ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
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2019
·Vol. 25
·期 4
·693-701
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IF 1.731
Kuang Yizhu,He Hui,Chen Shuixia,Wu Jingjie,Liu Fenglei
Using efficient and stable solid amine adsorbents to capture CO 2 has been considered as an effective technology to reduce the CO 2 concentration in the atmosphere. In this paper, a series of solid amine-containing fibrous adsorbent for CO 2 capture were prepared by direct modification of polyacrylonitrile (PAN) fibers with amination reagents, including diethylenetriamine (DETA), triethylenetetramine (TETA), tetraethylenepentamine (TEPA) and polyethyleneimine (PEI). Abundant amine groups can be introduced on the PAN surface owing to the reactivity between cyano group and amino group. The effects of the type and structure of amination reagents on the swelling properties and CO 2 adsorption capacities of the as-prepared adsorbents were investigated. The results indicated that chemical modification of PAN fibers with amine compounds could greatly increase the CO 2 adsorption capacity of the aminated adsorbents. The adsorption capacities of the adsorbents were correlated well with the content of amino groups. PAN–TETA and PAN–TEPA showed higher CO 2 adsorption capacities and better stability than PAN–DETA and PAN–PEI. Besides, as water molecules could take part in and facilitate the CO 2 adsorption, the CO 2 adsorption capacity of amine-modified fibers would be strongly dependent on the swelling property.
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JOURNAL OF MATERIALS SCIENCE
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2018
·Vol. 54
·期 5
·3805-3816
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IF 2.993
Yin Fengqin,Wu Zhejia,Luo Xianyong,Zhuang Linzhou,Ou Haozhen,Chen Shuixia
The nitrogen-rich hollow microspheres (MFM) with different pore sizes have been synthesized by using melamine, m -phenylenediamine and paraformaldehyde as monomer, different particle sizes of SiO 2 microsphere as template, and water as solvent. The specific surface area, pore volume and average pore size of the synthesized MFM were 183.67 m 2 /g, 0.91 cm 3 /g and 19.8 nm, respectively. After loading polyethyleneimine (PEI), its CO 2 adsorption capacity could reach 2.68 mmol/g at 60 °C, with the corresponding utilization efficiency of amino as high as 40.66%. The kinetic simulation of pseudo-first-order, pseudo-second-order and Avrami kinetic model showed that the Avrami model could better describe the adsorption process of CO 2 , indicating both physical adsorption and chemical adsorption in the whole process. The diffusion mechanism was simulated by using the Boyd model, the intermolecular diffusion model and the intraparticle diffusion model, showing that the porous structure of MFM was beneficial to the diffusion of CO 2 in the particles. After 5 cycles, 10 cycles, 15 cycles and even after 20 cycles of adsorption–desorption, the adsorption capacity of MFM-PEI at 30 °C was nearly the same as the capacity of the fresh one, indicating the regeneration stability of the adsorbent, with great advantages in practical production.
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ADVANCED MATERIALS
·
2019
·Vol. 31
·期 17
·1807807
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IF 25.809
Xueyuan Wang,Jiafang Xie,Muhammad Arsalan Ghausi,Jiangquan Lv,Yiyin Huang,Maoxiang Wu,Yaobing Wang,Jiannian Yao
Metal–CO 2 batteries represent a promising priority for sustainable energy and the environment. However, CO 2 utilization in nonaqueous electrolytes mostly involves difficult CO 2 electrochemistry, leading to poor selectivity and limited cycle performance. Herein, an aqueous rechargeable Zn–CO 2 electrochemical cell that tunably produced CO fuel gas (90% Faradaic efficiency) during cell discharge (cathodic reaction: CO 2 + 2e − + 2H + → CO + H 2 O) and O 2 during cell charge at ≈2 V (cathodic reaction: H 2 O → 1/2O 2 + 2e − + 2H + ), mimicking the separate steps of CO 2 fixation and water oxidation during photosynthesis while exhibiting the advantages of high efficiency, tunable products, and operation independent of sunlight is proposed and realized. The cell achieves a remarkable energy efficiency of 68% with fuel generation, providing an alternative for the green, efficient, and safe utilization of CO 2 by metal–CO 2 batteries.
