SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yuan Li,Yang Zhou,Yuze Zhang,Xiaoqing Wang,Jinping Li,Jiangfeng Yang
Although zeolite adsorbents are widely used for gas separation, current studies predominantly focus on single-phase topological structure. Herein, an intergrowth T zeolite with ERI and OFF topologies was synthesized in a template-free system, and the results showed the CH 4 adsorption capacity and CH 4 /N 2 selectivity were 34.4 cm 3 /g and 5.3 (298 K, 1 bar), respectively. The exceptional performance was attributed to its high microporosity and the 6-member ring (6-MR) structure at the intergrowth interface, which synergistically optimize the distribution of adsorption sites, as evidenced by density functional theory (DFT) calculations. Breakthrough experiments demonstrated that intergrowth T zeolite can effectively separate CH 4 /N 2 mixtures (50/50 and 20/80; v/v) with actual separation times of 7.0 min and 10.4 min. Furthermore, two-bed six-step pressure swing adsorption (PSA) simulations further indicated that 20 % of the pristine CH 4 could be enriched to over 50 %, with a recovery rate of 87 %, demonstrating significant potential for upgrading low-concentration coal-bed methane.
研究领域:
化学工程
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材料科学
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物理化学
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分离技术
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能源工程
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Peng Hu,Hao Wang,Chao Xiong,Hao Liu,Jun Han,Jie Zhou,Zhenxia Zhao,Yongqing Wang,Hongbing Ji
We demonstrate a novel microwave-assisted strategy to in situ functionalize the node chemistry of Zr-based metal–organic frameworks (Zr-MOFs) with a 2-aminobenzimidazole (2-AMI) agent. The novel strategy can concomitantly weaken the Lewis acidity of Zr6O8 nodes of Zr-MOFs through bonding with 2-AMI, contributing to admirable surface hydrophobicity with an ultrahigh water contact angle of 151.7° and enhanced stability. The successful coordination process was jointly verified by thermogravimetry analysis, 1H nuclear magnetic resonance spectroscopy , and X-ray photoelectron spectroscopy analyses. Meanwhile, the tailor-made pore microenvironment enabled highly efficient CO2/CH4 separation via a synergetic equilibrium-kinetic effect. Gas adsorption isotherms and time-dependent kinetic profiles cooperatively reveal that UiO-66(N10%-Zr) exhibits an advanced ideal adsorbed solution theory selectivity of 326, an excellent diffusion selectivity of 60.7, and a dynamic selectivity of 195 for CO2/CH4 separation, confirming the unwanted equilibrium-kinetic effect. Breakthrough experiments and modeling simulations further confirm the enhanced hydrophobic nature and high CO2/CH4 separation performance of UiO-66(N10%-Zr) even under humid conditions. The node-based engineering strategy is here demonstrated to be highly effective for CO2/CH4 separation, providing a new direction to achieve advanced MOF structures with sustainable advantages including high adsorption capacity, high selectivity, and hydrophobicity, which are of crucial significance for industrial applications.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Minghu Zhao,Jiuhu Zhao,Ran Ding,Rongshu Zhu,Haiyan Li,Zhi Li,Jingwen Zhang,Yongji Zhu,Huiying Li
The existence of sulfur dioxide and water vapor in the flue gas generated from waste-to-energy stations could lead to catalyst deactivation , which has adverse effects on NO x removal. It is thus particularly important to study the reaction mechanism of catalyst resistance to poisoning. Herein, we report the mechanism of In-Co 3 O 4 -Ga 2 O 3 /H-Beta catalyst to SO 2 and H 2 O resistance in the selective catalytic reduction (SCR) of NO x by CH 4 . The catalyst could achieve 74.6% NO x removal efficiency in the presence of 100 ppm SO 2 and 5% H 2 O. In this catalyst, Co 3 O 4 is attributed to enhancing the reversible poisoning of SO 2 and CH 4 activation and increasing the number of Brønsted acid sites by decomposing H 2 O. However, the InO + active center was still eroded by a small amount of water vapor, leading to a reduction in NO x removal efficiency. The addition of Ga 2 O 3 primarily provided an important intermediate NO 2 for CH 4 -SCR reaction and reduced the aggregates of Co 3 O 4 to increase the exposure of indium sites, and could reduce a part of SO 2 to S 2− . This study provides a good candidate for preparing catalysts with superior resistance towards SO 2 and H 2 O for CH 4 -SCR.