CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
·
IF 3.171
Xionghui Liu,Jianfeng Du,Yu Ye,Yuchuan Liu,Shun Wang,Xianyu Meng,Xiaowei Song,Zhiqiang Liang,Wenfu Yan
Nitrogen-rich porous organic polymers have shown great potentials in gas adsorption/separation, photocatalysis , electrochemistry, sensing and so on. Herein, 1,2,3-triazole functionalized triazine-based porous organic polymers (TT-POPs) have been synthesized by the copper-catalyzed azide-alkyne cycloaddition (Cu-AAC) polymerization reactions of 1,3,5-tris(4-azidophenyl)-triazine with 1,4-diacetylene benzene and 1,3,5-triacetylenebenzene, respectively. The characterizations of N 2 adsorption at 77 K show TT-POPs possess permanent porosity with BET surface areas of 666 m 2 ·g −1 (TT-POP-1) and 406 m 2 ·g −1 (TT-POP-2). The adsorption capacities of TT-POPs for CO 2 , CH 4 , C 2 H 2 and C 2 H 4 , as well as the selective separation abilities of CO 2 /N 2 , CO 2 /CH 4 , C 2 H 2 /CH 4 and C 2 H 4 /CH 4 were evaluated. The gas selective separation ratio of TT-POPs was calculated by the ideal adsorbed solution theory (IAST) method, wherein the selective separation ratios of C 2 H 2 /CH 4 and C 2 H 4 /CH 4 of TT-POP-2 was 48.4 and 13.6 (298 K, 0.1 MPa), which is comparable to other adsorbents (5.6–120.6 for C 2 H 2 /CH 4 , 10–26 for C 2 H 4 /CH 4 ). This work shows that the 1,2,3-triazole functionalized triazine-based porous organic polymer has a good application prospect in natural gas purification.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Peng Yan,Jucai Yang,Deyun Ma,Siyun Zhang,Shigong Zeng,Liting Feng,Sihui Zhan,Qiaquan Lin
A water-stable porous cobalt(II)–organic framework functionalized by ethoxyl groups with a chemical formula, {[Co 6 (5-EIA) 5 (tmbpy)(OH) 2 (H 2 O) 2 ]∙4(H 2 O)} n ( 1 ) (5-H 2 EIA = 5-ethoxy-isophthalic acid; tmbpy = 3,3′-dimethyl-4,4′-bipyridine) has been constructed and studied in terms of structure and performance. 1 shows a 3D framework, and has a 1D channel of 8.1 × 6.0 Å 2 along the a axis. The framework 1 exhibits high humid and thermal stability according to PXRD and TGA results. The C 2 H 2 and CO 2 uptakes of the activated 1 ( 1a ) were up to 2.07 mmol g −1 and 1.89 mmol g −1 at 273 K (100 kPa), respectively. More importantly, 1a shows excellent C 2 H 2 /CH 4 (1:1) and CO 2 /CH 4 (1:1) separations with IAST selectivity of 23.7 and 11.4 at 298 K (100 kPa), respectively. Furthermore, 1a showed good reuse performance, suggesting that 1a could be applied to the separation of C 2 H 2 /CH 4 or CO 2 /CH 4 .
