DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 6
·2526-2533
·
IF 3.5
Jia-Min Lyu,Shen Yu,Zhan Liu,He-You Du,Ming-Hui Sun,Chun-Mu Guo,Yi-Long Wang,Yu Li,Li-Hua Chen,Bao-Lian Su
Excessive emission of CO2 into the atmosphere has severely impacted the global ecological environment. Converting CO2 into valuable chemicals and fuels is of great significance for sustainable development. However, low activity and undesirable selectivity often result from the inherent inertness of CO2. Herein, K- or/and Zn-modified Fe-based catalysts were prepared by an incipient-wetness impregnation method for CO2 hydrogenation via a cascade reaction. The results indicate that K species exist as K2O while Zn species exist as ZnFe2O4. In the CO2 hydrogenation pathway, K2O facilitates the adsorption of CO2 and restrains the adsorption of H2, accelerating the transformation of CO2 into C2–C4 olefins rather than paraffins while Zn species promote the dispersion of Fe species, leading to improved activity. Synergistically, a K- and Zn-modified Fe-based catalyst (2Zn–10K–Fe/Al) shows excellent catalytic CO2 hydrogenation activity, achieving a CO2 conversion of 77% which is 1.8 times that (42%) of the unmodified Fe-based catalyst (Fe/Al). Our catalyst also shows a significantly promoted selectivity to C2–C4 olefins of 17% in comparison with the Fe/Al catalyst (0%). It is envisioned that such a binary effect of elements might contribute to the low-cost and industrial production of Fe-based catalysts for selective CO2 conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Luotian Lv,Yao Liu,Yankai Huang,Tong Li,Han Feng,Yongqing Wang
Since the intensification of global environmental pollution and energy shortages, photocatalytic CO 2 reduction reaction (CO 2 RR) has emerged as a promising strategy to convert solar energy into clean chemical energy. Herein, we construct a robust and efficient heterojunction construction photocatalyst for CO 2 RR, composed of the highly reactive CeNi quantum dots (CeNi QDs) and nickel metal–organic layer (Ni-MOL) ultrathin nanosheets. This design facilitates the rapid separation of photogenerated charge carriers, as confirmed by X-ray photoelectron spectroscopy (XPS), photoluminescence spectroscopy (PL) and other characterizations. Mechanistic studies with in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and the d-band center calculation indicate that the propensity of photocatalyst for CO 2 absorption and CO desorption, leading to high performance and selectivity. The optimized loading amount of CeNi quantum dots and modified structure result in a CO yield of 30.53 mmol·g −1 within 6 h under irradiation. This work not only paves a new and convenient way for developing high-activity quantum dot materials for CO 2 RR but also exploits novel avenues to fabricate more heterojunction composites for solar energy conversion.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yuanye Zhuang,Shiyang Bai,Meng Ge,Jingjing Sun,Yingying Cheng,Jihong Sun,Yanmin Yu
An environmentally friendly polymer catalyst (PAS) was synthesized via inverse emulsion polymerization using acrylic acid (AA) and 1-vinyl imidazole (VI) as monomers. The excellent catalytic activity of PAS was attributed to the synergistic effects of the carboxyl groups (-COOH) as hydrogen bond donors and N-heterocyclic carbene (NHCs) as electron donor, as well as the swelling properties of the polymer, which can enrich the substrate into the polymer network, increasing the contact between the substrate and active sites. Characterization results from thermogravimetric (TG) analysis and small-angle X-ray scattering (SAXS) showed that the excessive imidazole addition disrupted the polymer's chain-like structure, significantly reducing its swelling properties. And, the catalytic performance is influenced by both the amount of imidazole in PAS and the swelling properties of the polymer. Finally, the reaction mechanism of the CO 2 cycloaddition reaction catalyzed by PAS was proposed and validated through density functional theory (DFT) calculations.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Hanwen Wang,Jiawei Wang,Hangyuan Zhang,Xinyang Wang,Xiaoping Rao
