POLYMER
·
2024
·
IF 4.1
Biao Li,Hao Li,Dexuan Xiang,Yuejun Ouyang,Jingao Wu,Gui Chen,Zaixing Zhang,Hongwei Lin,Nonglin Zhou
Converting CO 2 into precious chemicals is considered to be a fundamental and effective tool for controlling the abundant CO 2 emitted. One of the most compelling methods for CO 2 conversion is the synthesis of cyclic carbonates by cycloaddition of CO 2 with epoxides. However, the development of materials with specific functionalities for CO 2 capture and conversion is still considered to be a significant challenge. Herein, a novel imidazolium salts and pyridine skeleton bifunctionalized hypercrosslinked polymers were prepared by FeCl 3 -catalyted Friedel-Crafts alkylation reaction. Various analytical techniques were used to investigate the properties of the catalysts. The bifunctionalized heterogeneous catalysts exhibited outstanding catalytic performances for CO 2 cycloaddition under mild conditions with an excellent yield of up to 99 %. Besides, the catalyst could bear various epoxides and no significant loss of activity after 6 cycles. The properties of metal-free, solvent-free, cocatalyst-free, easy-to-prepare, mild conditions, facility separation and recyclability make the bifunctionalized hypercrosslinked polymers useful for CO 2 cycloaddition.
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Greenhouse Gases-Science and Technology
·
2024
·
IF 2.7
Fa-Ping Liu,Ai-Rong Li,Cheng Wang,Yu-Ling Ma
CO 2 hydrate technology can be applied to seawater desalination. However, the kinetics of CO 2 hydrate formation were inhibited in the aqueous solution with inorganic salts, and the kinetic mechanism of CO 2 hydrate formation for inorganic salts with different metal cations and anions was still unclear. In this work, CO 2 hydrate nucleation and growth were studied in aqueous solutions of metal chlorides. Instead of Na + and K + ions, CO 2 hydrate nucleation was promoted in the presence of Ni 2+ , Mn 2+ , Zn 2+ and Fe 3+ ions due to the co-ordination bonds between transition metal ions and water molecules to enhance the formation of the critical crystal nuclei. The induction time was increased by 61.1% in aqueous solution with 0.32 mol/L NaCl, while it was shortened by 55.6% in FeCl 3 aqueous solution at the same concentration of Cl − anions. In the process of CO 2 hydrate growth, Cl − ions played a more important role than the metal ions in affecting the stability of CO 2 hydrate cages. The gas storage capacity was reduced by 10.3% in the presence of NaCl, and was lower than that of other metal chlorides. Cl − anions were absorbed on the hydrate surface and involved in hydrate cages to inhibit the hydrate growth due to the hydrogen bonds between the Cl − ions and water molecules of the hydrate cages. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Tianyue Wang,Jia Liu,Bining Tian,Lulu Yan,Zhanfeng Li,Yue Tian
Engineering surface reaction kinetics plays a vital role in promoting CO2 photoreduction reaction (CO2 PRR) efficiency but remains formidably challenging. Here, we demonstrate that the regulation of the surface oxidation state is an effective strategy for the unification of the adsorption sites and reactive centers, which significantly improves the reaction kinetics and CO2 PRR efficiency. Taking advantage of the concept, we further propose p–p orbital hybridization between P atoms and the adjacent O atoms in BiVO4 at the interface constructed in the O-RP/BiVO4 Z-scheme heterostructure to create the oxidation state of RP. Theoretical calculations and spectral characterizations reveal that the interfacial atomic orbital hybridization lowers the CO2 activation energy barrier through the stabilization of the COOH* intermediate and facilitates the charge separation and transfer. Consequently, the optimized photocatalyst exhibits an excellent performance for sacrificial reagent-free CO2 PRR, with a production rate of 208 and 26.2 μmol g–1 h–1 for CO and CH4, respectively, ca. 21-fold higher than that of pristine RP and topping most of the hybrid photocatalysts with a noble metal as cocatalysts. This work provides critical insight for the design of high-efficiency photocatalysts for CO2 PRR.
