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POLYCYCLIC AROMATIC COMPOUNDS · 2016 · IF 0.959

Characterization of Phenol Metabolization by P. stutzeri N2

Hongyun Nie,Maiqian Nie,Yongzhe Yang,Jing Zhao,Xinyi Zhang,Yutao Guo,Yi Wan,Jing Zi

Characterization of phenol metabolization by P. stutzeri N2 was proposed based on the identification of relevant metabolites and enzyme activities of catechol 1,2-oxygenase and catechol 2,3-dioxygenase. P. stutzeri N2 started to grow on 400 mg l−1 phenol with no obvious lag phase, and then phenol decomposition was rapidly completed within 32 h. Results of enzyme activities, UV spectrums of cultures, and the mass spectrum identification of cis, cis-muconic and 2-HMS, which showed that catechol C12O and C23O were acting simultaneously on the fission of the phenol ring. The existence of P-hydroxybenzoic acid and straight-chain saturated dicarboxylic acids in the culture medium showed that carboxylation and hydrogenation were involved during the phenol degradation. Metabolites containing five or four carbons indicated that catechol and its immediate ring-cleavage intermediates could be furthermore metabolized by P. Stutzeri N2. Therefore, P. stutzeri N2 which could degrade phenol with high efficiency and diverse pathways could have potential applications in the treatment of wastewater containing phenol.

CAS / MDL: 10416-59-8
研究领域: 环境微生物学 · 生物化学
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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Highly permeable MOF NH2-MIL-101(Cr) fragment membranes for CO2/N2 separation

Yunqi Zhou,Ye Yuan,Xinlei Liu,Zhi Wang

Metal-organic framework (MOF) membranes with proper pore size distribution and functional groups are generally more suitable for separation. Most MOFs are characterized by a hierarchical pore structure, which possesses large cavities surrounded by small windows. Fabrication of MOF membranes only retaining microporous fragment structure is a workable method to narrow pore size distribution. In this study, well-grown NH 2 -MIL-101(Cr) fragment membranes were fabricated for CO 2 separation by adjusting acetic acid – ligand – metal ratio to balance the nucleation and growth. NH 2 -MIL-101(Cr) fragment has a similar chemical structure to NH 2 -MIL-101(Cr) as expected, but only small pores with size around 0.56 nm is retained. The NH 2 -MIL-101(Cr) fragment membranes exhibited CO 2 /N 2 selectivity of about 37 with CO 2 permeance up to 6104 GPU.

研究领域: 材料科学 · 化学工程
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 43 ·20777-20785 · IF 3.925

Promoting the effects of CuSO4 on N2 selectivity in selective catalytic oxidation of ammonia over Pt/TiO2 catalysts

Yanke Yu,Mengqiao Geng,Desheng Wei,Chi He

Selective catalytic oxidation of NH3 (NH3-SCO) is a promising method to reduce NH3 pollution. The Pt-based catalysts exhibited excellent activity in the NH3-SCO reaction under low temperatures. However, it was easy for the NH3 to be oxidized to N2O and NOx (NO and NO2) over the Pt-based catalyst, causing a low N2 selectivity. The CuSO4, which could supply both Brønsted and Lewis acid sites on the catalyst, was used to promote N2 selectivity. The N2 adsorption–desorption, X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), inductively coupled plasma mass spectrometry (ICP-MS), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were used to characterize the catalyst. The addition of CuSO4 could suppress the formation of N2O and NOx, thus the highest N2 selectivity on the catalyst increased from 21.2% to 78.1%. An imide mechanism was the main reaction mechanism on the Pt/TiO2 catalyst. After adding CuSO4, the NH3-SCO reaction over the CuSO4-Pt/TiO2 catalyst mainly followed an i-SCR mechanism where NH3 was oxidized to N2O and NOx, and then the newly formed N2O and NOx were reacted with NH3/NH4+ adsorbed on the Lewis and Brønsted acid sites via an NH3-SCR reaction over the catalyst, and finally N2 was formed. The acid sites performed an important role in the formation of N2 and this work should provide an effective method to promote N2 selectivity in a NH3-SCO reaction.