Emulsion-based delivery systems are extensively employed for encapsulating functional active ingredients, protecting them from degradation, and enhancing bioavailability and release efficiency. Here, a CO 2 -responsive surfactant synthesized from rosin displays rapid responsiveness to CO 2 at room temperature, transitioning reversibly switches between active and inactive states multiple times. The dual tertiary amines on the rosin rigid structure contributes to its CO 2 sensitivity. When in its active cationic form, in conjunction with silica nanoparticles , it exhibits desired Pickering emulsification performance across various oil phases. In the Pickering emulsion loaded with quercetin , the encapsulation efficiency and loading efficiency reached 80.50% and 0.69%, respectively, with stability lasting at least 30 days. The system provides robust protection for quercetin against external factors, such as UV and heat, revealing sustained release effects. This study investigated the potential of using rosin-based CO 2 -responsive surfactants alongside nanoparticles to design stable Pickering emulsion systems for active substance encapsulation and sustained release.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shuzhuang Sun,Bocheng Yu,Yanmei Shen,Yu Liu,Hongman Sun,Xuan Bie,Mengna Wu,Yongqing Xu,Chunfei Wu,Hui Zhou
Integrated CO 2 capture and utilization (ICCU) using “capture-conversion” dual functional materials (DFMs) paves a cost-effective path for restricting CO 2 emissions by eliminating the energy-intensive intermediate processes. The interactions between catalysts and absorbents are believed pivotal in ICCU; however, there is a lack of environment-friendly strategy to fabricate the interaction for industrial applications. Here, we propose a solvent-free mechanochemical approach to promote the interaction by improving the proximity between natural calcium and iron sources. The interaction was systemically investigated and confirmed using XRD, XPS, TEM, TPR, etc. As a result, the mechanochemical approach derived DFM achieved 5.5 mmol g −1 CO 2 capacity, 87 % CO 2 conversion, and 100 % CO selectivity at 650 °C, significantly outperforming the CaO-alone benchmark (CO 2 capacity < 4.5 mmol g −1 , CO 2 conversion < 73 %). Further incorporating MgO would alleviate the sintering and promote the CO 2 capture stability (< 15 % decrease after 20 cycles) by acting as a thermal-stable barrier. Based on in situ XRD, it is further confirmed that Fe-Ca interaction exhibits a dynamic looping mechanism in ICCU. The techno-economic analysis strongly supports the superiority of ICCU catalyzed by naturally sourced DFMs on eliminating the energy and H 2 consumption for CO 2 capture and upgradation. As a result, producing CO via ICCU using mechanochemical derived DFMs exhibits 20 % and 10 % cost decrease compared to the conventional CCU and ICCU using CaO alone scenarios, pointing out the potential of ICCU technology in industrial applications.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Ziwen Mei,Kejun Chen,Yao Tan,Qiuwen Liu,Qin Chen,Qiyou Wang,Xiqing Wang,Chao Cai,Kang Liu,Junwei Fu,Min Liu
ABSTRACT Electrocatalytic CO 2 reduction reaction (CO 2 RR) holds significant promise for sustainable energy conversion, with cobalt phthalocyanine (CoPc) emerging as a notable catalyst due to its high CO selectivity . However, CoPc's efficacy is hindered by its limited ability to provide sufficient proton for the protonation process, particularly at industrial current densities . Herein, we introduce defect-engineered carbon nanotubes (d-CNT) to augment proton feeding for CO 2 RR over CoPc, achieved by expediting water dissociation. Our kinetic measurements and in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy reveal d-CNT significantly enhances proton feeding, thereby facilitating CO 2 activation to *COOH in CoPc. Density functional theory calculations corroborate these findings, illustrating that d-CNT decreases the barrier to water dissociation. Consequently, the CoPc/d-CNT mixture demonstrates robust performance, achieving 500 mA cm –2 for CO 2 RR with CO selectivity exceeding 96%. Notably, CoPc/d-CNT remains stability for a duration of 20 h under a substantial current density of 150 mA cm –2 . The study broadens the scope of practical applications for molecular catalysts in CO 2 RR, marking a significant step towards sustainable energy conversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiaofen Wei,Jun Liu,Huangyu Yan,Tianshan Li,Ying Wang,Yuqiong Zhao,Guoqiang Li,Guojie Zhang
