ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Hongbing Song,Yongjie Wang,Yule Liu,Lei Chen,Bingxiao Feng,Xin Jin,Yu Zhou,Tingting Huang,Meng Xiao,Fangmin Huang,Hengjun Gai
Three ionic liquid (IL) monomers consisting of one, two, and four benzene rings were designed with 2-phenylimidazole and polymerized with α,α′-dichloro-p-xylene (DCX) and formaldehyde dimethyl acetal (FDA) to form a series of novel poly(ionic liquid)s (PILs). In this process, the designed ILs were employed as active ionic sites, and DCX and FDA were selected as cross-linkers. Self-condensation of the cross-linker provided a large specific surface area for the hypercross-linked organic framework, while co-condensation between the cross-linker and IL introduced active sites to the framework. The obtained porous hypercross-linked PILs not only promoted CO2 capture and the selective absorption of CO2/N2 but also showed good activity for the cycloaddition of epoxide with CO2. HP-[BZPhIm]Cl-DCX-1 with a large surface area (763 m2·g–1) showed a CO2 uptake capacity of 1.47 mmol·g–1 and offered a 98.9% yield of the CO2 cycloaddition product with epichlorohydrin at 80 °C for 24 h under 0.1 MPa CO2 pressure. The designed PILs provide an important reaction for CO2 utilization.
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2017
·
IF 2.813
Ling Zhang,Xue Liu,Rui-Xia Yang,Nian-Yu Huang,Wei-Qiao Deng
Covalent triazine-based frameworks (CTFs) are important microporous materials with a wide range of applications. Here, we demonstrate an environmentally benign and economic synthetic pathway to CTFs. The monomers used for CTFs, aromatic nitriles , were obtained by cyanation using nontoxic potassium hexacyanoferrate(II) in place of commonly used toxic cyanides. Then, the CTFs were synthesized by trimerization of the corresponding cyano monomers in molten zinc chloride . A series of CTFs was synthesized, and the highest Brunauer-Emmett-Teller surface area measured in this series was 2404 m 2 /g. Among the synthesized CTFs, CTF DCP exhibited excellent CO 2 adsorption properties, with a CO 2 uptake of 225 mg/g at 0 °C.
研究领域:
材料科学
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环境科学
·
化学工程
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DOI
高影响因子
APPLIED ENERGY
·
2017
·
IF 7.182
Ke Wang,Zhongyun Zhou,Pengfei Zhao,Zeguang Yin,Zhen Su,Ji Sun
Highly efficient NaF-doped Li 4 SiO 4 sorbents were synthesized by sacrificial carbon template technology to overcome their typical kinetic limitations at low CO 2 concentrations. The samples were characterized by XRD , SEM , N 2 adsorption, XPS , differential scanning calorimetry (DSC), and thermogravimetric analyses (dynamic and isothermic). The results showed that co-doped sodium and fluorine were substituted for lithium and oxygen, respectively. Such doped features induced a high concentration of Li-O sites on the molten surface when absorbing CO 2 in a relatively wide temperature range (475–575 °C). This favorable characteristic greatly facilitated surface chemisorption processes, accelerated the transport of Li + and O 2− , and decreased the CO 2 diffusion resistance. Therefore, 3 wt.% NaF doping was used to reach a maximum absorption capacity (>33.0 wt.%) in a wide temperature range (475–575 °C) in 15 vol.% CO 2 . Moreover, the high capacity was maintained over 10 sorption/desorption cycles, suggesting that NaF-doped Li 4 SiO 4 sorbents have high potential for CO 2 capture.
