ACS Applied Polymer Materials
·
2025
·
IF 4.7
Yanling Liu,Xiao Peng,Yuan Li,Fei Wang,Xue Ai,Yuxi Huang,Xin Sun,Jie Zhao,Kai Li
Membrane separation technology has garnered significant attention for CO2 separation and purification, with mixed matrix membranes (MMMs) emerging as promising candidates due to their advantages of ease of processing, high mechanical strength, and thermal stability. The development of effective fillers for separation performance becomes one of the key foci in this area. In this work, CC3, a type of porous organic cages (POCs), was synthesized and functionalized with two amino-containing materials of different chain lengths. Polyethylenimine (PEI) and diethylenetriamine were used as modification agents to successfully graft amino groups onto the CC3 crystals to form defect-free Pebax mixed matrix membranes containing amino-functionalized CC3. The special porous structure of CC3 increases the gas permeability of the mixed matrix membrane by providing extra channels for the transportation of CO2. Besides, amino groups on functionalized CC3 interact with the chains of Pebax through hydrogen bonding, thus improving the compatibility between filler and matrix. The amino groups can further facilitate the transport of gases across the membrane through reversible reactions with CO2, which is further enhanced under humid conditions. Under optimal conditions, at 1 bar and 30 °C, the CO2 permeability of Pebax/PEI@CC3-MMMs was 342.33 Barrer with a selectivity of 33.38, while Pebax/DETA@CC3-MMMs exhibited a CO2 permeability of 273.34 Barrer and a selectivity of 35.77. This work demonstrates that amino-functionalized POCs (CC3) can effectively enhance the CO2 permeability and the CO2/N2 selectivity, which may provide a way to develop high-performance mixed matrix membranes with superior separation properties.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Zhenghao Zhang,Bo Peng,Yupeng Zhang,Jiaxin Xiong,Jingwei Li,Jianwei Liu
A CO2/N2-responsive emulsion provides milder reaction conditions, nontoxicity, and economic feasibility compared to other switchable surfactants. In this study, CO2/N2-responsive pickering emulsions were fabricated by using a compounded dispersion containing SiO2 nanoparticles (NPs) and superamphiphiles as the emulsifying agents. The synergistic effects of the SiO2 NPs and superamphiphiles significantly stabilized the emulsion at all of the tested concentrations and prevented complete phase separation of oil and water. The electrostatic interaction between the SiO2 NPs and superamphiphiles was disrupted after bubbling with CO2 for 30 s, resulting in the breaking of the emulsion. However, the dispersion recovered its interfacial activity after the introduction of N2 and again emulsified the emulsion. This reversible switching behavior was validated through three consecutive cycles of bubbling CO2/N2. The protonation and deprotonation of the SiO2 NPs and superamphiphiles in response to CO2/N2 facilitated reversible assembly and disassembly, which enabled the switching of the emulsions between inactive and active forms. The novel highly stable Pickering emulsions demonstrated rapid demulsification and emulsification in response to CO2/N2 and are promising for a wide range of applications.
研究领域:
材料科学
·
化学工程
·
胶体与界面科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Huimin Shi,Hang Zhang,Zhi Chen,Tao Wang,Lei Wang,Wei Zeng,Guanhua Zhang,Huigao Duan
Titanium nitride (TiN) has been attracting increasing interest as an anode material for electrochemical energy storage and conversion systems due to its superior thermal stability, electrical conductivity and chemical durability. The most commonly used strategy to synthesize TiN nanostructures is nitriding TiO 2 nanostructures using ammonia gas as the nitrogen source, and thus is not environmental friendly. Herein, we report an ammonia-free strategy to synthesize TiN nanomaterials using TiO 2 precursors via a magnesium-assisted nitriding reaction using nitrogen gas (N 2 ) as the nitrogen source. Systematical studies were conducted to reveal the mechanism of magnesium-assisted nitriding process in constructing TiN nanostructures under N 2 atmosphere. The as-synthesized TiN NRs were directly used as the anodes for lithium ion batteries and delivered an excellent reversible capacity of 710 mAh g −1 at the current density of 100 mA g −1 after 200 cycles. In addition, the TiN NRs also exhibited excellent cycling stability and rate capability. Our work provides a low cost, environmental friendly and reliable strategy to synthesize TiN materials from TiO 2 by using N 2 as the nitrogen source, which may facilitate the practical applications of TiN materials in electrochemical/photo-electrochemical energy storage and conversion systems.
