LANGMUIR
·
2025
·
IF 3.9
Yingying Cheng,Yuanye Zhuang,Shiyang Bai,Meng Ge,Jihong Sun,Jingjing Sun,Xufeng Gong
The removal of CO2 from biogas is critically important for environmental protection and energy applications yet remains technically challenging in the chemical industry. In this work, novel composite adsorbents featuring ZIF-8 uniformly dispersed on randomly oriented clinoptilolite lamellae (LCP) were designed and fabricated through a straightforward composite method. The synthesis sequentially incorporated metal precursors into LCP via ion exchange and salt addition and then introduced organic ligands to generate ZIF-8. Comprehensive characterizations, including XRD, FT-IR, N2 adsorption–desorption isotherms, SEM, and TG analyses, confirmed the physicochemical properties and structural features of the composites. The synthesized Zn-LCP/ZIF-8 materials exhibited exceptional CO2/CH4 separation performance, demonstrating ultralow CH4 adsorption capacity (<0.1 mmol/g) coupled with superior CO2/CH4 selectivity (≈28). Complementary molecular simulations using Material Studio software provided mechanistic insights into the adsorption and separation behavior, which further confirmed the superiority of the composite structure in CO2/CH4 separation. These results establish an effective strategy for biogas purification, while offering new perspectives for enhancing the CO2/CH4 adsorption selectivity.
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Zhishuncheng Li,Yongheng Yuan,Guangfei Qu,Keyi Xiang,Ping Ning,Wanyuan Du,Keheng Pan,Yingying Cai,Junyan Li
Catalysts for the generation of methane in electrochemical CO 2 reduction reactions (CO 2 RR) must have suitable adsorption energies for the intermediate products. In this study, we used a one-step electrodeposition method to prepare nitrogen(N) and phosphorus(P)-doped copper(Cu)-based catalysts. The introduction of P to the catalyst resulted in a significant change in the CO 2 RR pathway, leading to efficient and highly selective methane production. The Cu-N 2 -P 2 electrocatalyst exhibits a CH 4 Faradaic efficiency (FE) of 73 % at a potential of −1.6 V vs RHE, and it was found to be more effective in promoting the hydrogenation process of *CHO-*CH 2 O-*CH 3 O, which was confirmed by in-situ IR, X-ray absorption techniques and DFT calculations. P serves as the primary electron donation site in the catalyst, thereby influencing the charge distribution properties of the surrounding Cu atoms. This, in turn, facilitates the regulation of intermediate adsorption, representing the primary factor in the notable enhancement of methane selectivity.
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DOI
高影响因子
Journal of the American Chemical Society
·
2024
·
IF 14.4
Xiaolan Duan,Yang Li,Jiahua Zhao,Mengyuan Zhang,Xiaopeng Wang,Li Zhang,Xiaoxuan Ma,Ying Qu,Pengfei Zhang
The catalytic properties of unary to ternary metal oxides were already well experimentally explored, and the left space seems like only high entropy metal oxides (HEOs, element types ≥5). However, the countless element compositions make the trial-and-error method of discovering HEO catalysts impossible. Herein, based on the study of the crystal phase and catalytic performance of the ACr2Ox catalyst system, the strong correlation between the single spinel phase and good catalytic activity of CH4 oxidation was inferred owing to the similar element importance sequences, which were acquired by the corresponding high accuracy machine learning models (cross-validation score >0.7). Furthermore, searching for negative data and choosing the proper training data resulted in high-quality regression models to search for better catalysts. Finally, the screened irregular catalyst Ni0.04Co0.48Zn0.36V0.12Cr2Ox with outstanding sulfur and moisture resistance and long-term stability (>7000 h, T90 = 345 °C) envisions the potential of applying the machine learning method to discover HEOs for target processes.
研究领域:
材料科学
·
催化
·
化学工程
·
机器学习
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Longkai Pan,Minggang Zhang,Hui Mei,Li Yao,Zhipeng Jin,Hongxia Liu,Shixiang Zhou,Ziyi Yao,Gangqiang Zhu,Laifei Cheng,Litong Zhang
Use of 3D photocatalytic reactor has been widely explored for development of efficient photocatalytic systems. In the present study, a bionic palisade cells BiOBr/Sr 2 Nb 2 O 7 /Al 6 Si 2 O 13 photocatalytic reactor with high strength was prepared through combination of 3D printing technology and solvothermal method. The carefully designed and optimized bionic palisade cell structure exhibited a periodic porous structure with high surface area. The controllable periodic structure effectively regulated the internal photon transfer and mass transfer. Photon transfer ensured that light is fully scattered within the structure, which improved light utilization. High mass transfer ensured smooth flow of reactant inside the structure, which increased reactant adsorption on the surface of photocatalysts. The interface electric field of the BiOBr/Sr 2 Nb 2 O 7 p-n heterojunction effectively separated the photogenerated electrons and holes. The BOB/SNO/ASO structure had high photocatalytic CO 2 reduction performance under the simulated sunlight. The CO yield for the reaction was 13.68 μmol/g/h, whereas that of CH 4 yield was 6.37 μmol/g/h. Therefore, the findings of the present study provide a basis for design and preparation of high-performance 3D photocatalytic reactors.
