnO nanorods was investigated. In addition, the density functional theory calculation was used to explore the potential mechanism for the improvement of gas-sensing performance. The results show that ZnO treated with oxygen plasma for 60 s has more oxygen vacancies (45.53 %) and higher adsorption energy (−1.06 eV) to NMP. The ZnO-60 gas sensors have excellent selectivity to 100 ppm NMP at 210 °C, with a response value up to 197.58, low detection limit (94 ppb), and short response/recovery time (75 s/27 s). This study not only provides important theoretical and experimental basis for further optimizing the design and manufacture of gas sensors, but also provides strong support for environmental monitoring and human health protection.
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FUEL
·
2017
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IF 4.601
Yafei Guo,Chuanwen Zhao,Jian Sun,Weiling Li,Ping Lu
Silica aerogel supported K 2 CO 3 sorbents with different K 2 CO 3 loadings were synthesized by sol-gel and wet impregnation processes. The sorbents were characterized by N 2 adsorption-desorption, X-ray diffraction (XRD), and field emission scanning electron microscopy (FESEM) techniques. CO 2 capture performances of the sorbents were tested in a simulated ultra-dilute flue gas stream of 1.0%CO 2 and 2.0%H 2 O at 20 °C, using a fixed-bed reactor coupled with an online infrared gas analyzer. Sorbent regeneration performances of the samples were evaluated in a pure N 2 atmosphere at 200 °C with a heating rate of 10 °C/min. CO 2 capture capacity and K 2 CO 3 utilization efficiency increased first and then decreased with the increase in K 2 CO 3 loading. The desired sorbent with 20 wt% K 2 CO 3 was screened for investigating the effects of acid impurities. The presence of 500 ppm SO 2 and 500 ppm NO in the simulated flue gas stream was found to adversely affect the CO 2 capture, sorbent regeneration and multiple cyclic performances. Detailed mechanisms of the irreversible sorbent deactivation process were discussed. SO 2 could be chemically absorbed by K 2 CO 3 under a moist condition to form byproduct of K 2 SO 3 ·H 2 O, and the byproduct was stable and would be accumulated in the sorbent during the repeated cycles. This further attenuated the physical properties and K 2 CO 3 utilization efficiency of the sorbent. These results would lay a solid foundation for further application of the sorbent in ultra-dilute flue gas treatment.
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FUEL
·
2017
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IF 4.601
Yiquan Guo,Yongchun Zhao,Shaolong Wang,Cheng Jiang,Junying Zhang
Fly ash fine particles emitted from flue gas during coal combustion are the primary atmospheric pollutants in China. The purpose of this study was to investigate the characteristics of the zeta potential of fine particle suspensions. The relationship between the zeta potential and the fine particle removal efficiency was also discussed. Batch experiments were conducted to evaluate the zeta potential of fine particle aqueous solutions under various pH, ion concentration, surfactant, polymer, and chemical agglomeration solution conditions. A chemical agglomeration system was designed to simulate the removal process of the fine particles. The test results indicated that the zeta potential absolute value of the solution decreased initially and then increased as the pH increased. As the pH increased from 4 to 12, the zeta potential decreased from Zp = 9.4 mV to Zp = −45.4 mV. The isoelectric point (IEP) was 4.3. Also at the IEP, the highest fine particle removal efficiency of 25.9% was achieved. The zeta potential increased as the metal cation concentration of the solutions increased. The trivalent cation Al 3+ exhibited the best performance, which increased Zp from −32.1 mV to −11.2 mV and produced the highest fine particle removal efficiency of 9.2%. Polymers significantly impacted the zeta potential. As the concentration of kappa-carrageenan (CAR) increased from 0.01% to 5%, the zeta potential increased from −30.1 mV to 12.6 mV. The highest fine particle removal efficiency of 41.8% was acquired at a concentration of 0.5%, which had the lowest zeta potential absolute value of 3.5 mV. It can be inferred that the increase in the zeta potential induced the growth of the energy barrier, which prevented particle agglomeration. The suspension with a lower zeta potential exhibited a better fine particle removal efficiency.
