Separations
·
2025
·Vol. 12
·期 2
·42
·
IF 2.7
Huihui Wang,Yuqiong Zhao,He Lian,Qi Wang,Zhihong Shang,Guojie Zhang
The separation of CH4and N2is essential for the effective use of low-concentration coalbed methane (CBM). In this study, a series of nitrogen-doped porous carbons were synthesized using an in situ nitrogen doping method combined with K2CO3activation. The study systematically examined how changes in the physical structure and surface properties of the porous carbons affected their CH4/N2separation performance. The results revealed that in situ nitrogen doping not only effectively adjusts the pore structure and alters the reaction of K2CO3on the carbon matrix, but also introduces nitrogen and oxygen functional groups that significantly enhance the adsorption capabilities of the materials. In particular, sample S3Y6−800 demonstrated the highest methane adsorption capacity of 2.23 mmol/g at 273 K and 1 bar, outperforming most other porous carbons. This exceptional performance is attributed to the introduction of N-5, N-6, C-O, and COOH functional groups, as well as a narrower pore-size distribution (0.5–0.7 nm) and the formation of carbon nanotube structures. The introduction of heteroatoms also provides additional adsorption sites for the porous carbon, thus improving its methane adsorption capacity. Furthermore, dynamic breakthrough experiments confirmed that all samples effectively separated methane and nitrogen. The Toth model accurately described the CH4adsorption behavior on S3Y6−800 at 298 K, suggesting that the adsorption process follows a sub-monolayer coverage mechanism within the microporous regions. This study provides a mild and environmentally friendly preparation method of porous carbons for CH4/N2separation.
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
JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY
·
2019
·Vol. 30
·期 9
·1789-1800
·
IF 1.335
Zhang Guojie,Hou Peng,Sun Yinghui,Xu Ying,Cheng Haizhu,Zhang Yongfa
Different activated carbons and manganese-modified activated carbons were prepared as deoxidizers for the low-concentration coalbed methane deoxidation. The results show that the deoxidation performance of the different activated carbons is affected by raw materials for preparation of deoxidizers. One type of activated carbon exhibited the best performance of oxygen removal, due to the relatively low ash content and better adsorption performance. Experimental results show that the manganese-modified deoxidizers exhibit an excellent deoxidation efficiency at low temperature. At 200 ºC, one kind of manganese-modified activated carbons decreased the oxygen content to less than 1 vol%, which could maintain about 600 min. This indicated that the addition of manganese greatly improved the reactivity of oxygen with activated carbon. Characterization results demonstrated that the physical structure and species types of oxygen of activated carbons, and manganese have important effects on the activity of deoxidizers in different temperature ranges.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Zhijie Zhou,Yanting Gao,Wei Xia,Wenbo Shi,Yizhou Liu,Fang Zheng,Zhiguo Zhang,Qiwei Yang,Qilong Ren,Zongbi Bao
The development of advanced adsorbents for methane (CH4) and nitrogen (N2) separation is critical for the efficient utilization of coal-bed methane (CBM), which is a key alternative energy resource. Herein, we report a bimetallic copper–indium-based metal–organic framework (MOF), CuIn(3-ain)4, featuring high-density nitrogen and oxygen sites distributed along its pore surface. These negatively charged atom sites, derived from CuN4 and InO8 clusters, form multiple hydrogen-bonding interactions with CH4, significantly enhancing its adsorption affinity. CuIn(3-ain)4 demonstrates a high CH4 uptake of 1.56 mmol g–1 and excellent CH4/N2 selectivity under ambient conditions, outperforming many reported materials. Dynamic