APPLIED ORGANOMETALLIC CHEMISTRY
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2026
·Vol. 40
·期 4
·e70543
·
IF 4.3
Xinhao Zhang,Qiang Wang,Haoyang Lin,Dingkai Hu,Biao Liu,Dezhi Cao,Guorong Zhao
The excessive consumption of fossil fuels has triggered a dramatic surge in CO 2 emissions, prompting the development of diverse mitigation strategies. Among these, the functionalization of metal–organic frameworks (MOFs) with polar amine moieties has emerged as a promising approach to substantially enhance their CO 2 capture capacity. In this study, HKUST-1 was synthesized via a solvothermal method and then modified with three different amines (DEA, TEPA, and PEI) by impregnation to prepare a series of solid amine adsorbents. The effects of the amine type, amine loading, and environmental parameters, including temperature, gas flow rate, CO 2 concentration, and humidity, on the CO 2 adsorption performance were systematically studied. Thermal stability, cycling performance, and adsorption kinetics were also evaluated. The results show that the PEI-modified adsorbent exhibits the best performance, with an optimal amine loading of 20%. Excessive amine loading leads to pore blockage and reduces adsorption capacity. Compared to unmodified HKUST-1, PEI20@HKUST-1 shows a 92% enhancement in CO 2 adsorption, attributed to PEI's bidentate adsorption mechanism and flexible polymeric chains, which contribute to a high amine utilization efficiency. Among the environmental factors studied, higher temperatures lower the CO 2 uptake due to thermodynamic constraints, whereas increasing flow rate and humidity first promotes and then suppresses adsorption. The optimal adsorption conditions are identified as 30°C, 20 mL min −1 flow rate, and 45% relative humidity. Moreover, PEI20@HKUST-1 displays good thermal stability and excellent cycling performance, retaining 88% of its initial adsorption capacity after 15 consecutive adsorption–desorption cycles. Kinetic analysis confirms that the adsorption process follows the Avrami model, which indicates a combined physisorption and chemisorption mechanism.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122217
·
IF 7.5
Yingnan Ma,Zhen Xu,Renjie Huang,Yulu Zhang,Jihong Tian,Zijian Zhang,Shuyan Meng,Panliang Zhang,Kewen Tang
Efficient CO 2 separation is pivotal to lowering the energy consumption and costs of carbon capture, utilization, and storage (CCUS), and thin-film composite membranes (TFCMs) with high permeance have emerged as a preferred solution for carbon neutrality and global climate change mitigation. Polyethyleneimine (PEI) exhibits excellent CO 2 adsorption capability owing to its unique amino structure, however, its excessive accumulation on the substrate surface and pore penetration lead to an overly thick functional layer, which significantly impairs the gas permeability of TFCMs. This work successfully developed a novel ultrathin polyethyleneimine (PEI) composite membrane based on MOFs nanosheets gutter layer via interfacial polymerization. Benefiting from the significant improvement of the surface properties of substrate by the MOFs nanosheets gutter layer, the prepared PEI functional layer exhibited an ultrathin thickness less than 135 nm with a highly ordered structure. The CO 2 permeance reached 779.6 GPU, with excellent selectivities of 59.1 for CO 2 /N 2 and 54.1 for CO 2 /CH 4 . The resulting TFCMs demonstrated excellent CO 2 separation performance, surpassing the 2008 and 2019 upper bound while maintaining long-term separation stability. The study provided new insights into the precise design and controllable preparation of gas separation membranes, offering valuable reference for the industrial development of high-performance CO 2 separation membranes.
