ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Chongyang Wei,Yidan Wang,Haoting Liang,Ting Li,Jing Lv,Mei-Yan Wang,Yue Wang,Shouying Huang,Xinbin Ma
Direct conversion of CO2 to aromatics has received considerable attention as a typical CO2 utilization technology for mitigating climate change. Efficiently regulating the distribution of aromatics remains a significant challenge. Here, we report on a series of bifunctional catalysts composed of Na/Fe and Ni/ZSM-5 zeolites with varying Ni content, which achieve a controlled distribution of aromatics in direct CO2 hydrogenation to aromatics. The hydrogen spillover effect of Ni on ZSM-5 accelerates the cracking of aromatics and consequently increases the BTX (benzene, toluene, xylene) content in the aromatics to as much as 78.4% (mol %). Ethylbenzene dealkylation as a model reaction reveals that introduction of Ni facilitates the removal of branched chains from aromatics in the form of CH4, leading to a positive correlation between CH4 selectivity and the BTX ratio in aromatics with the amount of spillover hydrogen. The hydrogen spillover effect also significantly reduced the coke content on HZSM-5, prolonging the catalyst life. However, excessive hydrogen spillover increases the hydrogen coverage on Fe species, inhibiting the carburization of Fe, which is unfavorable for CO2 conversion. These insights offer a new strategy for controlling the distribution of aromatics over bifunctional catalysts over the conversion of C1 to aromatics.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
·
IF 7.8
Pan Zhang,Zhongfa Zha,Jiawen Yang,Xinbo Wang,Jianwen Song,Shuming Du,Liwen Li,Kun Zhao,Dong Fu,Lemeng Wang,Jun Ke,Pengfei Qu
High energy consumption during CO₂ desorption remains a critical bottleneck limiting the industrial application of monoethanolamine (MEA)-based carbon capture technologies. To address this issue, a novel high-efficiency catalyst, the 1:4-Ti@D composite catalyst based on diatomite and TiO(OH) 2 surface modification, was developed. Catalytic performance was evaluated in 30 wt% MEA solution at 90 °C. Compared with non-catalytic processes, the 1:4-Ti@D catalyst enhanced total CO₂ desorption amount by 46.2 % and maximum desorption rate by 125.1 %, while reducing desorption energy consumption by 39.2 %. Notably, it maintained stable catalytic efficiency after 10 consecutive adsorption-desorption cycles, confirming its durability for industrial use. The physicochemical characteristics of the catalysts were comprehensively elucidated through various multi-dimensional characterization techniques. The experimental findings revealed that the synergistic effect of TiO(OH) 2 and diatomite substantially augmented the surface acid site density, while the optimized mesoporous structure facilitated efficient reactant transport, thereby underpinning the catalyst's exceptional performance. By the study of desorption mechanism, the stronger interaction between Ti and O of reactants can lead easier H 2 O and RNHCOO - absorption and activation. Moreover, an assessment of the catalyst's impact on thermal and oxidation degradation as well as the corrosion rate of MEA indicated minimal influence on amine degradation and corrosion processes. This work provides a new strategy for developing low-cost, high-stability clay-based catalysts and offers technical support for advancing energy-efficient industrial carbon capture systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Ruqing Chong,Xiangyan Dou,Zhaoqi Deng,Zhangzhou Luo,Zihui Meng,Wenfang Liu
With formate dehydrogenase (FDH) as the biocatalyst and reduced nicotinamide adenine dinucleotide (NADH) as the cofactor, enzyme catalysis achieves high-selectivity CO 2 reduction to formic acid under ambient conditions. However, this route relies on susceptible and costly enzyme and cofactor, and faces difficulties in their recovery and reuse. Enzyme immobilization and cofactor regeneration are essential strategies to address these issues. Herein we designed a dual-function Ti 3 C 2 T x /graphene (GA)/TiO 2 (TGT) composite aerogel, after amino modification, FDH was immobilized on the aerogel via glutaraldehyde chemistry. Then it was innovatively applied in a photo-enzyme coupled system (PECS) that mimics natural photosynthesis and engenders sustainable CO 2 reduction by integrating photocatalytic NADH regeneration with enzymatic CO 2 reduction. Porous GA aerogel not only enables high specific surface area that facilitates enzyme immobilization and substrate adsorption, but also extends the light response of TiO 2 from ultraviolet to visible light range and reduces band gap. Ti 3 C 2 T x contributes simultaneously to photocatalysis and enzyme reaction through its excellent electronic conductivity, large two-dimension surface and good CO 2 affinity. Ultimately, TGT demonstrated photocatalytic activity of 58.8 μM/(g·min) and NADH yield of 14.9 %. TGT immobilized FDH exhibited an enzyme activity recovery of 81.4 % and produced 0.24 mM formate. With 2 mM cofactor, formate yield reached 12.4 % in the PECS, surpassing most reported systems.
