Greenhouse Gases-Science and Technology
·
2015
·Vol. 5
·期 5
·682-694
·
IF 2.147
Tao Wang,Wei Yu,Mengxiang Fang,Hui He,Qunyang Xiang,Qinhui Ma,Menglin Xia,Zhongyang Luo,Kefa Cen
Nanoparticles suspended in solutions are considered to have the potential to enhance gas-liquid mass transfer and have been studied for gas separation. In order to reveal the mechanisms of kinetics enhancement, the diffusion and reaction process should be carefully examined. In this paper, CO 2 absorption kinetics of amine-based solutions with additive of SiO 2 and Al 2 O 3 nanoparticles were investigated by wetted-wall column experiments. Measurements at different conditions, including solid loading, pressure, and solvent flow rate, show a significant enhancement on CO 2 absorption kinetics. The experiment and model analysis indicate that the micro convective motion induced by particle Brownian movement plays a primary role in mass transfer enhancement. Three solutions, MEA, MDEA, and PZ which have different kinetics were selected to study the impact of nanoparticles on absorption kinetics of solutions with different reaction rate. It is interesting to find that the increased ratio of absorption kinetics by nanoparticle follows the same order with increased solvent reaction rate with CO 2 , which is PZ > MEA > MDEA. The wetted-wall kinetic model indicates that a diffusion controlled kinetics for PZ solution could result in much more significant kinetic enhancement with additives of nanoparticles. By operation conditions optimization, the liquid side mass transfer rate of MEA solution can be increased over 15%.© 2015 Society of Chemical Industry and John Wiley & Sons, Ltd
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KEY ENGINEERING MATERIALS
·
2015
·
IF 0
Peng Peng Lv,Feng Wang,Yu Hai Guo,Hong Yan Tang
In this study, hydrophilic PTFE hollow fiber membranes were prepared and applied for CO2 desorption via a membrane flash process, which is a new CO2 desorption process by utilizing waste thermal energy. The methyldiethanolamine was selected as the absorbent. Effects of the flashing temperature, flashing pressure, rich solution flow rate and MDEA concentration on CO2 release ratio and CO2 desorption flux were deeply investigated. The results show that flashing temperature is positive to the CO2 release ratio and CO2 desorption flux. However, the flashing pressure, rich solution flow rate and MDEA concentration are negative to the CO2 release ratio and CO2 desorption flux.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 6
·1504-1511
·
IF 2.726
He Kai,Liu Shijia,Zhao Guiyan,Qin Yucai,Bi Yanfeng,Song Lijuan
A series of Ni-W catalysts supported on mesoporous SBA-15 with different Ni:W ratios(Ni x W/SBA-15, Ni-5%, x =1, 10, 50) was prepared and fully characterized by powder X-ray diffraction(PXRD), Brunner-Emmet-Teller(BET), transmission electronic microscopy(TEM), H 2 -temperature programmed reduction(H 2 -TPR), and X-ray photoelectron spectroscopy(XPS). High-resolution TEM images, XPS measurements, H 2 -TPR experiments coupled with PXRD results determined the evolution of Ni and W species. It is found that a trace amount of W from H 2 WO 4 can significantly improve Ni dispersion on SBA-15 (Ni 50 W/SBA-15) with Ni 0 and non-stoichiometric WO x species as small as ca . 3.6 nm. The prepared Ni x W/SBA-15 was utilized for CO 2 hydrogenation, which showed that a higher W content restrained the CO 2 hydrogenation while a lower W ratio promoted both conversion rate and selectivity for methane compared with Ni/SBA-15. The Ni 50 W/SBA-15 catalyst showed the best performance with a 93.3% CO 2 conversion rate and 99.7% selectivity for methane at 400 o C under 0.1 MPa and maintained ca . 97% initial performance for 24 h. Tracking product evolution experiments by in-situ Fourier transform infrared spectrascopy(FTIR) indicated that a small amount of W can modify the surface of Ni particles by geometric coverage and electronic modification, which facilitates the adsorption of the CO intermedia and results in the formation of CH 4 . This work provides a new clue to fabricating efficient CO 2 conversion bimetallic materials.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Haozhan Chu,Guoxiong Zhan,Kuilin Peng,Yinge Bai,Pengfei Gao,Hongyu Zhang,Zehua Wei,Xiangping Zhang,Shaojuan Zeng