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APPLIED CLAY SCIENCE
·
2026
·
IF 5.2
Xiaoyu Li,Haiyang Xue,Hui Ma,Chenyu Wang,Kang Peng
Solid amine adsorbents play an important role in separating CO 2 from flue gas and can be used in post-combustion CO 2 capture. However, their effective regeneration capabilities and long-term stability remain significant challenges. Herein, a hydroxyl-functionalized polyethyleneimine on graphene/vermiculite-derived porous silica nanosheets with good structural tunability was reported as a solid amine adsorbent. The optimized adsorbent possesses a high working capacity (1.50 mmol/g) and long-term stability in practical temperature swing adsorption processes. After 20 adsorption-desorption cycles, the adsorption capacity decreases by only 3.2%, demonstrating good cyclic stability. The formation of hydrogen bonds between the hydroxyl groups of glycerol and the amino groups of polyethyleneimine significantly reduces the irreversible conversion of amine groups to urea groups, thereby greatly enhancing the cycling stability of the adsorbent. The incorporation of graphene enhances the thermal conductivity of porous silica nanosheets by 42.8%, allowing for rapid thermal transmission and preventing local overheating during the CO 2 adsorption process. The combined strategy of amine functionalization and porous support design in this work offers an effective approach to improving the cycling stability of solid amine adsorbents.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Guangli Yu,Zhiqi Zhu,Fei Ni,Xingfei Song,Xuming Qin,Xiaoguo Wan,Kangjun Wang
Porous organic frameworks (POFs) have garnered significant attention as potential filler materials for gas separation applications. Nevertheless, most available POFs predominantly possess a single type of adsorption site, which limits their overall performance. In this study, two ferrocene-based POFs, termed FcDA POF-1 and FcAc POF-2, were synthesized using ferrocene derivatives and pyrrole as monomeric precursors. The resulting POFs exhibited dual Lewis acid-base sites and high specific surface area. Extensive characterization validated excellent interfacial compatibility when these POF fillers were incorporated into 6FDA-DAM polymer matrix. The optimized mixed-matrix membrane (MMMs) based on FcDA POF-1 achieved exceptional CO 2 permeability of 3278.1 Barrer, coupled with an ideal CO 2 /N 2 selectivity of 58.4. These metrics represent enhancements of 260% and 208%, respectively, compared to the pristine 6FDA-DAM membrane, notably exceeding the 2019 Robeson upper bound. Density functional theory (DFT) calculations supported the hypothesis that multiple weak interactions between CO 2 molecules and FcDA POF-1, occurring at the electron-rich nitrogen atoms (Lewis base sites) and electron-deficient cyclopentadienyl groups (Lewis acid sites), synergistically enhance selective CO 2 recognition. Further evaluations under mixed-gas conditions, varying pressures and temperatures, as well as long-term stability tests, substantiated the membranes’ practical applicability. This work underscores rational design principles for constructing high-performance MMMs and presents a viable avenue for efficient CO 2 separation.
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PLANT BIOTECHNOLOGY JOURNAL
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2026
·
IF 12.8
Shubin Li,Tao Sun,Dailin Liu,Tong Zhang,Lei Chen,Weiwen Zhang
The single crossover occurring via homologous recombination is a common phenomenon existing among microbes like Escherichia coli , Bacillus subtilis , Vibrio natriegens , Gluconobacter oxydans and most cyanobacteria species, threatening the stability of engineered strains and challenging iterative genetic engineering. Among them, we take the fast-growing cyanobacterium Synechococcus elongatus UTEX 2973 (Syn2973) as a representative study due to its promising roles for CO 2 fixation and bioconversion. We established three marker-free platforms to achieve stable genome recombination: (i) T4CROSS, which employs two plasmids and four rounds of single crossover; (ii) TRIPLEARM, which uses a single plasmid containing three homologous arms for three rounds of single crossover; and (iii) CRISPRARM, which integrates CRISPR/Cpf1-mediated genome editing with homologous recombination. As proof of concept, we employed the CRISPRARM platform for a three-step sequential engineering of the sucrose biosynthetic pathway. The final engineered strain produced 7.12 g L −1 of sucrose within 4 days.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Chaoying Zhang,Qian Jia,Guoqiang Li,Feng Li,Haitao Cui,Congming Li,Lei Li
An ultramicroporous variant of Mg-MOF-74 is synthesized through a mixed-linker strategy incorporating ethylenediaminetetraacetic acid (EDTA) as exotic linker. • An exclusive H 2 O adsorption site is created based on the uncoordinated oxygen atoms of EDTA. • The hydrogen-bonding network within EDTA-modified frameworks enhances CO 2 adsorption by 14.3 % via the formation of carbonates. • Incorporating EDTA molecules increases the CO 2 /N 2 selectivity by a factor of 2.28 compared to pristine Mg-MOF-74. • The EDTA-modified Mg-MOF-74 outperforms the pristine Mg-MOF-74 with a two-fold enhancement in CO 2 uptake under humid conditions. Mg-MOF-74 ([Mg 2 (DOBDC)]) represents a high-performance solid adsorbent for carbon capture, however, its CO 2 uptake decreases significantly under humid flue gas conditions due to competitive adsorption between H 2 O and CO 2 molecules. Herein, a mixed-linker modification strategy is employed by integrating ethylenediaminetetraacetic acid (EDTA) into the Mg-MOF-74 framework. This approach preserves the original one-dimensional pore structure while altering the coordination environment of Mg 2+ sites, reducing their coordination number to five. The resulting structure with uncoordinated oxygen atoms from EDTA serves as exclusive adsorption centers for H 2 O thereby protecting the CO 2 adsorption capacity. The optimized MOFs exhibits a high CO 2 adsorption capacity (6.4 mmol/g, at 1 bar) and outstanding CO 2 /N 2 selectivity (346). In humid CO 2 /N 2 (15:85, v:v, at 314 K, RH% = 86%) breakthrough experiment, the EDTA-modified frameworks maintain stable CO 2 uptake (3.92 mmol/g), consistent with dry performance, whereas the pristine Mg-MOF-74 shows a great reduction (2 mmol/g). In-situ FTIR further reveals that the incorporation of EDTA facilitates the formation of hydrogen bonding and carbonate species, synergistically enhancing the moisture resistance of MOF materials. Moreover, the modified material retains stable breakthrough times over six consecutive adsorption-desorption cycles under high-humidity conditions, demonstrating its great potential for scalable industrial carbon capture applications.
