RESEARCH ON CHEMICAL INTERMEDIATES
·
2018
·Vol. 44
·期 5
·3613-3627
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IF 1.674
Sun Zhiguo,Feng Run,Zhang Li,Xie Hongyong
A new method of carbon capture and sequestration (CCS) by sodium humate (HA–Na) and Ca(OH) 2 from carbide slag (CS) solution was proposed. The effects of various operating parameters, such as the additive amount of HA–Na, pH, temperature, gas flow rate, CO 2 inlet concentration, and stirring rate on both the Ca ion concentration and Ca conversion rate were investigated in a lab-scale bubbling reactor. The synergistic mechanism of HA–Na and Ca(OH) 2 from CS on CCS is also put forward and demonstrated. The experimental results indicate that HA–Na may improve significantly the CCS capability of CS since the Ca conversion rate of CS is increased 10% by HA–Na additive. The pH is a key factor for the CO 2 absorption process and HA–Na may lower the rate of pH decrease of Ca(OH) 2 solution. The increasing temperature, stirring rate, and CO 2 inlet concentration are favorable to CO 2 capture, as well as low gas flow rate. Ca(OH) 2 from CS mixed with HA–Na solution shows good performance in CO 2 uptake, and the Ca conversion rate reaches 99% with 100 mL of Ca(OH) 2 (1.5 g/L) solution mixed with 0.1 g HA–Na at 40 °C, a gas flow rate of 0.1 L/min, and an inlet CO 2 concentration of 100% at ambient pressure. Moreover, calcite CaCO 3 is is identified as the main product of CO 2 capture by X-ray diffraction and scanning electron microscopy analysis.
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CARBOHYDRATE POLYMERS
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2024
·
IF 10.7
Wenjing Li,Jilun Guan,Huayang Fang,Yuheng Jiang,Yu Zhong,Shaohong Shi,Fangchao Cheng
Cellulose possesses numerous favorable peculiarities to replace petroleum-based materials. Nevertheless, the extremely high hygroscopicity of cellulose severely degrades their mechanical performance, which is a major obstacle to the production of high-strength, multi-functional cellulose-based materials. In this work, a simple strategy was proposed to fabricate durable versatile nanocellulose films based on sustaining CO 2 capture and in-situ calcification. In this strategy, Ca(OH) 2 was in-situ formed on the films by Ca 2+ crosslinking and subsequent introduction of OH − , which endowed the films with high mechanical strength and carbon sequestration ability. The following CO 2 absorption process continuously improved the water resistance and durability of the films, and enabled them to maintain excellent mechanical properties and promising light management ability. After a 30-day CO 2 absorption process, the water contact angle of the films can be increased from 43° to 79°, and the weight gain rate of the films in a 30 h water-absorption process can be sharply decreased from 331.2 % to 52.2 %. The films could maintain a high tensile strength of 340 MPa, and result in a CO 2 absorption rate of 3.5 mmol/g cellulose after 30 days. In this study, the improvement of durability and carbon sequestration of nanocellulose films was achieved by a simple and effective method.