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
Carbon Capture Science & Technology
·
2023
·
IF 0
Wufeng Wu,Jiang Fan,Dongyue Wang,Yali Zhao,Xinglei Zhao,Yanying Wei
MOF membranes exhibit impressive performance in gas separation due to their large surface area, controllable pore size and unique affinity. Here, the ultrathin UiO-66-NH 2 polycrystalline membranes with thickness of ∼320 nm are successfully prepared within 1 h using a combination of ultrasound-assisted and microwave synthesis strategies. During the reaction, high-density small MOF nuclei are produced by sodium formate ultrasound-assisted, which act as sufficient nucleation sites for heterogeneous nucleation during membrane growth, aiming for development of a continuous MOF membrane on the porous substrate. The obtained UiO-66-NH 2 membrane shows an ideal CO 2 /CH 4 selectivity of 40 due to the enhanced the interaction between CO 2 molecules and the membrane. Moreover, the narrowed pore structure further hinders the diffusion of larger-sized molecules owing to -NH 2 occupying the pore channels, resulting in elevated CO 2 /CH 4 selectivity. Compared to many other MOF membranes, the UiO-66-NH 2 polycrystalline membranes exhibit a well balance of gas permeance and CO 2 /CH 4 selectivity, which presents a new route for CO 2 capture.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Ruoxing Liao,Yumin Guo,Liqiu Yang,Haoli Zhou,Wanqin Jin
Membrane technology , a successful technology for separating gases such as CO 2 /CH 4 mixture, has attracted much attention because of its low energy consumption, and membrane performance is an important factor affecting its industrial application. Herein, the solvent-induced microstructure of a polyimide membrane was employed to enhance its CO2/CH4 separation performance. The effect of solvents on the membrane structure and gas separation performance was investigated by using different solvents (such as tetrahydrofuran, N,N-dimethylacetamide) to dissolve a newly synthesized polyimide polymer, which was fabricated into a membrane. Various characterization methods, such as positron annihilation lifetime spectroscopy (PALs) and X-ray diffractometry (XRD), were conducted to reveal changes in the microstructure of membranes prepared with different solvents. The interaction of solvents with groups of polymer backbones was also analyzed for the explanation of the effect of solvents on the membrane performance for the separation of different gas pairs, such as CO2/CH4 mixture. The results showed that a membrane with optimal separation performance was obtained by optimizing the solvent composition, which exceeded the 2018 mixed-gas CO2/CH4 upper bound. The induced effect of solvents on the polymer membrane structure provides a new research path for the optimization of polymer membranes to enhance separation performance.
研究领域:
材料科学
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化学工程
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气体分离技术
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhenghui Huang,Peng Hu,Jia Liu,Fang Shen,Youquan Zhang,Kungang Chai,Yunpan Ying,Chengjun Kang,Zhaoqiang Zhang,Hongbing Ji
Efficient CH 4 /N 2 separation is necessitated for obtaining purified methane from natural gas. Aluminum-based metal–organic frameworks (Al-MOFs) have potential for industrial separation applications due to their structure-tunable, low-cost, and scalable features. Intrigued by the impressive selectivity of a recently reported Al-MOF (Al-CDC) toward CH 4 over N 2 , we herein further study the potential of Al-MOFs as adsorbent for CH 4 /N 2 separation, mainly considering the effects of pore geometry and linker polarity. Utilization of two bent ligands and two linear ligands with different polarity afforded two one-dimensional square-shaped Al-MOFs i.e., CAU-10-H, MIL-160, and two rhombic-shaped counterparts i.e., Al-Fumarate (Al-Fum), MIL-53(Al)), respectively. Afterward, pure CH 4 and N 2 adsorption experiments were conducted at 273–313 K for assessing the CH 4 /N 2 separation performance. The results indicated that all the Al-MOFs exhibited superior affinity toward CH 4 over N 2 , and the CH 4 uptake followed the sequence of Al-Fum > CAU-10-H > MIL-53(Al) > MIL-160. Exhilaratingly, Al-Fum exhibited unprecedented CH 4 /N 2 selectivity (17.2) and high CH 4 uptake at 273 K and 1.0 bar. The mechanism underlying the disparity of Al-MOFs affinity toward CH 4 was deciphered via theoretical simulation, suggesting that the synergetic effects of accessibility of strong affinity sites (μ 2 -OH) on AlO 6 chains and polar pore surface induced by varying linkers highly promoted the CH 4 uptake. Furthermore, the results of cyclic adsorption–desorption experiments and binary breakthrough tests validated the feasibility of Al-Fum for practical application.