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ANALYTICA CHIMICA ACTA
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2025
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IF 6
Wen-Qi Tang,Yue-Wen Gu,Xiang Qi,Ye-Qin Zhou,Wang Li,Ming Xu,Zhi-Yuan Gu
The separation of xylene isomers in capillary gas chromatography (GC) is essential and a significant challenge in analytical chemistry. Metal-organic frameworks (MOFs), as emerging porous materials, exhibit great potential for separation applications. However, the effective utilization of MOF-based stationary phases in GC is heavily constrained by their morphology and particle size. Larger particles lead to uneven coating on the inner wall of chromatographic columns, reducing the mass transfer efficiency and diffusion of analytes, which severely compromises chromatographic separation performance. Reducing the channel length of the MOFs are crucial methods for the development of GC stationary phases. In this study, by optimizing the amount of pyridine modulator, we successfully reduced the length of the MOF-74 nanorods, subsequently reduced the one-dimensional channel length in MOF-74. Compared to the longer hexagonal-shaped MOF-74-1, the nano-MOF-74-3 stationary phase showed a more uniform deposition on the inner wall of the capillary column. The MOF-74-3 column provided high separation performance for xylene isomers, achieving a separation factor of 6.11 for p X/ o X, which outperformed both MOF-74-1 and commercial columns such as HP-5MS and VF-WAXMS. The MOF-74-3 column demonstrated excellent separation performance after five injections of xylene isomers, indicating good reproducibility in the separation process. The xylene molecules exhibited a smaller mass transfer coefficient and faster diffusion in nano-MOF-74-3 than in MOF-74-1 column, effectively reducing chromatographic peak tailing. Moreover, the MOF-74-3 column also provided baseline separation for various alkane isomers and substituted benzene isomers. This work successfully decreased the aspect ratio of MOF-74-1 and MOF-74-3 from 2.6 to 1.1 through the addition of pyridine. The high-efficiency MOF-74-3 separation column achieved high-resolution separation of xylene isomers, alkane isomers, and substituted benzene isomers. This method offerd a new direction for the design of high-resolution stationary phases, which were essential for advancing GC-based analytical methods.
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Acta Biomaterialia
·
2024
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IF 9.4
Lianying Zhang,Xiaotong Chen,Beixian Zhou,Wei Meng,Haifeng Zeng,Yongjian Chen,Guoqin Huang,Yingshan Zhang,Huimin Wang,Ming Chen,Jinxiang Chen
Immunotherapy has emerged as a highly promising strategy in the realm of cancer treatment, wherein immunogenic cell death (ICD) is considered a potential trigger for anti-tumor immunity by inducing adaptive immunity to dying cell antigens. This process is often accompanied by the exposure, active secretion, or passive release of a large number of damage-associated molecular patterns (DAMPs), which activate dendritic cells (DCs) and enhance their antigen-presenting capacity. Subsequently, it promotes the recruitment and activation of cytotoxic T lymphocytes, ultimately leading to tumor growth inhibition. In addition, polarizing the M2 phenotype of tumor-associated macrophages (TAMs) to the M1 phenotype is another way to activate anti-tumor immunity, which can further enhance the effect of anti-tumor immunotherapy. In this study, we engineered a composite nanoparticle of UiO-66-NH 2 @Gold nanoshells@GOx-P-Arg (denoted as UGsGP). The gold nano shells in UGsGP exhibit a broad Near-Infrared-II (NIR-II) absorption to give a high photothermal conversion efficiency and achieve photothermal therapy (PTT). The GOx in UGsGP involves the breakdown of glucose, which results in a decrease in ATP levels and an inhibition of HSP90 and HSP70 production, ultimately enhancing the heat sensitivity of the tumor for PTT. In addition, GOx-mediated starvation therapy by glucose exhaustion produces a substantial amount of hydrogen peroxide (H 2 O 2 ), which can then react with P-Arg to produce intratumoral NO Thus, the synergistic effect of PTT resensitization, the photothermally-enhanced GOx-mediated starvation, and NO-based gas therapy promote the induction of ICD and the polarization of TAMs. The combination therapy exhibits significant antitumor effects both in vitro and in vivo. Statement of significance (1) Gold nanoshells on the surface of UiO-66-NH 2 display a broad absorption spectrum ranging from 900 to 1700 nm, combined with a high photothermal conversion efficiency of 74.0 %, demonstrating their remarkable ability to harness and convert light energy into heat for effective tumor ablation. (2) Under laser irradiation, GOx within the UGsGPs effectively consumes glucose, increasing intratumoral H 2 O 2 levels, which then reacts with P-Arg to produce NO within the tumor. Concurrently, the reduction in ATP levels suppresses HSP90 and HSP70 production, thereby enhancing the tumor's sensitivity to photothermal therapy. (3) The synergistic combination of NO gas therapy, starvation therapy, and PTT promotes ICD induction and TAM polarization, thereby improving the therapeutic outcomes for primary and distant tumors.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xiaoxia Zhang,Zhipeng Zhou,Junjie Liao,Liping Chang,Jiancheng Wang,Weiren Bao
