Journal of the American Chemical Society
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2025
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IF 15.6
Deyun Sun,Shangqing Chen,Miao He,Hongxue Xu,Yongxiang Sun,Lijuan Shi,Hongbo Zeng,Qun Yi
Efficient extraction of high-purity CO2 from humid flue gas via adsorptive separation offers a promising and sustainable solution for carbon reduction and downstream applications. However, the coadsorption of H2O vapor and N2 from humid flue gas remains a persistent challenge that limits separation efficiency. To overcome this issue, this work introduces a novel concept of ionic hydrophobic gates on porous adsorbents, which enables one-step separation of high-purity CO2 directly from humid flue gas. By assembling hydrophobic ionic liquids and fluorine-rich terephthalaldehyde onto the surface of a metal–organic framework (MOF), this design establishes H2O barriers and CO2 channels on the outer shell while maintaining pore integrity in the core. The resulting core–shell material demonstrates exceptional CO2 adsorption capacity and an extraordinary CO2/N2 selectivity of 1780 (15/85, v/v), surpassing conventional adsorbents. Notably, dry CO2 with 99.999% purity is successfully extracted from humid flue gas (relative humidity, RH = 100%) in a single breakthrough experiment. In situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and density functional theory calculations reveal that fluorine-rich hydrophobic sites act as effective H2O barriers, while ionic liquid segments facilitate the transport of CO2 through hydrogen bonding and electrostatic interactions. Owing to its excellent scalability and broad compatibility with diverse MOF platforms, this ionic hydrophobic gating strategy offers a robust and versatile approach for constructing advanced gas separation materials, holding great promise for industrial applications in carbon capture, clean energy, and sustainable chemical processes.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Ge-liang Xie,Yang Cao,Sheng-ren Li,Qian-qian Lu,Wei Chen,Shuai Gao,Wei Qiu,Chao He,Zhen Fang,Lujiang Xu
Lignin valorization through catalytic upgrading to nitrogen-containing aromatics represents a critical pathway for sustainable chemical production. Using vanillin, a key lignin depolymerization product, as a platform molecule, we demonstrate the first integrated strategy combining cyanide-free cyanation and gas-phase hydrodeoxygenation (HDO) to synthesize hydroxybenzonitriles (HBNs). Bond dissociation energy (BDE) analysis revealed the cyano group’s selective retention (C≡N: 136.21 kcal/mol vs C–O: 62.44–116.17 kcal/mol), guiding targeted HDO pathway design. A green H2O/HCOOH system achieved 99.2 mol % vanillonitrile yield under mild conditions (85 °C, 12 h), surpassing conventional DMF-based methods. Engineered Mo/TiO2 catalysts with triple functional sites (oxygen vacancies, suitable content of Mo5+, strong metal–support interaction) achieved 57.6% HBN yield in continuous gas-phase HDO, outperforming Mo/ZrO2. The catalyst retained 90% of its initial activity over eight cycles due to enhanced metal–support interactions. This work establishes a sustainable route for lignin-to-chemical conversion, advancing catalyst design principles for biomass upgrading.
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Mengyuan Liu,Bo Ran,Ping Hu,Jialu Fang,Jun Sun,Yuqing Bai,Qingshan Ma,Xiaoman Ma,Zhaofeng Wu,Haiming Duan
s This study presents an eco-friendly fabrication method for high-performance room-temperature (RT, 25 °C) gas sensors by integrating biomass-derived N-doped carbon quantum dots (N-CQDs) with biochar (BC). The N-CQDs were hydrothermally synthesized from waste milk and the BC substrate was devrived from carbonized Lyocell fiber mask waste. The constructed N-CQDs@BC heterostructure through simple mechanical mixing and milling exhibited better trimethylamine (TMA) sensing capabilities, achieving a remarkable response magnitude of 21k% to 500 ppm TMA gas at RT with a moderate response/recovery time of 82.24 s/10.71 s. The sensor demonstrated outstanding stability by maintaining 21k% response after 45 days of ambient storage and achieved a low detection limit of 1.07 ppm. Density functional theory calculations revealed that N-doping significantly enhanced the material’s adsorption capabilities for both O 2 and TMA. This improvement in adsorption energy, combined with increased charge transfer, underscores the effectiveness of N-doping in optimizing the material’s electronic structure and reactivity. By exclusively utilizing biomass waste resources, this work establishes a simple solution for developing eco-friendly semiconductor gas sensors that combine high sensitivity cost-effectiveness, and environmental sustainability with promising applications.