Ionic liquids (ILs) show great potential for carbon dioxide (CO2) capture due to their designable structures and dual roles as absorbents and catalysts. Our previously designed IL solvent ([Cho][Triz]/TMS) showed good absorption performance but a slow regeneration rate. Here, a novel strategy to promote CO2 desorption in IL absorbents at lower temperatures using homogeneous Lewis acid IL (LAIL) catalysts was proposed. The cobalt (Co)-based LAIL [Bmim]2[CoCl4] exhibited superior performance, with the CO2 desorption amount enhanced by 54.1% and activation energy reduced by 30.3% compared with the blank test, leading to low regeneration energy consumption (0.90 GJ/t CO2), which was ascribed to a simultaneous increase in Brønsted and Lewis acid sites, promoting C–N bond cleavage by C2–H in [Bmim]22+ and Co sites in [CoCl4]2–. The environmental impact of IL-based CO2 capture processes, evaluated by the green degree method, demonstrated that the green degree production value of the IL-LAIL system is 79.6 and 673.6 gd/h higher than that of the IL and MEA systems, respectively, indicating greater environmental sustainability. This study provides a viable strategy for employing homogeneous catalysts to facilitate energy-efficient CO2 capture.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Ning-Ya Wang,Yi-Hong Liu,Xiao-Jie Jiang,Hui-Li Guo,Li-Xiao Wang,Bei-Bei Li,Xue Liu,Xiao-Bo Zheng,Jing-Yu Pang,Dong-Bin Dang,Yan Bai
The catalytic activity of single-atom catalysts (SACs) is strongly influenced by their local coordination environment. In this study, a series of Mn-N-C SACs with tunable coordination structures were synthesized via pyrolysis of Mn-doped metal-organic frameworks (MOFs) at different temperatures. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption spectroscopy (XANES and EXAFS) confirmed the atomic dispersion of Mn and the formation of Mn-N 4 moieties as the active sites. Among the catalysts, Mn-NC-1000°C with high Pyridine-N content exhibited the best performance, achieving a maximum Faradaic efficiency (FE) of 94.9% for CO at –0.47 V vs. RHE in an H-type cell, along with a current density of ∼15 mA . cm −2 . And in a flow cell, the current density increased significantly to ∼100 mA . cm −2 while maintaining high CO selectivity (FE CO =95%) and operational stability (24 h). The density functional theory (DFT) studies further reveal that the Mn-NC-1000°C with high Pyridine-N content effectively reduces the reaction barriers for the formation of *COOH and thus accelerates the reduction of CO 2 .This work provides a controllable strategy for regulating the coordination microenvironment of SACs and offers valuable insights for the development of efficient CO 2 electroreduction system.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhipeng Qie,Minghui Hu,Wenqi He,Yao Zhang,Zhongbao Liu,Huaizhong Xiang,Zepeng Wang,Dafeng Yang,Shuyi Yao,Xinxin Pi,Hongxing Dai
Capturing CO 2 from humid flue gas remains a major challenge due to the severe competitive adsorption between CO 2 and H 2 O on zeolites. In this study, a novel chelation-assisted K + ion exchange strategy was proposed to simultaneously enhance both the CO 2 adsorption capacity and moisture resistance of mordenite (MOR) zeolites. Compared to the conventional ion exchange, this approach induced the mild surface dealumination, effectively removed the hydrophilic extra-framework Al(VI), and increased the K + exchange content. Structural refinement revealed that in the resulting MOR-EDTA-2K sample, K + ions were distributed in both the 12-membered ring (12MR) channels and the 8MR side pockets, which favored CO 2 adsorption. MOR-EDTA-2K achieved comparable uptake of 15 vol% CO 2 (46 mg/g) but with lower H 2 O uptake than conventional ion-exchange derived MOR sample, resulting in an improved CO 2 /H 2 O selectivity. Furthermore, DRIFTS analysis confirmed a mechanistic shift in CO 2 adsorption status from the HCO 3 − to CO 3 2− species, attributed to the inhibited water adsorption on MOR-EDTA-2K. For practical application, monolithic adsorbents prepared with MOR-EDTA-2K demonstrated prolonged CO 2 breakthrough time, excellent cyclic stability, and well regeneration at 75 °C. This facile and scalable method, with the advantage of low-temperature regeneration, renders the prepared zeolite a highly promising candidate for industrial CO 2 capture under humid conditions.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Qingnan Wang,Yueyangchao Yu,Longjie Liu,Yi Ye,Xinglei Zhao,Chongshan Yin,Bin Liu,Shaofei Wang
