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CHEMICAL ENGINEERING SCIENCE · 2025 · IF 4.3

Development of novel HNIW/N2 host-guest explosives with enhanced stability and performance via pressure-temperature strategy

Xiaomin Song,Donghan Jia,Shanhu Sun,Xiaoyu Sun,Haobin Zhang,Shiliang Huang,Huiyang Gou,Jie Sun,Jinjiang Xu

Supramolecular assembly has emerged as a promising strategy to drive the development of high-performance energetic materials (HEDMs). In this study, we reported the fabrication of novel HNIW/N 2 host–guest explosives using DAC combined with pressure–temperature (P-T) strategy. The molecular composition and crystal structure were analyzed through Raman spectroscopy, synchrotron radiation XRD and DFT calculations. High-pressure Raman spectroscopy and quantum chemical calculations confirmed the stabilizing effect of nitrogen on structural stability of explosive crystals. Remarkably, HNIW/N 2 exhibited superior detonation performance (D V  = 9646 m/s, P = 43.4 GPa), and the formation mechanism of host–guest explosives was illustrated from the perspective of crystal stacking. The newly constructed HNIW/N 2 host–guest explosives realized the green and safe incorporation of nitrogen, as well as enhanced the structural stability and detonation performance for explosive crystals. The study can offer valuable insights into the design of advanced energetic materials and underscore the potential of supramolecular assemblies in this field.

研究领域: 材料科学 · 化学
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JOURNAL OF APPLIED POLYMER SCIENCE · 2019 ·Vol. 136 ·期 28 ·47755 · IF 2.188

Effects of preparation parameters on CO2/N2 gas permselectivity of polyether thin film composite membrane

Yixuan Wang,Jiawen Fu,Qingfu Zhang,Liping Lin,Chunhai Yi,Bolun Yang

In this work, ether oxide (EO)-based multilayer composite membranes were prepared via interfacial polymerization (IP) of trimesoyl chloride (TMC) and polyetheramine (PEA) on polydimethylsiloxane precoated polysulfone support membrane. The effects of preparation parameters, such as monomer concentrations, reaction time, and heat-treatment temperature on the membrane performance were investigated. The optimal preparation parameters have been concluded. The results showed the increasing monomers concentration of both PEA and TMC can lead to the decrease of CO 2 permeance and increase of CO 2 /N 2 selectivity. The optimal monomers concentration was found. When monomer concentrations are higher than the optimal values, the CO 2 permeance decreases continually while CO 2 /N 2 selectivity only shows a very limited improvement with the further increase of monomers concentration. The reaction time has similar effects on membrane performance as the monomers concentration. The effect of heat-treatment temperature was also studied. With the increasing heat-treatment temperature, the CO 2 permeance shows a decrease tendency, while the CO 2 /N 2 selectivity shows a maximum at 80 °C. When PEA is 0.013 mol L −1 , TMC is 0.020 mol L −1 , reaction time is 3 min, and heat-treatment temperature is 80 °C, the optimum preparation conditions are achieved with CO 2 permeance of 378.3 gas permeation unit (GPU) and CO 2 /N 2 selectivity of 51.7 at 0.03 MPa. This work may help to design and fabricate gas separation membranes with desired performance. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47755.

CAS / MDL: 77-58-7 497-19-8 78-10-4
研究领域: 材料科学 · 环境工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Heterophase structure of ZnSnO3 (rhombohedral and orthorhombic) for efficient dye degradation and N2-to-NH3 conversion via piezocatalysis and piezo-photocatalysis

Chunran Zhao,Chenrui Wang,Xujie Ren,Shude Yuan,Leihong Zhao,Lvchao Zhuang,Botao Teng,Ying Wu,Yiming He

