DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 36
·15330-15337
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IF 3.5
Fangzheng Qi,Zengsheng Guo,Yuhan Zhang,Xue-Na Tang,Yiqiang Sun,Bo Xu,Guang-Ning Liu,Cuncheng Li
The stable contact of heterogeneous interfaces and the substantial exposure of active sites are crucial for enhancing the photocatalytic performance of semiconductor catalysts. However, most reported two-dimensional (2D)/2D CsPbBr3 and BiOCl heterostructures are fabricated using electrostatic self-assembly methods, which exhibit significant deficiencies in precise interface quality control and effective active site exposure. In this study, we fabricate a zero-dimensional (0D)/2D CsPbBr3/BiOCl heterojunction via a two-step calcination method, achieving an efficient direct S-scheme configuration. Optimizing interfacial contact and band alignment between CsPbBr3 quantum dots and BiOCl nanosheets enhances cross-plane charge transfer, promoting superior charge separation. This 0D/2D CsPbBr3/BiOCl heterojunction exhibits enhanced carrier mobility and high conversion rates without cocatalysts or sacrificial agents. The mechanism underlying the accelerated S-scheme charge transfer is comprehensively elucidated through a combination of analytical techniques and density functional theory (DFT) calculations. This study offers a novel approach for managing charge carrier segregation and mobility in CO2 reduction photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Guorui Liu,Guorui Ma,Haiqiang Mu,Jing Li,Feng Li,Min Zhu,Jin Zhang
Significant carrier recombination has severely limited the development of the most potential photoelectrocatalytic CO 2 reduction reaction (PEC-CO 2 RR). Herein, coral-like CuBi 2 O 4 -Bi 2 O 3 photocathodes are prepared using the strategy of the construction of heterojunction to improve the efficiency of carrier separation. As expected, its faradic efficiency of CO (FE CO ) at the lower potential (0.1 V vs. RHE) is 86.03 %, which is about 1.49 times higher than that of the original CuBi 2 O 4 film. The increased catalytic activity of CuBi 2 O 4 -Bi 2 O 3 can be attributed to the high surface area of the distinctive coral-like structure of Bi 2 O 3 , which enhances light absorption efficiency. Additionally, the higher degree of band bending in CuBi 2 O 4 -Bi 2 O 3 and the built-in electric field can speed up the transport rate of electrons, slow down the recombination of photogenerated electrons with holes and extend the lifetime of photogenerated electrons, allowing electrons to continuously participate in the reaction. This study proposes a novel strategy to optimize the efficiency of photoelectrocatalytic CO 2 reduction by CuBi 2 O 4 -based photocathodes.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 7
·2957-2963
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IF 3.5
Peng Zhang,Sai Ma,Yujuan Zhang,Chaohui He,Tuoping Hu
The energy-saving separation of CO2/N2 and CH4/N2 in the energy industry facilitates the reduction of greenhouse gas emissions and replenishes energy resources, but is a challenging separation process. The trade-off between adsorption capacity and selectivity of the adsorbents is one of the key bottlenecks in adsorption separation technologies’ large-scale application in the above separation task. Herein, we introduced a series of fluoroborate or fluorosilicate salts (Cu(BF4)2, Zn(BF4)2 and ZnSiF6) into the open coordination nitrogen sites of aluminum-based metal–organic frameworks (MOF-253) to create multiple binding sites to simultaneously enhance the adsorption capacity and selectivity for the target gas. By the synergistic adsorption effect of metal ions (Cu2+ or Zn2+) and fluorinated anions (BF4− or (SiF6)2−), the single-component adsorption capacity and selectivity of salt-modified MOF-253 (MOF-253@Cu(BF4)2, MOF-253@Zn(BF4)2 and MOF-253@ZnSiF6) for CO2 and CH4 were effectively improved when compared to pristine MOF-253 at 298 K and 1 bar. In addition, the salt-modified MOF-253 has a moderate adsorption heat (<30 kJ mol−1) which could be rapidly regenerated at low energy by evacuation desorption. As confirmed by the ambient breakthrough experiments of MOF-253 and MOF-253@ZnSiF6, the real separation performance for both CO2/N2 (1/4) and CH4/N2 (1/4) was obviously improved. This work provides a feasible post-modification strategy on uncoordinated sites of the framework to improve adsorption separation performance and promote the development of ideal adsorbents with a view to realizing their application in the energy industry.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xinqi Zhang,Duoyong Zhang,Chen Zhang,Rongjie Ma,Xuancan Zhu,Liwei Wang