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ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Xianghai Song,Xiaoying Liu,Zhixiang Ren,Xiang Liu,Mei Wang,Yuanfeng Wu,Weiqiang Zhou,Zhi Zhu,Pengwei Huo
Photocatalytic carbon dioxide (CO 2 ) reduction represents a hopeful approach to addressing global energy and environmental issues. The quest for catalysts that demonstrate both high activity and selectivity for CO 2 conversion has attracted significant attention. In this study, ultrathin N-doped BiOBr was synthesized using a simple straightforward method. Systematic experimental results indicated that N-doping reduced the thickness of the BiOBr nanosheets and increased their specific surface area. Moreover, the efficiency of photogenerated charge carrier migration and the CO 2 adsorption capacity were significantly enhanced, contributing to improved CO 2 photoreduction performance. Experimental results showed that the 2N-BiOBr exhibited the best catalytic performance, with a CO evolution rate of 18.28 μmol·g −1 ·h −1 and nearly 100% CO selectivity in water, which was three times higher than that of pure BiOBr. The potential photocatalytic mechanism was investigated using in situ FTIR analysis and DFT simulations. Mechanistic studies revealed that N atoms replaced O atoms as adsorption centers, enhancing the strong adsorption selectivity towards CO 2 over O–H in BiOBr and facilitating the formation of key reaction intermediates. This study provides new perspectives on the creation and developmen of effective photocatalytic materials, offering theoretical support for the application of photocatalytic technology in energy and environmental science.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xianghui Zeng,Hui Chen,Wei Fang,Zhaohui Huang,Daheng Wang,Xuan He,Xing Du,Weixin Li,Haijun Zhang,Lei Zhao
CO 2 photoreduction into highly value-added chemicals over metal-free h -BCN has emerged as a promising strategy to address the issue of global warming. However, the serious carrier recombination caused by disordered charger transfer has limited its practical application. To circumvent this issue, fluorine modified h -BCN were synthesized using a facile heat treatment method. The surface halogenation created local spatial polarized electric field, which facilitated the local charge separation and transmission efficiency. Among them, BCN-F-4 exhibited the best photocatalytic CO 2 reduction activitiy with CO and CH 4 yield of 25.38 and 14.11 µmol g −1 h −1 , respectively. The turnover number (TON) of BCN-F-4 reached up to 163.6 μmol g −1 h −1 , 4.4 times that of BCN. Both theoretical simulation and experimental analysis demonstrated a strong covalent interaction between the F atoms and the h -BCN matrix, which gain deep understanding of the mechanism of prominent photocatalytic CO 2 reduction activity boosted by surface halogenation.
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JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Tao Chen,Fei Shan,Lingting Ye,Kui Xie
Due to their excellent high Faraday efficiency, perovskite solid oxide cells (SOECs) have attracted considerable attention. Nevertheless, they still face significant challenges in terms of stability and electrocatalytic activity during CO₂ electrolysis. In this study, Ni particles in La 0.65 Ba 0.35 Mn 1-x Ni x O 3-δ are successfully separated by a unique in-situ exsolved method of metal nanoparticles, which are uniformly anchored to the electrode surface as Ni nanometal particles. This effectively suppresses the generation of carbon deposits on the cathode surface. Under test conditions of 850 °C, 1.6 V and 50 sccm flow rate, the CO yield of the modified cathode material reached 5.9 mL min −1 cm −2 , which is nearly four times higher than that before doping. The synergistic effect of in-situ exsolution of Ni metal nanoparticles with oxygen defects generated by the perovskite, creating more active locations for CO 2 adsorption and electrolysis, is responsible for the significant improvement in electrochemical performance. This work provides new strategies and ideas for the development of efficient and durable SOEC cathode materials.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
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IF 8.4
Yanting Tang,Qingnan Wang,Xiaohe Tian,Chenlu Liu,Keming Zhang,Xiaoting Feng,Rui Zhang,Yueyangchao Yu,Shaofei Wang
