Polymers
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2024
·Vol. 16
·期 3
·393
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IF 4.7
Xiaoyu Du,Shijun Zhao,Yanqing Qu,Hongge Jia,Shuangping Xu,Mingyu Zhang,Guoliang Geng
Imidazole ionic liquids (ILs) have good affinity and good solubility for carbon dioxide (CO2). Such ionic liquids, combined with polyimide membrane materials, can solve the problem that, today, CO2is difficult to separate and recover. In this study, the ionic liquid (IL) of 1-ethyl-3-methylimidazolium tetrafluoroborate (IL1), 1-pentyl-3-methylimidazolium tetrafluoroborate (IL2), 1-octyl-3-methylimidazolium tetrafluoroborate (IL3), and 1-dodecylimidazolium tetrafluoroborate (IL4) with different contents were added to a polyimide matrix, and a series of polyimide membranes blended with ionic liquid were prepared using a high-speed mixer. The mechanical properties and gas separation permeability of the membranes were investigated. Among them, the selectivity of the PI/IL3membrane for CO2/CH4was 180.55, which was 2.5 times higher than the PI membrane, and its CO2permeability was 16.25 Barrer, which exceeded the Robeson curve in 2008; the separation performance of the membrane was the best in this work.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Liang Fu,Zhenping Qu,Lingling Zhou,Yue Ding
Interface engineering is demonstrated to lead to significant improvement in the catalytic performance for electrochemical CO 2 reduction reactions (CO 2 RR). In this work, we demonstrate a heterogeneous In(OH) 3 -Ag interface catalyst in which the appropriate In(OH) 3 clusters modified on metal Ag nanoparticles surface greatly improves the CO selectivity in CO 2 RR, realizing a CO faradaic efficiency (FE CO ) of 93% at − 0.7 V vs. RHE. The performance enhancement is attributed to the preferentially CO 2 adsorption and activation by the In(OH) 3 -Ag interface sites. In situ Raman spectroscopy reveals that the formation of In(OH) 3 -Ag interface sites is significantly favorable for the generation of key *CO 2 − intermediate at low overpotential. Further theoretical calculation confirms that the In(OH) 3 -Ag interface could enhance the adsorption of *COOH species on catalyst by means of tailoring the surface properties and electronic structures. This work shows that hydroxide-metal interface engineering is a promising pathway to regulate the activity for selective CO 2 RR properties.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Mengyuan Zhang,Li Zhang,Jian Ye,Hailong Li,Ying Qu,Chuandong He,Qiang Niu,Pengfei Zhang
ZnZrO x was a potential catalyst for CO 2 hydrogenation to methanol. However, the micrometer bulky morphology and low surface areas (e.g., <10 m 2 g -1 ) by traditional synthesis methods obstructed their way. This work demonstrated the electrospinning method for fabricating ZnZrOx nanofibers, with 30ZnZrOx-ES showing a significantly higher specific surface area (113.5 m²/g). The CH₃OH yield of 30ZnZrOx-ES was 1.6 times higher than that of 30ZnZrOx-CP, with good stability over 600 hours (300°C, 5 MPa, GHSV = 24,000 mL g⁻¹ h⁻¹). In situ infrared spectroscopy indicated that 30ZnZrO x -ES was easier to produce formates than 30ZnZrO x -CP. DFT calculations and experimental results (EPR, Raman) confirmed that the oxygen-rich surface with abundant oxygen vacancies would enhance H₂ activation of 30ZnZrOx-ES.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Long Cheng,Rong Wang,Ya Wang,Xingxia Yang,Yanxi Deng,Junhua Li
Formic acid (HCOOH) production from direct CO 2 electrolysis is suggested to be one of the most economically viable products. However, its commercial viability remains challenging in highly active and selective electrocatalysts. Here, we report that palladium (Pd) doping has a profound positive impact on the electrocatalytic activity of bismuth oxide (Bi 2 O 3 ). The introduction of Pd increases the current density and Faradaic efficiency of HCOOH (FE HCOOH ) in flow cell system. As a result, the optimized Pd-Bi catalyst exhibits a FE HCOOH of 99.1 % at −0.7 (V vs RHE). Operating experimental studies coupled with theoretical calculations reveal that the Pd modified active sites exhibit near-optimal binding energy for the key *OCHO intermediate, which is more conducive to the generation of formic acid. Furthermore, the use of an asymmetric low-frequency pulsed strategy stabilizes the active sites, ensuring sustained catalytic performance. This study highlights the potential of Pd-doped Bi 2 O 3 as a promising candidate for efficient and selective CO 2 electroreduction to formic acid.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Guangming Wang,Junnan Chen,Ye Qu,Yingjun Dong,Keting Wang,Lihua Qian,Rong Fu,Ying Zhang,Hui-Ming Cheng,Xiaolong Zhang
Electrochemical CO 2 reduction (ECR) to produce chemicals and fuel is a promising technique to build a net-zero carbon circular economy. The performance of ECR has largely advanced in the past decade along with the application of gas diffusion electrodes (GDEs). However, the gas-liquid balance in GDEs is highly fragile due to inefficient CO 2 mass transfer in catalyst layers, which is prone to cause the decay of catalytic performance. In this study, integrated Cu electrodes with controllable mesopores are designed and prepared by copolymer mediated electroless deposition. The optimized Cu electrode shows a selectivity of 81 % (including 65 % for C 2 H 4 ) towards C 2+ products, with a maximum C 2+ partial current density of 232 mA∙cm −2 . Further characterization and simulations reveal that the interconnected mesoporous channels stacked by in-situ reduced Cu nanoparticles leads to an improved CO 2 supply near catalytic sites. In addition, a micro-environment boosting the retention, protonation of *CO intermediates and a unique *CO-CHO coupling step is formed. Our findings provide valuable guidance for enhancing mass transfer and C-C coupling in ECR by creating and controlling intrinsic mesoporous structures in catalyst layers.