研究领域:
材料科学
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化学工程
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气体分离
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产品关联
DOI
高影响因子
Energy Materials
·
2024
·Vol. 4
·期 6
·N
·
IF 11.8
Zuwei Xu,Ze Zhang,Fuchang Gao,Yuhan Zhu,Haibo Zhao
Catalytic combustion is an effective approach to remove air pollutants from various emission sources. For this purpose, supported noble metal catalysts are preferred in commercial applications due to their outstanding catalytic activity for eliminating CO, hydrocarbon compounds and NOx. In this paper, we employ the flame spray pyrolysis method to prepare a series of Pt-based catalysts with four different supports (TiO2, ZrO2, MgO and ZnO) and variable low Pt loadings for catalytic combustion of CO and CH4. The performance of 0.5 Pt/TiO2 is the best in all samples, in which the T90 temperatures are 107 and 500 °C for 90% conversion of CO and CH4, respectively. To examine its thermal stability, a time-on-stream test at 700 °C for 420 min is carried out, resulting in a decrease of about 5% in the final conversion of CH4. The X-ray diffraction results show that TiO2 support is a mixed phase with a major amount of anatase and a small amount of rutile other than a pure phase of ZrO2, MgO and ZnO. Furthermore, X-ray photoelectron spectroscopy analysis and high-angle annular dark-field scanning transmission electron microscopy observation show that when the Pt loading is low, the Pt species exist as highly dispersed single atoms on the surface of the TiO2 support. As the Pt loading gradually increases, the state of the Pt species transitions from single atoms to Pt clusters, resulting in a decrease in dispersion. Ultimately, the Pt can successfully accumulate on the surface of the TiO2 nanoparticles, providing abundant active sites for efficient catalytic combustion reactions.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2024
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IF 4.4
Wei Li,Jingyun Wang,Mengmeng Han,Shanshan Xu
Obtaining pure clean energy methane (CH 4 , 3.80 Å) from natural gas is a great challenge task at present due to the similar kinetic diameter with nitrogen (N 2 , 3.64 Å). Herein, a well-defined rod-like bimetallic MOF (Cu 0.5 Ca 0.5 -SBMOF) with an excellent adsorption performance for CH 4 was successfully prepared and blended as filler with Matrimid® 5218 (PI) for preparing mixed matrix membranes (Cu 0.5 Ca 0.5 -SBMOF@PI MMMs). In the separation experiment of N 2 /CH 4 binary gas mixture, both filler loadings and trans -membrane pressure have significant effects on the separation performance of MMMs. When the filler loading is 20 wt%, Cu 0.5 Ca 0.5 -SBMOF@PI MMMs exhibits an excellent separation performance with a separation factor of CH 4 /N 2 up to 17.03, and the permeability of 22.57 barrer for N 2 , which significantly preceded the most reported MMMs. Moreover, the prepared MMMs also show excellent stability. This work has taken an important step towards practical application in the field of separating N 2 /CH 4 gas mixture using MMMs method.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Zhiwei Zhao,Yating Wang,Yuhao Tang,Xiaoqing Wang,Feifei Zhang,Jiangfeng Yang
Unconventional natural gas has become an important supplement to conventional energy sources, and the process of enrichment and purification of methane from low concentration coalbed methane is crucial. To this end, we report a copper-based metal–organic framework (MOF), ZJNU-119Cu, featuring two methane traps constructed with uncoordinated carboxylic acid oxygens and open metal sites. ZJNU-119Cu exhibits a high methane adsorption capacity (58.2 cm 3 ·g –1 ) at 298 K and 0.1 MPa and excellent CH 4 /N 2 separation performance under dynamic conditions. Density-functional theory calculations combined with grand canonical Monte Carlo simulation theory reveal the interaction mechanism for the uncoordinated carboxylic acid oxygen atoms and open metal sites in ZJNU-119Cu with CH 4 . The gas adsorption isotherms, heat of adsorption calculations, and breakthrough separation experiments indicate that this MOF is a very promising adsorbent for CH 4 /N 2 separation.
研究领域:
材料科学
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能源化学
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理论计算
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产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2024
·
IF 2.8
Ye Liu,Lei Zhang,Yubo Kuang,Xiaoqian Xiang,Haohan Tao,Guangran Di,Xiaojing Yin,Meicheng Li,Xiao-Jun Lv
The photocatalytic CO 2 reduction has the problems of low selectivity of single product. Here, the preparation of Cu modified tubular C 3 N 4 (CTN) was studied. The increase of the active site inhibits the recombination of electrons (e-) and holes (h + ) and improves the selectivity of CO 2 reduction products. Finally, the CO and CH 4 yields of 1.5 % CTN photocatalyst are 11.55 μmol·g −1 and 4.72 μmol·g −1 , respectively, which are 5 times higher than that of tubular C 3 N 4 photocatalyst. The selectivity of 2 % CTN to CH 4 is up to 68 %, indicating that the prepared CTN photocatalyst has high CO 2 reduction activity and CH 4 selectivity.