研究领域:
材料科学
·
环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 30
·41103-41112
·
IF 7.8
Sun Jiping,Zhang Hong,Wang Zhixing,Li Guangchao,Wu Bichao,Yang Sheng,Liu Min,Wang Jiexi
Developing acidic electrochemical CO 2 reduction reaction (CO 2 RR) systems can alleviate carbonate clogging in gas diffusion electrodes (GDEs), offering an efficient way to convert CO 2 at industrial-level current densities ( J > 200 mA cm –2 ). However, it comes at the cost of aggravating competitive hydrogen evolution reactions (HERs). Breaking this intrinsic selectivity–stability trade-off requires synergistic H 2 O/CO 2 management. As a central component of GDEs, the gas diffusion layer (GDL) critically governs gas (CO 2 )–liquid (H 2 O) transport balance. This work proposes a gradient pore-hydrophobicity cooperation strategy for synergistic H 2 O/CO 2 management to achieve efficient acidic CO 2 RR. Paired with commercial Ag catalysts, the Ag-GDEs exhibit an impressive CO Faraday efficiency of 97.26% at 400 mA cm –2 within a pH = 2.0 environment. Furthermore, in situ differential electrochemical mass spectrometry confirms the distinct mass transfer kinetics induced by GDL architectures. Lattice Boltzmann modeling simulations corroborate the effects of the gradient pore-hydrophobicity synergy on CO 2 and H 2 O distribution in GDLs. This work presents an effective approach to the rational design of GDLs and the collaborative liquid–gas management for efficient CO 2 RR.
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DOI
PubMed
高影响因子
FUEL
·
2021
·
IF 6.609
Hao Shen,Zihao Yang,Xiaochen Li,Ying Peng,Meiqin Lin,Juan Zhang,Zhaoxia Dong
Hydraulic fracturing and CO 2 flooding are extensively used in low-permeability reservoirs to enhance oil recovery (EOR). However, due to the serious heterogeneity of the formation, CO 2 is prone to break through the oil-bearing zone prematurely, which leads to the decrease of the swept volume. Conventional blocking agents have some defects such as difficult injection, poor stability and weak sealing strength. Therefore, it is critical to developing a new type of channeling blocking agent for low-permeability fractured reservoirs. In this study, ten kinds of chemicals with tertiary amino groups are filtered for the most effective CO 2 -responsive agent, which turns out to be N, N-Dimethyl erucamide tertiary amine (DMETA). Subsequently, rheological properties, response performance, and microstructure of the optimum agent are researched systematically through rheological experiments, CO 2 -response processes and Cryo-TEM. The results show that the viscosity of the DMETA solution can increase to nearly 605,700 mPa·s by self-assembly into wormlike micelles (WLMs). And it can be reversibly circulated between low viscosity and high viscosity by alternately introducing and removing CO 2 , which endows it with the ability to healing its viscoelasticity under an environment full of CO 2 . A new method based on optical microrheology is proposed to study the viscoelastic properties of WLMs under no external force. The experiments prove that the network structure is not stable after formation, but remains in a continuous process of separation and reconstruction as “a living polymer.” Furthermore, the plugging performance and EOR capacity are evaluated using fractured tight cores. The experiments demonstrate that the optimum agent can effectively restrain gas channeling and enhance recovery factor by 21.7%. We expect our work can provide insights for the synthesis of CO 2 -responsive WLMs and guidance for retarding gas channeling during CO 2 flooding in low permeability reservoirs.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2023
·
IF 2.6
Xiudong Zhang,Xianqiang Li,Chundong Zhang,Leiyu Zhang,Ruxing Gao
In order to achieve deep decarbonization for the purification process of coal-based syngas, developing efficient and clean solvents with strong CO2 absorption ability is essential. Considering this point, this work measured the vapor–liquid equilibrium (VLE) data of the CO2 + diisopropyl ether (DIPE), CO2 + methyl tert-butyl ether (MTBE), and CO2 + 1,2-dimethoxy ethane (1,2-DME) binary systems at 253.15 K, with an experimental pressure ranging from 0.30 to 1.85 MPa. From the experimental results, it can be seen that 1,2-DME has the strongest CO2 absorption capacity, followed by MTBE and DIPE. Meanwhile, it is found that the ether bonds can significantly improve the absorption ability of the solvent for CO2, whereas the increase in molecular weight can result in a negative impact. Finally, the Soave–Redlich–Kwong (SRK), Peng–Robinson (PR), and perturbed-chain statistical associating fluid theory (PC-SAFT) models were used to correlate the VLE data and obtain the binary interaction parameters kij. From the results, it is found that PR and SRK models are more suitable to correlate the VLE data of the CO2 + ether system. This work not only can provide a crucial reference for the selection of solvents with stronger CO2 absorption capacity but also provides accurate basic data for process simulation and optimization in the purification process of raw syngas.
