MOLECULES
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2024
·Vol. 29
·期 5
·1006
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IF 4.2
Xia Wang,Wulan Zeng,Peidan Hu,Shengxin Liu,Yuechao Lin,Zhaowen He,Chunling Xin,Xiangjun Kong,Jinghan Xu
Organic amine-modified mesoporous carriers are considered potential CO2sorbents, in which the CO2adsorption performance was limited by the agglomeration and volatility of liquid amines. In this study, four additives of ether compounds were separately coimpregnated with polyethylene polyamine (PEPA) into MCM-41 to prepare the composite chemisorbents for CO2adsorption. The textural pore properties, surface functional groups and elemental contents of N for MCM-41 before and after functionalization were characterized; the effects of the type and amount of additives, adsorption temperature and influent velocity on CO2adsorption were investigated; the amine efficiency was calculated; and the adsorption kinetics and regeneration for the optimized sorbent were studied. For 40 wt.% PEPA-loaded MCM-41, the CO2adsorption capacity and amine efficiency at 60 °C were 1.34 mmol/g and 0.18 mol CO2/mol N, when the influent velocity of the simulated flue gas was 30 mL/min, which reached 1.81 mmol/g and 0.23 mol CO2/mol N after coimpregnating 10 wt.% of 2-propoxyethanol (1E). The maximum adsorption capacity of 2.16 mmol/g appeared when the influent velocity of the simulated flue gas was 20 mL/min. In addition, the additive of 1E improved the regeneration and kinetics of PEPA-loaded MCM-41, and the CO2adsorption process showed multiple adsorption routes.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2011
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IF 2.089
Jun Li,Yinmei Ye,Lifang Chen,Zhiwen Qi
The solubilities of CO2 in solvent poly(ethylene glycols) (PEGs) with molecular weights of 150, 200, 300, and 400 were measured over the range of pressure from (100 to 1200) kPa and temperature from (303.15 to 333.15) K. Henry's constant was obtained by linear fitting of the experimental data, and thermodynamic properties of solutions were calculated from the correlation of Henry's constant. It indicates that the solubility of CO2 increases with increasing molecular weights of PEGs. Henry's constant based on mole fraction and the molality of CO2 in PEG400 vary from (4.78 to 7.09) MPa and (1.56 to 2.48) MPa·kg·mol–1 from (303.15 to 333.15) K, respectively.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
·
IF 4
Miao Jiang,Peng-Li Zhao,Yong-Ning Yue,Xue-Qin Song,Li Wang
With the acceleration of industrialization and energy consumption, global concerns for the safety of ecological system and sequent human health have attracted consideration attention increasingly in view of the severe contamination both in aqueous environment and aerosphere. Therefore, the development of multifunctional species for efficient adsorption of pollutants and chemical fixation of CO 2 receives increasing attention. Herein, an anionic Er III metal organic framework ( Er-MOF ) with large hexagonal channels, is obtained based on a benzene-spaced tetracarboxylate ligand, H 4 L (H 4 L = 1,4-bis(2′,2′′,6′,6′′-tetracarboxy-1,4′:4,4′′-pyridyl) benzene). Adsorption analysis indicates that Er-MOF behaves as an excellent adsorbent for selectively absorbing MB in water with a maximum adsorption capacity of 494.1 mg·g ‒1 . The adsorption mechanism could be a combination of size matching, electrostatic interaction, π···π stacking and hydrogen bonding. In addition, Er-MOF is demonstrated to be an efficient catalyst in the cycloaddition of CO 2 with epoxides under mild conditions due to its excellent stability, substantial specific surface area, confined space and well-exposed Lewis acid/base sites. The findings presented herein had great significance for enriching the multifunctional lanthanide MOFs in environmental applications.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
·
IF 6.9
You-yun Gong,Zi-ang Jia,Yiwen Fan,Jin-ping Cheng
Rational chemical modification engineering of metal-organic frameworks (MOFs) is an effective means to improve their CO 2 capture efficiency. In this study, we prepare UiO-66 MOF impregnated with different types of aliphatic amines using solvothermal and impregnation techniques, respectively, and investigated their performances in CO 2 adsorption and CO 2 /N 2 separation using the isothermal adsorption method. Aliphatic amines successfully chemically modifies UiO-66, and their molecules effectively occupied the pores of the UiO-66 framework, which has been confirmed by material characterization, experiments, and DFT-FMO calculations. There are significant improvements in the ability to capture CO 2 when aliphatic amines were added to UiO-66 compared to pure UiO-66 (1.39 mmol/g up to 2.11 mmol/g-2.53 mmol/g), attributed to the different types and numbers of amines, and there were also differences in the Zr metal clusters and BDC ligands. Meanwhile, The material has better CO 2 /N 2 adsorption IAST selectivity(98) because its surface area is changed and N 2 does not interact specifically with the adsorbent. Furthermore, the CO 2 adsorption capacity remains constant across multiple adsorption cycles, highlighting the adsorbent's stability and reliability during repetitive CO 2 capture. This study provides new ideas and perspectives for improving the CO 2 capture efficiency of UiO-66.