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Lingxiang Huang,Yue Ma,Mufan Niu,Shenyong Ren,Qiaoxia Guo,Chunming Xu,Baojian Shen
Dry reforming reaction of greenhouse gas CH 4 and CO 2 was studied over Ni-Fe bimetallic catalyst, in which the composite support of C12A7-O 2- in MCM-41 was used. The isotope 13 CH 4 /D 2 O tracing experiment showed CO mainly comes from 13 CHx oxidation reaction and DH comes from CHx and D 2 O reaction, exhibiting lattice oxygen promotes CH X oxidation and water accelerate methane conversion. XPS and TPSR-MS studies exhibited the existence of lattice oxygen in catalysts produces a little H 2 O to facilitate a lower starting point at the reaction temperature. On-line MS investigation found that the trace water addition in the system accelerated the adsorption of CO 2 on support and promoted methane dissociation, the H 2 signal appears later than CO, indicating the oxidation reaction of CHx occurs after the dissociation of CO 2 . Besides, TG analysis tells us the H 2 O may consume Cα on the catalyst in time during the reaction process to remove carbon deposition.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2018
·Vol. 2018
·期 8
·1047-1052
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IF 2.507
Xiaoxia Jia,Ning Yuan,Li Wang,Jiangfeng Yang,Jinping Li
Graphical Both high selectivity and adsorption capacity in the adsorptive separation of CO 2 , CH 4 , and N 2 were achieved by means of (CH 3 ) 2 NH functionalization of the unsaturated metal sites of the MOF Ni-HKUST-1. Ni-HKUST-1, with the same topological structure as Cu-BTC (HKUST-1), was synthesized by a (CH 3 ) 2 NH-assisted method. Ni-HKUST-1 with high purity (> 90 %), yield (85 %), and BET surface area (1088 m 2 /g) was successfully synthesized for the first time by using NiCl 2 . The pure-component adsorption isotherms of CO 2 , CH 4 , and N 2 on Ni-HKUST-1 were measured by the volumetric method and the data used to estimate the separation selectivity for CO 2 /CH 4 , CH 4 /N 2 , and CO 2 /N 2 binary mixtures according to the ideal adsorbed solutions theory. At 273 K and 1 atm, the selectivities for CO 2 /CH 4 , CH 4 /N 2 , and CO 2 /N 2 were 14.49, 5.36, and 183.41, respectively, and the adsorption capacities for CO 2 and CH 4 were 223.87 and 67.89 cm 3 /g, respectively. This is a rare demonstration of both high selectivity and adsorption capacity in the separation of CO 2 , CH 4 , and N 2 .
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
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2023
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IF 3.7
Jiuhu Zhao,Huiying Li,Yungang Wang,Rongshu Zhu,Senlin Sun,Jingwen Zhang,Chaolin Li,Mei Hong
Mesoporous In/Hβ-X series catalysts were prepared by desilication method with tetrapropylammonium hydroxide (TPAOH) and indium incorporation for selective catalytic reduction of NO with methane (CH 4 -SCR). The post desilication treatment conditions for preparing In/Hβ-X were optimized. Etching time is the most important desilication parameter influencing the resulting CH 4 -SCR performance of the catalyst. The In/Hβ-3 sample which was etched for 3 h presents the highest NO x conversion, 22% higher than In/H-Beta counterparts using commercial microporous beta. Obvious analysis reveals that besides generating mesopores, controlled desilication can modulate the proportion of InO + active sites and surface oxygen species, allowing more active sites to be exposed.
