INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
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IF 2.843
Lei Wang,Zhiming Zhou,Yuanwu Hu,Zhenmin Cheng,Xiangchen Fang
A series of nanosheet MgO-based sorbents promoted by mixed-alkali-metal nitrate and carbonate were prepared by a simple precipitation–deposition method and applied to CO2 capture. The structural properties of these sorbents were characterized by various techniques, and their CO2 capture performance was evaluated using a thermogravimetric analyzer. Compared to the sorbent derived from commercial MgO, the nanosheet MgO-based sorbent had faster and higher CO2 uptake, because of its thin-sheet structure. Among various alkali-metal-salt-promoted nanosheet MgO, the sorbents promoted with mixed-alkali-metal nitrates (LiNO3 and KNO3) and carbonates (Na2CO3 and K2CO3) exhibited a high total CO2 uptake at a respectable rate. In particular, the sorbent with a MgO content of 73 wt % and a nitrate/carbonate molar ratio of 2 possessed the highest total CO2 uptake and the best cyclic stability, with a total uptake of 0.52 gCO2/gsorbent and MgO conversion of 65% after 20 cycles (60 min of absorption in 40% CO2/60% N2 at 350 °C, 15 min of regeneration in 100% N2 at 400 °C). Based on the structure–activity relationship of the sorbents, a possible mechanism consisting of three stages was presented for the CO2 absorption process, in which the dissolution of CO2 and carbonation in the molten nitrate played an important role.
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NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 13
·5297-5304
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IF 3.269
Fengqin Yin,Peixuan Peng,Wenjie Mo,Shuixia Chen,Teng Xu
A porous amino resin melamine–formaldehyde (MF) with a high content of hydroxymethyl groups was prepared via the polycondensation of an excess of formaldehyde with melamine. Polyethylene imine (PEI) was then grafted onto the porous amino resin via a Mannich reaction between the active hydroxymethyl groups on the MF resin and the amino group on PEI to synthesize a solid amine adsorbent (MF-g-PEI). A large amount of hydroxymethyl groups were generated on the synthesized amino resin due to the excess formaldehyde used in the polycondensation reaction, which will provide abundant active sites to firmly combine with PEI and thus, enhance the stability of the MF-g-PEI adsorbent. The BET surface area and the pore volume of MF-g-PEI prepared using the optimal conditions were 460 m2 g−1 and 0.76 cm3 g−1, respectively. The CO2 adsorption capacity of MF-g-PEI, with a PEI loading of 11.35% can reach 1.32 mmol g−1 at 10 °C, while its amine utilization efficiency can reach up to 48.9%. The adsorbents also exhibited significantly improved adsorption kinetics and regeneration performance. This work provides a novel method that can achieve a promising solid amine adsorbent by directly grafting PEI onto porous material in the absence of an intermediate.
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International Journal of Greenhouse Gas Control
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2017
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IF 3.741
Lidong Wang,Shanlong An,Songhua Yu,Shihan Zhang,Yifeng Zhang,Meng Li,Qiangwei Li
CO 2 from coal-fired flue gas is one of the main components of greenhouse gases. Using phase change absorbents as a solvent can effectively decrease the consumption of regeneration energy for CO 2 capture process. This study employed a mixed solution of diethylenetriamine (DETA) and diethylaminoethanol (DEEA) as the new phase change absorbent for CO 2 absorption. The impact of the phase change behavior on the mass transfer characteristics of CO 2 absorption was investigated in a wetted-wall column. Effects of the temperatures, CO 2 loadings, and gas flow rate on the mass transfer coefficient were also conducted. The results indicated that temperature and CO 2 loading had relatively remarkable effects on the total mass transfer coefficient; whereas the gas flow rate had a smaller effect. Kinetic analysis revealed that the mass transfer resistance of CO 2 absorption into the DETA/DEEA phase change absorbent mainly concentrated at the liquid film side. The findings provide a theoretical reference for the development of new CO 2 phase change absorption technology .