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APPLIED CLAY SCIENCE
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2024
·
IF 5.3
Xiaoyu Li,Kang Peng,Xueqi Zhao,Keping Zhao,Haoran Li,Yanrong Zhao,Bo Zhang
Amine-functionalized mesoporous silica is considered as one of the most promising solid amine adsorbents for post-combustion carbon dioxide (CO 2 ) capture due to their high specific surface area, large pore volume and adjustable pore structure . However, the high costs associated with silica precursors and synthesis techniques of amine-functionalized mesoporous silica have extremely limited their practical applications. In this work, a facile and feasible approach was proposed to construct polyethyleneimine (PEI)-impregnated of Al-MCM-41 derived from natural flake-like kaolinite (FK) clay. The effect of PEI loadings and adsorption temperature on CO 2 uptakes, adsorption/desorption kinetics and stability for Al-MCM-41/PEI x adsorbents were specifically discussed. The optimal Al-MCM-41/PEI (AP30) adsorbent exhibited a high CO 2 uptake of 1.27 mmol/g at 75 °C and stable cyclic stability with a mere 1.1% decline per cycle over 10 adsorption-regeneration cycles, resulting from the unique ordered porous structure and spatial confinement effect of as-prepared Al-MCM-41 support to suppress excess PEI agglomeration and avoid blocking CO 2 adsorption in the resultant adsorbents. The good PEI dispersions provided abundant CO 2 affinity sites, which is beneficial to efficient CO 2 diffusion and adsorption, and thus greatly improving the CO 2 capture performances. This approach has enormous potential for cost-effective large-scale practical applications for CO 2 capture and separation processes.
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Progress in Natural Science-Materials International
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2024
·
IF 4.8
Shijia Liu,Haibin Wang,Xi Wang,Jieshu Zhou,Hongyan Liang
Electroreduction of CO 2 for formic acid production has been regarded as an efficient option for CO 2 utilization. However, under high current, achieving high selectivity for formic acid is challenging, which cannot meet industrial demands. Herein, we reported a type of Bi/In(OH) 3 (BIO) heterojunction reconstructed from Bi 2 S 3 /In(OH) 3 during electrochemical process, in which In(OH) 3 was applied to modulate the electronic structure of Bi. This strategy efficiently enhanced the ∗OCHO intermediates adsorption and lead to a decent selectivity towards formic acid under high current density. BIO displays faraday efficiency of formic acid beyond 95 % across a wide range current density of 200–400 mA cm −2 , where the highest value reached 97.7 % at 400 mA cm −2 . This work clarified the mechanism of CO 2 electroreduction to HCOOH on heterojunction, guiding the design of advanced catalysts.