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高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Yu Su,Qian Zhou,Ting Hu,Peng Li,Yu Zhu,Qing-Wen Han,Ru-An Chi,Dong-Sheng Li
Tin-oxo clusters, as molecular model compounds of tin oxide materials, have attracted increasing attention. Although various tin-oxo clusters have been obtained, the systemic studies on ligand functionalization of tin-oxo clusters remain to be well developed. In this study, we adopted 3-aminopyrazine-2-carboxylic acid (HAPZC) as the functionalized ligand, and successfully synthesized a novel tin-oxo cluster [( n -BuSn) 12 (OH) 6 O 14 (APZC) 2 ]·2H 2 O ( CTGU-SnC-3 ). Due to the functionalization of the APZC ligands, the structure and charge of Sn 12 cage in CTGU-SnC-3 are all different from those of reported cationic football cage. This Sn 12 cage in CTGU-SnC-3 presents the interesting low-symmetrical football framework with the functionalized ligands. Different from the reported cationic football cages, the CTGU-SnC-3 is charge-neutral structure without any counteranions. Moreover, the CTGU-SnC-3 exhibits hydrophobic behavior and catalytic activity in electrocatalytic CO 2 reduction reaction.
研究领域:
材料化学
·
分子簇化学
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DOI
高影响因子
Nano Research
·
2021
·Vol. 15
·期 2
·1310-1318
·
IF 8.897
Ullah Sami,Liu Yu,Hasan Maria,Zeng Wenwen,Shi Qitao,Yang Xiaoqin,Fu Lei,Ta Huy Q.,Lian Xueyu,Sun Jingyu,Yang Ruizhi,Liu Lijun,Rümmeli Mark H.
Graphene doping continues to gather momentum because it enables graphene properties to be tuned, thereby affording new properties to, improve the performance of, and expand the application potential of graphene. Graphene can be chemically doped using various methods such as surface functionalization, hybrid composites (e.g., nanoparticle decoration), and substitution doping, wherein C atoms are replaced by foreign ones in the graphene lattice. Theoretical works have predicted that graphene could be substitutionally doped by aluminum (Al) atoms, which could hold promise for exciting applications, including hydrogen storage and evolution, and supercapacitors. Other theoretical predictions suggest that Al substitutionally doped graphene (AlG) could serve as a material for gas sensors and the catalytic decomposition of undesirable materials. However, fabricating Al substitutionally doped graphene has proven challenging until now. Herein, we demonstrate how controlled-flow chemical vapor deposition (CVD) implementing a simple solid precursor can yield high-quality and large-area monolayer AlG, and this synthesis is unequivocally confirmed using various characterization methods including local electron energy-loss spectroscopy (EELS). Detailed high-resolution transmission electron microscopy (HRTEM) shows numerous bonding configurations between the Al atoms and the graphene lattice, some of which are not theoretically predicted. Furthermore, the produced AlG shows a CO 2 capturability superior to those of other substitutionally doped graphenes.
研究领域:
材料科学
·
物理化学
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DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yang Liu,Meng Zhang,Qingsong Tang,Peng Zhao,Kai Li,Xiaoming Jiang
Amino acids are widely involved in the processes of biosynthesis and physiological activities, as important basic substances for synthesis and metabolism in living organisms. The content of free amino acids in food, environment and clinical medicine fields, is of great significance for nutritional evaluation and health monitoring. Herein, a new method was proposed for rapid and sensitive determination of total free amino acids (TFAA), through detecting the carbon optical emission spectrometry (OES) of CO 2 , which was converted from the amino acids reacted with ninhydrin. All the free amino acids were converted into CO 2 without any pre-separation steps. To improve the sensitivity and convenience, headspace injection was utilized to pre-concentrate the generated CO 2 , and subsequently directly transported to a miniature microplasma excitation source for detecting the characteristic emission line of carbon at 193.04 nm. Under the optimal experimental conditions, the achieved limit of detection (LOD) was 0.17 μM, and the relative standard deviation (RSD) was 4.9% (65 μM, n = 7). It has been successfully applied to the determination of TFAA in a variety of certified reference materials (CRMs) and real samples to prove its accuracy and reliability. Moreover, owing to the small size, low power and reduced time consumption of the proposed method and instrument, it is promising for rapid screening and on-site analysis in various fields.