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AICHE JOURNAL
·
2024
·
IF 3.5
Tong Luo,Qi Liu,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Aqueous amine solution is a promising absorbent for CO 2 capture, yet irreversible reaction, that is, degradation can happen for amine and leads to performance decrease and many operating difficulties. Despite numerous research on reaction between amine and CO 2 for absorption, the reaction of amine degradation is not fully understood, especially for tertiary amine which is a vital component in constructing high-performance CO 2 absorbent. Considering the variety of tertiary amines, this article studied the thermal stability of five tertiary amine solutions at different temperatures to mimic the regeneration condition. The density functional theory (DFT) calculation was applied to reveal the degradation mechanism. The alkylation reaction that triggered the degradation of tertiary amine was deemed as the limiting step. Then the molecular simulation method was extended to 12 tertiary amines, aiming to further illustrate the influence of molecular structure on the alkylation reaction. These results provide basic data and theoretical guidance for developing the anti-degradation CO 2 absorbent.
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BIOTECHNOLOGY PROGRESS
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2025
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IF 2.5
Xiuyuan Zhou,Linqing Li,Shengjie Sun,Peng Xiong,Xiutao Liu
Redesigning metabolic pathways to enhance the efficiency of carbon fixation during chemical biosynthesis is a promising approach for achieving cleaner and greener production of multi-carbon compounds. In this study, we established a model of cell growth in Escherichia coli that is dependent on the RuBisCO-Prk pathway by regulating its central metabolism. This rewiring ensures that growth depends on RuBisCO's carboxylation, allowing heterotrophic growth to rely on carbon fixation. This model was verified by detecting the growth curve, and it was used to screen four RuBisCO genes, of which the gene from Rhodospirillum rubrum ATCC 11170 serves as a growth advantage for E.coli . In addition, this model was applied to construct an efficient succinate biosynthetic pathway that can produce two moles of succinate from one mole of xylose and three moles of CO 2 . Compared to conventional succinate biosynthesis, this strategy has a CO 2 fixation capacity that is 1.5 times greater. Furthermore, to optimize succinate production, various approaches were employed, including the optimization of key enzymes, substrate transport, and the supply of inorganic carbon. The resulting strain was capable of producing succinate at a level of 2.09 ± 0.14 g/L, which is nearly 22.4 times that of the original strain. In conclusion, this study was developed for the production of two moles of succinate by implementing three moles of carbon fixation reactions and demonstrated the feasibility of various optimization strategies in biological carbon fixation.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ning Liu,Na Lu,Kun Zhao,Pengxiao Liu,ZhuMei Sun,Jing Lu
The conversion of methane (CH 4 ) and carbon dioxide (CO 2 ) into high-value products under mild conditions is crucial for addressing the greenhouse effect and advancing C1 chemistry. In this study, Cu/ZnO catalysts were prepared through a one-step wet reduction process, and the catalytic conversion of CH 4 and CO 2 into acetic acid molecules (CH 3 COOH) was achieved via photon activation at ambient temperature. The yield of acetic acid was 411.6 μmol/Lg cat −1 h −1 with a selectivity of 89.5 % under optimal conditions (100 mWcm −2 light intensity, 25 ± 2 °C, 2 MPa pressure, and a 1:1 CH 4 :CO 2 volume ratio). Enhanced solubility of CH 4 in aqueous under increased pressure and temperature was observed to improve acetic acid production. Additionally, the catalytic mechanism involved surface chemisorption of CH 4 and CO 2 , facilitated by ZnO and Cu in the catalyst, leading to C-C coupling and subsequent acetic acid formation, driven by photogenerated electron-hole migration. This study provides a foundational understanding for the synthesis of value-added chemicals through CH 4 and CO 2 conversion via C-C coupling in mild environments.
