MICROPOROUS AND MESOPOROUS MATERIALS
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2017
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IF 3.615
Jun Liu,Yunfei Liu,Xiaowei Jiang,Yali Luo,Yinong Lyu
Two kinds of POSS-based microporous organic polymers (PMOPs) were prepared by cost-effective Friedel-Crafts reaction of octaphenylsilsesquioxanes with p -dimethoxybenzene (PMOP-1) or cyanuric chloride (PMOP-2). PMOP-1 with high surface area of 806 m 2 g −1 exhibited reasonable CO 2 adsorption (2.59 mmol g −1 , 273 K/1 bar) and selectivity, whereas PMOP-2 with lower surface area (559 m 2 g −1 ) showed a higher CO 2 /N 2 selectivity (30.0) and CO 2 /CH 4 selectivity (6.8) at 273 K/1 bar due to the high amount of nitrogen incorporated within the structure. The correlation between the performance of PMOPs in CO 2 capture/separation and their properties such as surface area, surface active sites, and heat of adsorption was investigated. The combination of a cost-effective method, high thermal stability, and reasonable selective adsorption make these materials potential candidates for application in CO 2 capture and separation technology.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2015
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IF 2.679
Dong Fu,LeMeng Wang,Pan Zhang,ChenLu Mi
The saturated solubility of CO 2 in monoethanolamine (MEA) promoted 2-diethylaminoethanol (DEAE) aqueous solution was investigated at temperatures ranging from (303.2 to 323.2) K. The mass fraction and temperature dependences of the saturated solubility and CO 2 loading are illustrated. The viscosities of both CO 2 -unloaded and CO 2 -loaded DEAE–MEA aqueous solutions were measured and then calculated by using the Weiland equation. The effects of temperature, mass fraction and CO 2 loading on viscosities are demonstrated.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2017
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IF 2.726
Shufeng Shen,Yue Zhao,Yangyang Bian,Yong Wang,Hui Guo,Hui Li
The solubility of CO 2 in aqueous potassium lysinate (LysK) solutions was measured in a stirred reactor at temperatures from 298 to 353 K, for 9.0, 17.4, 25.3, 33.1 and 41.2 mass% LysK and CO 2 partial pressures up to 110 kPa. The vapor-liquid equilibrium (VLE) data were interpreted using the modified Kent-Eisenberg model. The apparent equilibrium constants of carbamate hydrolysis and amino acid deprotonation were correlated as a function of temperature, CO 2 loading (expressed as mole CO 2 per mole LysK) and LysK concentration to fit the experimental solubility data. The proposed model satisfactorily predicted the VLE data for the H 2 O-LysK-CO 2 system, especially at moderate to high CO 2 loading, with an average absolute deviation within 3.2%. Liquid species in the CO 2 -loaded LysK solutions were also qualitatively characterized by 13 C NMR experiments.
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Journal of Materials Chemistry A
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2017
·Vol. 5
·期 37
·19954-19962
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IF 8.867
Yiming Zhang,Huixian Wang,Jindun Liu,Jingwei Hou,Yatao Zhang
In this work, carbonic anhydrase (CA) molecules were embedded into metal–organic frameworks (MOFs) via physical absorption and chemical bonds, which could overcome the enzymatic inactivation and the poor separation property of pristine MOF materials. And then, these nanocomposites (enzyme-embedded MOFs) as the crystal seeds were in situ grown on oriented halloysite nanotube layers to develop novel biocatalytic composite membranes. These membranes exhibited optimal separation performance with a CO2/N2 selectivity of 165.5, about 20.9 fold higher than that of the membrane without embedded CA molecules, surpassing the Robeson upper bound (2008). At the same time, the CO2 permeance increased about 3.2 fold (from 7.6 GPU to 24.16 GPU). Importantly, the biocatalytic composite membranes showed good stability and mechanical properties and were easily scalable, which could be extended to industrial applications.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Jiasheng Tong,Miao Wang,Xuejun Qiu,Shizhen Li,Hangqi Yang,Chuang Peng
Deep eutectic solvents (DESs) are promising media for CO2 electroreduction because of their high CO2 solubility, low cost, and eco-friendliness. However, the high viscosity and poor ionic conductivity severely limit their applications. In this study, low-viscosity polar aprotic solvents, propylene carbonate (PC) and sulfolane (SL), were used as diluents in Ethaline (ChCl:2EG) to prepare mixed electrolytes for electrochemical CO2 reduction. Raman and infrared spectra indicate that PC and SL can participate in the eutectic network of Ethaline through intermolecular hydrogen bonding, thereby decreasing the viscosity. The current density of the Ag cathode increases from 1.7 to 8.0 and 5.3 mA/cm2 with the addition of PC and SL, respectively. The two diluents also result in improved CO faradaic efficiency (FECO) and suppressed HER because the C═O and S═O bonds in the molecular frameworks of PC and SL can disrupt the hydrogen bonds of accumulated water molecules during electrolysis. At −2.0 V, FECO increases from 63% to over 90% upon the addition of PC and SL. This study provides new insights into the design of high-performance DES electrolytes for CO2 electroreduction.