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ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Pengxuan Wang,Yuming Gao,Haoyu Yan,Zhengwu Yang,Chaoping Xu,Dawei Tang,Bo Jiang
CO 2 methanation offers a practical solution for sustainable, renewable energy storage and long-term space exploration missions. However, conventional direct solar-driven photothermal systems suffer from thermal response hysteresis and dynamic temperature fluctuations, undermining methane yield stability and limiting their applicability under high gas hourly space velocity (GHSV) conditions. Herein, a round-the-clock CO 2 methanation system is pioneered that integrates photovoltaic power generation with induction heating by a rapid-response electromagnetic metamaterial (EEM), serving as both a catalyst and a susceptor. The EMM assembles single atoms, nanoclusters, and nanotubes into a macrostructure by a 3D-printed strategy and rapidly reaches the methanation temperature of 300 °C within just 36 s at a frequency of 297 kHz with an input power of 461 W, achieving a substantially great CH 4 space-time-yield of 821 mmol g cat −1 h −1 at an ultra-high GHSV of 150 000 mL g cat −1 h −1 . The outdoor photovoltaic-driven induction heating system maintains stable production with a cumulative CH 4 output of 1373.2 L over one week, shielding the system from environmental instability. Notably, this system exhibits a solar-to-chemical energy efficiency of 13% and achieves 20% energy savings compared with conventional electric heating technologies, offering a prospective avenue for efficient and stable CO 2 methanation.
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ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Yaju Xue,Boxia Guo,Xiuling Ji,Bowen Li,Yuhong Huang
Glycine serves as a crucial element in basic metabolic processes and acts as a precursor in the production of numerous industrial chemicals. Here we developed a streamlined artificial cascade enzyme catalysis pathway for converting CO2 into glycine through improving the CO2 activation and employing direct C–C condensation. After the optimization of enzyme combinations and dose-dependent regulation, the integration of reduced nicotinamide adenine dinucleotide regeneration and ionic liquids were introduced and facilitated the construction of an artificial cascade ionozyme catalysis system. Consequently, the glycine yield reached a remarkable 17.87-fold increase compared to that of the initial reaction system. Additional molecular simulations further demonstrated that the ionozyme possessed enhanced structural stability and substrate affinity, as indicated by an increase in hydrogen bonds and a diminished interference from water molecules in protein–ligand binding. This innovative approach holds great promise for sustainable CO2 bioconversion to glycine and other valuable chemicals.
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Catalysis Science & Technology
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2025
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IF 4.2
Sizhuo Chen,Haoyu Wang,Zhuoyang Fang,Shuang Song,Jie Gao,Weiting Yu
The electrochemical reduction of CO2 (CO2RR) to CO is a highly promising strategy for addressing both environmental and energy challenges. Identifying catalysts with excellent catalytic performance in CO2RR and facile preparation procedures is currently a hot research topic. Herein, a unique series of halogen‐containing polymorphic AgX (X = Cl, Br, I) nanocatalysts with high CO selectivity, activity, and stability in CO2RR have been synthesized via a one-step wet chemical co-precipitation method. A combination of DFT calculations and electrochemical measurements has illustrated that halogen element doping turns the d-band center of Ag shifting closer to the Fermi level, facilitates the interaction between the *COOH intermediate and the catalyst, lowers Gibbs free energy difference (ΔG) for the rate-determining step, and achieves enhanced CO2RR efficiency (CO faradaic efficiency at 93.24%). This study highlighted halogen doping as a strategy for designing efficient and stable electrocatalysts.