The capture of CO 2 from flue gas has emerged as the most effective technology for carbon reduction. The relatively low partial pressure of CO 2 in flue gas necessitates the development of CO 2 -selective adsorbents, which provide a direct pathway to obtaining pure CO 2 in one-step, thereby reducing energy consumption. Herein, an amino-rich deep eutectic solution (DES) is dispersed on the surface of formate ligand-removed MOF-808 using a self-assembly approach for post-combustion carbon capture. The high solubility of DES towards CO 2 enables the composite to effectively capture CO 2 , with MOF-808 serving as a porous gas storage tank. Material characterization confirms the loading of DES on the surface of MOF support while retaining its microporous structure. Owing to their unique CO 2 solution-diffusion mechanism, DES-modified adsorbents exhibit promising performance on CO 2 capacity, kinetics, CO 2 /N 2 selectivity, and isosteric heat. The optimized sample DES-2@MOF-808-FR demonstrates a notable CO 2 adsorption capacity of 4.16 mmol/g at 298 K and 1 bar. When tested with simulated flue gas (15 vol% CO 2 ), it maintains a working capacity of 2.86 mmol/g and a CO 2 /N 2 selectivity of 1184, surpassing most of existed materials. DES-2@MOF-808-FR can also retain its capacities after 10 adsorption/desorption cycles in simulated flue gas. This solution-based modification approach circumvents the challenges associated with precise structural control of the adsorbent, thereby facilitating potential industrial applications.
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ENERGY & FUELS
·
2024
·
IF 5.2
Wei Zhang,Weiwen Zhang,Xinyang Li,Cheng Fu,Bin Huang,Yuxing Li,Peng Xie
In this paper, carbon dioxide (CO2) absorption by monoethanolamine (MEA) solutions in a rotating packed bed (RPB) is simulated using the computational fluid dynamics (CFD) approach. First, a new gas–liquid–solid three-phase interaction force model is developed based on the modified Kołodziej model. Then, the new interaction force model is combined with the interfacial area model, mass transfer model, chemical reaction model, and heat transfer model. Finally, a new simulation framework for RPBs based on the Eulerian multifluid approach is developed for modeling CO2 absorption in an RPB. The simulated CO2 absorption efficiency (η) and overall gas-phase volumetric mass transfer coefficient (KGa) by using the Eulerian multifluid CFD model are verified by experimental data, and the pressure drop is compared with a general pressure drop model. In addition, the pressure drop, η, and KGa are investigated considering the influences of the rotational speed, gas and liquid flow rates, and MEA concentration.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jiawu Huang,Cuiting Yang,Shengjun Du,Lin Zhu,Zhenglin Du,Guang Miao,Chunshan Song,Jing Xiao
Adsorption-based capture of carbon dioxide (CO 2 ) to upgrade natural gas offer a promising solution for energy crisis and the reduction of CO 2 emission. However, trade-off between high adsorption selectivity and rapid kinetic is an inherent shortcoming of size-sieving based adsorptive separation of gas molecules at similar sizes, hindering the launch of sieving adsorbent for practical challenging selective gas capture. Herein, a gradiently porous carbon nanofiber PCF-800 with interconnected sieving ultramicropores and low-proportion surficial mesopores is tailor-made to simultaneously realize the exclusive and rapid capture of CO 2 from CH 4 . Arising from the unique interconnected micro-mesoporous structure, the as-prepared PCF-800 not only achieves remarkable uptake ratio of 45 (298 K, 1 bar) for CO 2 /CH 4 separation via size-sieving effect but also shows fast kinetic with diffusion rate of 1.35 × 10 -3 s −1 , outperforming the conventional ultramicroporous counterpart. Moreover, the impressive dynamic CO 2 /CH 4 separation factor up to 21.7 and satisfying cycling durability revealed by the breakthrough experiments further imply the industrial potential of PCF-800 in practical CH 4 purification. This work may shed light on the design of gradient sieving carbonaceous adsorbent with high selectivity and fast kinetic for extensive high-performance small gas separation.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Junying Fu,Min Lu,Kejing Fang,Pengmei Lv,Zuhong Xiong