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CHEMISTRY OF MATERIALS
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2024
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IF 7.2
Shikai Liu,Chuqiao Shi,Chaokai Xu,Haichuan Zhang,Wenqi Li,Valentín Briega-Martos,Qian He,Yimo Han,Yao Yang
CO2 reduction reaction (CO2RR) facilitates the sustainable synthesis of fuels and chemicals. Although copper (Cu) enables CO2-to-multicarbon product (C2+) conversion, Cu-based electrocatalysts, particularly nanocatalysts, face challenges in poor selectivity and stability owing to the highly dynamic nature of Cu atoms under reaction conditions. Core–shell structures present a promising approach to address these issues by modulating the Cu overlayer–substrate interactions with atomic-level precision. Here, we report on Pd@Cu core–shell structures with atomically thin and nanometer-thick Cu overlayers on single-crystal Pd nanocubes with {100} facets promoting the CO2-to-C2+ conversion. The microstructures and surface compositions at the atomically sharp Pd/Cu interface were investigated by atomic-scale scanning transmission electron microscopy (STEM) imaging and electron energy-loss spectroscopy (EELS). Our results reveal that atomic-layer Cu epitaxially grows on Pd and adapts to the lattice of the Pd substrate. The reaction-driven migration of atomic-layer Cu is effectively suppressed on Pd due to the strong Cu–Pd interaction. While Pd only reduces CO2 to C1 products, atomic-layer Cu on Pd can initiate the C2+ production during the CO2RR. Thick Cu overlayers (∼15 nm) on Pd further enhance the C2+ faradaic efficiency while undergoing significant structural reconstruction, with only the 2–3 nm Cu layers near the Pd surface remaining stable and resistant to Cu migration after the CO2RR. We anticipate that Pd@Cu core–shell structures with intermediate Cu shell thickness hold significant potential for enhancing C2+ selectivity while maintaining high stability of nanocatalysts for CO2 reduction to liquid fuels.
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JOURNAL OF CATALYSIS
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2025
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IF 6.5
Jia Li,Yang Li,Yingshan Zeng,Yang Liu,Zhengguo Song,Zhi Liu
CO 2 photo reduction provides a feasible technique to solve climate issues and promote carbon neutrality. However, the efficiency of CO 2 photo reduction is severely depressed by the rapid recombination of photo generated carriers within photo catalysts, restricting the participation of electrons in the reduction process. In this study, we successfully construct a two-dimensional (2D) multilayer internal electric field (IEF) heterostructure by engineering the interface between NiAl-LDH and ZnV 2 O 6 (ZNA). Driven by the IEF, the separation of photo generated electron-hole pairs is significantly enhanced, leading to the increased utilization efficiency of carriers for active sites. The best-performing sample of ZNA-2 achieves a highest CO yield of 695.8 μmol g −1 , approximately 30.5-fold higher than that of pristine ZnV 2 O 6 . Photo electrochemical measurement and density functional theory (DFT) calculation results reveal that the 2D-2D stacked structure generates multiple interlayer built-in electric fields, which are crucial for enhancing carrier separation and suppressing recombination. Adsorption energy and intermediate COOH* analysis reveal that ZNA-2 significantly lowers the adsorption energy of CO 2 , promoting its stable adsorption and subsequent conversion. Moreover, the unique 2D multilayer IEF heterostructure greatly facilitates the formation of key intermediate COOH* and the desorption of CO during CO 2 photo reduction, leading to high CO activity and selectivity. The present work discloses the unprecedented potential of 2D multilayer IEF heterostructures for efficient CO 2 photo reduction, marking a significant advancement over conventional 2D counterparts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Guangcan Huang,Tongxin Liu,Haoxin Peng,Yabo Xie,Qiang Chen,Jian-Rong Li
Mixed-matrix membranes (MMMs) incorporating Metal-Organic Frameworks (MOFs) represent a promising approach for gas separation, which can combine the advantages of selective adsorbents and processable polymers, and display great potential in the gas separation process. However, the further application of MMMs is severely impeded owing to the non-ideal interface between fillers and polymer matrix . In this work, a series of MIL-101(Cr) nanofillers, equipped with different kinds of counter anions were introduced to regulate the chemical microenvironment of the MMMs and improve the interfacial relationship between inorganic filler and polymer. The filler of MIL-101-HNO 3 exhibits improved dispersibility in solvents and heightened interface relationship with the polymer matrix (PIM-1) due to its optimal particle size and distinctive exposure of crystallographic planes. Moreover, gas sorption isotherms reveal that the MIL-101-HNO 3 MOF show reduced N 2 adsorption capacity. Therefore, the MOF filler of MMMs were optimized rationally by microenvironment regulate strategy, leading to the MIL-101-HNO 3 /PIM-1 MMMs achieve high CO 2 permeability and exceptional CO 2 /N 2 ideal selectivity (CO 2 = 14879 barrer, CO 2 /N 2 = 24.3), surpassing the latest 2019 upper bound. That makes MIL-101-HNO 3 /PIM-1 a potential candidate for the selective removal of CO 2 from stack gas and provides new insights into the regulation of the MMMs nanofiller microenvironment.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
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IF 3.7
Yutong Pan,Pengju Gao,Shixiong Tang,Xiaoyu Han,Ziwen Hao,Jiyi Chen,Zhenmei Zhang,Heng Zhang,Xiaohui Zi,Maoshuai Li,Shiwei Wang,Yue Wang,Xinbin Ma
This work synthesized a series of Ni/CeO 2 /Al 2 O 3 catalysts with varying CeO 2 doping amounts to enhance low-temperature CO 2 methanation. The introduction of CeO 2 weakens the interaction between Ni and Al 2 O 3 , leading to the formation of Ni-CeO 2 active sites. This results in a high dispersion of Ni and CeO 2 , improved catalyst reducibility, increased number of active sites, and enhanced the CO 2 methanation. This work further investigated the impact of WHSV and catalyst stacking configuration to enhance the reaction. When the catalyst is stacked into three segments with a temperature gradient of 330 °C, 300 °C, and 250 °C under WHSV=9000 ml·h –1 ·(g cat) –1 , the CO 2 conversion significantly increases to 95%, which is remarkably close to the thermodynamic equilibrium (96%).