研究领域:
材料科学
·
环境科学
·
化学工程
·
光催化
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DOI
高影响因子
ChemSusChem
·
2026
·Vol. 19
·期 3
·e202502612
·
IF 5.9
Shiyin Sun,Shuangde Li,Yunfa Chen
Due to lower energy consumption, great separation performance, and simple operation process, membrane technology plays an important role in gas separation. However, separation membranes often face a trade-off between permeance and selectivity. For instance, the pure layered double hydroxide (LDH) or metal organic framework (MOF) membranes exhibit high gas permeance but suffer from low selectivity. However, conventional Pd membranes typically have a thickness exceeding 50 μm, resulting in high costs and limited permeance. This article develops a novel strategy to fabricate a CoAl LDH/zeolitic imidazolate framework (ZIF)-67 heterostructure on a polydopamine-modified substrate, following by the infiltration of Pd nanoparticles (Pd NPs) into the LDH/ZIF framework via magnetron sputtering, resulting in a well-integrated LDH/ZIF@Pd membrane for highly efficient H 2 /CH 4 separation. In this architecture, the LDH sheets not only create nanocorridors for gas permeation but also provide the nucleation sites for ZIF grains. The incorporated Pd NPs and LDH/ZIF network form a well-integrated heterostructure, which endows the LDH/ZIF@Pd hybrid membrane with exceptional comprehensive performance, achieving H 2 /CH 4 selectivity of 48.3 and ultrahigh H 2 permeance of 8.4 10 5 GPU (75°C, 1 bar). This result sets a new benchmark for membrane-based gas separation, demonstrating outstanding potential for advanced hydrogen purification and sustainable energy applications. Graphical A novel layered double hydroxide (LDH)/zeolitic imidazolate framework (ZIF)@Pd hybrid membrane is developed for H 2 /CH 4 separation by constructing LDH/ZIF heterostructure and infiltrating Pd nanoisland, which demonstrates a remarkable combination of excellent H 2 /CH 4 selectivity of 48.3 and ultrahigh H 2 permeance exceeding 8.4 10 5 GPU, achieving an order of magnitude improvement in separation performance, showing great potential for hydrogen purification and sustainable energy applications.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Danhong Gao,Shang Li,Xianjie Xu,Hongwei Liu,Hanling Deng,Qianyao Lu,Dusong Hou,Sheng Huang,Mingzhi Jiao,Xiaowei Li,Xinjian He
Rapid and reliable detection of methane (CH 4 ), a key clean energy source and potent greenhouse gas, is of great importance for industrial safety and environmental protection. In this work, a high-performance CH 4 gas sensor is developed based on hollow ZnO nanobowls decorated with Pd nanoparticles, synthesized via a template-assisted strategy followed by mild impregnation. The hollow nanobowl architecture features a uniform particle size (~350 nm), ordered mesopores (~3.4 nm), and a high specific surface area of 104.06 m 2 g −1 , which effectively enhances gas diffusion and surface reaction kinetics without relying on complex heterojunctions or bimetallic systems. The introduction of Pd increases the oxygen vacancy content from 29.41% to 41.48%, provides additional active sites, and facilitates electron transport. Moreover, Pd catalyzes O 2 dissociation via a spillover effect and lowers the activation energy for C H bond cleavage in CH 4 , while the work function difference between Pd and ZnO induces a Schottky barrier at the interface, dynamically modulating the sensor conductivity. Benefiting from the synergistic effects of morphological regulation and interfacial electronic modulation, the sensor exhibits a high response of 67% to 1000 ppm CH₄ at an operating temperature of 253.5 °C, along with an ultrafast response/recovery time of 2/10.5 s and a wide detection range of 20–10,000 ppm. In addition, the sensor demonstrates good selectivity and excellent long-term stability, with less than 10% signal fluctuation over 30 days. Building upon the reliable concentration discrimination validated by CNN-1D models, an LSTM-based short-term dynamic prediction framework was further introduced to evaluate temporal early-warning performance under rapid methane concentration variations. The results demonstrate that the proposed sensor–algorithm integration can effectively capture dynamic concentration evolution and accurately predict the 5000 ppm alarm threshold across multiple diffusion rates, highlighting its potential for early-warning applications in confined spaces.