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Yang Li,Dario R. Dekel,Xuezhong He
Amine-rich facilitated transport membranes (FTMs) attract great interest in intensifying the membrane-based CO 2 separation processes. The high-molecular-weight polyvinylamine (PVAm) polymers containing fixed-site carriers of the amino groups were used to prepare highly CO 2 -permeable membranes. The sterically hindered PVAm polymers of poly(N-methyl-N-vinylamine) and poly(N-isopropyl-N-vinylamine) were obtained by functionalization of PVAm to provide superior CO 2 solubility. By loading the mobile carriers of amino acid salt (AAS) and CO 2 -philic graphene oxide (GO), the prepared FTMs render enhanced CO 2 permeance and CO 2 /N 2 selectivity. The d-spacing of 8.8 Å and the ultramicropores of 3.5 Å from GO nanosheets provide the combination of both selective surface flow and molecular sieving mechanisms to achieve improved CO 2 permeance and CO 2 /N 2 selectivity. In addition, the intercalation of GO hinders N 2 transport through the membrane due to a longer pathway, while the mobile carriers of AAS introduced into the PVAm matrix facilitate CO 2 transport through the selective layer. Therefore, the CO 2 /N 2 selectivity of the prepared FTMs was significantly enhanced to 171 based on the intensified carrier-driving transport mechanism. It can be concluded that amine-rich membranes based on both fixed and mobile carriers of the amino groups together with intercalated GO can synergistically improve the CO 2 /N 2 separation performance, and be potentially applied for CO 2 capture from flue gas .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Furong Li,Gonghe Tong,Yanbin Li,Zhigang Wang,Xiaoyao Tan
Protonic ceramic electrochemical reactors (PCER), having the advantages of high efficiency, adjustability, and scalability, exhibit great potential in energy storage such as conversion of CO 2 into high-value chemicals. Designing critical components like the electrolyte and electrodes of electrochemical reactors is essential to widen commercial applications. The present work constructed a three-layer microtubular PCER (MT-PCER) for CO 2 hydrogenation. BaCe 0.5 Zr 0.3 Y 0.2 O 3-δ (BCZY) was used as the electrolyte material to prepare BCZY/Ni-BCZY/Ni triple-layer hollow fibers (TLHFs) by a phase-inversion based co-spinning/co-sintering process. Porous Ni-BCZY was the catalytic functional (cathode) layer, and the metallic Ni composed the current collector layer. Results indicated that CO 2 conversion and CH 4 selectivity were significantly enhanced when the NiO content in the cathode layer increased from 40 % to 60 %, while there was no significant change for the content continuously increasing to 80 %. Compared with the reactor employing dual-layer hollow fibers, the Ni collector layer in TLHFs presented a remarkable intensification of the methanation performance. As a result, the MT-PCER with 60 % NiO content in the cathode layer and utilizing the Ni current collector was the recommended reactor structure, which possessed the CO 2 conversion of 29.8 %, CH 4 selectivity of 50.9 %, CH 4 yield of 15.2 %, and faradaic efficiency of 43.6 % at 700 °C and 2 V applied voltage. The adjusted design of the TLHF facilitated the advancement of the performance and efficacy of the MT-PCER, promoting carbon capture, utilization, and storage processes.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Tongjun Yang,Junpeng Xu,Hailiang Sheng,Junqin Wang,Gang Hu,Songmiao Liang,Lijie Hu,Lihua Zhang,Haibo Xie
The CO 2 -based reversible ionic liquid solution of 1,1,3,3-tetramethylguanidine (TMG) and ethylene glycol (EG) in dimethyl sulfoxide (DMSO) after capturing CO 2 , (2[TMGH] + [O 2 COCH 2 CH 2 OCO 2 ] 2− /DMSO ( χ RILs = 0.1), provides a sustainable and effective platform for cellulose dissolution and homogeneous utilization. Highly porous cellulose aerogel beads and monoliths were successfully prepared via a sol-gel process by extruding cellulose solution into different coagulation baths (NaOH aqueous solution or alcohols) and exposing the cellulose solution in open environment, respectively, and followed by different drying techniques, including supercritical CO 2 -drying, freeze-drying and air-drying. The effect of the coagulation baths and drying protocols on the multi-scale structure of the as-prepared cellulose aerogel beads and monoliths were studied in detail, and the sol-gel transition mechanism was also studied by the solvatochromic parameters determination. High specific surface area of 252 and 207 m 2 /g for aerogel beads and monoliths were achieved, respectively. The potential of cellulose aerogels in dye adsorption was demonstrated.