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VACUUM
·
2024
·
IF 3.8
Xiu Wen,Zhixiu Yang,Lijing Gao,Ruiping Wei,Xiaomei Pan,Jin Zhang,Guomin Xiao
Electrocatalytic reduction of CO 2 affords a potential way to mitigate the greenhouse effect and fuel crisis. In this work, we compared highly-dispersed CuO nanocomposites and Cu–Cu 2 O nanocomposites which all derived from Cu x Al-LDH for CO 2 electrochemical reduction . The Cu–Cu 2 O based nanocomposites obtained through the restoration strategies still retain its layered structure, simultaneously increasing dual Cu–Cu 2 O active sites, which exhibit excellent performance in selective reduction of CO 2 to C 2 H 4 . The Cu 5 Al-ER obtained through in-situ electrochemical reduction is modified by bulk phase, which can regulate active species, increase surface active sites, enhance C–C coupling. Meanwhile, the electrochemical strategy offers numerous benefits, including gentle conditions, adjustable monitoring, exceptional efficiency and adaptability. We have confirmed that cost-effective Cu–Cu 2 O based nanocomposite derived from Cu 5 Al-LDH can effectively promote C–C coupling during electrochemical CO 2 conversion and improve FE C2H4 . The FE C2H4 of Cu 5 Al-ER reaches 36% at −1.2 V vs. RHE. And the current density reaches −172 mA·cm −2 at −1.6 V vs. RHE. The results showed that compared to Cu 5 Al-LDO, the FE C2H4 of Cu 5 Al-ER increased by 2.6 times. In addition, Cu 5 Al-ER exhibits excellent stability during the 12 hours CO 2 catalytic reduction process.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Xu Ji,Weicong Xu,Chao Liu,Xing Wang
The electrocatalytic CO₂ reduction reaction (CO₂RR) offers a promising pathway for carbon cycling and high-value fuel synthesis. However, the efficient production of ethylene (C₂H₄), a critical multicarbon product, remains constrained by insufficient catalyst activity and selectivity. Although copper-based materials enable C–C coupling, conventional CuO catalysts suffer from imbalanced *CO intermediate adsorption strength and sluggish charge transfer kinetics.In this study, a silica (SiO₂) doping strategy was employed to synergistically modulate the electronic structure and surface active site distribution of CuO, significantly enhancing CO₂-to-C₂H₄ conversion efficiency. Experimental results demonstrate that SiO₂ incorporation induces local electronic density rearrangement around Cu²⁺, stabilizing *CO adsorption, while the constructed Cu-O-Si interfaces accelerate charge transfer, enhances electron transfer and reduce the energy barrier for *COCHO formation. The optimized SiO₂-10%/CuO catalyst achieves a C₂H₄ Faraday efficiency of 42% and a partial current density of 6.3 mA/cm² at −1.4 V (vs. RHE), representing a threefold improvement over pristine CuO. Notably, the catalyst exhibits exceptional stability over 4 hours.Structural characterization and theoretical calculations reveal that SiO₂ doping promotes the self-assembly of CuO nanosheets into flower-like architectures with a high specific surface area and exposes synergistic (111)/(002) facets, which collectively enhance *CO intermediate enrichment and directional coupling. This work provides novel insights into designing high-performance CO₂RR catalysts through multidimensional modulation strategies.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Min Chen,Longgang Liu,Xueyan Chen,Xiaoxiao Qin,Kunlin Li,Jianghao Zhang,Xiaolei Bao,Lingjuan Ma,Changbin Zhang
The influence of metal particle size over heterogeneous catalysts on the catalytic performance has always been an interesting subject due to its significance from both fundamental and practical perspectives. In this work, we regulated the synthesis of TiO 2 by the hydrolysis of different titanium precursors, and as-prepared TiO 2 supports were employed to load Ru with impregnation method. Interestingly, we synthesized three Ru-TiO 2 catalysts with different Ru particle sizes of 1.1, 2.9 and 5.2 nm. The Ru-TiO 2 catalysts were next tested for CO 2 hydrogenation reaction, the results show that the medium Ru particles on TiO 2 exhibited the best CO 2 methanation activity. Based on the characterizations, we observed that the medium Ru particles exhibited the best redox properties compared with small and large Ru particles, which was beneficial to the H 2 dissociation; in addition, the medium Ru particles exhibited a moderate ability to activate CO 2 , resulting in the most favorable formation and decomposition of bidentate bicarbonate. Consequently, the Ru-TiO 2 catalyst with medium Ru particles showed the highest activity for CO 2 methanation. This study provides a new method to prepare Ru-TiO 2 catalysts with different Ru sizes and also presents an understanding of Ru particle size effects on CO 2 hydrogenation.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Zhibin Zhang,Lei Wang,Xixian Yang,Mengyuan Chu,Liyun Huang,Jiayi Fan,Wucheng Xie,Defei Liu,Wenbing Yuan,Yue Situ