Coal gasification fine slag (CGFS), a byproduct of the coal gasification process, is currently being recognized as a resource with significant potential for value addition and sustainable applications, especially in synthesizing CO 2 adsorbents. The overarching challenges in this domain include the attainment of high-efficiency, environmentally benign transformation of CGFS into useful products, and the development of cost-effective adsorbent materials featuring precisely engineered pore structures. In this study, a hierarchical porous nanostructured silica material is synthesized rapidly, efficiently, and cost-effectively through acid leaching and alkaline dissolution-assisted hydrothermal treatment, employing CGFS as the precursor. The mass ratios of sodium hydroxide (NaOH) to CGFS range from 0.4 to 1, resulting in varying morphologies and adsorption properties. Specifically, the sample with the NaOH to CGFS ratio of 0.6 (CGFS-0.6) shows the best adsorption performance. The adsorption capacities are 2.87 mmol/g and 8.49 mmol/g at 20 °C with 15 % and 45 % CO 2 concentration, respectively. The material is characterized by a well-developed pore structure shaped like a bouquet of flowers, with a specific surface area of 457 m 2 /g and pore volume reaching 2.34 cm 3 /g. During the hydrothermal processing, silicate/aluminosilicate entities self-organized into a Si-O-Na/Al network structure, endowing the synthesized adsorbent with optimal internal porosity and silanol functionalities. The adsorption equilibrium is achieved rapidly within 10 min, and CO 2 adsorption stability remains robust across 20 successive cycles. All isothermal models of the adsorbents conform to the Sips model. This study offers a promising pathway for the value-enhanced utilization of coal-derived solid wastes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhilv Chen,Tao Wang,Chao Li,Mengxiang Fang,Wei Chen,Ximing Hu,Wei Zhang,li Zhang,Wenyang Fan,Shaojuan Zeng
In recent years, a large number of studies have shown that amine based water-lean absorbents formed by amines and organic solvents exhibit high capture efficiency and low regeneration energy consumption in CO 2 capture. However, there is a lack of research that combines molecular level structure with macroscopic properties. In order to optimize the performance of amine based homogeneous water-lean absorbents by utilizing the properties of organic solvents, and to explore the correlation between the macroscopic properties of the absorbents (CO 2 capacity, removal efficiency, regeneration rate, regeneration efficiency, etc.) and the molecular structure of the absorbent components. We used experiments and molecular dynamics to study the linear terminal diamine DMEDA and non-proton polar solvent (DMF, DMPA, NMP, SFL, DMSO) system. It was found that the absorption and desorption performance of water-lean solvents was higher than that of aqueous solutions 30 wt% MEA and 30 wt% DMEDA, among which EFH with DMF as the solvent has better comprehensive performance. The molecular dynamics simulation was built to describe the solution structures of these absorbents. Through RDF calculations, the unique behavior of DMEDA in non-proton polar solvent was revealed on molecular level, it was found that organic solvents tend to aggregate with DMEDA molecules to form large molecular clusters, while CO 2 molecules may diffuse through ordered pore structures, resulting in a significant improvement in the capture performance. And it was found that there is a quantitative relationship between the intensity of intermolecular interaction between DMEDA and CO 2 and the removal efficiency change in DMEDA water-lean absorbents. A functional relationship was fitted, and a preliminary and rapid method for determining capture performance through molecular dynamics was proposed.
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ChemistrySelect
·
2024
·Vol. 9
·期 22
·e202401690
·
IF 1.9
Menghan Xue,Fazhan Li,Zhen Li,Yuxia Sun,Yiping Guo,Yuehui Li
Graphical Increase of graphitic-N doping and graphitization degree of outside shells encapsulating Ni nanoparticles was developed to efficiently promote cathodic reduction of CO 2 to CO. Despite of high conductivity and reducing ability, transition metal nanoparticles tend to aggregate and unavoidably impact the selectivity during the proton-coupled reduction process of CO 2 RR. New strategy to regulate and utilize the electronic property of transition-metal particles allows for effective tuning of eCO 2 RR activity. Through simple creation of N-doped carbon shells surrounding Ni nanoparticles and controlling the amount and arrangement of the N atoms, successful and long-lasting electrochemical reduction of CO 2 was accomplished. The inherent HER activity was almost completely suppressed. It exhibited FE CO above 90 % in a 500 mV potential window, with the optimal up to 96.5 % at −0.78 V vs RHE. In flow cell electrolysis, a current density of 289.4 mA/cm 2 was achieved with Faradic efficiency of 96.4 % towards CO. The results of control experiments using different catalysts imply that electron transfer between Ni core and shells was significantly influenced by the property of N atoms. High content of graphitic nitrogen is crucial for the catalytic performance.