Efficient separation of CO 2 from CH 4 is a critical unit operation for biogas upgrading and achieving carbon neutrality goals. While mixed-matrix membranes (MMMs) offer an energy-efficient alternative to traditional separation processes, their industrial deployment is often restricted by engineering challenges, specifically filler agglomeration and non-selective interfacial defects. Herein, we report a novel MOF (metal–organic framework) gel network templated polymerization strategy that effectively circumvents these limitations. In this approach, a continuous, pre-formed network of UiO-66 MOF gel serves as a structural scaffold, within which the 6FDA-ODA polyimide matrix is directly polymerized. This method fosters exceptional interfacial adhesion and uniform dispersion of the filler, successfully eliminating non-selective defects. The resulting MMMs exhibit remarkable gas separation performance, with the optimal membrane (MA-0.075, with 1.6 wt% UiO-66 gel loading) achieving a CO 2 permeability of 30.9 Barrer and a CO 2 /CH 4 selectivity of 135.5 under mixed-gas conditions. This represents enhancements of 212 % and 162 %, respectively, over the pristine 6FDA-ODA polyimide membrane, surpassing the 2008 Robeson upper bound. Furthermore, the membrane demonstrated excellent operational stability over 120 h. This work provides a scalable fabrication route for advanced MMMs, demonstrating significant potential for energy-efficient gas separation applications.
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JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Yingnan Ma,Zhen Xu,Yulu Zhang,Zixuan Guo,Juan Chen,Panliang Zhang,Kewen Tang
This study innovatively proposed an in-situ confined polymerization strategy of trimesoyl chloride (TMC) and piperazine (PIP) within MOFs nanosheets, successfully constructing a thin film nanocomposite (TFN) separation membrane with excellent interfacial compatibility. The method employed MOFs nanosheets as confined templates to achieve bottom-up in-situ construction of a continuous and dense polyamide matrix. By precisely controlling the number of polymerization cycles, the MOFs content in the functional layer was effectively regulated from 83.3 wt% to 42.6 wt%. Benefiting from the molecular-level interfacial compatibility between MOFs and the polymer phase, as well as the synergistic effect of efficient solution diffusion and fine molecular sieving mechanisms, the TFN membranes demonstrated significantly enhanced CO 2 separation performance, CO 2 permeance reached 1688.3 GPU with selectivities of 36.4 for CO 2 /N 2 and 38.9 for CO 2 /CH 4 , which surpassed the Upper bound (2008 and 2019). The TFN membranes exhibited outstanding long-term operational stability (selectivity fluctuation <3.6%) under rigorous conditions including prolonged 14-day continuous testing and variable temperature (35-75 °C) and pressure (0.1-0.5 MPa) conditions. This work provided a new paradigm for the precise design and scalable fabrication of gas separation membranes, opening new avenues for the development of high-performance separation membranes.
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JOURNAL OF CATALYSIS
·
2026
·
IF 6
Mufan Niu,Qiyu Sun,Chongbin Wei,Fubin Peng,Xiaohe Huang,Han Yang,Ying Cui,Shenyong Ren,Chunming Xu,Baojian Shen
To elucidate the active sites and reaction mechanism of CrO x /ZrO 2 catalysts in CO 2 -assisted oxidative dehydrogenation (CO 2 -ODH) of ethane, a combination of multiple characterization techniques, DFT calculations, and in situ FTIR spectroscopy was employed. Results reveal the coexistence of isolated and polymeric Cr 6+ species on the catalyst surface, with catalytic activity exhibiting a strong positive correlation with the content of polymeric Cr 6+ , confirming its role as the key active component. Further investigation uncovers a distinct and strong electronic interaction between CrO x and ZrO 2 that facilitates the formation and stabilization of polymeric Cr 6+ . This interaction is absent in CrO x /CeO 2 and CrO x /TiO 2 systems, offering a theoretical rationale for the rational design of catalyst supports. Mechanistically, CO 2 plays a dual role: it participates in both ethane ODH and the RWGS reaction, and reoxidizes coordinatively unsaturated Cr 3+ to Cr 6+ , thereby enhancing reaction stability. This work elucidates the CO 2 -ODH pathway and the regulatory role of CO 2 , offering new insights into the design of active sites in CrO x -based catalysts. However, pronounced catalyst deactivation currently limits industrial application, highlighting the need for future efforts to focus on improving catalyst stability.