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Chen Wang,Yan Zhu,Ling Zhao,Rui Wang,Jun Jin,Yansheng Gong,Huanwen Wang,Beibei He
Solid oxide electrolysis cells (SOECs) have emerged as a promising technology for CO 2 electrolysis. However, the sluggish kinetics of CO 2 electrolysis impedes their widespread commercialization. Here, a novel heterostructure of in-situ exsolved metal/high-entropy perovskite, Ni@Sr 2 Fe 1.0 Ti 0.2 Cr 0.2 Mn 0.2 Mo 0.2 Ni 0.2 O 6-δ (Ni@SFTCMMN), has been designed to enhance the efficiency of CO 2 electrolysis. The Ni@SFTCMMN, with its high-entropy configuration and embedded exsolution morphology, ensures high structural stability during continuous CO 2 electrolysis. As an application, the Ni@SFTCMMN-based electrolysis cell demonstrates a remarkable current density of 1.91 A cm −2 at 1.5 V and 800 °C, maintaining consistent performance over 160 h. By integrating theoretical calculation with experimental investigations, we aim to establish the link between the electronic structure of perovskite oxides with varying elemental compositions and the mechanism of the CO 2 reduction reaction. The findings from this work provide crucial insights into the role of conformational entropy strategies in CO 2 electrolysis and suggest potential pathways for developing efficient and durable cathode of SOECs.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Muhammad Sabir,Mahmoud Sayed,Zhuofan Zeng,Bei Cheng,Wang Wang,Chuanbin Wang,Jingsan Xu,Shaowen Cao
The photocatalytic conversion of carbon dioxide (CO 2 ) into valuable products holds great promise from environmental and economic perspectives. However, current photocatalytic materials still exhibit unsatisfactory efficiency. In this study, a notably efficient step-scheme (S-scheme) heterojunction was developed by combining the Co-MOFs with carbon nitride nanosheets (g-C 3 N 4 ). The electrostatic interaction between these components not only facilitates the exfoliation of g-C 3 N 4 layers but also enhances the stability of the photocatalyst structure. The optimal heterojunction Co-CN4 photocatalyst achieved a significantly enhanced CO production rate of 16.1 µmol g −1 h −1 , which is 4.7 times higher than that of pure g-C 3 N 4 . This improved activity is ascribed to the enhanced light absorption and mitigated charge carrier recombination. Density functional theory (DFT) computations in conjunction with experimental observations elucidate the establishment of a close contact interface. Additionally, electron paramagnetic resonance (EPR) and in situ X-ray photoelectron spectroscopy (XPS) characterization unveil the electron transfer pathway of Co-CN4 during photocatalytic CO 2 conversion. This study offers valuable insights into the design of S-scheme photocatalysts for enhancement of CO 2 photoreduction.
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JOURNAL OF POROUS MATERIALS
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2025
·
IF 3.2
Xiong Qingxing,Yu Lingling,An Ning,Cong Hang,Zhao Wenfeng
Conversion of greenhouse gas carbon dioxide to valuable products is important to reach carbon balance and sustainability, of which catalytic cycloaddition of CO 2 to cyclic carbonates has attracted much attention. Here, a biomass-derived zwitterionic polymer has been synthesized and characterized. The prepared polymer with porous structure was employed for the catalytic cycloaddition of atmospheric CO 2 and epoxides in excellent yields with a broad substrate scope under solvent-, co-catalyst, and metal-free conditions. The synthesized polymer with good thermostability could be readily recovered and recycled four times at least. Moreover, this catalytic system provided satisfactory performance with up to 96% yield of cyclic carbonate even in the gram-level scale-up reaction under the optimal standard conditions. The catalytic mechanism has also been preliminarily discussed.
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