研究领域:
材料科学
·
电化学能源存储
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Zhuangzhi Wu,Rongbin Zhang,Hao Fei,Ruoqi Liu,Dezhi Wang,Xinli Liu
The NH 3 is generally synthesized by the traditional Haber–Bosch method, which is energy-consuming and releases a lot of CO 2 . Electrocatalytic fixation of N 2 is highlighted as a carbon-free route to generate NH 3 by the nitrogen reduction reaction (NRR), but strongly demands highly efficient and durable electrocatalysts. Herein, we propose the multiphasic 1T@2H-MoSe 2 as a highly active NRR catalyst for the first time, which exhibits excellent activity for the NRR with a NH 3 yield of 19.91 ± 0.89 μg h −1 mg cat . −1 and a FE of 2.82% ± 0.1% at −0.6 V in 0.1 M Na 2 SO 4 . Moreover, a good durability is also demonstrated.
研究领域:
材料科学
·
化学工程
·
催化科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yu Fang,Yang Cao,Bihui Tan,Qianlin Chen
Solar energy can be used as “green” energy by photocatalysis for the nitrogen fixation under the atmospheric conditions compared with the traditional energy-intensive industrial production of ammonia. However, the complex kinetics and high reaction barriers greatly hinder the development of the photocatalytic N2 reduction reaction. Herein, a BiOBr/MXene-Ti3C2 composite catalyst is prepared by the simple electrostatic adsorption and self-assembly method. The as-prepared 10 wt % BiOBr/Ti3C2 exhibits the best performance for N2 fixation to NH3 by photocatalysis. The evolution rate of NH3 is up to 234.6 μmol·g–1·h–1, which is approximately 48.8 times and 52.4 times higher than those of pure BiOBr and Ti3C2, respectively. It is found that the designed double vacancies of oxygen and titanium for BiOBr/Ti3C2 composites, with the availability of localized electrons, have the ability to adsorb and activate N2, which can be efficiently reduced to NH3 by the interfacial electrons transferred from the excited BiOBr/Ti3C2 composite. In addition, the results of in situ Fourier transform infrared show the generation of NxHy species by the continuous protonation processes. Moreover, titanium vacancy (VTi) induces a strong absorption energy for nitrogen atoms on the surface of BiOBr/Ti3C2 according to the density functional theory calculations. In particular, the P-electron feedback caused by VTi could effectively promote the weakening of the N≡N triple bond and elongate the N2 bond length by ∼31.6%. This work might provide new insights into the synergistic effect of double defects and inspiration for the rational design of catalysts by defect engineering in the field of catalytic synthesis of ammonia.
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Kaifang Wang,Danlin Chen,Jiali Tang,Zihao Hong,Zhongtai Zhu,Ziyi Yuan,Zhihong Lin,Yuqi Liu,Raphael Semiat,Xuezhong He
Membrane gas separation technologies have emerged as highly prospective avenues for the selective separation of CO 2 . In this research, a novel array of mixed-matrix membranes (MMMs) was engineered, integrating two-dimensional nanosheets of MXene, specifically Ti 3 C 2 T x , into polymers of intrinsic microporosity (PIMs) to selectively separate CO 2 from N 2 . The inclusion of Ti 3 C 2 T x nanosheets, rich in polar functional groups, significantly increases the affinity between CO 2 molecules and the fabricated MMMs. Additionally, the precise modulation of the molecular diffusion channels for CO 2 and N 2 is achievable due to the interlayer spacing between MXene layers (∼0.35 nm) within the PIM-1 matrix. This innovation is predicated on the synergistic effect of solution-diffusion and molecular sieving mechanisms that underpin the gas separation process, leading to a marked improvement in both selectivity for CO 2 over N 2 and the permeability of CO 2 . Among the series, the MMMs with a 0.5 wt% MXene display exceptional separation efficiency, achieving a CO 2 permeability of 12475.3 barrer and a CO 2 /N 2 selectivity of 32.7. Notably, all the PIM-1/MXene membranes prepared with different compositions in this study exceed the Robeson upper bound defined in 2019, indicating their substantial promise for CO 2 separation and capture in industrial applications.