Fabricating heterophase junctions proves to be an efficient strategy for achieving efficient charge separation and enhancing the catalytic activity of photocatalysts. Surprisingly, this approach is rarely utilized in the field of piezocatalysis. In this work, a novel ZnSnO 3 heterophase junction catalyst was fabricated by combining rhombohedral (R-ZnSnO 3 ) and orthorhombic (O-ZnSnO 3 ) phases for efficient piezo and piezo-photocatalytic RhB degradation and N 2 fixation. The piezocatalytic RhB degradation rates of ZnSnO 3 heterophase catalysts are 5.6 and 3.6 times higher than those of O-ZnSnO 3 and R-ZnSnO 3 , respectively, with similar enhancements observed in piezocatalytic N 2 fixation. The coupling of R-ZnSnO 3 and O-ZnSnO 3 does not increase the piezoelectric properties; however, an S-scheme structure formed at the interface. Under the combined effects of band bending, interface electric fields, and Coulomb attraction, electrons and holes migrate and achieve effective spatial separation. This result supports the energy band theory over the induction charge theory, contributing to the ongoing debate in piezocatalytic mechanisms. Electrochemical analyses and piezo-photocatalytic tests further indicate that ZnSnO 3 heterophase junctions exhibit a synergistic effect between piezocatalysis and photocatalysis. This synergy can be attributed to the complementary effects of photoinduced carrier generation and piezoelectric field-assisted carrier separation. Hydroxyl radicals, superoxide radicals, and holes serve as the primary active species responsible for piezocatalytic RhB degradation through a mechanism similar to photocatalysis. Theoretical calculations reveal that the Sn site on the surface of O-ZnSnO 3 acts as the active site within the ZnSnO 3 heterophase junction, providing valuable insights for future catalyst development. This work offers a deeper understanding of the synergistic mechanisms in piezo-photocatalysis, presenting a promising route for efficient environmental and energy applications.

CAS / MDL: 10026-06-9 12209-98-2
研究领域: 材料科学 · 环境科学 · 催化化学
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SEPARATION SCIENCE AND TECHNOLOGY · 2025 · IF 2.3

Mixed matrix membranes based on MIL-100(Cr) for removal of N2 from CH4

Xiaoli Ding,Qiankun Zhang,Hongyong Zhao,Qingping Xin,Yuzhong Zhang

Two series of mixed matrix membranes (MMMs) have been synthesized via in situ UV polymerization for the removal of N2 from CH4. MIL-100(Cr) particles activated at different temperatures were used as fillers. MIL-100(Cr) activated at 150°C with CH4-selective adsorption was incorporated with poly(ethylene oxide)-based polymer to improve the CH4/N2 separation performance, and that activated at 250°C with N2-selective adsorption and diffusion was incorporated with fluoropolymer to improve the N2/CH4 separation performance. The effects of the filler loadings on the gas permeation and separation performances were investigated. The optimum MMMs with 5 wt.% loading of MIL-100(Cr) activated at 150°C exhibited a 70% increased CH4/N2 permselectivity of 5.0 with a 37% increased CH4 permeability of 11.2 Barrer (tested at 0.2 MPa and 35°C). The optimum MMMs with 5 wt.% loading of MIL-100(Cr) activated at 250°C exhibited a 106% increased N2 permeability of 71.5 Barrer with an 89% increased N2/CH4 permselectivity of 1.9.

研究领域: 化学工程 · 材料科学 · 膜技术 · 气体分离
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SEPARATION AND PURIFICATION TECHNOLOGY · 2017 · IF 3.359

Thin film composite membranes functionalized with montmorillonite and hydrotalcite nanosheets for CO2/N2 separation

Yiming Zhang,Huixian Wang,Yatao Zhang,Xiaoxu Ding,Jindun Liu

Montmorillonite (MMT) and Mg-Al hydrotalcite (HT) nanosheets were prepared via vigorous agitation and ultrasonic, respectively. In order to increase the permeability of CO 2 , poly (PEA-MMT-TMC)/PS and poly (PEA-HT-TMC)/PS composite membranes were prepared via interfacial polymerization by adding the dimensional (2D) inorganic nanosheets (MMT and HT) into the aqueous phase of PEA. And in consequence, the poly (PEA-MMT-TMC)/PS composite membrane showed CO 2 permeability of 15.87 barrer and the CO 2 /N 2 selectivity of 37 at 1.0   bar when the MMT concentration was 0.068   wt%. The poly (PEA-HT-TMC)/PS composite membrane also showed CO 2 permeability of 15.3 barrer and the CO 2 /N 2 selectivity of 40 at 1.0   bar when the HT concentration was 0.25   wt%. Compared with the controlled membrane (CO 2 permeability: 6.9 barrer, CO 2 /N 2 selectivity: 103), the CO 2 permeability increased after incorporating the inorganic nanosheets into the membranes and maintained the pretty CO 2 /N 2 selectivity. The addition of exfoliated MMT and HT could facilitate the gas permeation to improve the gas separation performance of the composite membranes. Also, the combination of inorganic nanosheets with organic membrane has a great potential application in the gas separation.

