Journal of Energy Chemistry
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2017
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IF 2.594
Haiying Ran,Jiexin Wang,Ahmed A. Abdeltawab,Xiaochun Chen,Guangren Yu,Yinghao Yu
We synthesized one quaternary ammonium polymeric ionic liquids (PILs)P[VBTHEA]Cl and three imidazolium PILs of P[VEIm]Br, P[VEIm]BF 4 , P[VEIm]PF 6 by free-radical polymerization in solution. These PILs were characterized by FT-IR, 1 H-NMR, 13 C-NMR, TGA, XRD and SEM. Their CO 2 adsorption capacities were measured under different pressures and temperatures by constant-volume technique. It was observed that quaternary ammonium PILs of P[VBTHEA]Cl have higher adsorption capacity for CO 2 than those imidazolium PILs, following P[VBTHEA]Cl > P[VEIm]PF 6 > P[VEIm]BF 4 > P[VEIm]Br, which may be ascribed to higher positive charge density on ammonium cation than that on imidazolium cation and thus stronger interaction with CO 2 , consistent with the results from dual-mode adsorption model that ammonium PILs have much higher CO 2 bulk absorption than imidazolium PILs. CO 2 adsorption capacity of P[VBTHEA]Cl is 9.02 mg/g under 295 K and 1 bar, which is comparable to that of some other PILs, and is much higher than that of the corresponding ILs monomer . These PILs have good adsorption selectivity for CO 2 over N 2 and regeneration efficiency.
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JOURNAL OF MEMBRANE SCIENCE
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2014
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IF 4.908
Wenjuan He,Zhi Wang,Wen Li,Shichun Li,Zhiheng Bai,Jixiao Wang,Shichang Wang
Fixed carrier membranes containing amino groups show attractive performance in CO 2 separation for clean energy supply and greenhouse gas reduction. However, the separation performance of fixed carrier membranes at high feed pressure is limited by the facilitated transport ability of membranes as well as the CO 2 -induced plasticization. In this work, the tertiary amino group containing fixed carrier membranes were prepared by interfacial polymerization (IP) with hexane-soluble trimesoyl chloride (TMC) and aqueous-soluble 1,4-bis (3-aminopropyl) piperazine (DAPP), N -aminoethylpiperazine (EAP) and 3,3′-diamino- N -methyldipropylamine (DNMDAm). The results show that the membrane prepared with TMC and DAPP exhibits the highest CO 2 separation performance due to efficient CO 2 facilitated transport and high plasticization resistance. Efficient facilitated transport of CO 2 in the membrane is due to the high content of cyclic tertiary amino groups which possess high stoichiometric CO 2 loading and high rate constant of amine-CO 2 reaction. Moreover, high plasticization resistance of the membrane is attributed to the appropriate stiffness of polymer chains provided by IP. The membrane prepared with TMC and DAPP shows promising applications in high-pressure fuel gas purification.
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BIOMASS & BIOENERGY
·
2024
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IF 5.8
Yonghui Xu,Yufei Liu,Wei Zhan,Dingle Zhang,Yiyun Liu,Yi Xu,Zhengshun Wu
This study explores the transformation of peanut shells, an abundant agricultural waste, into high-efficiency activated carbon for CO 2 capture using a two-step pyrolysis and K 2 CO 3 activation method. Observations indicated that with an increasing impregnation ratio, the activated carbon demonstrates remarkable improvements in structural properties, achieving specific surface areas and pore volumes of 1150.02 m 2 /g and 0.46 cm 3 /g, respectively. Among the prepared samples, the activated carbon obtained with a peanut shell to K 2 CO 3 impregnation mass ratio of 1:2 exhibits superior CO 2 adsorption capacity at 1 bar, with values of 3.76 mmol/g at 25 °C and 5.70 mmol/g at 0 °C. The CO 2 adsorption isotherms of the activated carbon conform to the Langmuir and Freundlich models. These results demonstrate the potential of this method in addressing environmental concerns, particularly in mitigating CO 2 emissions, and highlight the broader application prospects of biomass-derived activated carbon in environmental management.