Biodiesel, a renewable liquid fuel, is undergoing eco-transition in catalyst research and development. Calcium oxide (CaO) was a widely studied heterogeneous catalyst due to its considerable activity. However, the poor stability of CaO during storage in air, especially by CO2 and H2O poisoning, presents a challenge. This research successfully developed a high-activity CaO/La2O3 catalyst for biodiesel production with CaO nanoparticles well-dispersed on the La oxide support (Ca/La=0.12). Under mild reaction conditions, a fatty acid methyl esters (FAMEs) yield of 96.9% was achieved. After exposure to air for two weeks, the CaO/La2O3 (Ca/La=0.12) catalyst absorbed 49% less CO2 and 91% less water than pure CaO and keeps 71.4% of the original activity. Thermogravimetric and in-situ Fourier Transform Infrared Spectroscopy analysis reveal that CO2 and H2O will preferentially be captured by La oxides and keep the supported CaO active sites safe. DFT calculations confirmed that CO2 and H2O adsorption on CaO terrace sites became an unfavoured process due to lattice compression of CaO nanoparticles on La2O3, which imparts the CO2/H2O-proof property to CaO/La2O3 catalyst. Methanol adsorption, dissociation, and migration pathways on CaO/La2O3 that produce active methoxy anions at Ca-La interfaces were identified as key steps in achieving efficient catalytic reactions.
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FOOD HYDROCOLLOIDS
·
2024
·
IF 11
Haiyu Du,Xinru Liu,Xiaoli Sun,Heng An,Yiyi Li,Zhu Zhu,Yongqiang Wen
Microbial infections result in significant postharvest losses of fresh produce. Microbial metabolism and variation in the quality of fruit and vegetables caused by microbial infection are accompanied by significant carbon dioxide (CO 2 ) production, contributing to a decreased pH value of the headspace microenvironment. Hence, the work aimed to design a CO 2 -responsive label with freshness indication, stimuli-responsive release antimicrobials, and adhesion for postharvest preservation. The multifunctional label (Eug/CPDH) was prepared by incorporating a mixed methyl red/bromothymol blue dye as an indicator and eugenol (Eug) as an antimicrobial agent into a matrix constructed by crosslinking 3-carboxyphenylboronic acid-grafted chitosan and dopamine-grafted hyaluronic acid (CPDH) through acid-sensitive borate bonds. The microbial infection could be indicated to visualize the freshness. Meanwhile, the label showed a CO 2 -responsive release ability, as confirmed by the release experiment. The antimicrobial test showed that the label had excellent inhibition properties against Escherichia coli , Staphylococcus aureus , and Botrytis cinerea . More importantly, the label could be conveniently adhered to the inner surface of the packaging and its effectiveness was verified by strawberry preservation experiments. At room temperature, the strawberry's reduction in hardness, vitamin C , total phenolic content, anthocyanins , and antioxidant capacity was effectively suppressed, and the shelf life was extended to 5 days. Overall, the CO 2 -responsive label provided a new strategy for developing multifunctional freshness preservation materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Leiqing Hu,Jun Cheng,Yannan Li,Jianzhong Liu,Junhu Zhou,Kefa Cen
Surface grafting modification was proposed to improve the surface polarity of polyacrylonitrile hollow fiber-supported polydimethylsiloxane (PDMS) membrane. The initiator 3-aminopropyltriethoxysilane containing one amine group was integrated into PDMS, and polyvinyl pyrrolidone (PVP) with strong polarity was connected to the surface by reacting with amine groups. Surface grafting modification was proven on X-ray photoelectron spectroscopy. The sharp decrease (from ∼98° to ∼28°) in water contact angle of the PDMS membrane indicated the significant improvement in surface polarity after the modification. The surface roughness of the PDMS membrane increased with the modification, and the PDMS surface immersed for 40 s was almost covered with PVP. The membrane immersed in PVP solution for 10 s improved CO 2 /H 2 , CO 2 /CH 4 , and CO 2 /N 2 selectivities . While CO 2 permeance slightly decreased from ∼2500 GPU to ∼2440 GPU. For the separation of CO 2 /CH 4 and CO 2 /N 2 mixed gases , all CO 2 /CH 4 and CO 2 /N 2 selectivities were improved after the modification. For the separation of CO 2 /H 2 mixed gas, CO 2 /H 2 selectivity was improved when the immersion time was below 30 s.