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Solar RRL
·
2026
·Vol. 10
·期 2
·e202500917
·
IF 4.7
Lu Peng,Qiang Li,Siting Shao,Meng Zhang,Hongpeng Jia
The escalating CO 2 concentration and energy demand necessitate efficient CO 2 conversion strategies. Photothermal catalytic CO 2 methanation is a promising strategy, yet its efficiency is hindered by the inherent stability of CO 2 and the rapid recombination of photogenerated charge carriers. Among non-noble metal catalysts, Ni-based catalyst is a promising candidate for CO 2 methanation, with sintering and agglomeration remaining to be addressed. Herein, NiMn/TiO 2 bimetallic catalysts with varying Ni/Mn ratios were synthesized to overcome these issues. Characterization results demonstrate that Mn incorporation enhances CO 2 adsorption capacity by increasing oxygen vacancies and significantly improves the separation efficiency of photogenerated carriers. Furthermore, Mn doping optimizes the electronic structure of the catalyst, narrowing its bandgap for improved light absorption. But the catalytic performance is highly dependent on the Ni/Mn ratio. The synergistic effect of Ni and Mn can be maximized when the Ni/Mn ratio is 1:1, which is specifically manifested as the best catalytic activity. Excessive Mn loading covers active Ni sites and impedes electron transfer, thereby degrading activity. Therefore, this work highlights the importance of Mn as a promoter in designing efficient non-noble metal catalysts for photothermal CO 2 conversion.
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Small
·
2026
·
IF 12.1
Yu Liu,Yi Xin,Teng Zhang,Yunlong Li,Junhong Jian,Shoufu Cao,Jian Luan,Xiaosa Zhang,Wenze Li,Wei Qi
Tailoring bimetallic synergy in azo-functionalized porous organic polymers for enhanced electrocatalytic CO 2 reduction porous organic polymers (POPs) have emerged as promising candidates for electrocatalytic applications due to their structural tunability and high surface areas. In this study, we report a coordination-driven assembly strategy to construct a Cu/Co bimetallic azo-phenolic polymer (denoted as Cu@Azo-CoPG) through chelation of azo-phenolic motifs with Cu 2 + ions. Systematic evaluation reveals that the bimetallic Cu@Azo-CoPG outperforms its monometallic counterparts (Cu-PG and Co-PG) in CO 2 reduction reaction (CO 2 RR), achieving a remarkable CO Faraday efficiency (FE CO ) of 94.3%. First-principles calculations elucidate that the Cu─Co dual sites synergistically modulate reaction energetics: the Co center lowers the energy barrier for * COOH intermediate formation, while adjacent Cu sites facilitate CO desorption. This work establishes a design paradigm where the electronic interplay between heterometallic sites in POPs enhances both CO 2 adsorption/activation and product desorption kinetics, offering new insights into the rational engineering of dual-active-site catalysts for sustainable energy conversion.
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高影响因子
ADVANCED MATERIALS
·
2026
·
IF 26.8
Kangwang Wang,Jie Zhan,Jun Liu,Zaichen Xiang,Wanyi Zhang,Lingyong Zeng,Kai Yan,Yan Sun,Huixia Luo
The photochemical CO 2 reduction reaction (CRR) represents a zero-carbon pathway for converting CO 2 into value-added chemicals, yet its industrial implementation has been constrained by low selectivity and product diversity. Dirac nodal arc semimetals characterized by ultrahigh carrier mobility (>25 000 cm 2 ·V −1 ·s −1 ) offer a promising platform to search for efficient catalysts for CO 2 conversion. Herein, we demonstrate that strategic Pt incorporation into PdSn 4 optimizes the electronic structure and carrier dynamics of this Dirac semimetal. Experimental and theoretical analyses reveal that the resulting Pd─Sn─Pt local electronic structure redistributes charge density around Pd and Pt atoms, which facilitates C─C coupling via *OC─COH and *OC─CHOH intermediates and enhances carrier mobility by 40% versus the pristine PdSn 4 single crystal. The optimized Pd 0.4 Pt 0.6 Sn 4 single crystal achieves C 2 H 4 i) formation rate of 328 µmol∙g −1 ∙h −1 ; ii) product selectivity of 73.1%; iii) electron-based selectivity of 89%. This work establishes electronic-structure-tunable Dirac semimetals as a new paradigm for multi-carbon photochemical CO 2 reduction, providing a design strategy for next-generation photocatalysts.
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