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ENERGY & FUELS
·
2025
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IF 5.3
Xiaoteng Cui,Mingsheng Luo,Zhi Yang,Roshni Rahman,Ziyuan Li,Wenshuai Yang,Lingman Xia
As a greenhouse gas, carbon dioxide is also a rich carbon resource that can be effectively utilized to tackle the global warming crisis. This paper presents an in-depth investigation of the impact of the Cu content on the structure of Cu–Zn–Al layered double hydroxides (LDHs) from a novel perspective. The CO2 hydrogenation performance of the derived catalyst, the LDO, is also evaluated in the methanol synthesis reaction. All catalysts were evaluated at 3.0 MPa, a carbon dioxide to hydrogen ratio of 3, and a space velocity of 3600 mL·g–1·h–1. The results from this work indicate that the catalyst with a Cu:Zn ratio of 11:4 exhibited the highest methanol selectivity of 63.9% at 230 °C. At 250 °C, the catalysts also yielded the highest methanol selectivity of 50% only, along with a CO2 conversion as high as 17.8%. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) data suggest that the CO2-to-methanol reaction follows the formate (HCOO*) mechanism for this catalyst. Results from this work offer a novel approach to designing Cu-LDH-based catalysts, which offers valuable insights for the efficient chemical utilization of CO2.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jing Lei,Wei Bi,Mitang Wang,Hao Jiang,Yanjie Hu,Chunzhong Li
How to achieve controllable preparation of heterostructure and in-situ optimize the interface and internal electron transfer by a fast and economic synthesis method has become a big challenge in the practical application of photocatalysis. Herein, an island-shaped SrTiO 3 (STO) perovskite nanodots and TiO 2 (T) compounded S-scheme SrTiO 3 /TiO 2 (ST) heterostructure was successfully developed. During the millisecond reaction process, the decomposed Sr 2+ penetrated into the TiO 2 lattice causing the lattice expansion and inducing local atomic rearrangements, resulting in the generation of STO phase. Owing to the synergy of the efficient electron transport at the perovskite nanodots interface and the stronger reduction capacity, the performance of the optimized ST1 sample is greatly improved to 86.90 μmol g −1 for CO 2 -to-CO and 21.31 μmol g −1 for CO 2 -to-CH 4 . The utilization of electrons reached up to 119.74 μmol g −1 h −1 , which was 3.13 times higher than that of T. Detailed characterizations and density functional theory (DFT) calculations proof that the formation of intermediates HCOO − and CO 3 2− is the key to the performance improvement critically. Overall, this work originally reports a feasible strategy for flame synthesis of S-scheme heterostructure photocatalyst.
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MOLECULES
·
2024
·Vol. 29
·期 3
·578
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IF 4.2
Hengxin Jian,Mengyu Lu,Haowen Zheng,Shengrui Yan,Mei Wang
Mimicking the photosynthesis of green plants to combine water oxidation with CO2reduction is of great significance for solving energy and environmental crises. In this context, a trinuclear nickel complex, [NiII3(paoH)6(PhPO3)2]·2ClO4(1), with a novel structure has been constructed with PhPO32−(phenylphosphonate) and paoH (2-pyridine formaldehyde oxime) ligands and possesses a reflection symmetry with a mirror plane revealed by single-crystal X-ray diffraction. Bulk electrocatalysis demonstrates that complex1can homogeneously catalyze water oxidation and CO2reduction simultaneously. It can catalyze water oxidation at a near-neutral condition of pH = 7.45 with a high TOF of 12.2 s−1, and the Faraday efficiency is as high as 95%. Meanwhile, it also exhibits high electrocatalytic activity for CO2reduction towards CO with a TOF of 7.84 s−1in DMF solution. The excellent electrocatalytic performance of the water oxidation and CO2reduction of complex1could be attributed to the two uniqueµ3-PhPO32−bridges as the crucial factor for stabilizing the trinuclear molecule as well as the proton transformation during the catalytic process, while the oxime groups modulate the electronic structure of the metal centers via π back-bonding. Therefore, apart from the cooperation effect of the three Ni centers for catalysis, simultaneously, the two kinds of ligands in complex1can also synergistically coordinate the central metal, thereby significantly promoting its catalytic performance. Complex1represents the first nickel molecular electrocatalyst for both water oxidation and CO2reduction. The findings in this work open an avenue for designing efficient molecular electrocatalysts with peculiar ligands.Keywords:transition metal complex;water oxidation;carbon dioxide reduction;electrocatalysis;synergistic catalysis