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PubMed
高影响因子
APPLIED ENERGY
·
2019
·
IF 8.426
Hui Guo,Chenxu Li,Xiaoqin Shi,Hui Li,Shufeng Shen
High energy consumption for CO 2 capture using aqueous amines is still a major drawback limiting its deployment on a global scale. In this work, the absorption-desorption performance of CO 2 into several blends of monoethanolamine (MEA) or diethanolamine (DEA) with glycol ethers (2-methoxyethanol (2ME) and 2-ethoxyethanol (2EE)) as nonaqueous solvents has been investigated at ambient pressure. Reaction mechanisms and the relative heat duty for these nonaqueous systems were also explored and compared with those of the aqueous MEA. Results showed that the nonaqueous absorbents with 5.0 M MEA had comparable absorption capacity with aqueous 5.0 M MEA and higher desorption efficiency resulting in a larger cyclic capacity (1.45 mol kg −1 ). Higher partial pressure ratio of CO 2 to solvent vapor under the desorption conditions was also observed for these nonaqueous systems. 13 C NMR, FTIR spectra and online conductivity analysis provided evidences that CO 2 can react with MEA in nonaqueous solvents forming the ionic couples (i.e. protonated MEA and carbamate) as well as carbamic acid at high CO 2 loading. The mixture of MEA and 2ME or 2EE could significantly reduce the energy consumption by about 55% as compared to the benchmark aqueous 5.0 M MEA system.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Cheng Wang,Xinwei Liu,Wei Li,Xin Huang,Sen Luan,Xiaojian Hou,Mengnan Zhang,Qian Wang
Hierarchically porous metal-organic frameworks with micropores, mesopores , and macropores have been successfully fabricated by using compressed CO 2 . Not any acid or addition but compressed CO 2 was added into the synthesis system for achieving hierarchically porous materials. TEM , SEM, N 2 adsorption, XRD , TG, FTIR, and EDX were employed to character structural and component of the obtained materials. The mesopores size of resultant MOFs prepared by this approach can be expanded as large as 28 nm, which is rather difficult to obtain by conventional syntheses method. In addition, the amount and proportion of micropores, mesopores, and macropores distributed in the obtained samples can be controlled by adjusting CO 2 pressure. Furthermore, the resulting hierarchically porous MOFs (HP-MOFs) can be utilized to absorb selectively on CO 2 and CH 4 , which demonstrate the enhanced adsorption behavior. The liquid phase adsorption performances of the as-prepared HP-MOFs samples are evaluated by using methylene blue as a model adsorbate. The possible mechanism of formation of HP-MOFs by using compressed CO 2 was proposed according to results of the experiments. Compared with traditional synthetic methods, the compressed CO 2 plays many roles in the synthesis of HP-MOFs. Notably, this versatile approach can be applied to prepare other hierarchically porous materials in the organic solvent–water miscible system.
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Jove-Journal of Visualized Experiments
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2019
·
IF 1.108
XiaoXiang Fang,Zhihong Gao,Hanfeng Lu,Qiulian Zhu,Zekai Zhang
We demonstrate a method for the enhancement of CO2 photoreduction. As the driving force of a photocatalytic reaction is from solar light, the basic idea is to use concentration technology to raise the incident solar light intensity. Concentrating a large-area light onto a small area cannot only increase light intensity, but also reduce the catalyst amount, as well as the reactor volume, and increase the surface temperature. The concentration of light can be realized by different devices. In this manuscript, it is realized by a Fresnel lens. The light penetrates the lens and is concentrated on a disc-shaped catalyst. The results show that both the reaction rate and the total yield are efficiently increased. The method can be applied to most CO2 photoreduction catalysts, as well as to similar reactions with a low reaction rate at natural light.