The ultra-deep removal of thiophene from coke oven gas (COG) is critical for the conversion of COG to methane. Currently, Cu/ZnO/Al 2 O 3 is considered as a promising sorbent for thiophene removal; however, its desulfurization performance is currently unable to meet the requirements for industrial applications. Here, a zirconium modification strategy is proposed to overcome this problem, allowing zirconium loaded copper-based sorbents (Cu/ZnO/Al 2 O 3 /ZrO 2 ) with significantly improved thiophene removal performance and high activity to be obtained. Characterization results showed that zirconium improved both the dispersion of copper and the concentration of Lewis acid sites on the sorbent surface. A ZrO 2 concentration of 2 % resulted in stronger Cu-Zn interaction, and the dispersion of Cu on the surface of the sorbent reached its maximum value (49.20 %). Additionally, the Lewis acid strength was also maximized, which greatly improved the desulfurization activity and resulted in a breakthrough adsorption capacity of thiophene (Q b-thiophene ) of 36.24 mg/g, which was about 17 % higher than that of the unmodified Cu/ZnO/Al 2 O 3 sorbent. These results demonstrate that the sulfur capacity of the sorbent can be increased by increasing the number of acidic sites on its surface, paving the way for ultra-deep thiophene removal in industrial applications.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Kunpeng Song,Xue Bi,Chuang Yu,Ye-Tang Pan,Henri Vahabi,Vera Realinho,Jiyu He,Rongjie Yang
Up to now, metal–organic frameworks (MOFs) with open nanostructures have shown outstanding capabilities in trapping smoke particles compared to the original MOFs. However, only a few MOF-based strategies have been reported to synthesize hierarchical porous cages thus far, which are mainly restricted to environmentally unfriendly wet-chemical liquid methods. Herein, as a proof-of-concept, a gas-steamed metal–organic framework approach was designed to fabricate a series of cheeselike open cages with hierarchical porosity. Briefly, zeolitic imidazolate framework-67 (ZIF-67) and phytic acid were employed as precursor and etchant, respectively. Abandoning the conventional wet-chemical method, the coordination bond of ZIF-67 was cleaved by acidic steam, forming an open framework with a high specific surface area and a hierarchical porous structure. The universality of this method was also confirmed by the selection of different etchants. Impressively, they also show outstanding fume-toxic adsorption capability and labyrinth effects based on abundant and complex porous channels. At only 5 wt % loading, Co3O4@open ZIF-67 cage-2 (Co3O4@OZC-2) imparted polyurea (PUA) composites with a 21.2% limiting oxygen index, and the peak of heat release rate, total heat release, and total smoke production were reduced by around 37.5, 25.5, and 40.4%, respectively, compared to neat PUA. This work will shed light on the advanced structural design of polymer composites with high fire safety, especially smoke suppression performance, so as to obtain more feasible applications.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Qianfeng Wang,Jiayi Li,Yunxiao Dong,Han Hu,Drow Lionel OYoung,Di Hu,Yufang Zhang,Dong-Qing Wei,Jinggang Wang,Jin Zhu
2,5-Thiophenedicarboxylic acid (TDCA) is a biobased building block for aromatic–aliphatic copolyesters. This study synthesized poly(propylene succinate-co-thiophenedicarboxylate) (PPSTh) and poly(propylene adipate-co-thiophenedicarboxylate) (PPATh) via two-step melt polycondensation. PPATh70 exhibits the highest melting temperature at 144.8 °C. Crystallization kinetics indicate that diol-TDCA segments primarily form crystalline phases in PPXThs, with long aliphatic units enhancing crystallization. PPXThs containing over 50 mol % TDCA have a higher tensile modulus than poly(butylene adipate-co-terephthalate) (PBAT) and possess excellent gas barrier properties, outperforming PBAT by over 200 times. Dynamic mechanical analysis links the superior gas barrier properties to reduced free volumes. PPAThs degrade faster than PPSThs, with hydrolytic differences explained by Fukui function analysis and DFT calculations. Molecular dynamics simulations clarified the degradation mechanism catalyzed by Candida antarctica lipase B, showing that residues at the entrance interact with PPXTh50 residues, hindering the carbonyl carbon from approaching the catalytic nucleophile, while the flexible PPXTh40 more easily achieves an ideal Bürgi–Dunitz angle for nucleophilic attack.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
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IF 9
Mengchen Wang,Jiayou Liao,Chengyun Gao,Jiwei Ma,Xianjie Meng,Yinghua Shen,Xu Wu,Yong Wang,Jinping Li
Hyperbranched polyimide (HBPI) membranes have emerged as promising materials for gas separation due to their loose interchain structure and large free volume. However, their widespread application is hindered by challenges such as complex synthesis procedures, high-cost monomers, and poor resistance to plasticization. In this study, a series of Trimesoylchloride (TMC)-branched 6FDA-based PI membranes were successfully synthesized using different contents of TMC as a branching agent to regulate the pore distribution. The molecular structure and degree of branching (DB) of HBPI were characterized using FTIR and 1 H NMR. The incorporation of TMC into the HBPI structure effectively enhanced the permeability and selectivity of the acyl chloride-branched PI membranes while improving thermal stability. The optimized membrane (A5-TMC content is 5%), exhibits the improving O 2 and CO 2 permeabilities of 176.52 and 930.94 Barrer combined with the O 2 /N 2 , CO 2 /N 2 and CO 2 /CH 4 selectivities of 4.68, 24.65 and 23.85, respectively. Particularly, the A5 HBPI membrane, with a DB value of 85.71%, demonstrated superior anti-aging properties compared to linear 6FDA-DAM membrane over 365 days. Most importantly, the 6FDA-DAM-TMC HBPI membranes significantly enhanced the resistance to plasticization at elevated CO 2 feed pressures, maintaining stability up to 300 psi and significantly outperforming the linear 6FDA-DAM membrane. This study provides an effective method for the fabrication of high-performance gas-separated polymer membranes with enhanced plasticization resistance and long-term durability for advanced gas separation applications.
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