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2024
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IF 5.9
Yongheng Ren,Yang Chen,Hongwei Chen,Lu Zhang,Jiangfeng Yang,Qi Shi,Lin-Bing Sun,Jinping Li,Libo Li
The identical molecular size and similar physical properties of carbon dioxide (CO 2 ) and acetylene (C 2 H 2 ) make their adsorptive separation extremely challenging to achieve with most adsorbents. Reports on the separation of CO 2 and C 2 H 2 mixtures by zeolites are even rarer with the mechanism of adsorptive separation requiring further exploration. In this paper, we report that ion modulation of zeolite 5A promotes the difference in kinetic diffusion of CO 2 and C 2 H 2 , realizing the inverse separation of zeolite from selective adsorption of C 2 H 2 to selective adsorption of CO 2 . Creating a compact pore space restricting the orientation of gas molecules enables charge recognition. The positive electrostatic potential at the pore openings was utilized to hinder the diffusion of C 2 H 2 between the cages while ensuring the transfer of CO 2 , increasing their diffusion differences in pore channels and leading to the CO 2 /C 2 H 2 kinetic selectivity of 31.97. Grand canonical Monte Carlo (GCMC) simulation demonstrates that the CO 2 distribution in K-5A- β is significantly higher than that of C 2 H 2 . Dynamic breakthrough experiments verify the excellent performance of material in practical CO 2 /C 2 H 2 separation, for CO 2 /C 2 H 2 (50/50 and 1/99, V/V) mixtures can be separated in one step, thus directly generating high purity C 2 H 2 (> 99.95%), which provides a promising thought for the zeolite-based separation of CO 2 and C 2 H 2 .
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Qi Tan,Yiwen Liu,Ruifeng An,Heping Wu,Zhiqiang Tian,Bingliang Gao
Reducing greenhouse gas emissions is a crucial step in mitigating global warming. Carbon dioxide (CO 2 ) represents one of the most pivotal greenhouse gases contributing to climate change. Many researchers are actively engaged in the development of effective and reversible CO 2 absorbents to control and reduce CO 2 gas emissions. In this paper, we synthesized a series of molecular solvents (MSs) based on the superbase 1,5-diazabicyclo [4.3.0]-5-nonene (DBN) and used them for CO 2 capture. The CO 2 capture capacity of MSs composed of DBN and different alcohols was systematically investigated, with DBN-Methanol (1:1.25) demonstrating superior absorption performance by achieving a maximum absorption capacity of 0.263 g CO 2 /g MS. The effects of temperature, pressure, the molar ratio of the hydrogen bond acceptor (HBA) to hydrogen bond donor (HBD), and moisture on the absorption process were studied. The experimental results were corroborated by NMR spectra analysis and FTIR spectra analysis, confirming that these MSs can effectively react with CO 2 to produce carbonate and carbamate compounds through synergistic absorption involving hydroxyl group as primary component and amino group as secondary component. In addition, it is worth noting that the MSs studied in this work exhibit only glass transition at low temperatures and transform into ionic liquids (ILs) after capturing CO 2 , resulting in a significant increase in conductivity and demonstrating considerable electrochemical potential.
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AICHE JOURNAL
·
2024
·Vol. 70
·期 8
·e18471
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IF 3.5
Xiaoyu Wang,Fangxu Fan,Yongchao Sun,Jingfa Zhang,Canghai Ma,Gaohong He
Polymer-based membrane technology holds immense promise for CO 2 separation. However, it faces persistent challenges, including the high CO 2 pressure-induced plasticization and permeability-selectivity trade-offs, which significantly hinder the development of polymeric membranes. To tackle this issue, we synthesized a novel polyimide 6FDA-DAT:DABA(6FDD) containing triptycene and carboxylic groups. Upon de-carboxylation induced cross-linking, the membrane demonstrated a simultaneous enhancement of gas permeability and selectivity. Specifically, compared to the uncross-linked 6FDD, the 400°C-24 h cross-linked membrane exhibited a remarkable increase in CO 2 permeability by 177% (93.1 Barrer) and a significant rise in CO 2 /CH 4 selectivity by 47% (57.5), reaching the CO 2 /CH 4 upper bound. More importantly, the cross-linked membrane displayed vastly improved CO 2 plasticization resistance, withstanding up to 42 bar of CO 2 feed pressure. The design of decarboxylated cross-linked membranes in this work paves the way for creating high-performing and plasticization-resistant membranes with potential applications in high-pressure CO 2 separations.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yunpeng Wang,Tao Liu,Chun Cheng,Yachen Xie,Cheng Lan,Wenchuan Jiang,Zhiyu Zhao,Shuo Zhai,Yiri Li,Yifan Wu,Heping Xie