CAS / MDL: 13463-67-7 18497-13-7
研究领域: 催化化学 · 环境科学
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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

PIM-1 membrane incorporated cPIM-1 grafted PP-DETA for high-efficiency CO2/N2 separation

Shuangqi Song,Hong Li,Jingde Li,Yanqin Yang

Mixed-matrix membranes (MMMs), developed through the combination of solid fillers with polymer matrices, represent an effective approach addressing the persistent challenge of balancing permeability and selectivity in polymer membrane. Diethylenetriamine-functionalized porous material of PP-DETA, which is synthesized from porous organic polymer of PP via one-step diethylenetriamine grafting, is an ideal material for MMMs production. However, designing and optimizing PP-DETA for high-performance CO 2 separation membranes remains a challenge. Herein, we develop an improved PP-DETA material, designated as PP-DETA-cPIM-1, by covalently attaching a carboxylated polymer of intrinsic microporosity (cPIM-1) network layer onto the PP-DETA surface. Membranes prepared from this PP-DETA-cPIM-1 filler and PIM-1 matrix demonstrate enhanced interfacial adhesion and stronger mechanical properties in comparison to the counterparts with the same loading of PP-DETA. The incorporation of PP-DETA-cPIM-1 into MMMs establishes an enhanced filler/polymer interface that facilitates the selective transport of CO 2 through the filler, while simultaneously improving membrane stability and suppressing physical aging. Specifically, with 5 wt% loading of PP-DETA-cPIM-1 filler, the MMM is able to enhance the CO 2 /N 2 selectivity and CO 2 permeability by 52.3 % and 25.3 %, respectively, exceeding the upper bound established in 2008. Furthermore, PP-DETA-cPIM-1/PIM-1 MMMs display superior anti-aging ability for 180 days of aging.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2018 · IF 3.927

Preparation of Ni-MOF-74/SBS mixed matrix membranes and its application of CH4/N2 separation

Shumin Wang,Qingping Guo,Shujun Liang,Peng Li,Jujie Luo

A series of mixed matrix membranes (MMMs) were fabricated with Ni-MOF-74 as filler and poly (styrene-b-butadiene-b-styrene) (SBS) polymer as matrix materials for CH 4 /N 2 separation. MMMs were characterized by Fourier transform infrared (FTIR) spectra, X-ray diffraction (XRD), scanning electron microscopy (SEM), and thermogravimetric analysis (TGA). Gas separation behavior was investigated by measuring single and mixed gases. For the single gas, the CH 4 permeability of the MMMs incorporated with 15 wt% Ni-MOF-74 (Ni-MOF-74/SBS-15) reached 83.5 Barrer, which was 116% higher than that of SBS (38.6 Barrer), while its ideal selectivity remained the same. CH 4 permeability can further increase to 176.6 Barrer with the increase in temperature to 55 °C. For the CH 4 /N 2 (50/50 vol%) mixed gas, the Ni-MOF-74/SBS-15 sample exhibited increasing CH 4 permeability (74.7 vs 36.7 Barrer), while selectivity remained unchanged relative to that of the pure SBS membrane.

CAS / MDL: 67-56-1 109-99-9
研究领域: 材料科学 · 化学工程
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Journal of Environmental Sciences · 2023 · IF 6.9

Remarkable N2-selectivity enhancement of NH3-SCR over HPMo modified MnCo-BTC@SiO2 catalyst

Songjin Ko,Xiaolong Tang,Fengyu Gao,Honghong Yi,Hengheng Liu,Ning Luo

In this work, the phosphomolybdate (HPMo) modification strategy was applied to improve the N 2 selectivity of MnCo-BTC@SiO 2 catalyst for the selective catalytic reduction of NO x , and further, the mechanism of HPMo modification on enhanced catalytic performance was explored. Among MnCo-BTC@SiO 2 -x catalysts with different HPMo concentrations, MnCo-BTC@SiO 2 -0.75 catalyst exhibited not only the highest NH 3 -SCR performance (∼95% at 200-300°C) but also the best N 2 selectivity (exceed 80% at 100-300°C) due to the appropriate redox capacity, greater surface acidity. X-ray photoelectron spectrometer (XPS) and temperature programmed reduction of H 2 (H 2 -TPR) results showed that the modification with HPMo reduced the oxidation-reduction performance of the catalyst due to electron transfer from Mo 5+ to Mn 4+ /Mn 3+ and prevent the excessive oxidation of ammonia adsorption species. NH 3 temperature-programmed desorption of (NH 3 -TPD) results showed that the modification with HPMo could significantly improve the surface acidity and NH 3 adsorption, which enhance the catalytic activity and N 2 selectivity. In-situ diffused reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) revealed that modification with HPMo increased significantly the amount of adsorbed NH 3 species on the Bronsted acid site and C B / C L , it suppressed the production of N 2 O by inhibiting the production of NH species, the deep dehydrogenation of ammonia adsorption species. This study provided a simple design strategy for the catalyst to improve the low-temperature catalytic performance and N 2 selectivity.