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Algal Research-Biomass Biofuels and Bioproducts
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2025
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IF 4.5
Jirong Long,Wenguang Zhou,Jing Cao,Yuxuan Mao,Peilun Xu,Jin Liu,Yanghong Yao,Chenguang Wang,Yong Liu
Sporopollenin is a chemically robust biopolymer known for its resistance to environmental degradation and diverse functional potential. This study pioneers the successful extraction of sporopollenin from Chlorella vulgaris cultured in coal-fired flue gas using an innovative alkali-acid two-stage protocol. Multiscale characterization revealed that, despite its irregular morphology, microalgal sporopollenin shares high structural similarity with pollen-derived counterparts. Fourier-transform infrared spectroscopy and elemental analysis confirmed similar functional groups and elemental profiles. Liquid chromatography–mass spectrometry and pyrolysis–gas chromatography–mass spectrometry identified fatty acids as the major structural units, while solid-state 13 C SSNMR spectroscopy revealed a hybrid architecture comprising aliphatic, aromatic, and heterocyclic components. These findings provide molecular insight into the evolutionary continuity of sporopollenin and highlight a scalable, green approach for transforming industrial emissions into high-value biomaterials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Ning Zhang,Yingmei Meng,Zhiying Li,Chuanlong Jin,Junjiang Bao,Xiaopeng Zhang,Gaohong He
High free-volume microporous membranes constructed by intrinsically microporous polymers (PIMs) are up-and-coming in efficient carbon capture, but their practical applications are limited by plasticization and physical aging issues. This work we proposed a CO 2 -solution-compensated cross-linking strategy to construct microporous membranes with both crosslinking network and enhanced CO 2 solubility via the Hoffmann alkylation reaction between the bromomethylated PIM matrix and Ethylenediamine (EDA) only at 80 °C. The enhanced CO 2 solubility could compensate the reduced CO 2 diffusion by the crosslinking network. Accordingly, the crosslinked microporous membranes with CO 2 -solubility compensation achieved a superior decarbonization from natrual gas (CO 2 permeability of 898.9 Barrer, CO 2 /CH 4 separation factors of 204.1) surpassing the 2019 Robeson upper and excellent anti-plasticization (plasticizing pressure up to 0.8 MPa) and anti-aging (CO 2 permeability loss < 10 % after 30 days) performance. The CO 2 -solubility-compensation crosslinking strategy will promote the development of high-performance microporous membrane for efficient decarbonization.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Bei Liu,Mingxing Zhou,Zhinan Wu,Xulong Song,Tong Zhou,Shipeng Cao,Chongjian Jiang,Xinwei Zhang,Xiwen Zhang,Liwen Mu,Han Lin,Xiaohua Lu,Tuo Ji,Shuandi Hou,Jiahua Zhu
Amine-based sorbents are promising for low-concentration CO 2 capture, yet their practical application has long been hindered by poor stability. In this study, amidated tetraethylenepentamine (TEPA) network (ATN) sorbents were synthesized by crosslinking TEPA with 4 binary organic acids in the molded alumina-silica (MAS) supports. Characterizations confirm the successful formation of amide bonds between the primary amines of TEPA and binary acids within the pore channels, a key innovation that reconfigures TEPA distribution—shifting from a wall-attached state (as in conventional systems) to an aggregated polymeric network. This structural breakthrough yields remarkable stability enhancements: unlike TEPA/MAS, which loses ∼90 % of its initial capacity after 50 cycles, TEPA/MAS- t , t -MA, and TEPA/MAS-FA retain ∼80 % of their capacity under the same conditions. Experimental results and DFT calculations further reveal a novel mechanistic insight: acids containing double bonds form more stable amide networks with stronger p-π conjugation than straight-chain acids. By integrating molecular crosslinking with porous support engineering, this strategy offers a robust framework for designing durable, high-performance CO 2 capture materials for actual applications.
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Science China-Chemistry
·
2025
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IF 9.7
Li Ran,Yin Hang,Jing Wen-Kai,Cheng Jia-Lin,Qin Xue-Rong,Lu Tong-Bu,Wang Hong-Juan,Yu Zi-You
As important catalysts for C–C coupling, copper-based materials have great potential for electrocatalytic reduction of CO 2 to C 2+ products. In this work, Cu 2 O catalysts modified with different lanthanide hydroxides were successfully synthesized and used for CO 2 electroreduction. The results showed that compared with Cu 2 O/Gd(OH) 3 and Cu 2 O/Yb(OH) 3 catalysts, Cu 2 O/La(OH) 3 exhibited the highest electrocatalytic performance for CO 2 reduction. This catalyst was able to maintain a high Faraday efficiency for C 2+ products ( \({\rm FE}_{{\rm C}_{2+}}\) ) of about 60% within the current density range of 400–800 mA cm −2 . The highest \({\rm FE}_{{\rm C}_{2+}}\) reached 66% at 600 mA cm −2 and the partial current density for C 2+ products reached a maximum of 488 mA cm −2 . Meanwhile, the catalyst could run stably for 40 h with a remained \({\rm FE}_{{\rm C}_{2+}}\) of about 60%. Multiple characterizations reveal that the introduction of La(OH) 3 promotes the formation of *CO intermediates, and also helps to stabilize the Cu(I) species in Cu 2 O under cathodic potentials, thus facilitating the C–C coupling for C 2+ production. This work provides a new strategy to enhance the C 2+ production via stabilizing Cu(I).
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