研究领域:
催化
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环境科学
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2024
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IF 5.6
Xueyu Zan,Shiqi Tao,Chaoyu Zhang,Yixiao Wu,Yongjun Liu,Wei Huang
Direct conversion of methane and carbon dioxide into acetic acid is a dream way to address the two greenhouse gases, but is challenged by their chemical inertness. Cu and Pd are promising candidates both in CH 4 and CO 2 activation as well as the subsequent C-C coupling reactions at low temperature. Herein, we report that acetic acid can be produced by the direct coupling of CH 4 and CO 2 in the presence of H 2 O 2 over Cu-Pd/Al 2 O 3 catalysts at 50 °C. Results show that the acetic acid yield reaches 48.1 μmol·g cat −1 ·h −1 on the optimized reaction condition over Cu 3.8 -Pd 1.6 /Al 2 O 3 catalyst, which is higher than that of either mono-Cu or mono-Pd catalyst. Extensive characterization indicates the higher activity of Cu 3.8 -Pd 1.6 /Al 2 O 3 catalyst is attributed to the strong synergistic effect between Cu and Pd, which results in the formation of CuPdO 2 phase, and thus promoting the electron transfer from Cu to Pd. DRIFTS experiments reveal that acetic acid is produced by the coupling of CH 3 * and COOH* over CuPdO 2 active sites via Langmuir-Hinshelwood mechanism, where CH 3 * is originated from CH 4 dehydrogenation step, and COOH* may formed by the activation of CO 2 by H 2 O 2 . This study provides a new approach for the co-conversion of CH 4 and CO 2 into acetic acid at low temperature.
研究领域:
化学工程
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催化
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环境科学
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产品关联
DOI
高影响因子
Journal of Natural Gas Science and Engineering
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2018
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IF 2.803
Tengyang Zhu,Xing Yang,Yi Zhang,Yayun Zheng,Xiaoqi He,Jujie Luo
Air pollution gradually aggravated, which accelerates the demand of clean energy (in particular clean natural gas) because of its abundant storage worldwide. However, raw natural gas commonly contains impurity gases, such as CO 2 and N 2 , which reduce the heat of its combustion. Here, we reported new polyamide-poly(propylefne glycol) (PA-PPG) random and block copolymer materials with excellent CO 2 /CH 4 separation performance. These copolymers were characterised by Fourier-transform infrared spectroscopy (FTIR), nuclear magnetic resonance spectroscopy ( 1 H NMR), UV–vis absorption spectrum and X-ray diffraction (XRD). The gas permeation properties of these copolymers were investigated by using five single gases (CO 2 , H 2 , O 2 , CH 4 and N 2 ) at different temperatures (298–328 K) and a feed pressure of 76 cmHg. The effects of chemical structure, PPG content and operating temperature on the gas permeation properties of these copolymers were also further discussed. Results showed that PA-PPG random copolymer membranes exhibited better gas permeation properties than those of PA-PPG block copolymer membranes. PA-PPG random copolymer membrane with 20 wt% PPG exhibited the highest selectivity (CO 2 /CH 4 = 37.31 and H 2 /CH 4 = 33.44) at 298 K and 76 cmHg. The CO 2 and H 2 permeability values were 5.97 Barrer and 5.19 Barrer, respectively.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Li Yin,Meiling Li,Hailun Xia,Shanshan Mao,Fangyuan Gai,Hao Wang
The gas separation performance of hybrid carbon molecular sieve membranes is critically influenced by the particle size of the fillers. Herein, ZIF-8 crystals of different sizes (≈50 nm, ≈500 nm, and ≈1 µm) are used as fillers to synthesize a series of ZIF-8-derived-carbon hybrid carbon molecular sieve membranes with high filler loading. As the ZIF-8 crystal size increases from nanoscale to microscale, the CO 2 permeability of the resulting hybrid carbon molecular sieve membrane for a CO 2 /CH 4 binary mixture increases, reaching 9965 Barrer with a selectivity of 28.05. This trend highlights a clear correlation between filler size and gas separation performance of the hybrid carbon molecular sieve membranes. Microscale ZIF-8-derived-carbon offers synergistic advantages by providing abundant hierarchical pores for molecular sieving and continuous, long pathways for efficient gas transport, while preventing particle aggregation under high loading. Our finding provides valuable insights for the further development of high-performance hybrid carbon molecular sieve membranes.