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Science Advances
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2025
·Vol. 11
·期 48
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IF 12.5
Kaifang Wang,Zhongtai Zhu,Yuqi Liu,Weiran Zheng,Ziyi Yuan,Zhihong Lin,Raphael Semiat,Lu Shao,Xuezhong He
Carbon membranes are emerging as a versatile platform for the selective separation of gas mixtures with similar molecular sizes. Here, a high-performance carbon membrane is developed from an asymmetric, rigid copolyimide precursor via a precisely controlled carbonization process. Membranes carbonized at 800°C exhibit exceptional CO 2 separation performance, with CO 2 permeabilities up to 15,700 barrer and CO 2 /N 2 and CO 2 /CH 4 selectivities of 63 and 52, respectively—surpassing the 2019 upper bounds. Molecular dynamic simulations, in conjunction with in situ thermogravimetric analysis-mass spectroscopy and thermogravimetric analysis-Fourier transform infrared spectroscopy, reveal the evolution of a bimodal carbon matrix with micropores (7 to 20 angstroms) and ultramicropores (4 to 7 angstroms). Gas transport is dominated by synergistic adsorption-selective and molecular sieving mechanisms, enabling subangstrom discrimination between CO 2 and larger gases. This work demonstrates a facile, tunable strategy to engineer carbon membranes with outstanding CO 2 separation capabilities, offering previously unexplored opportunities for energy-efficient gas separation processes in industrial applications.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Bowen Xu,Chao Xu,Qiongqiong Jiang,Huajing Zhang,Fei Jin,Hailin Zhang
The isothermal thermochemical redox cycle is a promising route for solar-driven CO 2 splitting, as it enables stable heat input and simplifies reactor design. However, achieving high redox activity and long-term stability remains a challenge for oxygen carrier materials. In this study, spinel FeAl 2 O 4 foam ceramics were synthesized at three calcination temperatures for 1300 °C (FA-13), 1400 °C (FA-14), and 1500 °C (FA-15), to investigate the redox performance. X-ray diffraction patterns were tested and confirmed that FA-14 and FA-15 both exhibited a pure FeAl 2 O 4 phase, while FA-13 retained residual Al 2 O 3 . The structure characteristics and scanning electron microscopy analyses revealed that FA-14 exhibited optimal porosity (74.41 %) and uniform grain distribution. In contrast, FA-15 showed densification and reduced porosity (71.75 %), while FA-13 displayed structural defects and poor crystallinity. Isothermal CO 2 splitting tests at 1400 °C demonstrated that FA-14 achieved the highest CO yield of 206 μmol/g, outperforming CeO 2 , FA-13 and FA-15. Long-term cycling tests over 50-cycle redox test(>100 h) showed that FA-14 maintained stable CO and O 2 yields of 170 ± 10 μmol/g and 97 ± 5 μmol/g, respectively indicating excellent thermal stability under high-temperature operation condition. These results demonstrate that tuning the calcination temperature of FeAl 2 O 4 ceramics can optimize their redox performance by balancing crystallinity and porosity.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10389
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IF 15.7
Zhai Yanjie,Gong Shanhe,Li Weisong,Xia Qing,Li Tingting,Guan Jianyu,Leu Shao-Yuan,Wu Zhen-Yu,Lau Shu Ping,Zhang Xiao
Electrochemical carbon capture offers a sustainable pathway for carbon management, yet current systems are hindered by low concentration of atmospheric carbon dioxide (CO 2 ), resulting in inefficiencies and limited stability. Here, we develop an electrochemical system employing a modular porous solid electrolyte (PSE) reactor for continuous, scalable carbon capture from diverse sources, including ambient air and flue gas, while regenerating high-purity CO 2 ( >99%) without additional chemical input through a recirculation mode. By leveraging oxygen evolution and reduction reactions (OER/ORR) and employing sodium (bi)carbonate as a reversible cyclic mediator, the system achieves continuous CO 2 capture from flue gas, delivering high Faradaic efficiencies for Na⁺ transport (~85%), and high carbon capture rates (3060 ml h − 1 at 10 A, 100 cm 2 ). Notably, direct air capture is demonstrated using ambient air, showing a long-term stability of over 2000 hours while maintaining high carbon removal efficiency (>93%) at 30 mA cm -2 and a large air treatment capacity (approximately 8820 kg air day -1 m -2 ), thus contributing to the goal of achieving net-zero emissions.