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Journal of Materials Chemistry A
·
2026
·
IF 9.2
Yangyang Zhao,Yijian Wang,Xiaoyu Wang,Xingchen Feng,Tao Cong,Juntao Feng,Pei Wang,Kai Yang,Xifeng Ding
Solid oxide electrolysis cells (SOECs) offer a promising route for electrochemical CO 2 conversation to sustainable fuels, but their widespread adoption is hindered by the lack of cathodes combining high catalytic activity and stability. To address this challenge, we developed an in-situ interface-engineered La 0.6 Sr 0.4 Fe 0.95 Ti 0.2 O 3-δ cathode (R-LSF 0.95 T) cathode featuring exsolves Fe nanoparticles. The optimized R-LSF 0.95 T-based cell delivers a current density of 780 mA cm -2 at 1.5 V and 800 °C in pure CO 2 atmosphere, representing a 23.2% improvement over mechanically mixed electrode. This performance enhancement arises from synergistic metal-oxide hetero-interfaces, where the reduced perovskite substrate promotes CO 2 adsorption and oxygen-ion transport, while the Fe nanoparticles provide abundant active sites and reduce activation barrier for CO 2 reduction. Notably, the Fe-decorated perovskite demonstrates superior carbon deposition compared to Ni-based cathodes owing to its moderate activity. Consequently, the electrolysis cell maintains exceptional stability over 100 h at 1.5V and 800 ℃, with interfacial robustness further enhanced through redox cycling due to reinforced anchoring effect with more minute Nano-Fe exsolution. This work establishes a novel materials design paradigm that reconciles the activity-stability trade-off in SOEC cathodes through the combination of moderately active catalysts with interface reinforcement, offering new pathways for developing durable, high-performance CO 2 electrolysis systems.
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Plasma Processes and Polymers
·
2026
·Vol. 23
·期 5
·e70179
·
IF 3.2
Liangping Xiao,Rui Zhang,Tianyu Li,Jiahui He,Yu Liang,Xiubin Luo,Fuxue Wang,Xiao Liu,Jiannian Yao,Rusen Zhou
Two-dimensional (2D) materials have demonstrated excellent application prospects in electrocatalysis due to their unique anisotropy, high densities of exposed atoms, and tunable surface chemistry. However, the top-down exfoliation of few-layer nanosheets by breaking van der Waals interactions often introduces external intercalating molecules or solvent molecules, which adversely affect their performance in electrocatalytic reactions. Herein, we report a liquid-phase plasma bubbles treatment method for the exfoliation and preparation of few-layer Bi 2 Se 3 nanosheets. As no external intercalating molecules are introduced, and the as-exfoliated few-layer nanosheets possess a higher density of unsaturated bonds, they exhibit outstanding performance in the electrocatalytic carbon dioxide reduction reaction (CO 2 RR). The Faradaic efficiency for CO 2 electroreduction to formate exceeds 90%, with catalytic stability maintained for up to 100 h. Furthermore, this exfoliation method demonstrates broad applicability, successfully producing few-layer MoS 2 , WS 2 , and WSe 2 nanosheets. This work provides a new strategy for the synthesis of high-performance few-layer nanosheets for electrocatalysis.
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Eun Kyu Sun,Kyungwhan Min,Ook Choi,Senthil Kannan,Tae-Hyun Kim
Polymer of intrinsic microporosity-1 (PIM-1) is recognized for its exceptional gas permeability, attributed to its high free volume and microporosity. However, it presents several disadvantages, including low selectivity, plasticization, and poor aging properties. To address these challenges, PIM-nPI-Tz, a series of composite membranes containing triazine cross-links, was developed herein by spin-coating nitrile-functionalized polyimidazolium (PI-CN) onto a PIM-1 membrane, followed by heat treatment. The resulting coating layer increased the selectivity of the PIM-1 membrane, given its CO2 affinity, while the formation of triazine increased the backbone-to-backbone spacing, enhancing the diffusivity and permeability of the membrane. Notably, PIM-5PI-Tz (involving PIM-1 coated with a 5% PI-CN solution) exhibited a 73% increase in CO2 permeability (7539 barrer) and a 34% rise in CO2/N2 selectivity (24.4), nearly equivalent to the 2019 Robeson upper bound in terms of overall gas separation. Moreover, the plasticization of the membrane was effectively suppressed, even at a feed gas pressure of 20 bar. Further, its gas separation performance was retained over 300 days under CO2/N2 mixed-gas conditions, demonstrating its superior antiplasticization and antiaging characteristics. The coating material used herein, PI-CN, exhibits a significantly higher CO2-philicity than conventional coating materials, such as Pebax, PEG, and PDMS. Moreover, during the spin-coating and subsequent heat treatment processes, molecular rearrangement within PI-CN facilitates CO2 diffusion, further enhancing the gas transport performance of the PIM membrane.