Covalent organic frameworks (COFs), characterized by their well-organized porous structure, exhibit promising prospects for carbon capture. Nevertheless, their weak film-forming property and relatively large pore sizes constrain their utilization as gas separation membranes. This study introduced a facile approach to fabricating COF membranes tailored for CO 2 separations. By introducing an extra monomer, trimesoyl chloride (TMC), together with COF monomers, a thin and defect-free layer of COF-polyamide was synthesized by interfacial polymerization process. The amide structure embedded into the COFs layers was expected to mend the defects, strengthen the binding forces, and improve the stability of the COFs layers. To further enhance the performance, imidazolium ionic liquid (IL) was adopted to modify the COF-polyamide layer. The introduction of TMC rendered the COF-polyamide layer more negatively charged, facilitating stronger binding to the positively charged cations in the IL. This modification with IL effectively reduced the pore size of the COFs and increased the affinity for CO 2 . The resultant COF composite membranes exhibited a high CO 2 permeance of 125.9 GPU and CO 2 /N 2 selectivity up to 35.0, accompanied by robust long-term stability. Our method paves a new way for the fabrication and application of interfacial polymerized COF membranes for gas separation applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Gangan Wang,Chaoyi Chen,Junqi Li,Yuanpei Lan,Xin Lin
Red mud and carbide slag, strongly alkaline solid wastes, are produced during the manufacturing of alumina and acetylene gas, respectively. Improper management of these wastes can pose significant environmental hazards. This study proposed a novel method for the collaborative treatment of red mud and carbide slag, enabling the recovery of constituent elements with CO 2 sequestration. During the hydrochloric acid leaching process, Si was reclaimed as Si-rich residue, whereas Ti, Al, Ga, Fe, and Sc were stepwise recovered as Ti-rich product, Al/Ga-rich filtrate, and Fe/Sc-rich product via the subsequent hydrolysis, co-precipitation, and alkali leaching processes, respectively. Utilizing carbide slag to replace the energy-intensive NaOH for pH adjustment in the leaching solution resulted in a Ca 2+ concentration of 21,922 mg/L in the filtrate after co-precipitation. Through further mineralization process, CO 2 sequestration was achieved alongside the production of CaCO 3 with the content reaching 98.5 % along with a whiteness of 94.4 %. Furthermore, by adjusting the experimental parameters in the mineralization process, controlled manipulation of the phase and morphology of the CaCO 3 product could be achieved to meet various industry requirements. To summarize, the complete resource recovery of red mud and carbide slag was achieved in this study, demonstrating the promising potential in practical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Zezhong Xie,Qiushi Wang,Rongge Yang,Jingnan Zhang,Shanqiang Ou,Gangfeng Ouyang,Mingyang Li,Jianxin Shi,Yexiang Tong
Local pH near the catalyst surface exerts a substantial influence on both catalytic selectivity and activity in electrocatalytic CO 2 reduction (CO 2 RR). While the investigation of local pH remains challenging in the aspect of in-situ imaging and monitoring. In this study, a novel lateral-type surface-enhanced Raman spectroscopy (L-SERS) system with a wide pH testing range from acidic to alkaline, is developed for the in-situ observation of local pH distributions with high spatial and temporal resolution during CO 2 RR. Excellent in-situ imaging of local pH near the catalyst surface is obtained, showing good consistency with simulation results. Besides, the gradual pH elevation and stabilization can be monitored via this time-resolved local pH investigation. This study presents a direct visualization of local pH distribution and variation at the Nernst layer during CO 2 RR, providing direct evidence in local pH for the feasibility of acidic electrolyte and offering theoretical guidance for optimizing CO 2 RR conditions.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-15
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IF 15.7
Xu Ting,Yang Hao,Lu Tianrui,Zhong Rui,Lv Jing-Jing,Zhu Shaojun,Zhang Mingming,Wang Zheng-Jun,Yuan Yifei,Li Jun,Wang Jichang,Jin Huile,Pan Shuang,Wang Xin,Cheng Tao,Wang Shun
Creating and maintaining a favorable microenvironment for electrocatalytic CO 2 reduction reaction (eCO 2 RR) is challenging due to the vigorous interactions with both gas and electrolyte solution during the electrocatalysis. Herein, to boost the performance of eCO 2 RR, a unique synthetic method that deploys the in situ reduction of precoated precursors is developed to produce activated Ag nanoparticles (NPs) within the gas diffusion layer (GDL), where the thus-obtained Ag NPs-Skeleton can block direct contact between the active Ag sites and electrolyte. Specifically, compared to the conventional surface loading mode in the acidic media, our freestanding and binder free electrode can achieve obvious higher CO selectivity of 94%, CO production rate of 23.3 mol g −1 h −1 , single-pass CO 2 conversion of 58.6%, and enhanced long-term stability of 8 hours. Our study shows that delivering catalysts within the GDL does not only gain the desired physical protection from GDL skeleton to achieve a superior local microenvironment for more efficient pH-universal eCO 2 RR, but also manifests the pore structures to effectively address gas accumulation and flood issues.