研究领域:
材料科学
·
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Zhan-Kuo Guo,Han-Qing Chen,Hui-Lin Jiang,Bao-Xia Dong,Yun-Lei Teng
Storing and hydrogenating CO2 to CH4 is an efficient solution to alleviate the greenhouse effect and energy shortage. This work demonstrated that the CaO-captured CO2 could be selectively converted to CH4 by Ni- and hydrogen-assisted calcium looping (CaL) processes in a batch reactor. The Ni/CaO composite was first synthesized in one step at room temperature by calcium-induced hydrogenation of Ni-mixed calcium carbonate without the use of any solvent and CO2 emission. The CO2 capture properties over the Ni/CaO composite and the methanation properties of the Ni/CaCO3 composite produced after CO2 capture were then studied in a batch reactor. It was proved that the CO2 capture properties of CaO can be improved, the CaO recovering temperature can be significantly lowered, and valuable CH4 can be selectively produced by Ni- and hydrogen-assisted calcium looping processes at moderate/high temperature. The 68.58% methane yield and 100% methane selectivity were achieved under relatively mild conditions. After five Ni- and hydrogen-assisted CaL processes, the methane yield still reaches 45%. This study offers a novel energy-saving CaL process, which can be utilized for facile and selective conversion of the CaO-captured CO2 to CH4.
研究领域:
化学工程
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环境科学
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能源技术
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产品关联
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 11
·8541-8552
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IF 4.6
Hui Zhang,Yi Hui Sun,Sheng Li An,Rui Hua Guo,Rui Fen Wang,Yu Wei Ma
S-type heterojunction photocatalysts (CeCux-BTC/CN) of cerium-copper bimetallic organic framework (CeCux-BTC) and graphitic carbon nitride (g-C3N4) were constructed by a simple solvothermal method using cerium nitrate, copper nitrate, and urea as the raw materials, and 1,3,5-benzene-tricarboxylic acid as the ligand for the photocatalytic CO2 reduction to CO and CH4. The results show that the built-in electric field constructed by Fermi energy level flattening transfers the electrons in an S-type manner, which not only preserves the strong reducing properties of the electrons in the material but also provides the maximum redox capacity and enables the composite samples to obtain higher visible-light trapping capacity and improve the separation efficiency of the carriers while refining the crystal particles. With the addition of only 1 mL of H2O as the proton supply source, CeCu0.05-BTC/CN exhibits the optimal photocatalytic performance. The CO and CH4 yields were 64.44 and 0.5575 μmol g−1, which were 7.56 and 2.42 times higher than those of g-C3N4, respectively, and the catalytic performances were basically stable after cycling tests.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Wenjiao Chang,Honghuo Wang,Tingting Wu,Shuting Zhang,Yifan Li,Junying Wang,Yongqiang Yang,Lei Wang
Photocatalytic CO 2 reduction reaction is regarded as a potential strategy to convert greenhouse gases into valuable chemicals. However, achieving photocatalysts with high efficiency and target product selectivity under visible light still faces great challenges. Herein, sub-2 nm RuO 2 @TiO 2 (RTO) nanorods with lattice matching interface are rationally designed and prepared via a hydrothermal reaction step-by-step. Due to the strong interaction of the lattice-matched interface with the Ru-O-Ti bond, new energy levels have emerged at the interface, leading to effective visible light absorbance. Moreover, the photo-generated electrons could be transferred to the RuO 2 efficiently via the lattice-matched interface. As a result, the RTO photocatalyst exhibits superior CO 2 -to-CH 4 conversion performance of 15.6 µmol g −1 with a selectivity of 87.9% under visible light irradiation. Density functional theory (DFT) calculation reveals that the energy barrier of CO* to CO is significantly higher than that of *CHO, resulting in the preferential production of CH 4 . This work provides an effective strategy for designing photocatalyst with promoted visible light absorption and improved product selectivity.
研究领域:
材料科学
·
环境科学
·
催化化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）