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高影响因子
CARBON
·
2025
·
IF 11.6
Mengjie Cao,Shuangde Li,Shikun Wang,Xin Zhou,Guangxin Ma,Yunfa Chen
Catalytic decomposition of CH 4 is expected to yield pure hydrogen and carbon, which is important for reducing greenhouse gas emissions. Nickel-based catalyst are currently the most common catalyst for methane cracking but sintering and carbon accumulation can cause catalyst deactivation. Therefore, stabilizing the particle size of nickel-based catalysts by enhancing the metal-support interaction is crucial for designing methane cracking catalysts. In this study, the effect of added Cr and Cu on the performance of NiAl catalyst was studied. The results indicated that the co-doping of Cu and Cr improved the metal-support interaction and promoted the formation of oxygen vacancies. Cu doped NiAl catalyst increased the Ni–Ni bond length and decreased the coordination of Ni–Ni by alloying with Ni. This effectively stabilized the catalyst size during the CH 4 cracking reaction. It was showed that the smaller the variation in particle size of the catalyst during the reaction, the higher the stability of methane decomposition. The Ni 2.4 Cu 0.3 Cr 0.3 Al catalysts retained 60 % hydrogen yield for up to 630 min at 600 °C. By coupling “hydrogen preparation” and “carbon production”, this paper is expected to open up a new path for the integration of clean energy production and advanced carbon materials manufacturing in a resource-efficient and environmentally friendly way.
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DOI
高影响因子
Reaction Chemistry & Engineering
·
2023
·Vol. 8
·期 10
·2632-2640
·
IF 3.9
Han-Qing Chen,Zhan-Kuo Guo,Shu-Xiang Xiang,Hui-Lin Jiang,Yun-Lei Teng
Directly converting metal oxide-adsorbed CO2 to CH4 at low temperatures is a more energy-saving method for achieving carbon capture and utilization. In this study, an Al2O3-supported Ni/CaO composite was greenly prepared by a mechanochemical method. It is found that CO2 capture and selective methanation can be realized over the Ni/CaO/Al2O3 composite at as low as 200 °C under static pressure conditions. The methane yields over the 10Ni/10CaO/γ-Al2O3 composite reach 70.05 and 388.5 μmol CH4 per g at 200 and 350 °C with approximately 100% selectivity to CH4. The experimental results show that the reaction time and temperature obviously affect the methanation yield over the Ni/CaO/Al2O3 composite. This work provides a facile energy-saving strategy for converting CO2 to CH4 at low temperatures.
研究领域:
环境催化
·
能源化学
·
材料科学
·
工业化学
·
碳捕集与利用
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yi Huang,Meng Cao,Lingfei Ye,Jie Liao,Haonan Wu,Lan Yi,Shangqing Chen,Fanpeng Cheng,Huijuan Guo,Liwei Cheng,Lijuan Shi,Qun Yi
Mixed matrix membranes (MMMs) incorporating porous fillers offer transformative potential for gas separations, yet their practical implementation is often hindered by interfacial defects and the inherent permeability–selectivity trade-off. Herein, we propose a covalent organic framework (COF) engineering strategy that integrates ionic functionalization with alkyl chain length modulation (C2, C8, C12) to fabricate high-performance 6FDA-DAM-based MMMs. By grafting bromoalkanes onto the pyridinic sites of TpDp COF, the resulting ionic COFs (iCOF TpDp–CnBr) synergistically eliminate interfacial voids through Br − -mediated electrostatic attraction and alkyl-dependent van der Waals interactions, while the bromide anions establish CO2-philic nanochannels via ion–quadrupole interactions. At 10 wt% loading, the 6FDA-DAM/TpDp–C8Br MMM achieves a CO 2 permeability of 363.7 Barrer and a CO 2 /CH 4 selectivity of 48.7, representing a 2.4-fold increase in permeability and a 2.7-fold enhancement in selectivity over the pristine polymer. This dual improvement transcends the 2008 Robeson upper bound, driven by optimized interfacial adhesion and tailored redistribution of free volume. Long-term stability tests (35 °C, 0.2 MPa) confirm structural integrity under the evaluated conditions. Density functional theory simulations reveal that the C8 alkyl chain minimizes interfacial energy by balancing steric hindrance and polymer–filler compatibility, establishing a charge–chain molecular design paradigm for next-generation membranes with promising application in natural gas purification.