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Foods
·
2024
·Vol. 13
·期 11
·1719
·
IF 4.7
Yadan Chen,Yanbin Wang,Liang He,Liling Wang,Jianchen Zhao,Zhenya Yang,Qin Li,Rui Shi
This study aimed to investigate the efficacy of supercritical CO2(SC-CO2) extraction in enhancing the extraction rate, purity, and antioxidant activity ofIndocalamus latifolius(Keng) McClure (Poaceae) leaf terpenoids (ILLTs). Crude extracts obtained from leaves were subjected to qualitative and quantitative analyses, revealing neophytadiene, phytol, β-sitosterol, β-amyrone, squalene, and friedelin as the primary terpenoid constituents, identified through gas chromatography–mass spectrometry (GC-MS). Compared with steam distillation extraction (SD), simultaneous distillation extraction (SDE), ultra-high pressure-assisted n-hexane extraction (UHPE-Hex), ultra-high pressure-assisted ethanol extraction (UHPE-EtOH), ultrasound-assisted n-hexane extraction (UE-Hex), and ultrasound-assisted ethanol extraction (UE-EtOH), SC-CO2exhibited a superior ILLT extraction rate, purity, and antioxidant activity. Scanning electron microscopy (SEM) observations of the residues further revealed more severe damage to both the residues and their cell walls after SC-CO2extraction. Under optimal parameters (4.5 h, 26 MPa, 39 °C, and 20% ethyl alcohol), the ILLT extraction rate with SC-CO2reached 1.44 ± 0.12 mg/g, which was significantly higher than the rates obtained by the other six methods. The subsequent separation and purification using WelFlash C18-l, BUCHI-C18, and Sephadex LH-20 led to an increase in the purity of the six terpenoid components from 12.91% to 93.34%. Furthermore, the ILLTs demonstrated cytotoxicity against HepG2 cells with an IC50value of 148.93 ± 9.93 μg/mL. Additionally, with increasing concentrations, the ILLTs exhibited an enhanced cellular antioxidant status, as evidenced by reductions in both reactive oxygen species (ROS) and malondialdehyde (MDA) levels.
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Materials
·
2025
·Vol. 18
·期 2
·244
·
IF 3.2
Zhong Li,Zhiming Yin,Dingzhao Zhou,Zhiqiang Wu,Daohang Wang,Shuwen Guan,Guangyan Du
Ensuring long-term wellbore integrity is critical for carbon dioxide geological storage. Ordinary Portland cement (PC) is usually used for wellbore primary cementing and plug operation, and set cement is easily corroded by acidic fluids, such as carbon dioxide, in underground high-temperature and high-pressure (HTHP) environments, resulting in a decrease in the mechanical properties and an increase in permeability. In order to achieve long-term wellbore integrity in a CO2-rich environment This study introduces materials such as thermosetting vinyl ester resin (TSR), filler composite resin (FCR), and low-cost resin cement (RC). Corrosion experiments were conducted using four materials in 28 days under supercritical carbon dioxide gas and water phase conditions of 60 °C and 10 MPa. The samples were characterized through mechanical property testing machines, core permeability measuring instruments, FTIR, XRD, and SEM. The results proved that after corrosion, PC mechanical properties decreased, the permeability increased, and the microscopic composition and morphology changed greatly. Penetrating corrosion occurs in the sample in the gas phase environment, and propulsive corrosion from outside to inside occurs in the water phase environment. However, TSR, FCR, and RC materials all maintain excellent resistance to carbon dioxide corrosion in gas and water environments. They have higher compressive strength and extremely low permeability compared to ordinary Portland cement. These three materials’ compressive strengths can be maintained around 131, 99, and 58 MPa, and permeability can be stabilized at <6 × 10−7, <6 × 10−7, and 0.16 mD levels. In summary, the above three materials all show better performance than ordinary Portland cement and are promising alternative materials that can be used in primary cementing and plug operations of carbon dioxide geological storage wells.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Wanqi Lian,Ying Huang,Qiaoqiao Yin,Zhicheng Guo,Yun Xu,Tifang Miao
To enhance the economic viability of photocatalytic materials for carbon capture and conversion, the challenge of employing expensive photosensitizer must be overcome. This study aims to improve the visible light utilization with zirconium-based metal–organic frameworks (Zr-MOFs) by employing a multi-component post-synthetic modification (PSM) strategy. An economical photosensitiser and copper ions are introduced into MOF 808 to enhance its photoreduction properties. Notably, the PSM of MOF 808 shows the highest CO yield up to 236.5 μmol g −1 h −1 with a HCOOH production of 993.6 μmol g −1 h −1 under non-noble metal, and its mechanistic insight for CO 2 reaction is discussed in detail. The research results have important reference value for the potential application of photocatalytic metal–organic frameworks.
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