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PubMed
高影响因子
Nano Energy
·
2019
·
IF 15.548
Yecan Pi,Jun Guo,Qi Shao,Xiaoqing Huang
Perovskite oxides are a class of attractive materials for their broad applications in many energy conversion and storage fields, while their catalytic performance of CO 2 electroreduction (CO 2 ER) has been rarely investigated. Herein, all-inorganic SrSnO 3 perovskite nanowires are constructed and utilized to catalyze the CO 2 ER for the first time. Inspiringly, such SrSnO 3 NWs demonstrates impressive selectivity and activity for formate production, with considerable Faradaic efficiencies (~80%) over a broad potential range, and the highest formate partial current density of 21.6 mA cm −2 , much better than that of the SnO 2 nanoparticles . Further analyses reveal that the notable CO 2 ER activity of SrSnO 3 NWs is linked to the efficient stabilization of formate intermediate (CO 2 •− ) as well as the slow kinetics for hydrogen evolution reaction (HER). This work can inspire the development of highly efficient perovskite catalysts for CO 2 ER and beyond.
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Journal of CO2 Utilization
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2019
·
IF 5.189
Weiqi Liu,Zhichao Miao,Zhenbin Li,Xiaozhong Wu,Pengfei Zhou,Jinping Zhao,Huahua Zhao,Weijiang Si,Jin Zhou,Shuping Zhuo
A series of Co@N-C materials are synthesized from pyrolysis of ZIF-67 at different temperatures and employed as catalyst for electrochemical reduction of CO 2 (CO 2 RR) to syngas. Through a systematical investigation of the relationship between structure of Co@N-C catalysts and their catalytic activity, it could be found that the Co species exposed on the material surface mainly promote the hydrogen evolution reaction (HER) process to produce H 2 , while the Co particles packaged by N-C skeleton provide electrons and transfer them to CO 2 molecule through the Co -N- C skeleton, promoting the CO 2 reduction reaction. Following this thinking, the pristine Co@N-C materials are treated by aqua regia to remove the surface exposed Co species. After acid treatment, the affinity of H species sharply decreases, and adsorption of CO 2 and transfer of electron to CO 2 are successfully improved. The acid-treated Co@N-C catalysts exhibit improved catalytic activity, faradic efficiency of CO, and stability in CO 2 RR process. Among all these catalysts, the obtained Co@N-C-700-A shows highest CO 2 reduction activity and stability, achieving a specific current of 25 A∙g (cat) −1 and a productivity of 0.266 mol (CO) h −1 ∙ g(cat) −1 at a mild potential of -0.57 V vs. RHE. The ratio of CO/H 2 in products could be adjusted in the range of 1/4 to 1.5/1.
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POLYMER
·
2018
·
IF 3.483
Jin Wang,Hongming Zhang,Yuyang Miao,Lijun Qiao,Xianhong Wang,Fosong Wang
CO 2 based waterborne polyurethane (CO 2 -WPU), especially high CO 2 content one, suffered from the poor flexibility at low temperature due to high content of rigid carbonate segment. Here a microphase separation idea was proposed by introducing poly(butyl acrylate) (PBA) as soft phase to toughen CO 2 -WPU via an organic solvent free route, i.e., the polymerizable butyl acrylate acted as a pseudo-solvent during CO 2 -WPU prepolymer synthesis, it then experienced radical polymerization after formation of CO 2 -WPU, and finally forming a material with multi-phase structure. Benefiting from the separation of soft PBA phase and hard CO 2 -WPU phase in micro-size, a 368% increase in elongation at break (ε b ) and nearly 65 times increase in toughness at -10 °C was observed when PBA loading increased from blank to 65 wt%. As a comparison, the tensile strength (σ m ) and ε b of the PBA/CO 2 -WPU blending film at room temperature was only 4.4 MPa and 383% when PBA loading was 50 wt%, while the PBA/CO 2 -WPU multi-phase film showed σ m of 18.8 MPa and ε b of 489%, respectively. The toughening effect was attributed to the more uniform micro-phase separation structure caused by molecular level inter-migration between PBA and CO 2 -WPU during preparation process.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 40