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Energy Technology
·
2025
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IF 3.6
Hui Huang,Qi Xu,Liangyun Yu,Lidong Li,Ying Zhang,Fennv Han,Qi Zhang
Currently, there is a thermodynamic and kinetic mismatch between carbon dioxide methanation. Carbon dioxide is stable in nature and requires a highly active catalyst to facilitate its reduction reaction. In this article, Ru/ZrO 2 catalysts are prepared by a structure-directed derivatization strategy using zirconium-based metal-organic frameworks (MOFs) (UiO-66) as precursors. The porous framework structure of MOFs was utilized to construct Ru nanoparticles with a large size (≈9.7 nm). Photothermal catalysis is employed, and the photoexcitation induced the transfer of electrons from the conduction band of ZrO 2 to Ru, which elevated the electron density of Ru to the enriched state and promoted the activation of CO 2 adsorption, while the photothermal effect facilitated the warming of the catalyst bureau, which provided a favorable condition for CO 2 methanation. The compositional valence, morphology, specific surface area, bandgap and other properties of the catalysts were evaluated by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscpe, Brunner-Emmet-Teller measurements, hydrogen temperature-programmed reduction, CO 2 -TPD, ultraviolet–visible, photoluminescence, and photocurrent response characterization. The experimental results showed that 99% methane selectivity and 120.354 mmol g cat −1 h −1 methane yield were achieved at 1 MPa and photothermal (250 °C) conditions.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2025
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IF 4.7
Xiaoxia Zhang,Congmei Chen,Meng Rong
The development of advanced microporous organic polymers with high CO 2 capture efficiency and efficient removal of toxic volatile organic compounds under high-humidity conditions remains a significant challenge. In this work, three highly hydrophobic fluorinated tetraphenyladamantyl microporous organic polymers (FMOPs) were fabricated via C – H arylation of 1,3,5,7-tetra(4-bromophenyl)adamantane with 1,2,4,5-tetrafluorobenzene, 1,2,4,6-tetrafluorobenzene, and 1,3,5-trifluorobenzene, respectively. The effects of fluoroaromatic linking units on the porosity, chemical properties, static and dynamic gas/vapor adsorption performance under dry and high humidity conditions were systematically investigated. It was found that fluoroaromatic linkers with isomerism and higher functionality facilitate the formation of highly porous network. The fluorinated FMOPs demonstrated strong hydrophobicity with minimal water vapor adsorption (0.06–0.17 wt%, 298 K/0.9 P/P 0 ). Among them, FMOP-3 exhibited the highest BET surface areas of 1373 m 2 /g and a narrow pore size distribution (0.55 nm and 0.93 nm). FMOP-3 also showed remarkable CO 2 uptake (12.2 wt%, 273 K/1.0 bar) and CO 2 /N 2 selectivity (46.4). Notably, the FMOPs simultaneously possess exceptional adsorption capacities for benzene (122.5-149.6 wt%) and cyclohexane (95.3-122.8 wt%), significantly surpassing most previously reported porous organic polymers. Moreover, dynamic breakthrough experiments under high humidity (85% RH) confirmed the high capture efficiency of FMOPs. Experimental characterizations and theoretical calculations confirmed that fluorination enhances the interactions of CO 2 @FMOPs and benzene@FMOPs through dipole–quadrupole interactions and fluorine-induced strengthened π-π interactions. These findings highlight the potential of FMOPs for highly efficient CO 2 capture and toxic volatile organic vapor removal under high-humidity conditions. In addition, this work also provides some insights into developing advanced functional adsorbents for gas molecule capture under high-humidity conditions.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
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IF 9
Qingnan Wang,Yanting Tang,Longjie Liu,Chenlu Liu,Keming Zhang,Xiaohe Tian,Xiaoting Feng,Rui Zhang,Yueyangchao Yu,Tianhe Gu,Bin Liu,Shaofei Wang
The scalable fabrication of large-area, defect-free metal-organic framework (MOF) membranes for precise gas separation is hindered by their intrinsic brittleness and polycrystalline defects. Herein, we present a molecular weaving strategy to construct an interwoven mixed matrix membrane of rigid 3D UiO-66 gel and flexible polyethyleneimine (PEI) polymers, achieving both structural robustness and tunable porosity. Glutaraldehyde crosslinking further stabilizes the hybrid framework, enhancing mechanical durability while refining pore dimensions to 0.35 nm, ideal for H 2 /CO 2 sieving. The resultant ultrathin (∼50 nm) but flexible membranes, with UiO-66 content up to 46 wt%, exhibit superior separation performance, achieving a H 2 permeance of 845 GPU and H 2 /CO 2 selectivity of 16.8, surpassing the 2008 Robeson upper bound. Additionally, we demonstrated the fabrication of defect-free membranes ∼160 cm 2 , showcasing the scalable potential of this method. This work introduces a promising strategy for designing flexible, high-performance MOF-based separation systems, addressing urgent challenges in energy-efficient gas purification and carbon capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Li Peng,Zhaofeng Duan,Shumin Cen,Xuehong Gu