CO 2 batteries offer a promising avenue for mitigating CO 2 emissions and conversion, but encounter challenges such as high costs, dendrite, corrosion, flooding and slow kinetics stemming from the use of metal electrodes. CO 2 mineralization is thermodynamically favorable (ΔG CO2 ), presenting an opportunity for processing solid waste and reducing CO 2 emissions while potentially producing energy. However, the lack of direct electron transfer in the CO 2 mineralization reaction hinders the direct generation of electrical energy. Here, we propose an organic CO 2 mineralization battery (OCMB) without using metal, which efficiently harnesses CO 2 to mineralize solid waste carbide slag, maximizing the recovery of mineralization reaction energy to generate electricity and produce carbonate products, without requiring renewable electricity charging. We employ a high-solubility, stable under strong alkaline conditions, and fast kinetics organic phenazine derivative—DSPZ as the electron and proton carrier, which facilitates the conversion of ΔpH between electrodes by interacting with alkaline wastes and CO 2 into electricity. Simultaneously, the OCMB undergoes regeneration cycles through mineralization reactions. The theoretical model predicted the open circuit voltage (OCV) and discharge behavior of OCMB, offering insights for improved battery engineering. We demonstrate an impressive peak power density exceeding 227.5 W/m 2 for the OCMB, with an estimated electricity production of ∼ 178.03 kWh per ton of CO 2 mineralization. This research underscores the potential integration of OCMBs into CO 2 energy systems, waste treatment processes, and chemical production, offering both economic and environmental benefits.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Dandan Hao,Ping Wang,Ju Liu,Huanhui Zhan,Tiantian Zhou,Bo Fu
MOF-199 is considered to be an excellent CO 2 adsorbent owing to its substantial specific surface area, suitable pore structure and abundant sorption sites. However, powdered MOF-199 is prone to agglomeration and has poor recyclability. Herein, we proposed a MOF-199-based adsorbent by combining the MOF synthesis process with traditional papermaking process. Through such a design, MOF-199 particles are adhered on the surface of wood pulp fiber. The sufficient hydroxyl groups and electrostatic forces of cellulose facilitates the homogeneous and tight adhesion of MOF crystals. The optimal MP-4 sample demonstrated a high CO 2 adsorption capacity (1.80 mmol·g ‐−1 at 25 °C) and good CO 2 /N 2 selectivity (30.06). Moreover, the composite sorbent can be easily regenerated. The adsorption mechanism was analyzed by the density functional theory approach. The simulation results showed that the carboxyl functional groups with a large number of oxygen atoms and active metal sites are the key to boost the CO 2 adsorption performance.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 23
·9724-9731
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IF 3.5
Ying Peng,Shuo Chen,Zhengli Hu,Mengqi Yin,Lishun Pei,Qiaohua Wei,Zailai Xie
Developing novel electrocatalysts for achieving high selectivity and faradaic efficiency in the carbon dioxide reduction reaction (CO2RR) poses a major challenge. In this study, a catalyst featuring a nitrogen-doped carbon shell-coated Ni nanoparticle structure is designed for efficient carbon dioxide (CO2) electroreduction to carbon monoxide (CO). The optimal Ni@NC-1000 catalyst exhibits remarkable CO faradaic efficiency (FECO) values exceeding 90% across a broad potential range of −0.55 to −0.9 V (vs. RHE), and attains the maximum FECO of 95.6% at −0.75 V (vs. RHE) in 0.5 M NaHCO3. This catalyst exhibits sustained carbon dioxide electroreduction activity with negligible decay after continuous electrolysis for 20 h. More encouragingly, a substantial current density of 200.3 mA cm−2 is achieved in a flow cell at −0.9 V (vs. RHE), reaching an industrial-level current density. In situ Fourier transform infrared spectroscopy and theoretical calculations demonstrate that its excellent catalytic performance is attributed to highly active pyrrolic nitrogen sites, promoting CO2 activation and significantly reducing the energy barrier for generating *COOH. To a considerable extent, this work presents an effective strategy for developing high-efficiency catalysts for electrochemical CO2 reduction across a wide potential window.
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