研究领域:
材料科学
·
环境工程
·
化学工程
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产品关联
DOI
高影响因子
RARE METALS
·
2025
·
IF 11
Yang Hui-Ying,Zhao Yu,Huang Ke-Lei,Meng Xiang-Chao
Combining interfacial solar evaporation with a three-phase photocatalytic system can theoretically improve the production efficiency of ammonia. Herein, we designed a simple solar evaporator via in situ growth of TiO 2 onto hydrophilic carbon paper using a fast Joule heating method. This system had porous channels for high water evaporation rates, wide light-responsive wavelength range, effective light absorption, and potentially high catalytic activity. The lattice disorder and oxygen vacancies created by the rapid heating and cooling process could be reaction sites for nitrogen adsorption and activation. The ammonia yield in the three-phase system was up to 360.37 mol·g −1 ·h −1 , which was higher than the two-phase system (17.14 μmol·g −1 ·h −1 ). Additionally, the ammonia yield rate was 73.65 μmol·g −1 ·h −1 in an outdoor test, demonstrating the potential for large-scale solar nitrogen reduction reaction (NRR). As detected, the activation energy for N 2 reduction to NH 3 was reduced to 26.3 kJ·mol −1 , indicating that this process was facilitated by the design of the photothermal–photocatalytic system. Furthermore, density functional theory (DFT) calculations confirmed the roles of oxygen vacancies as active sites in promoting the NRR. This work provided a new approach to applying solar evaporators for the highly efficient ammonia production by the synergistic effects of photothermal and photocatalytic processes. Graphical abstract
研究领域:
化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Meng Qiao,Yan-Fei Mu,Ji-Li Zhou,Su-Xian Yuan,Meng-Ran Zhang,Min Zhang,Tong-Bu Lu
Cu optimizes Co 3 O 4 d-orbital occupancy for symmetry-matched interactions with N 2 and CO 2 . • Cu-Co 3 O 4 reduces C − N coupling barrier from 2.34 to 1.19 eV. • Cu-Co 3 O 4 exhibits superior performance, ranking among the highest reported for photocatalytic urea synthesis. Photocatalytic CO 2 /N 2 co-reduction to urea is a green route for carbon‑nitrogen cycle closure, yet it is severely limited by the disparate orbital symmetry requirements of CO 2 /N 2 that impede synergistic activation on a single catalyst. Herein, Co 3 O 4 is doped with Fe/Cu/Ni to tailor the d -orbital configuration of its active sites, and Cu-Co 3 O 4 emerges as the optimal catalyst. It delivers a high urea yield of 25 μmol g −1 h −1 and a solar-to-urea conversion efficiency of nearly 0.035%, which ranks among the top efficiencies for photocatalytic urea synthesis. In situ diffuse reflectance infrared Fourier transform spectroscopy identifies *N 2 CO as the key reaction intermediate, while projected density of states calculations reveal that Cu 2+ ( d 9 ) optimizes d orbital occupation of catalyst to realize symmetry-matched adsorption of CO 2 /N 2 and strengthen orbital coupling. Density functional theory calculations further demonstrate that *N 2 CO formation is the rate-limiting step for urea synthesis, with Cu-Co 3 O 4 lowering the C − N coupling barrier to 1.19 eV (vs. 2.34 eV for pristine Co 3 O 4 ). This work establishes orbital symmetry matching between the d -orbitals of catalytically active sites and the π orbitals of reactants as a critical determinant for the selectivity of multi-molecule co-reduction reactions, thereby providing a general design principle for the development of high-performance photocatalysts. A Cu-doped Co 3 O 4 photocatalyst is rationally engineered, where incorporated Cu 2+ ( d 9 ) optimizes the occupation of active d xy / d xz orbitals in Co 3 O 4 , enabling symmetry-matched interactions with CO 2 and N 2 and reducing the C − N coupling barrier. This catalyst achieves a high urea yield of 25 μmol g −1 h −1 and a solar-to-urea conversion efficiency of ~0.035%, ranking among the top-performing systems for photocatalytic urea synthesis to date. Download: Download high-res image (115KB) Download: Download full-size image
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DOI
高影响因子
ACS Applied Polymer Materials
·
2026
·Vol. 8
·期 14
·12068-12079
·
IF 5.2
Chen Tao,Li Shuangjiang,Wang Bo,Yang Zhen,Xu Zhiyong,Zhao Wenbo
A highly potent greenhouse gas, sulfur hexafluoride (SF 6 ), requires efficient capture from industrial SF 6 /N 2 mixtures. Herein, a series of benzene-rich hyper-cross-linked
polymers (PPBx) were synthesized via a low-cost Friedel–Crafts
alkylation reaction using α,α ′ -dichloro- p -xylene (DCX) and triphenylbenzene (TPB) at different molar
ratios. The abundant benzene rings in the material enable strong F–π
interactions with SF 6 , while the hierarchical micromesoporous
structure ensures high adsorption capacity. Adsorption tests revealed
that PPB1, fabricated at a DCX/TPB molar ratio of 3:1, achieved a
remarkably high SF 6 uptake of 2.05 mmol/g at 298 K and
1 bar and an impressive SF 6 /N 2 ideal adsorbed
solution theory selectivity of 120 at 298 K. In addition, the dynamic
separation performance for SF 6 /N 2 was up to
1274.6 s/g, also demonstrating excellent properties under actual operating
conditions. The PPB1 material also demonstrates excellent thermal
stability and cycling performance. This work provides a cost-effective
and highly efficient hyper-cross-linked polymeric adsorbent with high
potential for industrial SF 6 separation and recovery.
