CHINESE CHEMICAL LETTERS
·
2014
·
IF 1.178
Wei Wang,Ye Yuan,Fu-Xing Sun,Guang-Shan Zhu
Novel porous aromatic frameworks (PAF-53 and PAF-54) have been obtained by the polymerization of amino compound ( p -phenylenediamine and melamine) and cyanuric chloride. They display a certain amount of CO 2 adsorption capacity and highly selective separation of CO 2 /CH 4 and CO 2 /N 2 as 18.1 and 83 by Henry Law respectively. They may be applied as ideal adsorbents to separate and capture CO 2 .
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 7
·2957-2963
·
IF 3.5
Peng Zhang,Sai Ma,Yujuan Zhang,Chaohui He,Tuoping Hu
The energy-saving separation of CO2/N2 and CH4/N2 in the energy industry facilitates the reduction of greenhouse gas emissions and replenishes energy resources, but is a challenging separation process. The trade-off between adsorption capacity and selectivity of the adsorbents is one of the key bottlenecks in adsorption separation technologies’ large-scale application in the above separation task. Herein, we introduced a series of fluoroborate or fluorosilicate salts (Cu(BF4)2, Zn(BF4)2 and ZnSiF6) into the open coordination nitrogen sites of aluminum-based metal–organic frameworks (MOF-253) to create multiple binding sites to simultaneously enhance the adsorption capacity and selectivity for the target gas. By the synergistic adsorption effect of metal ions (Cu2+ or Zn2+) and fluorinated anions (BF4− or (SiF6)2−), the single-component adsorption capacity and selectivity of salt-modified MOF-253 (MOF-253@Cu(BF4)2, MOF-253@Zn(BF4)2 and MOF-253@ZnSiF6) for CO2 and CH4 were effectively improved when compared to pristine MOF-253 at 298 K and 1 bar. In addition, the salt-modified MOF-253 has a moderate adsorption heat (<30 kJ mol−1) which could be rapidly regenerated at low energy by evacuation desorption. As confirmed by the ambient breakthrough experiments of MOF-253 and MOF-253@ZnSiF6, the real separation performance for both CO2/N2 (1/4) and CH4/N2 (1/4) was obviously improved. This work provides a feasible post-modification strategy on uncoordinated sites of the framework to improve adsorption separation performance and promote the development of ideal adsorbents with a view to realizing their application in the energy industry.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Hailong Tang,Yongqing Ma,Ganhong Zheng,Chuhong Zhu,Meiling Wang,Yilin Lu,Xiao Sun
Photocatalytic CH 4 conversion to CH 3 OH under mild conditions is undoubtedly an efficient strategy to realize CH 4 upgrading. In this work, in-situ formed highly reactive Fe IV =O complex with a bound Cl axial ligand was detected at ambient temperature and its contribution to CH 4 photoxidation to CH 3 OH was deeply investigated. Under optimized experimental condition, a high CH 3 OH yield of 3026.1 mmol mol Fe −1 (6.76 mmol g cat −1 h −1 ) with selectivity of 73.6 % was obtained during 8 h. Isotope labeling mass spectroscopy experiments manifested that O 2 was the only source of oxygen in products. The formation of Cl-(H 2 O) 4 Fe IV O complex was confirmed using low-temperature electron spin resonance spectroscopy and cryogenic Raman spectroscopy (ν(Fe O) = 828 cm −1 ). Through density functional theory (DFT) calculation, we showed that the Cl axial ligand acts as an “electron reservoir” during CH 4 conversion, i.e., electron acceptor during the process of CH 4 oxidation to CH 3 OH, while electron donor in CH 3 OH desorption. This not only lowered C-H cleavage energy, but also facilitated CH 3 OH desoption and inhibited overoxidation. As far as we know, Cl-(H 2 O) 4 Fe IV O is the first detected Fe IV O complex generated directly from O 2 and Fe 3+ at ambient temperature.
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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.
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ENERGY & FUELS
·
2025
·
IF 5.3
Zhuo Chen,Ze Zhang,Rongxin Xia,Junhu Zhou,Jun Cheng
To improve the conversion rate of carbon dioxide (CO2) to methane (CH4) in a microbial electrochemical system (MES), the zeolitic imidazolate framework ZIF-67(Co) with electron storage properties was first grown in situ on MIL-100(Fe) with excellent CO2 adsorption properties by a hydrothermal method. The obtained binary core–shell MIL@ZIF material was then adsorbed by carbon felt on a cathode to grow biofilms composed of electroactive microorganisms for characterization and testing in an MES. This system exhibited a CH4 production rate of 0.42 mmol LR–1 d–1, along with an impressive faradaic efficiency of 96.4%. Three-dimensional excitation–emission matrix spectra of extracellular polymeric substances indicated that those containing higher contents of humic acid shifted electron pairs and converted redox states to facilitate electron transfer. MIL@ZIF enriched hydrogenotrophic methanogens and electrogenic bacteria in microbial communities with enhanced gene expression of electrically conductive pili and cytochrome C to strengthen interspecies electron transfer. MIL@ZIF enhanced CO2 adsorption and electron storage, reinforcing electron transfer chains and boosting CH4 yield by a factor of 10.7.