CAS / MDL: 9046-10-0
研究领域: 材料科学 · 化学工程 · 环境科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2019 ·Vol. 25 ·期 38 ·9045-9051 · IF 5.16

Construction of a Stable Crystalline Polyimide Porous Organic Framework for C2H2/C2H4 and CO2/N2 Separation

Lingchang Jiang,Pengyuan Wang,Meiping Li,Panpan Zhang,Jialu Li,Jia Liu,Yanhang Ma,Hao Ren,Guangshan Zhu

Graphical Lapping it up : A thermally and chemically stable, crystalline polyimide porous organic framework, was constructed by imidization of linear naphthalene-1,4,5,8-tetracarboxylic dianhydride with triangular 1,3,5-tris(4-aminophenyl)benzene. This material is capable of selective adsorption of C 2 H 2 over C 2 H 4 and CO 2 over N 2 (see figure). Utilization of porous materials for gas capture and separation is a hot research topic. Removal of acetylene (C 2 H 2 ) from ethylene (C 2 H 4 ) is important in the oil refining and petrochemical industries, since C 2 H 2 impurities deactivate the catalysts and terminate the polymerization of C 2 H 4 . Carbon dioxide (CO 2 ) emission from power plants contributes to global climate change and threatens the survival of life on this planet. Herein, 2D crystalline polyimide porous organic framework PAF-120, which was constructed by imidization of linear naphthalene-1,4,5,8-tetracarboxylic dianhydride and triangular 1,3,5-tris(4-aminophenyl)benzene, showed significant thermal and chemical stability. Low-pressure gas adsorption isotherms revealed that PAF-120 exhibits good selective adsorption of C 2 H 2 over C 2 H 4 and CO 2 over N 2 . At 298 K and 1 bar, its C 2 H 2 and CO 2 selectivities were predicted to be 4.1 and 68.7, respectively. More importantly, PAF-120 exhibits the highest selectivity for C 2 H 2 /C 2 H 4 separation among porous organic frameworks. Thus PAF-120 could be a suitable candidate for selective separation of C 2 H 2 over C 2 H 4 and CO 2 over N 2 .

研究领域: 材料科学 · 化学工程
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-15 · IF 14.7

A unicellular cyanobacterium relies on sodium energetics to fix N2

Tang Si,Cheng Xueyu,Liu Yaqing,Liu Lu,Liu Dai,Yan Qi,Zhu Jianming,Zhou Jin,Jiang Yuyang,Hammerschmidt Katrin,Cai Zhonghua

Diazotrophic cyanobacteria can fix nitrogen gas (N 2 ) but are usually scarce in nitrogen-limited coastal waters, which poses an apparent ecological paradox. One hypothesis is that high salinities (> 10 g/L NaCl) may inhibit cyanobacterial N 2 fixation. However, here we show that N 2 fixation in a unicellular coastal cyanobacterium exclusively depends on sodium ions and is inhibited at low NaCl concentrations (< 4 g/L). In the absence of Na + , cells of Cyanothece sp. ATCC 51142 (recently reclassified as Crocosphaera subtropica ) upregulate the expression of nifHDK genes and synthesise a higher amount of nitrogenase, but do not fix N 2 and do not grow. We find that the loss of N 2 -fixing ability in the absence of Na + is due to insufficient ATP supply. Additional experiments suggest that N 2 fixation in this organism is driven by sodium energetics and mixed-acid fermentation, rather than proton energetics and aerobic respiration, even though cells were cultured aerobically. Further work is needed to clarify the underlying mechanisms and whether our findings are relevant to other coastal cyanobacteria.

研究领域: 微生物学 · 海洋生物学 · 生物化学
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INORGANICA CHIMICA ACTA · 2022 · IF 3.118

Comparative study of the electrocatalytic N2 reduction property of a Cu4 cluster with μ2-/μ3-OH and a Cu2 complex with μ2-OH