High-silica CHA (SSZ-13) zeolites membranes, with pore size between the molecular size of CO 2 and N 2 or CH 4 , are promising for some industrial CO 2 separation process. Considering water is typically present in these industrial gas feed and the negative impact of moisture on the membranes’ gas permeation, it is highly desirable to increase the surface hydrophobicity of membranes to reduce the adsorption of water. In this paper, a W-doping strategy was proposed to increase the hydrophobicity of SSZ-13 membranes by eliminating the silanols on the surface, and the W-doped high-silica CHA (W-SSZ-13) zeolite membranes were prepared for the first time. Characterizations such as SEM, XRD, and XPS confirmed the successful incorporation of W into CHA membrane. The incorporation of W reduced the pore mouth size, and the W-SSZ-13 zeolite membranes showed improved CO 2 /N 2 and CO 2 /CH 4 separation performance. After W-doping, the maximum separation factors ( α max ) for the CO 2 /N 2 mixture with equimolar composition under dry conditions increased from 8.8 to 16.9, and for the equimolar CO 2 /CH 4 mixture, the value increased from 105.9 to 176. The W-SSZ-13 membranes also showed better separation performance under wet conditions. For both systems, the W-SSZ-13 membrane showed higher α max and less CO 2 permeance reductions, indicating a more resistance in wet conditions.
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CELLULOSE
·
2020
·Vol. 27
·期 17
·10541-10551
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IF 4.21
Wang Mingyue,Liu Mao,Zhao Hongjuan,Xiong Xiaoqing,Zheng Laijiu
Abstract Modified curcumin, which has the advantages of low toxicity, high solubility, and little color change after modification, is very suitable for nonaqueous supercritical carbon dioxide cotton dyeing. However, the existing curcumin modification technology focuses on improving its solubility. Modified curcumin is directly adsorbed onto cotton fabrics, and the main interaction forces are van der Waals forces, which causes the poor fastness of modified curcumin to dyed cotton fabrics. In this study, reactive groups (hydroxyalkyls) were introduced into curcumin to enhance its fastness to cotton fabrics. The results showed that, similar to alkyl groups, hydroxyalkyl groups can enhance the color depth of dyed cotton fabrics by elevating the solubility of modified curcumin in supercritical carbon dioxide. The higher the solubility of modified curcumin in supercritical carbon dioxide was, the higher the K/S value of the dyed cotton fabric. Furthermore, the hydroxyl groups on the modified curcumin could form ether bonds with the hydroxyl groups on cotton fabrics. Therefore, the washing and rubbing fastness of hydroxyalkyl-curcumin-dyed cotton fabric was better than that of alkyl-curcumin-dyed cotton fabric. Graphic abstract
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CARBON
·
2019
·
IF 7.466
Hui Ning,Xiaoshan Wang,Wenhang Wang,Qinhu Mao,Zhongxue Yang,Qingshan Zhao,Yan Song,Mingbo Wu
Electroreduction of carbon dioxide (CO 2 ) to ethylene (C 2 H 4 ) is one of the most feasible approaches to reduce the carbon emissions and enhance carbon dioxide utilization , whereas the lack of efficient catalysts impedes the scale application. Cuprous oxide (Cu 2 O) is a promising catalyst for the formation of C 2 H 4 but with unsatisfied selectivity and stability. Herein, we prepared Cu 2 O/nitrogen-doped carbon shell (Cu 2 O/NCS) composite and employed it in the production of C 2 H 4 from CO 2 electroreduction. The ultra-thin NCS with graphene-like structure was prepared from petroleum asphalt by template method . The cubic Cu 2 O nanocrystals are uniformly dispersed on the surface of NCS with ca. 150 nm diameters. Cu 2 O/NCS loaded on glass carbon electrode showed a high faradaic efficiency of C 2 H 4 (24.7%) at −1.3 V ( vs . reversible hydrogen electrode) as well as remarkable stability. The excellent performance of Cu 2 O/NCS is attributed to the high dispersion of cubic Cu 2 O nanocrystals and the abundant pyridinic-N moieties in NCS. This work provides a new strategy to improve the selectivity and durability of Cu 2 O for production C 2 H 4 from electrocatalytic CO 2 reduction by fabricating composites with nitrogen-doped carbon materials.
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