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POLYMER
·
2025
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IF 4.5
Xiuyuan Wei,Chao Shan,Zhongying Liu,Zhiqing Liang,Hui Wu,Chanjuan Liu,Xiaohua Huang
A novel sulfur-and fluorine-containing dianhydride monomer 2,2-bis[4-(3,4-dicarboxyphenylthio)phenyl]hexafluoropropane dianhydride (6FDAPSA) was synthesized by molecular design, and a series of random co-polyimides were prepared from 6FDAPSA, 4,4-(hexafluoroisopropene)diphthalic anhydride (6FDA) and 4-(3-fluoro-4-(trifluoromethyl)phenyl)-2,6-bis(4-aminophenyl)pyridine (FTPPA). The obtained co-polyimides exhibited excellent thermal properties ( T g > 288 °C, T 5 % > 504 °C, T 10 % > 536 °C), good optical properties (λ cut-off > 342 nm, λ 80 % > 410 nm), commendable mechanical properties (tensile strength >75 MPa) and outstanding hydrophobic properties (contact angle >90.0°). They also showed excellent solubility in both high and low boiling point organic solvents. Besides, Wide-angle X-ray diffraction test and molecular simulation confirmed that the prepared co-polyimides possess a large molecular chain spacing, with d-spacing values ranging from 5.59 to 5.84 Å and fractional free volume from 0.237 to 0.280. Consequently, polyimide membranes exhibited commendable gas permeability values of He (up to 49.5 barrer) and CO 2 (up to 34.2 barrer), and good ideal gas selectivity values of He/N 2 (up to 34.2) and CO 2 /N 2 (up to 22.2). These results indicate that polyimide matrix materials have potential application prospects in the field of gas separation.
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CARBOHYDRATE POLYMERS
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2025
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IF 12.5
Xiaolei Luo,Linyue He,Longfei Sun,Xinxin Chen,Lin Liu,Juming Yao,Yurong Cai
Addressing the inherent flammability of cellulose aerogel (CA) remains crucial for ensuring its safety-critical application. Prevailing studies predominantly focuses on flame retardant synthesis and interfacial compatibility, yet neglect the fundamental analysis of cellulose's intrinsic thermal degradation behavior. Herein, a gas-solid dual barrier strategy was provided for enhancing the flame retardancy of CA according to its competitive thermal degradation process involving random chain scission and intramolecular dehydration reactions. Concretely, as the solid barrier, LDH was uniformly dispersed in matrix to alleviate the thermal decomposition process of CA and inhibit gas phase fuel generation at source during thermal exposure. Meanwhile, TP played the role of gas barrier to quench the combustion reaction chain and suppress the heat feedback. Under the dual action of gas-solid phase, a high-quality char layer that effectively blocked heat and mass transfer formed rapidly, the residual mass of the TP/LDH/CA at 800 °C in the air increased to 12.8 % compared with CA. As a result, the obtained TP/LDH/CA had extremely high fire safety, which could extinguish within 2 s after removal from the flame, and the total smoke release (TSR) decreased by 90.54 %.