The electroreduction of CO2 to formate is of significant interest due to its potential for sustainable fuel and chemical production. Hollow fiber electrodes, which integrate gas diffusion and catalytic layers, offer structural advantages. These advantages enhance gas–solid–liquid-phase reactions, making them particularly beneficial for CO2 electroreduction. This work reports a copper–bismuth alloy hollow fiber with a nanostructured surface, designed with specific metal ratios and transformed into a sulfur surface-modified copper–bismuth alloy hollow fiber (Cu7S4–CuBi HF) electrode with nanoflower structures. CO2-penetration mode enhances formate current density and Faradaic Efficiency (FE) while suppressing the hydrogen evolution reaction (HER), due to the fiber’s unique gas transport. The nanoflower morphology increases the electrochemical active surface area, boosting current densities. This design achieved a formate FE of 91.27% at −0.9 V vs RHE and a current density of 80.12 mA cm–2, outperforming many existing Cu@Bi electrocatalysts. This success is due to the innovative surface design and the distinct structural features of the hollow fiber electrodes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shuangqing Shang,Pengxiang Wang,Hanting Xiong,Xing Liu,Junhui Liu,Hua Shuai,Lingmin Wang,Zhenglong Zhu,Zhiwei Zhao,Yong Peng,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Jun Wang
The efficient separation of C 2 H 2 /CO 2 mixtures is critical yet and remains challenging owing to their closely similar physical properties and molecular sizes. Herein, we report a novel flexible microporous adsorbent, Zn-SDBA-bpy (SDBA=4,4′-sulfonyldibenzoic acid, bpy = 4,4′-bipyridine), for molecular sieving of C 2 H 2 from CO 2 . Zn-SDBA-bpy features contracted interlayer cavities with a highly negative electro-environment arising from abundant exposed oxygen atoms of SDBA. Charge transfers between C 2 H 2 and the framework result in strong C 2 H 2 -host interactions that induce a selective gate-opening effect towards C 2 H 2 . Therefore, Zn-SDBA-bpy exhibits substantial C 2 H 2 capture at low pressure (20.7 cm 3 g −1 at 0.1 bar) while excluding CO 2 , demonstrating high C 2 H 2 /CO 2 selectivity (490.2). Notably, Zn-SDBA-bpy features the lowest C 2 H 2 gate-opening threshold ( ca. 0.01 bar) among reported flexible adsorbents for C 2 H 2 /CO 2 separation. Dynamic breakthrough experiments confirm its excellent C 2 H 2 /CO 2 separation yielding high-purity C 2 H 2 (>99.5 %) products. Modeling studies reveal the strong host-C 2 H 2 interactions and underlying mechanisms of molecular sieving within Zn-SDBA-bpy.
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CATALYSIS TODAY
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2024
·
IF 5.2
Peng Bai,Yicheng Zhao,Yongdan Li
Photocatalytic N -formylation of amines with CO 2 is a promising strategy to convert CO 2 into value-added chemicals sustainably. In this work, Pd-Bi bimetallic modified ZnO enriched in oxygen vacancies is constructed for photocatalytic CO 2 formylation of benzylamine at room temperature without any reductants. The Pd and Bi sites reduce the band gap energy of ZnO, promote the separation of the photogenerated charge carriers and enhance the adsorption capacity of CO 2 . The yield of N -benzylformamide reaches 31.7 mmol g −1 with a selectivity of 85.3 % after 3-hour radiation in N , N -dimethylformamide (DMF) solvent. The aldehyde group involved in the formylation of benzylamine is derived from the decomposition of DMF, which is regenerated with the aldehyde group coming from the reduction of CO 2 . The decomposition-regeneration cycle of DMF solvent enlarges the reaction region, which is beneficial to the activity and selectivity of the formylation process. The synergistic photocatalytic system shows a good universality. This study provides a new approach to high-efficiency CO 2 utilization and formamide production.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhaohao Li,Tianjing An,Jiaxi Yang,Dan Gao,Hongyuan Zhang,Heng Zhang
Capturing CO 2 from the flue gas in the power plant is an important measure to realize the low-carbon combustion of the fossil energy. This paper presents a novel technique which combines traditional methods of the chemical absorption, the physical adsorption and the membrane absorption. The ionic liquid ([TEPA][MIm]) is utilized to improve the CO 2 absorption performance and reduce the energy consumption. While the porous skeleton (ZIF-8) is added to the ionic liquid to reduce the viscosity while introducing the physical adsorption. Moreover, the hydrophobic ceramic membrane is utilized as the separation interface between the gas phase and the liquid phase, which can avoid the entrainment and overflow of the liquid phase while increasing the specific surface area. In terms of the material preparation and the characterization, the addition of ZIF-8 does not destroy the original chemical composition of [TEPA][MIm]. The average contact angle of the hydrophobic ceramic membrane is 140.55°, and the failure temperature is greater than 400 K, which conforms to the application situation of the power plant. In terms of the CO 2 capture and the desorption performance, the maximum CO 2 capture amount reaches 2.03 mol/mol. The temperature of complete desorption is 70 °C. Furthermore, the capture performance after five cycles can reach 80 % of the initial performance. The performance is better than that of the CO 2 capture technology utilizing the traditional monoethanolamine solution.