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Nano Research
·
2024
·
IF 9.5
Li Jing,Jing Chuanyong,Wang Jin
Electrocatalytic CO 2 reduction to CH 4 remains challenging due to multi-electron transfer and intermediates adsorption. Herein, we synthesized electrocatalysts by growing Ni-Cu alloy structure on nitrogen-doped carbon nanotubes (Ni x Cu y -NCNT) for electrocatalytic CO 2 reduction reaction (CO 2 RR) via hydrothermal method followed by pyrolysis. The optimized Ni 1 Cu 1 -NCNT demonstrated a superior CO 2 RR performance, achieving 99.7% \(\text{FE}_{\text{CH}_{4}}\) (FE = Faradaic efficiency) and 11.54 mA • cm −2 current density at −1.2 V vs. reversible hydrogen electrode (RHE), which outperformed single metal counterparts. Its outstanding performance was due to the electrons transferred from Cu to Ni and Ni-Cu alloy shifted the d-band center toward the Fermi level, which was more conducive to the intermediate formation. In situ electrochemical attenuated total reflection (EC-ATR) and density functional theory (DFT) calculations revealed the appearance of *CHO intermediate and the pathway during the CO 2 RR process. The design of the bimetallic electrocatalyst in this study provides a new perspective for the highly selective reduction of CO 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ning Liu,Na Lu,Kun Zhao,Pengxiao Liu,ZhuMei Sun,Jing Lu
The conversion of methane (CH 4 ) and carbon dioxide (CO 2 ) into high-value products under mild conditions is crucial for addressing the greenhouse effect and advancing C1 chemistry. In this study, Cu/ZnO catalysts were prepared through a one-step wet reduction process, and the catalytic conversion of CH 4 and CO 2 into acetic acid molecules (CH 3 COOH) was achieved via photon activation at ambient temperature. The yield of acetic acid was 411.6 μmol/Lg cat −1 h −1 with a selectivity of 89.5 % under optimal conditions (100 mWcm −2 light intensity, 25 ± 2 °C, 2 MPa pressure, and a 1:1 CH 4 :CO 2 volume ratio). Enhanced solubility of CH 4 in aqueous under increased pressure and temperature was observed to improve acetic acid production. Additionally, the catalytic mechanism involved surface chemisorption of CH 4 and CO 2 , facilitated by ZnO and Cu in the catalyst, leading to C-C coupling and subsequent acetic acid formation, driven by photogenerated electron-hole migration. This study provides a foundational understanding for the synthesis of value-added chemicals through CH 4 and CO 2 conversion via C-C coupling in mild environments.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shengjun Du,Minglong Guo,Guangxing Yang,Qiao Zhang,Zhiting Liu,Feng Peng
The highly-efficient separation of CH 4 /N 2 mixture on carbon materials is significantly hindered by the inherent trade-off that exists between CH 4 adsorption capacity and CH 4 /N 2 separation selectivity. Herein, we have constructed a type of novel carbon materials (PGC- x ) with well-controlled ultramicropores ranging from 0.48 to 0.57 nm for CH 4 /N 2 separation. The Zn-based salt template was in-situ confined into the polymer framework during the co-assembly of phloroglucinol and glyoxylic acid. The subsequent evaporation of Zn at high temperature gives rise to the adjustable ultramicropore structure, effectively devoid of mesopores and macropores. Benefiting from the optimal pore size of 0.50 nm, PGC-1 demonstrated high CH 4 uptake of up to 1.50 mmol/g. Meanwhile, the CH 4 /N 2 (15/85 and 85/15, v/v) separation selectivity of PGC-1 at 298 K and 1.0 bar reached 5.8 and 6.0, respectively. Dynamic breakthrough experiments proved that PGC-1 could be used as efficient adsorbent for capturing low or high concentration of CH 4 from N 2 . This work offers a promising design principle for optimizing porous structure of carbon materials, with the aim of minimizing the selectivity-capacity trade-off that often arises in the separation of diverse gas pairs.
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ENERGY & FUELS
·
2025
·
IF 5.3
Dekang Li,Zhixian Bao,Lijun Jin,Haoquan Hu
Dry reforming of methane (DRM) can spontaneously use CO2 and CH4 to produce syngas, but minimal sulfur impurities in the feed gas can poison and deactivate the catalyst. Although the Ni/Al2O3 catalyst has excellent DRM activity, it is challenging to regenerate due to sulfation of the support. Besides that, the loading of sacrificial promoters used to improve sulfur resistance, such as Cu, may impact the DRM performance of active sites. Here, a spatial separation strategy was proposed to precisely design a sulfur-resistant catalyst, dividing the catalyst into a DRM zone and a H2S adsorption zone. The Ni@SiO2@NiCu catalyst prepared by this strategy shows stable DRM performance and significantly improved sulfur resistance and can be regenerated repeatedly. The Ni@SiO2@NiCu catalyst has the best sulfur resistance, 6.8 times that of the spatially adjacent NiCu@SiO2 catalyst and 1.4 times that of the Ni@SiO2@Cu catalyst. This spatial separation strategy introduces a novel concept for the controllable synthesis of sulfur-resistant catalysts and may inspire further applications in the design and development of such catalysts.