研究领域:
材料科学
·
膜技术
·
气体分离
·
高分子化学
·
可持续能源
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhengda Lin,Yijun Liu,Zhongming Zhang,Jie Yao
In this study we used a high-temperature steam-induced hydrolysis method to obtain a fluorinated OH/SiO 2 -TiO 2 /polyethersulfone (PES) composite hollow fiber membrane for CO 2 capture. The purpose of grafting SiO 2 and TiO 2 on the surface of PES by hydrolyzing silicon precursors and titanium precursors at high temperature, is to improve the alkali corrosion resistance and hydrophobicity of the PES membrane. The OH/SiO 2 -TiO 2 /PES composite hollow fiber membranes prepared by the high-temperature steam-induced hydrolysis method and the graft coating method were measured by SEM, EDS , FTIR, WCA, AFM , XRD and XPS in order to characterize the morphology and structure of the prepared membranes. In the CO 2 /CH 4 separation performance test experiment, the OH/SiO 2 -TiO 2 /PES membrane prepared by the high-temperature steam hydrolysis method showed better separation performance than the original PES membrane. The effects of absorbent flow rate, absorbent concentration and feed gas flow rate on CO 2 flux and CO 2 /CH 4 were selectivity investigated. When the flow rate of the absorbent (DEA) reached 16 L/h, the flow rate of the feed gas (CO 2 /CH 4 = 40 : 60) was 30 ml/min, the concentration of the absorbent was 1 mol/L, The CH 4 concentration was 99.88 % and the optimal separation factor was as high as 554.89. In general, the results obtained in this work may provide promising insights into the use of fluorinated OH/SiO 2 -TiO 2 /PES composite membranes for carbon capture and CO 2 /CH 4 separation in GLMC application.
研究领域:
材料科学
·
环境工程
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DOI
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Bingying Jia,Liujie Bing,Bang Xu,Jihong Sun,Shiyang Bai
The amine (NH2)-functionalized UiO-66 was successfully anchored on disorderly layered clinoptilolite (CP) via surfactant (poly(ethylene glycol) (PEG) and poly(vinylpyrrolidone) (PVP))-assisted induction. The structural features and physicochemical parameters of the resultant UiO-66-on-CPs were characterized by powder X-ray diffraction (XRD) patterns, scanning/transmission electron microscopy (SEM/TEM) images, Fourier transform infrared (FT-IR) spectra, N2 sorption isotherms, and small-angle X-ray scattering (SAXS) patterns. The results demonstrated that the growth of UiO-66-NH2 nanoparticles facilitated the disorder degree of the crystal plane of CP along the a-axis, while the addition of PEG in the hydrothermal synthesis system of CP was conducive to the formation of a flower-like microstructure and the introduction of PVP was beneficial to the nucleation and growth of UiO-66-NH2 nanoparticles with a small size (40 nm) on the surfaces of the obtained CP-PEG lamellas. Finally, the gas-selective adsorption and separation performances of CO2 and CH4 were evaluated using the synthesized disorderly layered UiO-66-on-CP heterostructures as adsorbents, indicating that the NH2-functionalized UiO-66-on-CP exhibited a superior selective factor (3.66) of CO2/CH4. These results elucidated that the proposed approach is a promising strategy for constructing MOF-on-zeolite heterostructures, which may open an avenue to expand CP application and improve their performance.
研究领域:
材料科学
·
化学工程
·
环境科学
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DOI
高影响因子
JOURNAL OF POROUS MATERIALS
·
2023
·Vol. 30
·期 6
·2129-2137
·
IF 2.6
Tao Ruyu,Liu Hao,Xiang Pan,Lin Yichao,Zhou Junjie,Zhou Chen,Zhao Yayun,Tian Ziqi,Zhang Qiuju
Nanoscale Zr-based metal-organic framework (MIP-202) particles were successfully prepared via a seeds-assisted hydrothermal secondary synthesis. The uniformly-shaped MIP-202 particles exhibit excellent performance on selective CO 2 adsorption from CO 2 /CH 4 and CO 2 /N 2 mixtures. At 298 K and 1 bar, the uptake ratios of CO 2 /CH 4 and CO 2 /N 2 of MIP-202 particles are as high as 32.6 and 65.2, respectively. The IAST (ideal adsorbed solution theory)-predicted selectivities of CO 2 /N 2 (50/50, v/v) and CO 2 /CH 4 (50/50, v/v) reach to 4.5 × 10 10 and 102.2, respectively. The breakthrough experiments further demonstrate that the CO 2 /CH 4 and CO 2 /N 2 mixtures can be efficiently separated through an adsorption column packed with MIP-202 particles. In addition, the as-prepared MIP-202 particles had a low iso-enthalpy of adsorption of CO 2 of 32.95 kJ/mol, which is favorable for the regeneration of the adsorbent. Herein the as-prepared MIP-202 is a potential material for efficient separation of CO 2 from CH 4 or N 2 through an energy- and cost-saving CO 2 capture process.
研究领域:
材料科学
·
环境化学
·
能源工程
·
纳米技术
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DOI
高影响因子
危险品化学品经营许可证（带存储）