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iScience
·
2026
·Vol. 29
·期 6
·
IF 4.5
Ziyu Wang,Xuejie Han,Baohao Qian,Xiulai Zhang,Jingyuan Ma,Ru Feng,Meiqin Shi,Guangbo Chen,Fanfei Sun
Photothermal catalytic reduction of CO 2 to CO has been regarded as a promising strategy for solar-to-chemical energy conversion, yet the dynamic evolution of active sites under realistic reaction conditions remains poorly understood. Herein, we synthesized CuO/ZnO (CuZnO) catalysts with intimate interfacial contact via co-precipitation followed by calcination method. Under photothermal conditions, CuZnO underwent in situ reconstruction into low-coordinated metallic Cu in close contact with ZnO, delivering a CO generation rate of ∼18.1 mmol g −1 h −1 with a selectivity as high as 99% at 200 °C, outperforming that achieved under purely thermal conditions. Operando photothermal X-ray absorption fine structure (XAFS) spectroscopy revealed the real-time evolution of both Cu and Zn coordination environments in CuZnO, illustrating the formation and stabilization of metallic Cu on ZnO during photothermal catalysis. This study elucidates the mechanisms underlying photothermal synergy in CO 2 reduction and provides mechanistic insights into active-site dynamics under photothermal conditions.
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Journal of the American Chemical Society
·
2026
·
IF 16.6
Jundi Cheng,Biao Zhou,Hao Zhang,Xupeng Liu,Hao Zhang,Furong Guo,Xiaoyi Zhang,Yuqing Hu,Jun Lin,Hao Li,Lizhi Zhang
Electrochemical CO2 reduction to multicarbon (C2+) hydrocarbons offers a promising route for value-added fuels and chemical feedstocks, yet its selectivity is usually limited by the sluggish symmetric C–C coupling. Herein, we demonstrate the synthesis of phosphidated Cu–Ni–Cu triangular single-atom cones (Ni1PCu2) by decorating Cu nanowires with Ni single atoms and P. These Ni1PCu2 can deliver an impressive CO2-to-C2+ hydrocarbon (C2H4 43%, C2H6 48%) Faradaic efficiency of 91% under solar light at an ultralow bias of −0.3 VRHE, and a stable C2+ hydrocarbon production rate of 370 μmol h–1 cm–2 for 4 days at 100 mA cm–2, where the Cu nanowires harness solar light to generate plasmonic electrons for the CO2 activation and its subsequent conversion to *CO, while electronegative phosphidation induces the formation of Cu+ sites to well stabilize *CO across high coverages. Strategically positioned Ni single atoms generate and confine active hydrogen (•H) for efficient hydrogenation of adjacent Cu+–*CO into Cu+–*CHO. The resulting Cu+–*CHO displays a weakened C–O bond and enhanced C nucleophilicity, allowing for solar-powered asymmetric C–C coupling with neighboring *CO toward efficient and selective C2+ hydrocarbon synthesis.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Zequn Li,Luogang Wu,Guangcan Huang,Xuetong Cui,Zilong Chen,Qiang Chen,Jian-Rong Li
Mixed matrix membranes (MMMs) incorporating metal–organic frameworks (MOFs) are attractive for molecular recognition and separations, but precisely engineering the MOF filler structure toward maximizing its inherent nanopore separation capability remains challenging. Here, we report a fluorination strategy to functionalize MIL-101 that synergistically optimizes its pore chemical environment and interfacial compatibility with the polymer matrix. Compared with the MIL-101/6FDA-DAM membrane, the incorporation of strong electron-withdrawing fluorinated ligands enhances both the CO2 adsorption affinity of MIL-101 and its hydrogen-bonding interaction with the 6FDA-DAM matrix. The optimized MIL-101-F/6FDA-DAM (10 wt %) membrane achieves a CO2 permeability of 2200 Barrer, a 150% enhancement over the pure 6FDA-DAM membrane, while maintaining a comparable CO2/CH4 selectivity of 21. The excellent separation performance surpasses the 2008 Robeson upper bound. This work provides a simple and effective approach to advancing the gas separation performance of MMMs.
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