研究领域:
分析化学
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生物医学
·
食品科学
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产品关联
DOI
高影响因子
Nano Energy
·
2025
·
IF 17.1
Zhao Sun,Huicai Wang,Xingxu Wang,Riguang Zhang,Zhiqiang Sun
Sorption-enhanced steam reforming of methanol (SE-SRM) offers a promising route for high-quality hydrogen production with in situ CO 2 capture; however, achieving an optimal balance between catalytic activity and CO 2 uptake capability, while ensuring catalyst stability, remains a significant challenge. In this study, a series of Zr-doped (0 wt%, 5 wt%, 15 wt%, 25 wt%) Cu-MgO catalytic sorbents are synthesized for SE-SRM. At 180℃, the hydrogen concentration and yield reach nearly 100 % and 10.35 μmol·g −1 ·s −1 . Moreover, the catalytic sorbent basically retains its catalytic activity and CO 2 uptake capacity after 30 cycles with merely slight deactivation. Results demonstrate that the doped Zr, presents as tetragonal ZrO 2 , enhances metal-support interactions with the formation of a Cu-O-Zr interfacial structure, promoting Cu nanocluster dispersion and altering the Cu + /Cu 0 distributions. Zr doping also enables the modulation of the medium-strong basic sites. Moreover, the AFM and TEM confirmed the formation of high-roughness MgO surface on the substrate, thereby facilitating CO 2 diffusion and adsorption. DFT calculation results further confirm the advantages of Zr-doped Cu-MgO catalytic sorbents due to its stronger capability on CH 3 OH activation and CO 2 adsorption.
研究领域:
催化化学
·
材料科学
·
能源化学
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DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Xiao-Chao Chen,Lin Guo,Guang-Hui Shi,Kai-Chun Zhao,Yong Lu,Ye Liu
Carbon dioxide (CO 2 ) was found to serve as a novel and green catalyst for the first time in N -formylation of amines with N, N -dimethylformamide (DMF), wherein only the aliphatic amines were applicable to afford the formamides in the yield of 71∼95%. The isotope labeling experiment with DMF- d 7 indicated that the N -formyl group in the formylated product was originated from DMF rather than CO 2 . The control experiments and the in situ high-pressure FT-IR spectra demonstrated that the formation of the carbamate salt of cyclohexylammonium cyclohexylcarbamate ( A ) derived from the reaction of CO 2 with cyclohexylamine was the driving force for this reaction. Accordingly, the mechanism of CO 2 -catalyed N -formylation of aliphatic amines with DMF was proposed, involving the formation of carbamate salt intermediate with enhanced nucleophilicity in anion in favor of the attack on carbonyl-group of DMF.
研究领域:
有机化学
·
绿色化学
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DOI
高影响因子
Advanced Energy Materials
·
2026
·
IF 25.5
Zhen Wang,Jun-Ke Liu,Li Deng,Gui-Zeng Liang,Kai Ying,Zhen-Mao Lai,Jing-Juan Wang,Chuan-Wei Wang,Yue-Feng Xu,Yao Zhou,Jun-Tao Li
When CO 2 undergoes a two-electron partial reduction during the discharging process of Li-CO 2 batteries, it produces thermodynamically active Li 2 C 2 O 4 , which readily decomposes during subsequent charging. This offers a promising opportunity to mitigate the large charging overpotential and enhance the battery's cycling stability. However, as an intermediate, Li 2 C 2 O 4 tends to transform to the inert Li 2 CO 3 readily. In this work, we report a high-performance cathode catalyst featuring ultrasmall RuO 2 and BiOCl uniformly co-decorated on an MXene substrate (RuO 2 -BiOCl). It effectively stabilizes Li 2 C 2 O 4 during discharge, facilitating the two-electron partial reduction of CO 2 ; meanwhile, it can also modulate the morphology of discharge products, resulting in an intimate and extensive solid–solid interface between the insulating discharging product and the electrocatalyst. This together avoids accumulation of bulky, highly inertial and insulating Li 2 CO 3 in the cathode during cycling, which decreases the charging polarization and prolongs the Li-CO 2 battery life span. The optimal Li-CO 2 battery delivers a high discharge capacity of 10.33 mAh cm −2 during the first full cycle, and extraordinary durability, sustaining over 10 000 h of operation with a fixed areal capacity of 0.10 mAh cm −2 at 0.02 mA cm −2 . By tuning the CO 2 reduction path, this work offers a novel approach for building high-performance, practically workable Li-CO 2 batteries.
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高影响因子
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