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ENERGY
·
2024
·
IF 9
Pengcheng Li,Dantong Wang,Yaoqi Hou,Zhan Hu,Danqing Chen,Yi Wang,Chunfeng Song
CO 2 absorption-microalgae conversion (CAMC) system can be a sustainable technology to achieve low-energy carbon capture and resource utilization in response to zero carbon. However, light stress could restrict the carbon utilization efficiency of CAMC system. In this study, melatonin (MT) and indole-propionic acid (IPA) as phytohormones, were used to promote the carbon fixation capacity and biomass yield of CAMC system under light stress, and the potential mechanism was also discussed. Both MT and IPA promoted the growth of Spirulina , and 10 mg-MT group obtained the highest biomass and carbon fixation capacity, which were 27.61 % and 30.62 % higher than control. MT and IPA promoted the activity of superoxide dismutase (SOD), catalase (CAT), and glutathione reductase (GR), enhancing antioxidant activity to avoid oxidative damage. The results of transmission electron microscopy (TEM) and cell apoptosis showed MT and IPA reduced cell membrane damage and apoptosis. Phytohormones induced the carbon flux flow to the synthesis of carbohydrate and protein, and increased carbohydrate and protein productivity. Moreover, the maximum phycocyanin content and yield were 13.74 % and 43.25 % higher than the control. Therefore, adding phytohormones was an effective strategy to achieve high-value bioresources of microalgae in CAMC system under light stress.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Shanyue Lu,Shengwei Zhang,Linlin Li,Cong Liu,Zhou Li,Dan Luo
Converting CO 2 into high-value-added chemicals by artificial photosynthesis technology effectively solves environmental problems and energy shortages. Nevertheless, it remains challenging to improve CO 2 conversion rates due to low photo-utilization and rapid electron-hole recombination. In this study, we successfully synthesized direct Z-scheme ZnIn 2 S 4 /BaTiO 3 heterojunction structure by a hydrothermal method. Specifically, compared with previous studies of various heterojunction catalysts, ZnIn 2 S 4 /BaTiO 3 heterojunction structure achieved a remarkably high yield of 105.89 μmol g -1 h - 1 , increasing 2.55 and 3.62-fold over the individual performance of ZnIn 2 S 4 and BaTiO 3 , respectively. Our investigation of photocatalytic mechanism suggest that the improved photocatalytic CO 2 reduction performance can be attributed to the synergistic effects of the piezoelectric effect and Z-scheme electron transfer mechanism. These effects can synergistically enhance space charge separation and retain photogenerated electrons, thereby facilitating a more efficient CO 2 reduction process. Consequently, this innovative piezoelectric effect-assisted Z-scheme heterojunction demonstrates immense potential to offer a novel strategy for addressing CO 2 reduction challenges and advancing sustainable energy development.
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ENERGY & FUELS
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2024
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IF 5.2
Yue Gu,Hongjun Tu,Ming Zhou
In this paper, a biobased ternary composite microgel (CS-DP-AA) was designed and prepared, which was based on chitosan and had a reversible response to CO2. The synthesis of CS-DP-AA microgel was proved by infrared spectroscopy, chromatography–mass spectrometry, X-ray photoelectron spectroscopy, and Raman spectroscopy. The structure and properties of CS-DP-AA microgel before and after CO2 response were characterized by scanning electron microscope, transmission electron microscope, ultraviolet visible spectrophotometer, laser particle size analyzer, zeta potentiometer, and other instruments, and the CO2 response mechanism was explored. The results show that CS-DP-AA microgel had great CO2 response performance and stability, and the UV transmittance could still reach 90.01% (relative) at 268.98 h after CO2 response. Subsequently, the rheological properties of CS-DP-AA microgel were evaluated by a rotary rheometer, which shows that CS-DP-AA microgel after the CO2 response had obvious viscoelasticity. Although shear thinning appeared with the increase in shear rate, the CS-DP-AA microgel after the CO2 response still had good viscosity under high temperature, high pressure, and high shear rate, which proves that it had great rheological properties. On the other hand, the ability of CS-DP-AA microgel to plug gas channeling in reservoirs was evaluated by a dual-core parallel-core physical simulation experimental device. The results show that the CS-DP-AA microgel injected into the core can indeed react with the CO2 adsorbed in the pores of the porous core and plug the larger pores. After the response, the resistance coefficient of the system increased significantly, reaching 80 times that of the previous value. It has been shown that CS-DP-AA microgel can indeed block gas channeling in oil reservoirs, expand the sweep efficiency and swept volume of the CO2 gas drive, contribute to the recovery rate of oil reservoirs, and ensure the smooth development of oil reservoirs, which has a good application prospect in plugging gas channeling in oil reservoirs.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