Wei Wang,Jing-Zhe Li,Shi-Jian Luo,Zi-Xuan Yao,Kuan-Guan Liu

Using the atomic precisely structurally characterized clusters as electrocatalysts can provide some possible structure information about the active intermediate during the electrocatalytic N 2 reduction reaction (NRR) process. A Cu4 cluster, named [(bpy) 4 Cu 4 (C 10 H 8 SO 3 ) 4 (OH) 4 ]•4H 2 O ( 1 ), has been synthesized and fully characterized by IR, SXRD, XPS, EPR, et al. Single crystal structural analysis reveals that the core structure of the cluster has a step-scheme conformation with two μ 2 -OH and two μ 3 -OH groups. Electro-catalysis studies of this cluster show that it can achieve a highest NH 3 yield of 2.18 μg h −1 mg −1 and a FE of 0.97 % at −0.6 V. The excellent NRR performance may be attributable to the additional μ 3 -OH groups, based on the contrastively study of the other electrocatalysts of the Cu powder and the Cu 2 complex, named [(μ 2 -OH)(μ 2 -Cl)(bpy) 2 Cu 2 Cl 2 ] ( 2 ), with one μ 2 -OH group in its structure. This work provides some structure information about the possible active sites during the NRR process and inspires us to develop new cluster as efficient electrocatalysts for advancing sustainable NH 3 production. Using the atomic precisely structurally characterized clusters as electrocatalysts can provide some possible structure information about the active intermediate during the electrocatalytic N 2 reduction reaction (NRR) process. A Cu4 cluster, named [(bpy) 4 Cu 4 (C 10 H 8 SO 3 ) 4 (OH) 4 ]•4H 2 O ( 1 ), has been synthesized and fully characterized by IR, SXRD, XPS, EPR, et al. Single crystal structural analysis reveals that the core structure of the cluster has a step-scheme conformation with two μ 2 -OH and two μ 3 -OH groups. Electro-catalysis studies of this cluster show that it can achieve a highest NH 3 yield of 2.18 μg h −1 mg −1 and a FE of 0.97 % at −0.6 V. The excellent NRR performance may be attributable to the additional μ 3 -OH groups, based on the contrastively study of the other electrocatalysts of the Cu powder and the Cu 2 complex, named [(μ 2 -OH)(μ 2 -Cl)(bpy) 2 Cu 2 Cl 2 ] ( 2 ), with one μ 2 -OH group in its structure. This work provides some structure information about the possible active sites during the NRR process and inspires us to develop new cluster as efficient electrocatalysts for advancing sustainable NH 3 production.

CAS / MDL: 7440-50-8
研究领域: 材料科学 · 电化学
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LANGMUIR · 2024 · IF 3.7

Preparation and Formation Mechanism of β-SiC Coatings Using a SiCl4–CH4–H2–N2 System

Tongguo Huo,Kai Cao,Jianxin Zheng,Dan Zhu,Yuan Lin,Yu Dai,Jian Wu

The mechanism of β-SiC preparation via chemical vapor deposition (CVD) of the SiCl4–CH4–H2–N2 system remains unclear. Consequently, the change of molar Gibbs free energy of the CVD β-SiC chemical reaction in the SiCl4–CH4–H2–N2 system has been studied by the Helsinki Software Corporation (HSC) Chemistry code for the first time. The role of nitrogen in the reaction was confirmed. Seven potential reaction pathways of CVD β-SiC were presented, and the thermodynamic equilibrium components of each reaction were calculated systematically. The most viable reaction pathway and corresponding optimal temperature range for CVD β-SiC were determined. In addition, a kinetic study of CVD β-SiC was conducted. The microscopic morphology and crystal structure of β-SiC coatings prepared on the graphite surface at different temperatures were charactered by scanning electron microscopy (SEM), X-ray diffraction (XRD), Raman, etc. Ultimately, through SEM, XRD, and Raman observation, uniform and dense β-SiC coatings with fine grains and high crystallinity were successfully obtained. Furthermore, large β-SiC-coated graphite trays with diameters of 230 and 465 mm were prepared by CVD using the SiCl4–CH4–H2–N2 system, and the average thickness of β-SiC was about 100.6 μm. This study provides a theoretical basis and technical recommendations for the fabrication of SiC-coated graphite trays used in metal–organic chemical vapor deposition (MOCVD) equipment.

CAS / MDL: 10026-04-7
研究领域: 材料科学 · 化学工程
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BIOCHEMICAL ENGINEERING JOURNAL · 2022 · IF 4.446

Promoting interspecies hydrogen/electron transfer in Bio-PdNPs-mediated denitrification with the selectivity towards N2