研究领域:
材料科学
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膜分离技术
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化学工程
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气体分离
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纳米材料
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多孔材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xing Yuan,Lingquan Meng,Chaohe Zheng,Haibo Zhao
Perovskites have been recognized as affordable substitutes for noble-metal catalysts for their tunable catalytic activity and thermal stability. Nevertheless, the highly demanding synthesis procedure still hinders the application of perovskites in catalytic combustion. In this work, a series of nanostructured SiTiO3 perovskites with B-site partial substitution by Co, Fe, Mn, Ni, and Cu are synthesized via flame spray pyrolysis in one step. The comprehensive characterizations on textural properties of nanostructured perovskites reveal that the flame-made perovskite nanoparticles all exhibit high crystal purity and large specific surface area (∼40 m2/g). Furthermore, the highest catalytic activity is achieved by SrTi0.5Co0.5O3 due to the formation of favorable oxygen vacancies, outstanding reducibility, and oxygen desorption capability. Additionally, the presence of 10 vol % water vapor during long-term testing indicates remarkable durability and water resistance. Finally, the CO oxidation and CH4 dehydrogenation on SrTiO3 incorporating Co atoms are more thermodynamically and kinetically favorable than those on other doped surfaces.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemical Engineering Journal Advances
·
2020
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IF 0
Jiuhu Zhao,Zhengzhong Wen,Rongshu Zhu,Zhi Li,Ran Ding,Yongji Zhu,Tingkun Gu,Rong Yang,Zhenye Zhu
In this paper, In-metal oxide/H-Beta catalysts were synthesized by ion exchange method and In-Co 3 O 4 /H-Beta exhibited the highest catalytic activity for the selective catalytic reduction of NO x with CH 4 in presence of H 2 O and SO 2 . Thus, the synthesis conditions of In-Co 3 O 4 /H-Beta were optimized. The results showed that In-Co 3 O 4 /H-Beta exhibited excellent catalytic performance and high CH 4 selectively when the synthesis was carried out by ion exchange method, the ratio of Si and Al in H-Beta was 25, the ratio of Co 3 O 4 and H-Beta was 5:40, the concentration of ion exchange liquid was 0.033 M and calcination temperature was 500 °C. The NO x removal efficiency was about 87.6 % and N 2 selectivity could reach 96.3% in the presence of H 2 O and SO 2 . Through a series of characterizations, it was concluded that In-Co 3 O 4 /H-Beta owned stable catalyst structure, abundant Brønsted acid sites and the highest ratio of InO + /In 2 O 3 under the optimal synthesis conditions. In addition, the doped of Co 3 O 4 could inhibit the adsorption of sulfate species on the surface of In/H-Beta catalyst, leading to the excellent H 2 O and SO 2 resistance property.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
REACTIVE & FUNCTIONAL POLYMERS
·
2018
·
IF 2.975
Xing Yang,Tengyang Zhu,Zongxiang Xu,Haiquan Shan,Jujie Luo
Poly(styrene-b-butadiene-b-styrene) triblock co polymer (SBS) crosslinked membranes containing poly(dimethylsiloxane- co -methylhydrosiloxane) (PDMS- co -PMHS) were prepared by hydrosilylation reaction toward CH 4 /N 2 separation. The effect of an additive amount of PDMS- co -PMHS on the structure, morphology, and thermodynamic stability of crosslinked membranes were investigated by using FT-IR, SEM and TGA . Soxhlet extraction experiments were also performed to explore the crosslinking degree of membranes. In this work, the single-gas permeability of CH 4 and N 2 was measured using the constant volume–variable pressure method. Our experimental results showed that crosslinked membranes can significantly enhance CH 4 permeability with increasing PDMS- co -PMHS content, whereas the CH 4 /N 2 selectivity remains unchanged. Among these crosslinked membranes, the SBS-c-PDMS- co -PMHS-70 membrane exhibited optimal CH 4 permeability at room temperature and the pressure of 1 bar. Specifically, the CH 4 permeability was > 10-folds higher than that of the SBS membranes (37.6 barrer versus 443.6 barrer). Moreover, investigation of the effect of test temperature on the gas permeation of crosslinked membranes revealed a preferable CH 4 permeability at 55 °C and 1 bar, at which the CH 4 permeability reaches 679.2 barrer without a substantial compromise in selectivity.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）