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Greenhouse Gases-Science and Technology
·
2017
·Vol. 7
·期 6
·1116-1125
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IF 1.676
Chao Chen,Samiran Bhattacharjee
Polyethylenimine (PEI) with different molecular weight such as 275, 800, 1800, and 25000, together with tetraethylenpentamine (TEPA) were impregnated into a mesoporous silica support (silica gel) using a wet impregnation method. These resultant solid amine sorbents with different amine types were compared in terms of CO 2 sorption kinetics and capacity at different temperatures, sorbent regeneration, and cyclic sorption-desorption performance, to study the effect of introduced amine types on the CO 2 capture performance. In the studied temperature range of 35–95°C for CO 2 sorption, samples with different amine types perform differently in CO 2 sorption kinetics and capacity. The largest CO 2 capture capacity for different solid amine samples appears at different temperatures, and there is evident difference on CO 2 capture capacity of different samples. In particular, PEI(25000)/silica gel showed the lowest CO 2 capture capacity among all samples. Compared to PEI/silica gel samples, TEPA/silica gel showed a relatively higher CO 2 sorption capacity. The regeneration of TEPA/silica gel is more difficult than PEI/silica gel samples, and 100°C was found suitable for complete regeneration of all sorbents. PEI(25000)/silica gel showed good reversibility and stability during 10 cyclic CO 2 sorption-desorption (sorption at 75°C and desorption at 100°C) tests, whereas PEI(275), PEI(800), PEI(1800), and TEPA/silica gel all suffered to various extents from amine leaching problems in cyclic CO 2 sorption-desorption performance under identical conditions. The cyclic CO 2 sorption-desorption performance can be improved by decreasing the desorption temperature to 75°C that leads to slightly loss of CO 2 uptake in the second run. © 2017 Society of Chemical Industry and John Wiley & Sons, Ltd.
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CATALYSIS LETTERS
·
2017
·Vol. 147
·期 7
·1654-1664
·
IF 2.799
Xu Fei,Cheng Weiguo,Yao Xiaoqian,Sun Jian,Sun Wei,Zhang Suojiang
Abstract A series of thiourea-based ionic liquids (TBILs) were developed as efficient catalysts for the synthesis of cyclic carbonates by the cycloaddition of CO 2 with epoxides under metal-, cocatalyst- and solvent-free conditions. Different substituted groups including electron donating and withdrawing groups were introduced onto the para-position of the aromatic ring in cation of TBILs. The effect of the catalyst structures on the reaction activity was systematically investigated. Among the ionic liquids, TBIL3 with substituted OCH 3 group showed the best performance with 99% propylene oxide conversion as well as 99% propylene carbonate selectivity under mild conditions (1.5 MPa, 130 °C and 3 h) without any co-solvent. It was demonstrated that two secondary amine groups of the thiourea unit could dually activate the epoxides and CO 2 and have a synergetic effect with the halide anion. Graphical Abstract
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Journal of CO2 Utilization
·
2017
·
IF 4.292
Yingjie Xu
Recently, chemical fixation of CO 2 catalyzed by protic ionic liquids (PILs) has been successfully achieved, suggesting that CO 2 absorption behavior plays an important role on CO 2 activation and transformation. For this reason, the influence of the alkalinity and physicochemical properties on CO 2 absorption behavior of four azole-based PILs, namely [DBNH][Pyr], [DBNH][Im], [DBUH][Pyr], and [DBUH][Im] was discussed in this work. The alkalinity of PILs was determined by potentiometric titration, and free space of PILs was evaluated by thermal expansion coefficient and refractive index. Solubility parameter of PILs was obtained from the activation energy for viscous flow. The results show that PILs with [Pyr] − exhibits stronger alkalinity and larger free space, which can help to improve CO 2 capture capacity. Whereas PILs with larger cation size [DBUH] + exerts higher viscosity, resulting in slower absorption rate of CO 2 . Furthermore, the CO 2 absorption capacity is inversely proportional to the solubility parameter of PILs. The absorption mechanism proved by FT-IR and 13 C NMR spectra indicates that [Pyr] − or [Im] − can react with CO 2 to form carbamate. Accordingly, considering the CO 2 capture capacity and absorption rate, [DBNH][Pyr] may be a good candidate for efficient CO 2 capture and activation with low enthalpy of absorption of −38.2 kJ mol −1 .
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