breakthrough experiments confirm that over 90% purity methane can be obtained in a single adsorption–desorption cycle. Grand Canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations reveal that the nitrogen and oxygen sites play a crucial role in selectively recognizing CH4 over N2, leading to a superior separation efficiency. Moreover, the material exhibits excellent cyclic stability and scalability, making CuIn(3-ain)4 a promising candidate for practical CH4/N2 separation in CBM purification. This study provides valuable insights into the design of MOFs for challenging gas separations, emphasizing the role of polar sites in facilitating selective adsorption.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY CONVERSION AND MANAGEMENT
·
2021
·
IF 9.709
Juan Yang,Pengyu Chen,Jun Dai,Yumei Chen,Liqing Rong,Dazhao Wang
Sunlight-driven photocatalysis is regarded as a promising strategy for direct conversion of methane in low concentration coal mine methane (LC-CMM) to value-added methanol, yet remains a grand challenge to efficiently activate and convert methane. Herein, WO 3−x nanosheets with gradient concentration of oxygen vacancy were synthesized and firstly served as full-spectrum responsive catalysts for transformation of LC-CMM to methanol at ambient conditions. Defect-rich WO 3−x -N2.0 shows a methanol yield of 1475 μmol·g −1 , roughly 4.5 times higher than WO 3 -A2.0 under simulated solar light irradiation. The selectivity of CH 3 OH on the optimal WO 3−x -N2.0 is up to 76%. More importantly, WO 3−x -N2.0 exhibits a methanol yield of 396 μmol·g −1 with the selectivity of 82% even under near infrared light irradiation while almost no CH 3 OH is detected over WO 3 -A2.0. Based on the results of energy-band structure, photoelectrochemical characterization, PLs and EPR tests, the significantly enhanced photocatalytic performance over WO 3−x -N2.0 is ascribed to the synergistic effect caused by the formation of oxygen vacancies, including extending light absorption into NIR region, improving separation of photoinduced electron-hole pairs and boosting production of hydroxyl radicals (key active species that drive CH 3 OH production). This work will offer a sustainable pathway to broaden the utilization of LC-CMM via efficient coupling of solar energy.
研究领域:
化学工程
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能源科学
·
环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Hua Shang,Honghao Bai,Xiaomin Li,Jinping Li,Jiangfeng Yang
Coalbed methane (CBM) emissions account for a large part of methane (CH 4 ) emission in the fossil energy area, and vacuum pressure swing adsorption (VPSA) is an effective method to recover low-concentration CBM. However, CBM supply can fluctuate in quality or quantity because of the constantly changing geological conditions, thus permanent large-scale factory mode is economically inappropriate. In this work, a highly integrated mobile skid-mounted prototype VPSA system was designed and installed, and site trials of low-concentration CH 4 capture were, for the first time, carried out in a coal mine site of Huayang New Material Technology Group Co. Ltd in China. Site trials including breakthrough tests and VPSA experiments were conducted in a fluctuating range of CH 4 (16–30%). The effects of flow rate, adsorption pressure, and feed concentration on the separation process were revealed using a breakthrough process, and their effects on the dynamic parameters were also analyzed. After purification, the CH 4 content in product gas was increased from 16–30% to 43.3–70.7% which all meet the requirements of 4T grade city gas in China, and maximum CH 4 productivity of 43.6 × 10 −3 m 3 /(kg·h) can be achieved. More importantly, multicycle breakthrough tests demonstrated that superhydrophobic zeolite TUTJ-1 is more resistant to the effects of water and has more potential for capturing CH 4 under humid conditions than activated carbon.