shuailong Song,Zhinan Wu,Tong Zhou,Yunxia Wen,Wei Cao,Han Lin,Xiaohua Lu,Tuo Ji,Jiahua Zhu
The major challenge that solid amine sorbents face in practical large-scale applications is their susceptibility to degradation under humid and oxygen-containing conditions. This study developed a superhydrophobic alkyl-silica by co-hydrolyzing alkyl-silane and tetraethyl orthosilicate and then immobilizing polyethyleneimine as a CO2 sorbent. By adjusting the chain length and density, the surface of the alkyl-silica has abundant alkyl chains, and the PEI molecules are intercalated into the surface alkyl layer. These alkyl chains effectively block the contact of O2 and H2O with the amine group, thereby selectively allowing the adsorption/desorption of CO2 molecules through the alkyl layer. The results showed that the working capacity of PEI/alkyl-silica was maintained at 86% by oxidation treatment and 85% by rinsing treatment, respectively, exhibiting excellent stability compared to unprotected PEI/SiO2. Meanwhile, the alkyl chain due to the steric hindrance effect weakens the interaction between CO2 and amine and does not reduce its original working capacity. The energy consumption of PEI/alkyl-silica during regeneration was lowered to 1.24 GJ·t-1-CO2. This interfacial building concept provides a new path for designing a long-term stable amine sorbent for cost-effective CO2 capture by avoiding the contact of O2 and H2O with the amine.
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iScience
·
2024
·
IF 4.6
Qi Xu,Wentao Wang,Yangyang Zhang,Huanhuan Liu,Xiaowen Wang,Suyuan Zeng,Genqiang Zhang
The production of high-demand syngas with tunable ratios by CO 2 electroreduction has attracted considerable research interest. However, it is challenging to balance the evolution performance of H 2 and CO with wide H 2 /CO ratios, while maintaining high efficiency. Herein, nitrogen-coordinated hierarchical porous carbon spheres with varying phosphorus content (P x NC-T) are assembled to regulate syngas production performance. The precise introduction of P modulates the local charge distribution of nitrogen-coordinated carbons, thereby accelerating the protonation process of ∗ CO 2 -to- ∗ COOH and promoting moderate H ∗ adsorption. Specifically, syngas with wide H 2 /CO ratios (0.60–4.98) is obtained over a low potential range (−0.46 to −0.86 V vs. RHE). As a representative, P 1.0 NC-900 presents a remarkable current density (−152 mA cm −2 ) at −1.0 V vs. RHE in flow cells and delivers a decent peak power density (1.93 mW cm −2 ) in reversible Zn-CO 2 batteries. Our work provides valuable insights into the rational design of carbon-based catalysts for CO 2 reduction.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Chen Min,Liu Longgang,Chen Xueyan,Qin Xiaoxiao,Zhang Jianghao,Xie Shaohua,Liu Fudong,He Hong,Zhang Changbin
Efficient heterogeneous catalyst design primarily focuses on engineering the active sites or supports, often neglecting the impact of trace impurities on catalytic performance. Herein, we demonstrate that even trace amounts of sulfate (SO 4 2− ) residuals on Ru/TiO 2 can totally change the CO 2 reduction from methanation to reverse-water gas shift (RWGS) reaction under atmospheric pressure. We reveal that air annealing causes the trace amount of SO 4 2− to migrate from TiO 2 to Ru/TiO 2 interface, leading to the significant changes in product selectivity from CH 4 to CO. Detailed characterizations and DFT calculations show that the sulfate at Ru/TiO 2 interface notably enhances the H transfer from Ru particles to the TiO 2 support, weakening the CO intermediate activation on Ru particles and inhibiting the further hydrogenation of CO to CH 4 . This discovery highlights the vital role of trace impurities in CO 2 hydrogenation reaction, and also provides broad implications for the design and development of more efficient and selective heterogeneous catalysts.
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