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FUEL
·
2025
·
IF 7.5
Wensheng Wei,Yuxin Wang,Guangwen Xu,Jinggang Zhao,Lei Shi
A series of novel imidazolium-based cationic metal complexes ([EIMBr-COO] n M, n = 1, 2, 3, 4 and M = Mg 2+ , Al 3+ , Ca 2+ , Ti 4+ , V 2+ , Cr 3+ , Mn 2+ , Fe 2+ , Co 2+ , Ni 2+ , Cu 2+ , Zr 4+ , Ag 1+ , Sb 3+ , Pb 2+ , La 3+ and Ce 3+ ) were successfully constructed through coordination-driven self-assembly by an efficient one-step grinding strategy. This self-assembly process occurs when hydroxyl oxygen atoms from [ECOOHIM]Br ligand donate electron pairs to empty orbitals in the metal ions, resulting in the formation of stable complexes. Notably, the prepared [EIMBr-COO] 2 Zn catalyst displayed excellent catalytic activity in the cycloaddition reaction of propylene oxide (PO) and CO 2 , and the propylene carbonate (PC) yield reached 83.55% with a TOF of 1461 h −1 within only 10 min. The synergistic effects of Zn 2+ centers (Lewis acid), imidazolinium groups (Lewis base) and Br - ions (nucleophilic site) in [EIMBr-COO] 2 Zn contributed the excellent catalytic performance. Meanwhile, the formation of a chemical bond (Zn-O) through the coordination-driven self-assembly strategy guarantees its stability. Moreover, a rational dual-activation mechanism of Lewis acid and Br - centers was proposed based on density functional theory calculations (DFT) to explain the acceleration mechanism of the rate-determining step. Besides, [EIMBr-COO] 2 Zn showed a wide range of catalytic universality in cycloaddition reactions and satisfactory stability. Therefore, this study is expected to present theoretical and practical support for the design and synthesis methodology of multifunction catalysts for CO 2 cycloaddition.
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CATALYSIS COMMUNICATIONS
·
2024
·
IF 3.4
Yu Sun,Jinxing Mi,Liang Li,Shuxiu Yu,Shixiong Yuan,Guimin Wang,Jianjun Chen,Junhua Li
The unique ability of Cu + to enhance C-C coupling makes it important in the field of CO 2 reduction reaction (CO 2 RR) over Cu-based catalyst, while Cu + is very prone to deactivation. Hereby, we propose a simple and feasible stabilization strategy to stabilize Cu + species through reducing Cu-Mg-Al hydrotalcite by adding ascorbic acid, which owns stable product selectivity in a span of 6 h at −0.95 V vs.RHE. Characterization results show that the excellent stability is promoted by the heterostructure of Cu 2 O and hydrotalcite with retained Cu + species, which derives from Cu 2 O and slow down the rapid reduction of Cu + to Cu 0 .
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Zhonghai Tang,Yunlan Chen,Changyong Cai,Shaoping Ma,Zhijian Tan
The extraction of Rosa roxburghii polysaccharides using conventional methods suffers from low extraction efficiency and poor selectivity. Recently, green and efficient methods of polysaccharide extraction have received increasing attention. In this study, a CO 2 -responsive ionic liquid (IL) was developed for the extraction of Rosa roxburghii polysaccharides. This IL can achieve efficient extraction, and can be recycled, and reused in the extraction process. The maximum polysaccharide extraction yield of the IL was 253 mg/g under optimal single-factor experiment conditions. Three fractionated polysaccharides, RTFP-1, RTFP-2, and RTFP-3, were obtained by further purification, and their preliminary structures were characterized. RTFP-2 and RTFP-3 showed higher antioxidant and hypoglycemic activities than RTFP-1. This IL maintains high extraction efficiency after 5 cycles and reuse. This extraction method based on a CO 2 -responsive IL provides an efficient and sustainable method for polysaccharide extraction.
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