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Advanced Science
·
2024
·
IF 14.3
Jia Shi,Andrew J. Tanentzap,Yuanze Sun,Jianjun Wang,Baoshan Xing,Matthias C. Rillig,Changchao Li,Ling Jin,Fang Wang,Tanveer M. Adyel,Jianying Shang,Xiang Wang,Jie Wang
Microplastic pollution in terrestrial ecosystems threatens to destabilize large soil carbon stocks that help to mitigate climate change. Carbon-based substrates can release from microplastics and contribute to terrestrial carbon pools, but how these emerging organic compounds influence carbon mineralization and sequestration remains unknown. Here, microcosm experiments are conducted to determine the bioavailability of microplastic-derived dissolved organic matter (MP-DOM) in soils and its contribution to mineral-associated carbon pool. The underlying mechanisms are identified by estimating its spectroscopic and molecular signatures and comparing its sorption properties on model minerals with natural organic matter (NOM). The results show that MP-DOM leads to 21–576% higher CO 2 emissions and 34–83% lower mineral-associated organic carbon in soils than NOM, depending on the type of plastic polymer. DOM from biodegradable microplastics induces higher CO 2 emissions than conventional microplastics. It is found that MP-DOM is 7.96 times more labile than NOM, making it more accessible for microbial utilization. The lower degree of humification, fewer polar functional groups, and higher H/C ratios in MP-DOM also led to 3.96 times less sorption with mineral particles. The findings provide insights into the effects of microplastics on soil carbon storage and highlight their consequences for wider terrestrial carbon cycling and climate warming.
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Journal of Energy Chemistry
·
2024
·
IF 14
Guan Wang,Shengtao Zhong,Xiaoqian Xiong,Jing Li,Fangyuan Wang,Li Huo,Daoxiong Wu,Xingqi Han,Zhitong Wang,Qi Chen,Xinlong Tian,Peilin Deng
Bismuth-based catalysts are highly promising for the electrochemical carbon dioxide reduction reaction (eCO 2 RR) to formate product. However, achieving high activity and selectivity towards formate and ensuring long-term stability remains challenging. This work reports the oxygen plasma inducing strategy to construct the abundant grain boundaries of Bi/BiO x on ultrathin two-dimensional Bi nanosheets. The oxygen plasma-treated Bi nanosheet (OP-Bi) exhibits over 90% Faradaic efficiency (FE) for formate at a wide potential range from −0.5 to −1.1 V, and maintains a great stability catalytic performance without significant decay over 30 h in flow cell. Moreover, membrane electrode assembly (MEA) device with OP-Bi as catalyst sustains the robust current density of 100 mA cm −2 over 50 h, maintaining a formate FE above 90%. In addition, rechargeable Zn-CO 2 battery presents the peak power density of 1.22 mW cm −2 with OP-Bi as bifunctional catalyst. The mechanism experiments demonstrate that the high-density grain boundaries of OP-Bi provide more exposed active sites, faster electron transfer capacity, and the stronger intrinsic activity of Bi atoms. In situ spectroscopy and theoretical calculations further elucidate that the unsaturated Bi coordination atoms between the grain boundaries can effectively activate CO 2 molecules through elongating the C–O bond, and reducing the formation energy barrier of the key intermediate (*OCOH), thereby enhancing the catalytic performance of eCO 2 RR to formate product.
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Plasma Processes and Polymers
·
2024
·Vol. 21
·期 7
·2400037
·
IF 2.9
Xuming Zhang,Yun Shan,Zhi Sun,Hua Pan,Yuzhen Jin,Zuchao Zhu,Liancheng Zhang,Wenhao Lin,Zhengbo Dai,Zhengang Lou,Huaming Li,Kai Li
Plasma catalytic CO 2 hydrogenation to methanol over MnO x /ZrO 2 catalyst was investigated in this work. A boosted methanol yield of 4.6 mg/h was obtained over MnO x /ZrO 2 catalyst, while it was only 0.0 and 0.7 mg/h for ZrO 2 and MnO x catalyst, respectively. The interaction between MnO x and ZrO 2 was responsible for the enhanced methanol yield. It resulted in sufficient oxygen vacancy. The in situ DRIFT spectra was conducted to reveal the plasma catalytic CO 2 hydrogenation to methanol reaction mechanism and the key intermediates of HCOO and CH 3 O species were determined. The sufficient oxygen vacancy promoted the formation of the key intermediates, especially the CH 3 O species.
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