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CHEMISTRY & BIODIVERSITY
·
2025
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IF 2.5
Yuanyuan Zhang,Haixin Liu,Xiang Xu,Xin Shen,Haolong Qi,Yilin Xing,Mengyi You,Tao Sun,Zhiqiang Cai,Xiaoyan Zhang
Leaning pillar[6]arene (LP6A) is an expanded version of pillar[6]arene (P6A), possessing not only the nanometer-sized cavity of P6A but also a unique desymmetrized leaning tower-like structure, which offers better structural flexibility and cavity adaptability. Here we report the first example of the utilization of imidazolium ionic liquid (IMIL) functionalized LP6A (LP6A-C10-IM-C8[NTf 2 ]) as a stationary phase in capillary gas chromatography (GC). The LP6A-C10-IM-C8[NTf 2 ] capillary column was prepared by the static coating method, showing medium polarity (average polarity 155) and high column efficiency (3758 plates/m). Using long alkyl chains modified LP6A (LP6A-C10) as a reference column, its retention behaviour and resolving performance were elucidated by a mixture of 30 analytes. Importantly, the LP6A-C10-IM-C8[NTf 2 ] column exhibited advantageous separation performance for the challenging isomers of halogenated benzenes, benzaldehydes, phenols, and anilines over the LP6A-C10 and commercial HP-5, HP-35, and DB-17 columns. In addition, the LP6A-C10-IM-C8[NTf 2 ] column has been used to determine the purity of isomer impurities in actual samples, demonstrating good potential in GC separations. Graphical This work reported the first example of utilization of imidazolium ionic liquid (IMIL) functionalized leaning pillar[6]arene (LP6A-C10-IM-C8[NTf 2 ]) as a stationary phase in capillary gas chromatography separations and obtained a high resolution performance for multiple anayltes.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2025
·Vol. 36
·期 21
·1-13
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IF 2.8
Zhou Mincong,Li Xu,Zheng Yichen,Wang Qingji
The in-situ growth of sensitive materials has progressively emerged as a prevalent trend. In this paper, SnW 3 O 9 nanosheet arrays are synthesized by aerosol-assisted chemical vapor deposition (AACVD), which is a method for in-situ preparation of sensitive films for gas sensors. Subsequently, Pt-Au is loaded onto the SnW 3 O 9 nanosheet arrays by the wet impregnation process. Ultimately, a H 2 sensor with high selectivity was successfully fabricated. At the optimum operating temperature of 310 °C, the response value of PtAu/SnW 3 O 9 -30 sensor to 100 ppm H 2 is 6.5 times of 100 ppm NH 3 , 7.6 times of 100 ppm CO and 10.1 times of 100 ppm CH 4 . Meanwhile, the sensor performs excellent anti-interference capability under the mixed gases between 100 ppm H 2 and 100 ppm CO, CO 2 and CH 4 , respectively. In addition, the sensor has good stability with different relative humidity. The excellent gas sensing performance of the sensor can primarily be attributed to the unique morphology of SnW 3 O 9 nanosheet arrays and the introduction of Pt-Au. The in-situ growth of PtAu/SnW 3 O 9 nanosheet arrays on planar substrate can be great potential for application in fabricating highly selective H 2 gas sensor.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Yuxiao Jiang,Kelin Hu,Jing Zhang,Tao He,Bin Yu,Xinyuan Li,Jiarong Yang
This research focused on the synthesis of In 2 O 3 /Ni x O y nanocomposites utilizing the conventional template method. The resulting gas sensor, designed for H 2 detection, demonstrates a sensing behavior that is dependent on temperature. Various characterization techniques were employed to analyze the synthesized In 2 O 3 /NiO composite materials. The results obtained from tests conducted at different temperatures reveal that the sensor maintains a stable n-type response for H 2 at temperatures exceeding 240°C, while exhibiting an atypical p-type response at lower temperatures. This transition in adsorption behavior enables the In 2 O 3 /Ni x O y composites to function as a dual-mode sensor capable of detecting H 2 . The temperature-induced transformation is likely attributable to the interplay of several mechanisms. This article elucidates this phenomenon by examining factors such as activation energy, TGA/DSC, adsorbed oxygen, heterojunction formation, and humidity effects. This study contributes to the understanding of the transformation mechanisms underlying MOS gas sensing behavior.
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RSC Advances
·
2024
·Vol. 14
·期 8
·5479-5491
·
IF 3.9
Yaqi Yao,Hongying Zhuo,Jinming Xu,Xiaofeng Yang,Yanqiang Huang
A method for synthesizing carbon spheres with a tunable particle size and internal structure from polyfurfuryl alcohol (PFA) was developed. By tuning the concentration of a structure directing agent (polypropylene glycol, PPG), we found a mechanism to tune the inner architecture of carbon spheres driven by water-solubility. A mixture of PFA and PPG transferred from the “water-in-oil” phase to an “oil-in-water” phase with an increasing content of PPG because of a difference in water-solubility between furfuryl alcohol (FA), PFA, and PPG. As a result, the internal morphology of the carbon sphere evolved from a “cheese-like” to a “pomegranate-like” structure, which was accompanied by an increasing specific surface area and pore volume. Furthermore, the separation of C2H2 and C2H3Cl was tested on the 25%-FACS (furfuryl alcohol-based carbon sphere) sample under different activation treatments with CO2 or CO2–NH3, with the coexisting “cheese-like” and “pomegranate-like” inner structures, owing to its moderate pore volume and mechanical strength. The maximum adsorption capacity of C2H3Cl reached 0.77 mmol g−1, while C2H2 was adsorbed in significantly lower quantities. It is believed that the high polarizability and high dipole moment of the C2H3Cl molecule primarily contribute to the excellent performance of C2H2 and C2H3Cl separation, and the introduction of polar N-containing groups on the carbon skeleton further promotes C2H3Cl adsorption.