研究领域:
能源工程
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环境科学
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Zaizheng Jiang,Zhiliang Tu,Zhihe Xin,Guodong Zhang,Fei Wang,Yongtao Zhang
Low-concentration coalbed methane (LCCBM) is an abundant unconventional natural gas resource, but the utilization efficiency of methane (CH4) is very low. Sodium dodecyl sulfate (SDS) enhances hydration for CH4 recovery but generates foams during hydrate dissociation, limiting continuous production. To address this issue, the –SO3– group was fixed on the polystyrene nanopolymers (named –SO3–@PSNS) for enhancing hydration to recover CH4 from 21.59 mol % CH4/78.41 mol % N2 in this work. The optimal CH4 recovery effect was obtained when SDS concentration was 4 mmol/L and –SO3–@PSNS concentration was 8 mmol/L. Due to the foams generated by the addition of SDS during the hydrate decomposition, THF in the system decreased from 1 mol % to 0.37 mol % after the reaction but only decreased to 0.96 mol % when –SO3–@PSNS was added. –SO3–@PSNS has important prospects for the application of hydrate-based CH4 recovery from LCCBM.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2018
·
IF 3.024
Yong Jiao,Liyang Wang,Liqin Zhang,Wenting An,Wei Wang,Wei Zhou,Moses O. Tadé,Zongping Shao,Jianping Bai,Si-Dian Li
This paper studies the electrochemical feasibility of the direct conversion of low-concentration, oxygen-bearing coal-bed methane (CBM, 30 vol % CH4) to electricity via solid oxide fuel cells (SOFCs). A fuel cell with the LiLaNi–Al2O3/Cu catalyst layer was developed, and a maximum power output of ∼1068 mW cm–2 was achieved at 850 °C using 30 vol % CBM fuel, which is only modestly lower than that from a cell based on hydrogen fuel. The stability test showed that the cell operation was quite stable during the 120-h test period, which is ∼40-fold longer than that of the cell without catalyst layer. The partial oxidation of methane (POM) occurring in the anode may play an important role when using 30 vol % CBM fuel, which not only supplies highly active gaseous fuels (H2 and CO) but also suppresses the carbon deposition on the anode. By modifying the anode with a LiLaNi–Al2O3/Cu catalyst layer, the POM of 30 vol % CBM was further promoted and the carbon deposition over the anode was mitigated more efficiently. Therefore, the strategy of direct conversion of low-concentration, oxygen-bearing CBM via the SOFCs with an anode catalyst layer may pave an alternative way to utilize this abundant resource efficiently and cleanly.
研究领域:
能源科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhiwei Zhao,Yuan Li,Yanjie Wang,Yating Wang,Yuhao Tang,Mengyue Lu,Xu Yang,Xiaoqing Wang,Feifei Zhang,Jinping Li,Jiangfeng Yang
The enrichment of low-concentration coal-bed methane is beneficial to solving the world’s energy concerns. However, most adsorbents used for CH 4 /N 2 separation from coal-bed methane are hydrophilic and ineffective under humid conditions. In this study, a hydrophobic nickel-based metal–organic framework (TUTQ-1Ni) was developed for efficient CH 4 /N 2 separation under humid conditions. Adsorption results show that, at 298 K and 1 bar, TUTQ-1Ni exhibits the highest CH 4 /N 2 selectivity (11.0) among the reported hydrophobic CH 4 -selective metal–organic frameworks. The results of theoretical calculations reveal that multiple O/S sites provide strong adsorption affinity for CH 4 over N 2 . Further, breakthrough experiments confirm the suitability of the material for CH 4 /N 2 separation, with the separation performance being maintained at even a high relative humidity of 100 %. The pressure swing adsorption simulation results indicate that TUTQ-1Ni is a potential candidate material for the selective capture of methane from coal-bed methane.
研究领域:
材料科学
·
能源化学
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产品关联
DOI
高影响因子
AICHE JOURNAL
·
2021
·Vol. 67
·期 9
·e17281
·
IF 3.993
Ze Dong,Bei Li,Hua Shang,Peixin Zhang,Shixia Chen,Jiangfeng Yang,Zheling Zeng,Jun Wang,Shuguang Deng
The adsorptive separation of CH 4 from low-grade coal-bed gas can be performed at decentralized and remote coal mines, and it uses more energy- and is cost-efficient than the traditional cryogenic distillation process. Herein, we present a facile method to prepare ultramicroporous carbon granules with a narrow pore-size distribution at 0.5–0.6 nm. To our knowledge, such centered and uniform pore-size distribution in carbon granules has never been reported. The carbon granules can be directly utilized in adsorption columns without a granulation or pelletization process. The granular oil-tea-shell-derived porous carbon (GOC-2) exhibited a record-high CH 4 uptake of 1.82 mmol/g and CH 4 /N 2 selectivity of 5.8 at 1.0 bar and 298 K among carbon granules. The excellent CH 4 /N 2 separation performances were confirmed from the results of dynamic breakthrough experiments and pressure swing adsorption simulations. This work provides a novel strategy for developing ultramicroporous carbon granules and guides the future design of efficient CH 4 /N 2 separation adsorbents.