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PubMed
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zikang Qin,Yulei Ma,Wentao Du,Jing Wei,Jia Song,Xinyue Fan,Lu Yao,Lin Yang,Yuanfa Zhuang,Wenju Jiang,Zhongde Dai
Amine-functionalized Metal-Organic Frameworks (MOFs) stand out as highly promising materials in membrane separation technology. Nevertheless, the incorporation of amine-functionalized additives may lead to uncontrollable alterations in MOF morphology. Two intact blade-like MOFs (PEI (Polyethylenimine)-ZIF-L and PAMAM (Polyamidoamine)-ZIF-L) were successfully synthesized by controlling the conditions and then introduced into Pebax 2533 to fabricate Mixed Matrix Membranes (MMMs). Hydrogen bonding and other interactions with Pebax can be formed by PEI-ZIF-L and PAMAM-ZIF-L to enhance interfacial compatibility. Simultaneously, a reversible reaction with CO 2 molecules can be undergone by the amine groups, resulting in facilitated transport in MMMs. The CO 2 separation performance of the MMMs is enhanced by this process, with the facilitation being more pronounced under humid conditions. Under humid conditions, the CO 2 permeabilities of Pebax-PEI-ZIF-L (2 wt%) and Pebax-PAMAM-ZIF-L (2 wt%) MMMs were 639.4 Barrer and 702.7 Barrer, respectively, while the CO 2 /N 2 selectivities were 26.68 and 24.35, respectively. Both permeability and selectivity exhibited a significant increase of 200% and 130%, respectively, compared to pure Pebax. Furthermore, the MMMs demonstrated excellent long-term stability during 72 h of continuous operation in a humid environment, showcasing significant potential for industrial applications, particularly in humid flue gas carbon capture.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
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IF 5.4
Guanhua Zhang,Shaocong Mo,Xiaowei Liao,Feng Liu,Hongtao Xu,Wei Lu
Metal-organic frameworks (MOFs) are interesting materials for carbon dioxide (CO 2 ) adsorption. Herein, novel nanocomposite materials comprising activated carbon (AC) and Magnesium-MOF-74 were synthesized by impregnating different loading ratios of activated carbon into synthesized Magnesium-MOF-74 to yield Magnesium-MOF-74@AC-X (where X represents the Magnesium/AC ratio set to 1:2, 1:1, and 2:1). Compared to Magnesium-MOF-74 alone, Magnesium-MOF-74@AC-X exhibited higher specific surface area, superior thermal stability, elevated CO2 adsorption capacity, and better adsorption selectivity. At 273 K, the adsorption of CO 2 by Magnesium-MOF-74@AC sample containing Magnesium to AC ratio of 1:2 reached 40.31 cm 3 /g, while that of pristine Magnesium-MOF-74 was only 21.01 cm 3 /g. At 298 K, the adsorption capacity reached 29.45 cm 3 /g, while that of pristine Magnesium-MOF-74 was 1.91-fold lower. The linear fitting of the adsorption isotherms of composite in the Henry adsorption region using Henry’s law yielded a CO 2 /N 2 selectivity adsorption capacity of 32.19, a value 4.55-fold higher than pristine Magnesium-MOF-74.
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