·19743-19749
·
IF 9.931
Chengcheng Yan,Long Lin,Dunfeng Gao,Guoxiong Wang,Xinhe Bao
The electrochemical CO2 reduction reaction (CO2RR) powered by renewable electricity has emerged as a promising approach to alleviate global warming and energy depletion simultaneously. Notably, efficient catalysts containing Earth-abundant elements to achieve high CO2RR performance are in great demand for future applications. Herein, carbon-supported gallia gel nanoparticles were synthesized by precipitating gallium nitrate on carbon black in an ethanolic ammonia solution. Nano-sized gallia nanoparticles uniformly dispersed on the carbon support achieved a maximum CO faradaic efficiency of 77.0% at −0.71 V vs. the reversible hydrogen electrode (RHE) in CO2-saturated 0.1 M KHCO3 solution, showing a dramatic improvement compared to a bulk Ga electrode with only 24.2% CO faradaic efficiency at −0.80 V vs. RHE. X-ray photoelectron spectroscopy measurements revealed that surface Ga3+ species were reduced to metallic Ga when subjected to a negative potential during the CO2RR, indicative of the formation of oxide-derived active gallium sites. Control experiments further highlighted the necessity of close coalescence between the nano-sized gallia particles and the conductive carbon support. The present study underscores the feasibility of improving the CO2RR performance of Ga-related materials through nanostructuring of oxide-derived gallium catalysts.
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SEPARATION SCIENCE AND TECHNOLOGY
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2018
·
IF 1.2
Libin Mei,Xinmin Liu,Jianjun Wu
A series of solid amine adsorbents were prepared by the template method with ion-exchange resin (D001) as the carrier and polyethyleneimine (PEI) as the modifier. The absorbents were characterized by energy disperse spectroscopy (EDS), scanning electron microscope (SEM), N2 adsorption–desorption, Fourier transform infrared spectroscopy (FTIR) and thermogravimetric analysis (TGA) techniques. The effects of PEI loading, adsorption temperature and influent velocities on CO2 adsorption capacity in a fixed-bed reactor were investigated. The results show that the solid amine adsorbent prepared by the template method had a better PEI dispersion, stability and CO2 adsorption capacity. The maximum CO2 adsorption capacity was 3.98 mmol·g−1 when PEI loading was 30%, the adsorption temperature was 65°C and the influent velocity was 40 mL·min−1. The CO2 adsorption capacity decreased only by 9.50% after 10 cycles of adsorption–desorption tests. The study of kinetics indicates that both chemical adsorption and physical adsorption occurred in the CO2 adsorption process. The CO2 adsorption process included fast breakthrough adsorption and gradually approaching equilibrium stage. The particle internal diffusion process was the control step for CO2 adsorption.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Zhihao Liu,Yachao Li,Kangzhou Wang,Yan Li,Yurong He,Jie Liang,Jianli Zhang,Tian-sheng Zhao,Noritatsu Tsubaki,Xinhua Gao
The design and preparation of highly active and stable Ni-based catalysts has attracted extensive attention. In this study, a series of embedded Ni@C catalysts were synthesized by a facile sol-gel method. After reduction at 400 °C, the optimized Ni@C-400 catalyst showed excellent performance in CO 2 methanation at a low temperature of 300 °C, with a CO 2 conversion of 74.3 % and good stability for 70 h. The characterization results indicated that after reduction treatment, the carbon species in the precursor were transformed into graphite carbon with more disorder defects. This structure facilitated the anchoring effect of the nickel components in the Ni@C catalyst, thereby forming a distinctive embedded structure that ensured the preservation of the nickel active phase in the catalyst following prolonged reaction. Therefore, the Ni@C catalyst prevented severe sintering and loss of loaded nickel. In addition, the interaction between Ni and C facilitated charge transfer, enhancing the CO 2 activation.
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