研究领域:
材料科学
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Yishuang Wang,Baolong Qin,Mingqiang Chen,Defang Liang,Zhiheng Lu,Hairan Wang,Chang Li,Gang Yuan,Jun Wang,Liang Yuan
Direct catalytic oxidation (DCO) of coalbed methane to methanol has been considered as a significant technology for highly efficient and clean utilization of coal resources. Herein, the Cu-based spherical micromesoporous material (Cu/SMMM) was successfully prepared by using a sepiolite-derived silica source, and the DCO of methane to methanol was achieved under a low-temperature gas-phase system. Under the optimal reaction conditions, the Cu/SMMM accomplished the maximum methanol production of 69.3 μmol/gcat/h and methanol selectivity of 81.2% with full activation at 450 °C in air for 4 h, and the reaction was carried out at 320 °C for 1 h. Various characterizations demonstrated that the unique SMMM promoted the dispersion of copper oxides to form more active copper species and Lewis acidic sites (LAS). The variable-temperature FTIR, XAS, and NO-IR analyses identified that the highly dispersed dimeric copper species such as ([Cu2(μ-O)]2+ or [(Cu2O2)2+]) in Cu/SMMM was the major active species for DCO of methane into methanol. Additionally, combined with in situ FTIR analysis, the catalytic mechanism was revealed, in which the adsorbed methane species could be converted to CH3* species. Subsequently, CH3* species bound to oxygen of the dimeric copper species to form CH3O* species, which was then converted to methanol in the presence of water.
研究领域:
化学工程
·
催化化学
✓ 已验证
DOI
高影响因子
Energies
·
2025
·Vol. 18
·期 18
·4854
·
IF 3.2
Kai Wang,Chenye Guo,Qisen Gong,Gen Li,Xiaoyue Zhuo,Peng Zhuo,Chaoxian Chen
To address the challenges of low permeability, high gas adsorption, and a fragile structure in coalbed methane reservoirs, this study developed a high-strength composite proppant with an activated carbon skeleton via nitric acid pretreatment, silica–alumina sol coating, and calcination. Orthogonal experiments optimized the preparation conditions: 30–40 mesh activated carbon, Si/Al molar ratio of 4:1, calcination at 650 °C for 2 h. The resulting proppant exhibited an excellent performance: a single-particle compressive strength of 55.5 N, porosity of 33.2%, crushing rate of only 2.3% under 50 MPa closure pressure, and permeability 48.5% higher than quartz sand. In simulated acidic coalbed environments (pH 3–5), its acid corrosion rate was <2.8%, and it enhanced methane desorption by 16.2% compared to pure coal. Additionally, the proppant showed a superior transport performance in fracturing fluids, with better distribution uniformity in fractures than ceramsite, and its hydrophobic surface (contact angle 115.32°) improved fracturing fluid flowback efficiency. This proppant integrates high strength, good conductivity, gas desorption promotion, and corrosion resistance, offering a novel material solution for efficient coalbed methane extraction.
研究领域:
能源工程
·
材料科学
·
石油工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 6
·e18079
·
IF 3.7
Feifei Zhang,Hua Shang,Bolun Zhai,Xiaomin Li,Yingying Zhang,Xiaoqing Wang,Jinping Li,Jiangfeng Yang
A robust aluminum-based metal–organic framework (Al-MOF) MIL-120Al with 1D rhombic ultra-microporous was reported. The nonpolar porous walls composed of para-benzene rings with a comparable pore size to the kinetic diameter of methane allow it to exhibit a novel thermodynamic-kinetic synergistic separation of CH 4 /N 2 mixtures. The CH 4 adsorption capacity was as high as 33.7 cm 3 /g (298 K, 1 bar), which is the highest uptake value among the Al-MOFs reported to date. The diffusion rates of CH 4 were faster than N 2 in this structure as confirmed by time-dependent kinetic adsorption profiles. Breakthrough experiments confirm that this MOF can completely separate the CH 4 /N 2 mixture and the separation performance is not affected in the presence of H 2 O. Theoretical calculations reveal that pore centers with more energetically-favorable binding sites for CH 4 than N 2 . The results of pressure swing adsorption (PSA) simulations indicate that MIL-120Al is a potential candidate for selective capture coal-mine methane.
研究领域:
材料科学
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化学工程
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能源技术
✓ 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）