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Molecular Catalysis
·
2024
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IF 3.9
Jiaqi Zhou,Qingrong Wang,Hong Liu,Ming Bao,Jiasheng Wang
Gas-phase selective oxidation of toluene with air is a promising method for producing high-purity benzaldehyde, but the yields of existing catalysts are limited, so the development of more efficient catalysts is of great importance to the chemical industry. Herein VMoNb/CeO 2 was prepared and characterized by SEM, XRD, Raman, XPS, H 2 -TPR, and NH 3 -TPD. The introduction of Mo generated V–O–Mo “asymmetric lattice oxygen” and thus brought high activity. Nb moderated the acidity and oxygen vacancy so as to improve the selectivity. The VMoNb/CeO 2 catalyst showed very high catalytic activity at 500 °C, with 35% toluene conversion and 82% benzaldehyde selectivity at an air flow rate of 30 mL/min for V:Mo:Nb =2:5:0.8. This work could serve as a reference for designing mixed metal oxide catalysts for selective oxidation of aromatic hydrocarbons.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
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IF 11.3
Jianping Sheng,Ye He,Fengyi Zhong,Chenyu Du,Guijie Liang,Xiaodan Ma,Yanjuan Sun,Fan Dong
Photo/electrocatalytic ammonia (NH3) synthesis via nitrous oxide (NOx) reduction is challenged by low NO solubility in electrolytes, inefficient electron and proton supply, and the high cost of separating NH3 from dilute NH4+ product solutions. In this study, we present a continuous, separation-free gas–solid photoreduction strategy for direct NH3 gas production from flue gas, enabled by dynamic band structure regulation of the photocatalyst. Comprehensive in situ characterization and theoretical analysis demonstrate that this approach utilizes photoexcited oxygen vacancies (PVO) in TiO2 to generate high-energy electrons in deep conduction bands, thereby enhancing the reduction capacity, accelerating electron transfer, and lowering the activation energy for both H2O dissociation and NO hydrogenation. The real-time tracking of NO radicals in a gas–solid system using operando EPR provides crucial mechanistic insights into high-energy electron behavior and the NO-to-NH3 conversion pathway, where these high-energy electrons not only promote efficient NO-to-NH3 conversion but also prevent toxic N2O byproduct formation, ensuring selective and efficient reduction. The optimized TiO2–PVO catalyst achieves an NH3 production rate of 79.86 ± 3.48 μmol g–1 h–1 with nearly 100% selectivity, a 16-fold improvement over pristine TiO2. This study offers valuable insights into solar-driven gas–solid NH3 synthesis from flue NOx.
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Results in Engineering
·
2025
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IF 7.9
Nuo Xu,Shuai-Xia Yuan,Yixin Liu,Zong-Yu Guo,Minghua Li,Duan-Chao Wang
Odors from sweat and skin secretions not only cause discomfort but may also signal microbial contamination in textiles, posing health risks. To address this, we report a multifunctional composite textile prepared via in-situ growth of two zeolitic imidazolate frameworks (ZIF-67 and ZIF-8) on cotton fabrics. Cotton was chosen for its comfort, hydrophilicity, and modifiable cellulose structure, with woven and knitted variants offering complementary mechanical and elastic properties. The integration of ZIFs imparts high surface area, tunable microporosity, and intrinsic antibacterial performance. Structural characterization confirms uniform deposition of ZIFs forming a functional shell on the cotton fibers. Notably, X-ray micro-computed tomography (Micro-CT) and BET analysis jointly reveal a hierarchical porous architecture from the textile macrostructure to ZIF microdomains, enabling efficient adsorption of both alkaline (NH 3 ) and acidic (CH 3 COOH) odor molecules. The ZIFs exhibit a surface area of 1451.0 m 2 /g, retaining 89.2 m 2 /g post-integration. The resulting fabrics demonstrate >90 % odor removal, excellent water absorbency and breathability, and 99.9 % antibacterial activity against S. aureus and E. coli. This study offers a promising strategy for designing next-generation functional deodorizing textiles for daily hygiene applications.
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