Sijing Bi,Huimin Liu,Yuancai Chen,Yongyou Hu

The palladium nanoparticles (Bio-PdNPs) were in-situ biosynthesized in denitrifying sludge at three Pd loading levels, and the denitrification performance was evaluated in terms of interspecies hydrogen/electron transfer (IHT/IET) and their pathway for the first time. The results showed that high selectivity towards N 2 (76.96%, 97.10% and 99.30%) were observed when conventional denitrifying sludge was embedded with appropriate amount of Bio-PdNPs at three C/N ratios (3, 7 and 10), respectively. In-situ fermented hydrogen could be consecutively provided for IHT at low H/N ratio, avoiding the production of NH 4 + . IHT related with Pd[H] mainly catalyzed the enzymic/nonenzymic transformation of NO 2 - , NO and N 2 O, in which NO could be directly/abiotically cracked to N 2 and O 2 /H 2 O. Moreover, IET was greatly accelerated via the bounded flavin (FBcyt) and cytochrome , riboflavin , as well as electron hopping. Nevertheless, enzymatic denitrification was depressed with excess Bio-PdNPs (Bio-PdNPs-10). This study shed light on IET/IHT and denitrification pathway in Bio-PdNPs-mediated denitrification system, and provided basis for engineering practice.

CAS / MDL: 13820-53-6
研究领域: 环境生物学 · 微生物学
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Composite membranes based on ether oxygen-rich polyimide with superior CO2/N2 separation properties prepared by interfacial polymerization

Xiaoli Ding,Weiji Wang,Xianyun Cheng,Xiaoqian Fan,Hongyong Zhao,Qingping Xin,Yuzhong Zhang

Ether oxygen-rich polymeric membranes emerge as promising membranes in CO 2 separation due to the high affinity between CO 2 molecules and ethylene oxide segments. However, there is a massive challenge in developing asymmetric membranes with high CO 2 permeation performance and CO 2 /light gas separation performance. This work revealed composite membranes with ether oxygen-rich polyimide separation layers were developed by interfacial polymerization between 1,2,4,5-benzenetetracarbonyl tetrachloride and commercial diamines named o,o'-bis(2-aminopropyl) polypropylene glycol-block-polyethylene glycol-block-polypropylene glycol followed by thermal imidization. The influences of the polymerization time and monomer concentrations on the gas transport and separation properties of the composite membranes were studied based on single-gas permeation. The optimum membrane possessed a superior high ideal CO 2 /N 2 separation factor of 429 accompanied with a moderate permeance of 150 GPU for CO 2 at 25 o C and 0.2 MPa. The performance stability was studied by operating the membrane at various pressures and temperatures. The result showed the composite membrane possessed excellent plasticization resistivity at high pressures. The separation property of composite membranes for CO 2 /N 2 binary mixture was also evaluated. The influences of the operation parameters, including stage-cut and pressure ratio on the product purity and recovery were investigated. The results showed great practical application potential in efficient separation of flue gas .

CAS / MDL: 110-54-3
研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

HOF-21 nanofillers incorporated mixed matrix membranes for high-performance N2/CH4 separation

Jun Ma,Jiahe Zhang,Ye Yuan,Yunqi Zhou,Shenzhen Cong,Guangyu Xing,Jixiao Wang,Zhi Wang

N 2 /CH 4 separation membranes based on N 2 preferential permeation can effectively reduce the recompression cost of CH 4 gas and show promising application prospects in the field of natural gas purification. However, the performance of N 2 /CH 4 separation membranes still needs to be improved. Here, we report a kind of mixed matrix membranes (MMMs) for N 2 /CH 4 separation via using HOF-21 as nanofiller and 6FDA-DAM polyimide as polymer matrix . In this work, the effects of HOF-21 loading, feed side pressure and temperature based on membrane performance were explored, and finally performance variation of the MMMs with operation time was tested. The incorporated HOF-21 nanoparticles with the most probable pore size of about 3.6 Å can significantly increase the diffusion rate of smaller N 2 molecules and enhance the N 2 /CH 4 diffusivity selectivity of the membrane. In addition, compared with polyimide, HOF-21 exhibits almost the same dynamic adsorption of N 2 and CH 4 , which can weaken the solubility of CH 4 and enhance the N 2 /CH 4 solubility selectivity of the membrane. When feed gas pressure was 0.2 MPa, the optimum membrane performance was achieved at the HOF-21 loading of 7 wt%, with N 2 permeance of 5.13 GPU and N 2 /CH 4 (50/50, vol%) selectivity of 20.52 at 298.15 K. Compared with N 2 permeation and N 2 /CH 4 selectivity of the 6FDA-DAM/PAN membrane, the MMMs increased by 67% and 54%, respectively, possessing potential applications in the field of N 2 removal in CH 4 purification.

研究领域: 材料科学 · 化学工程 · 天然气净化技术
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