研究领域: 催化化学 · 环境科学
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Sustainable Energy & Fuels · 2019 ·Vol. 4 ·期 1 ·164-170 · IF 4.912

An MOF-derived C@NiO@Ni electrocatalyst for N2 conversion to NH3 in alkaline electrolytes

Shijian Luo,Xiaoman Li,Wanguo Gao,Haiqiang Zhang,Min Luo

Today, industrial ammonia synthesis mainly depends on the Haber–Bosch process, which causes a lot of energy consumption and huge CO2 emissions. The electrochemical N2 reduction reaction (NRR) is considered a more sustainable and environmentally benign alternative to produce ammonia, but it requires an efficient catalyst to overcome the difficulty of N2 activation. In this work, we reported that MOF-derived C@NiO@Ni microtubes behaved as a high-efficiency electrocatalyst in 0.1 M KOH electrolyte. This electrocatalyst achieved a high NH3 yield of 43.15 μg h−1 mgcat.−1 and faradaic efficiency of 10.9% at −0.7 V vs. a reversible hydrogen electrode. The experimental results indicated that the excellent NRR performance originated from the oxygen vacancies in NiO. Moreover, the abundant NiO/Ni interfaces were conducive to proton adsorption and further enhanced the NRR performance.

研究领域: 材料科学 · 电化学 · 环境科学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2020 · IF 4.551

Functionalized ZIF-7/Pebax® 2533 mixed matrix membranes for CO2/N2 separation

Jie Gao,Haizhuo Mao,Hua Jin,Chen Chen,Armin Feldhoff,Yanshuo Li

Membrane-based separation technology has evolved as a competitive approach for CO 2 capture from flue gas (mainly N 2 ). To achieve high separation performance, three partially NH 2 -, OH- and CH 3 OH- functionalized mixed-linker-ZIF-7 were successfully synthesized, and incorporated into polyether-block-amide (Pebax® 2533) polymer to form mixed-matrix membranes (MMMs). As evidenced by the CO 2 adsorption isotherms , introducing functional groups in the ZIF-7 framework was indeed beneficial for CO 2 adsorption. All MMMs composed of ZIF-7-NH 2 , ZIF-7-OH and ZIF-7-CH 3 OH offered better CO 2 /N 2 separation performance than the parent ZIF-7-Pebax® 2533 membrane, suggesting the positive effect of functionalized ZIF-7 fillers on the gas separation performance. Among the three functionalized ZIF-7 based MMMs, the ZIF-7-OH-Pebax MMMs exhibited the best performance for CO 2 /N 2 separation, which might be ascribed to the highest adsorption selectivity of CO 2 over N 2 predicted by ideal adsorbed solution theory (IAST) for ZIF-7-OH fillers. The 14% ZIF-7-OH-Pebax MMM showed high CO 2 permeability of 273 Barrer and CO 2 /N 2 separation factor of 38, which increased by 60% and 145% as compared with the neat Pebax membrane. The strategy of preparing functionalized MOFs with strong affinity for CO 2 provides an effective method to develop MMMs for highly efficient CO 2 separation.

研究领域: 材料科学 · 环境工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Simultaneous efficient production of hydrogen peroxide, urea and H2 by bifunctional Cu-doped TiO2 electrocatalyst from CO2, N2 and water

Jiejie Bai,Yue Shi,Aixin Ma,Feifei Liu,Yanru Liu,Caixia Li,Jianping Lai,Lei Wang

The production of three separated, high-value chemicals (H 2 O 2 , urea and H 2 ) from CO 2 , N 2 , and H 2 O represents a significant challenge. It is a prospective and innovative way to simultaneously produce these chemicals in an anion exchange membrane (AEM) electrolyzer, which couples anodic 2e - water oxidation (2e - WOR) and cathodic CO 2 , N 2 and water reduction reaction (CNWRR), but has not yet been realized. Here, we found that bifunctional Cu x Ti 1-x O 2-y catalysts can be employed in the electrochemical production of H 2 O 2 , urea and H 2 from CO 2 , N 2 and water, and the optimized Cu 0.12 Ti 0.88 O 2-y catalyst exhibits an excellent productivity of 11.8 μmol cm −2 min −1 , 0.3 mg cm -2 h −1 and 0.82 mmol cm -2 h −1 for H 2 O 2 , urea and H 2 at 4.0 V (50 mA cm −2 ) in AEM electrolyzer, respectively. Theoretical calculations reveal that the superior performance of the 2e - WOR and CNWRR is attributed to the Cu doping effect, which not only promotes the coupling of *OH but also optimizes the adsorption energy barriers of COOH* and NNH*. It is worth noting that the AEM electrolyzer assembled by bifunctional Cu 0.12 Ti 0.88 O 2-y reaches a current density of 50 mA cm −2 with a cell voltage of 4.0 V and exhibits excellent stability of 50-hour continuous operation.