研究领域:
催化化学
·
化学工程
·
材料科学
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环境科学
·
能源技术
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Wei Liu,Bo Wang,Haifeng Dong,Mengyu Ren,Zongxu Wang,Dan Li,Yi Nie,Xiangping Zhang
Efficient CO₂/CH₄ separation is crucial for the value-added utilization of natural gas, shale gas, and biomethane. This work developed a series of tetramethylammonium-based ionic liquids (ILs) containing ethylene glycol (EG) as high-performance absorbents. Among them, the [N₁₁₁₁][1,2,4-Tz]/EG (1:1) system exhibited a high CO₂ capacity of 0.205 g/g at 40 °C and 100 kPa, together with exceptional CO₂/CH₄ selectivity (574). The separation performance was finely tuned by varying the EG content, which regulated the hydrogen-bond network within the hybrid system, leading to a remarkably low regeneration energy of 1.13 GJ·t −1 CO₂, superior to conventional ILs and amine solvents. Mechanistic studies unveiled that the hydrogen bonds between EG and IL anions not only promoted CO₂ activation but also directed the reaction pathway toward the formation of thermodynamically stable carbonate species (RCO₃ − ) rather than carbamates, thus facilitating the low-energy regeneration process. This study demonstrates that hydrogen bond modulation in EG-IL systems provides a sustainable and efficient strategy for CO₂ capture.
研究领域:
化学工程
·
环境科学
·
分离技术
·
可持续能源
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Small
·
2025
·
IF 12.1
Yuxing Luo,Yehui Ding,Xin Zhu,Meng He,Weiqun Shi,Xiangdong Ding,Xue Liu
2D coordination polymer membranes, characterized by ultrathin thickness and nanoscale porosity, exhibit exceptional selectivity and permeability for molecular separations. While amorphous coordination polymer (aCP) monolayers are particularly attractive for scalable fabrication, as their separation performance is less dependent on crystallinity, aCP monolayers have never been synthesized and their gas separation capabilities have been completely unexplored. Herein, we report an amphiphilic polyaromatic hydrocarbon (PAH) assisted interfacial assembly strategy to fabricate nanometer thick aCP monolayer. An amphiphilic hexa(terpyridine)hexaphenylbenzene (HTPHPB) monolayer is first formed at the air/water interface, which adsorbed pyrazine and coordinated with Co 2 ⁺ to generate an active layer, subsequently inducing the interfacial co-assembly of water-soluble pyrazine and tetracyanonickelate into continuous aCP films with a thickness of 2.2 nm. Remarkably, the six layer stacking aCP membranes exhibit unprecedented He/CH 4 separation performance with a He permeance of 136.6 GPU and a He/CH 4 separation factor of 110, representing a nearly threefold improvement in separation factor over the best-performing MOF materials reported to date. Furthermore, the membrane maintains its separation efficiency without significant performance loss under 50 times bending, demonstrating excellent structure stability. This work not only establishes a facile strategy for synthesizing aCP monolayers but also opens new avenues for designing high-performance gas separation membranes.
研究领域:
材料科学
·
膜技术
·
气体分离
·
配位聚合物
·
纳米材料
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yongliang Xu,Lei Xiang,Lanyun Wang,Zecheng lv,Yao Li,Hao Shao,Haidong Chen,Kun Zhang,Xiaodong Feng
Hydrate-based hydrogen storage technology enables the solid-state stabilization of hydrogen by encapsulating H 2 molecules within a clathrate lattice structure, representing a promising strategy for industrial-scale gas storage. This study focuses on enhancing the gas storage performance and stability of H 2 –CH 4 binary hydrate. Experiments on the formation and dissociation of H 2 –CH 4 hydrates were conducted under a pressure of 6.0 MPa. The study examines the effects of C 8 F 18 (6 wt%, 8 wt%, 10 wt%) and 1,3-DIOX (4mol%, 5mol%, 6mol%) on H 2 –CH 4 (with a ratio of 1:1) hydrate. The results indicate that in the composite systems containing 5mol%, 1,3-DIOX and 8 wt% C 8 F 18 , a synergistic promotion effect was observed. The nucleation temperature was further increased by 3.8 K compared to the single 1,3-DIOX system. The induction time was shortened by 146.9 min. Gas consumption improved to 0.14446 mol. Furthermore, In 4mol%1,3-DIOX and 6 wt% C 8 F 18 compound system prolonged the pre-dissociation 48.33min relative to the 1,3-DIOX system. C 8 F 18 enhances the self-preservation of the hydrate, an effect that is not present with only 1,3-DIOX. This effect becomes more pronounced as the concentration of C 8 F 18 increases. Generally, the 1,3-DIOX + C 8 F 18 can play a synergistic effect on enhancing the gas storage performance and stability of hydrates.
研究领域:
物理化学
·
能源材料
·
气体储存
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水合物化学
·
工业催化
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