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Siraj Ahmad,Yuan Ye,Wang Zhi
Natural gas, known for its cleanliness and cost-effectiveness, is primed to become a key energy source for the future. However, the high N 2 content in many natural gas reservoirs presents a significant challenge, necessitating the development of advanced N 2 rejection technologies. N 2 -selective membranes provide a cost-effective solution for reducing CH 4 recompression in natural gas purification, although further improvements in N 2 /CH 4 separation efficiency are still required. This work investigates the separation capability of advanced mixed PI-matrix composite (MMC) membranes for selective nitrogen (N 2 ) removal from methane (CH 4 ). A polyimide/polyacrylonitrile (PI/PAN)-based thin-film composite (TFC) membrane was fabricated, exhibiting enhanced interfacial compatibility and modified crystallinity, leading to a more ordered polymer network with a reduced intersegmental spacing of 4.1 Å, in contrast to 5.8 Å observed in the pristine PI. PALS analysis confirmed that incorporating TYUT-96Cr nanoparticles optimally improved fractional free volume (FFV) while decreasing the PI-matrix accessible pore size to below 0.39 nm. This structural adjustment results in a sevenfold increase in annihilation intensity for smaller microcavities (I 3 > I 4 ), suggesting improved N 2 over CH 4 separation via enhanced molecular sieving and faster N 2 diffusion. At a pressure of 1.5 bar and a TYUT-96Cr loading of 30 wt%, the membrane displayed an N 2 permeance of 3.68 GPU and a N 2 /CH 4 selectivity of 63.78. Upon decreasing the selective layer thickness from 19 to 13 μm, the N 2 permeance increased to 12.47 GPU, however, the N 2 /CH 4 selectivity declined to 51.96. These findings significantly advance membrane gas separation, with strong implications for efficient natural gas purification.
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2026
·
IF 5.6
Hao Zu,Chuanfeng Wang,Hui Liu,Jian Bian,Yuan Feng,Hui Huang,Laiming Wei,Guohua Cao
Due to the elevated sintering temperature, CaCu 3 Ti 4 O 12 ceramics are unsuitable for co-firing with copper electrodes, which has notable advantages including low production cost, high conductivity and broad high-frequency applicability. Therefore, the sintering of CaCu 3 Ti 4 O 12 ceramics should be conducted at temperatures below 1083 °C (the melting point of Cu) and under protecting atmosphere to prevent the oxidation of Cu. In this paper, CaCu 3 Ti 4 O 12 ceramics were sintered at only 1000 °C in high-purity N 2 , then reoxidized at 800 °C in air to restore their electrical properties. Among them, Ge 4+ -Ni 2+ co-doped CaCu 3 Ti 4 O 12 ceramics exhibited significantly increased grain-boundary resistivity, resulting in substantially decreased dielectric loss (about 0.055 at 1 kHz), while still remaining a large dielectric constant of 9.4 × 10 3 . Additionally, the nonlinear coefficient and breakdown strength field were also improved to values of 3.3 and 1360 V/cm, respectively. The results provide a promising candidate material for multilayer capacitor-varistor devices with Cu internal electrode.
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2019
·Vol. 136
·期 45
·48187
·
IF 2.188
Yan Zhang,Shili He,Jianing Wu,Junjie Ma,Shengdong Shao,Lingjie He,Xiaonan Li,Zhengping Fang,Hongwei Cao,Zhichao Xi
The waste silicon rubber composite insulator (WSiRC) was applied along with ammonium polyphosphate (APP) and pentaerythritol (PER) to improve the flame retardancy of polypropylene (PP) in this study. Considering the compatibility among PP, WSiRC, and flame-retardant additives, WSiRC was treated by acid and N 2 plasma to obtain the plasma-treated WSiRC (PLSiR), which decreases the amount of the inorganic additive and grafts amino groups onto the surface of the silicon rubber. The infrared spectrocopy (IR), scanning electron microscopy (SEM), and thermal gravimetric analysis (TGA) confirm that NH 2 groups have been grafted onto the surface of PLSiR. The TGA data also show that PLSiR had the char improving ability and promote the crosslink of APP, which results in its promotion for the flame retartancy of PP proved by the data of limiting oxygen index (LOI), UL94 rating and cone tests. It is also showed that PLSiR is superior than the WSiRC treated only by acid (ASiR) due to the differences in the structure and polarity. Moreover, the improvement of PLSiR on the flame retardancy of PP is dependent on its amounts. It is indicated that the 1 wt % loading of PLSiR in PP with APP and PER has the highest LOI value of 30.9 and reached UL94 rating V-0. The peak heat release rate (pHRR) and total heat release (THR) values are also decreased by 68.7 and 15%, respectively. SEM and Raman results show the condensed mechanism is ascribed to the PP/APP-PER/PLSiR system because the quality of char affect the flame retardancy of PP. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 48187.
研究领域:
高分子材料科学
·
阻燃化学
·
材料表面改性
·
环境功能材料
·
废弃资源再利用
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）