CAS / MDL: 298-14-6
研究领域: 电化学 · 催化 · 材料科学 · 可再生能源
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

Highly crystalline covalent organic frameworks for ratiometric fluorescent sensing of trace water in honey and N2 gas

Cong Guan,Jiaming Cai,Xiaotao Liu,Liangqia Guo

The detection of trace water (H 2 O) content is important and challenging in food and food-related industries. Herein, highly crystalline two-dimensional covalent organic frameworks (TAPT-BTCA-COF) with yellow-green fluorescence were prepared by using 1,3,5-tris(4-aminophenyl)triazine (TAPT) and 1,3,5-benzenetricarboxaldehyde (BTCA) as precursors. The fluorescence of TAPT-BTCA-COF is sensitive to the solvent polarity due to the intermolecular charge transfer (ICT) effect and can be quenched by trace H 2 O due to the block of ICT effect by H 2 O. On this base, TAPT-BTCA-COF is applied for sensing of trace H 2 O in common organic solvents such as DMF, acetonitrile , THF and acetone with fast response and high sensitivity. The limits of detection for H 2 O in DMF, acetonitrile, THF and acetone are 0.082 wt%, 0.0053 wt%, 0.0091 wt% and 0.0061 wt%, respectively. Furthermore, a ratiometric fluorescent sensor is proposed by using TAPT-BTCA-COF as the signal probe and red fluorescent tris(2,2′-bipyridyl)ruthenium(II) dichloride as the reference and successfully applied for quantitatively and semi-quantitatively sensing of trace H 2 O in honey sample and the moisture in N 2 gas.

CAS / MDL: 1314-56-3
研究领域: 材料科学 · 分析化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

K-RHO zeolite with high nitrogen selectivity for N2/CH4 separation by PSA process

Wang Boxuan,Bao Qiang,Chen Zhirui,Qiao Xue,Hu Yunfeng,Zhang Jian,Liang Dan,Sun Penglai,Xia Haiyue,Wang Xiangyang

Zeolite RHO, a microporous zeolite, has the great possibility for N 2 /CH 4 separation by regulating the size of the eight-membered ring window on the RHO framework. In this work, the ability of ion-exchanged RHO zeolites for N 2 /CH 4 separation is investigated, and a highly nitrogen selectivity adsorbents are developed. RHO samples were prepared by hydrothermal synthesis. Alkali metal cations (Na + , K + , Cs + ) was used for ion exchange. Adsorption equilibrium isotherms of N 2 and CH 4 were measured at normal temperature and fitted by the Langmuir equation. The adsorbent selection parameters ( S parameters) were calculated based on the working capacity and equilibrium selectivity of N 2 /CH 4 , which are used to comprehensively evaluate the selectivity of N 2 /CH 4 . The results indicate that the cations have effects on the regulation of the eight-membered ring window. In particularly, K-RHO no.2 sample which is obtained by ion exchange of K + cations exhibit the best N 2 /CH 4 separation performance, which is a potential nitrogen selective adsorbent. In addition, the product throughputs of RHO and the commercial adsorbent ETS-4 were compared by common PSA simulation process with essentially the same product purity and recovery. The results show that K-RHO no.2 has 36 % higher product throughput than ETS-4, which can compensate for the problem of low N 2 working capacity of ETS-4 in industrial application.

研究领域: 材料科学 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Highly porous MOF integrated with coordination polymer glass membrane for efficient CO2/N2 separation

Ning Li,Chao Ma,Ziyue Wang,Dudu Li,Zhihua Qiao,Chongli Zhong

The MOF crystal-glass composites (CGC) membrane, comprising a MOF crystal and MOF glass matrix, represents a novel self-supported membrane that has been effectively applied in gas separation. Nevertheless, the typical MOF glass matrix requires a higher operating temperature (>400 °C), which constrains its combination with a multitude of MOF crystals characterized by high porosity and low decomposition. In this work, Zn-P-dmbIm (coordination polymer) was chosen as the glass matrix, and MIL-101 crystal with high porosity were integrated at an operating temperature of 190 °C. Furthermore, the intrinsic low porosity of a g Zn-P-dmbIm can be enhanced by the incorporation of higher porosity MIL-101, which possessed a high specific surface area (from ∼1.7 m 2 /g to 401 m 2 /g) and porosity (from ∼0.0014 cm³/g/nm to 0.5605 cm³/g/nm) of the CGC. The intimate combination of MIL-101 and a g Zn-P-dmbIm by in - situ melting to reduce the interfacial defects, which also provides a robust foundation for effective CO 2 /N 2 separation. In CO₂/N₂ (50/50, v/v) mixed gas conditions, the MIL-101/ a g Zn-P-dmbIm membrane demonstrated a impressively high CO₂ permeability of 18670 barrer and CO₂/N₂ selectivity of 61, exceeding the CO₂/N₂ upper bound. The variable pressure (1-12 bar) and long-term stability (120 h) of the CGC membrane exhibited enhancing separation stability. Hence, the self-supported MIL-101/ a g Zn-P-dmbIm membrane demonstrated effective CO₂/N₂ separation performance, which had the potential to significantly extend the scope of applications for MOF crystal-glass matrices.

研究领域: 材料科学 · 环境工程
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