MATERIALS CHEMISTRY AND PHYSICS
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2023
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IF 4.6
Debin Zeng,Longtao Wang,Ruian Du,Zhen Wu,Xiting Wang,Chunguang Kuai,Yuzheng Guo,Changlin Yu
CO 2 photoreduction under mild conditions remains challenging, attributing to sluggish kinetics of complex coupling process of multi-electrons-protons and inefficient electron-hole pairs utilization. Herein, with Zn 3 V 2 O 8 as a phase transformation material, we construct an effective Zn 2 V 2 O 7 /Zn 3 V 2 O 8 /ZnO (OVZn) Z-scheme system by partial decomposition of Zn 3 V 2 O 8 into Zn 2 V 2 O 7 and ZnO. Time-resolved fluorescence decay (TRFD) spectra investigation shows that the photogenerated electrons of Zn 2 V 2 O 7 and ZnO recombine with the holes of Zn 3 V 2 O 8 , retaining more reductive electron of Zn 3 V 2 O 8 for CO 2 reduction. Moreover, in-situ Fourier-transform infrared spectroscopy suggests that the heterostructure can lower the energy barrier of CO desorption by changing bridge-bonded CO to linear-bonded CO and optimizing the energy barrier of CO production. Moreover, Cu, Ag and Au loading on OVZn greatly enhance light harvesting and promote photoelectric conversion, producing much photogenerated electron-hole pairs for CO 2 reduction. OVZn and metal loaded OVZn have better photocatalytic performance, showing application superiority on CO 2 photoreduction.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Qian Yi,Chunan Zhao,Cunbin Lv,Guanghao Wan,Miaomiao Meng,Lanyi Sun
The enhancement of gas–liquid mass transfer in the CO 2 absorption process by Low Transition Temperature Mixtures (LTTMs) based nanofluids was investigated. The effects of loading and size of TiO 2 nanoparticles on the CO 2 absorption rate were studied experimentally. The absorption rate was found to be improved significantly after adding nanoparticles. The maximum enhancement factor of 1.35 was observed when using nanoparticles with a particle size of 10 nm and a concentration of 0.6 kg/m 3 . The maximum absorption enhancement factor and mass transfer coefficient were observed when the loading of nanoparticles increased, hence there was an optimal concentration of TiO 2 nanoparticles in the CO 2 absorption process. For the size of nanoparticles, the CO 2 absorption rate was higher when the diameter of nanoparticles decreased. Furthermore, a three-dimensional unsteady mathematical model of gas–liquid mass transfer, which was based on the mechanisms of grazing effect and hydrodynamic effect in the gas–liquid boundary layer, was developed to describe the CO 2 absorption enhancement. The model predictions were well consistent with the experimental results, with a maximum deviation of less than 5%, which proved the reliability of the model. Finally, Molecular dynamics simulations were conducted on the absorbent-CO 2 system. The results showed that the addition of TiO 2 nanoparticles led to a reduction in the simulation box size at the same simulation time, but it did not significantly alter the interaction between LTTMs and CO 2 . Therefore, it can be inferred that TiO 2 nanoparticles enhance CO 2 absorption capacity by modifying the mass transfer rate. Through the aforementioned study, this paper explores the experimental and mechanistic aspects of nanoparticle-enhanced absorption of CO2 in LTTMs systems. The research demonstrates the feasibility of nanoparticle-enhanced absorption of CO2 in LTTMs solvents, providing insights into studying nanoparticle-enhanced gas–liquid mass transfer and offering a new research approach for CO2 capture.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Lulu Zhao,Huilin Hou,Lin Wang,Chris R. Bowen,Jinguo Wang,Ruifang Yan,Xiaoqiang Zhan,Hongli Yang,Man Yang,Weiyou Yang
Creating useful chemicals based on artificial CO 2 photoreduction is considered to be an attractive approach to address the environmental and energy crises. Currently, its selectivity with high conversion efficiency is still a grand challenge. Here, we report the refined substitution of Bi 3+ with Ag + in ultrathin Bi 2 WO 6 nanosheets through a liquid-phase cation exchange process, favoring a high selectivity towards the photocatalytic production of CO from CO 2 . The incorporation of Ag + could not only significantly promote the adsorption of both CO 2 and H 2 O molecules, but also facilitate the transfer of photogenerated carriers. The as-fabricated photocatalyst achieves a high CO generation rate of 116.96 μmol g −1 with a superb selectivity of 95.7 % after 6 h reaction without any sacrificial agent, approximate 4.2 times higher than that of pure Bi 2 WO 6 . The mechanism for photocatalytic CO 2 reduction is proposed, based on in-situ Fourier Transform Infrared spectrometry analyses and Density Functional Theory calculations.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Shuai Wang,Chunliang Shang,Yimin Deng,Jan Baeyens,Tatiana V. Plisko,Alexandr V. Bildyukevich,Tejraj M Aminabhavi,Xinying Liu,Mahluli Moyo,Helei Liu
The mass transfer plays a decisive role in screening and evaluation of amine solvents as well as in designing and scale-up of CO 2 capture. The influence of different operating parameters on mass transfer processes in CO 2 capture by EAE-1DMA2P amine solution was thoroughly investigated using a small-scale packed column. The mass transfer mechanism of EAE-1DMA2P amine solution in the capture of CO 2 was discussed by determining both mass transfer control steps and the reaction region between CO 2 and amine solvent, which provided a theoretical guidance for subsequent development of new solvents for large-scale applications. In addition, based on the experimental observations of K G a v , a prediction model for K G a v of EAE-1DMA2P composite amine solution was established by comparing two empirical models viz., Kohl-Riesenfeld-Astarita and Sheng of which Kohl-Riesenfeld-Astarita model provided a better fitting of the experimental results. The commonly used amine solvents and EAE-1DMA2P composite solvents were further compared and analyzed in terms of packed column size design and solvent consumption. The required packed column volume using EAE-1DMA2P composite solvent was only 4.95 m 3 , while the EAE-1DMA2P composite solvent has the smallest solvent consumption among all the solvents, indicating that this solvent has a lower operating cost than the other solvents, suggesting better industrial application.
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Advanced Science
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2023
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IF 15.1
Bo Gao,Changqing Tian,Linfeng Guo,Jinchen Zhou,Zixian Wang,Chengfan Fu,Hongmei Ran,Wei Chen,Qiang Huang,Daofu Wu,Xiaosheng Tang,Zhongtao Luo
In order to deal with the global energy crisis and environmental problems, reducing carbon dioxide through artificial photosynthesis has become a hot topic. Lead halide perovskite is attracted people's attention because of its excellent photoelectric properties, but the toxicity and long-term instability prompt people to search for new photocatalysts. Herein, a series of <111> inorganic double perovskites Cs 4 Mn 1-x Cu x Sb 2 Cl 12 microcrystals (x = 0, 0.1, 0.2, 0.3, 0.4, and 0.5) are synthesized and characterized. Among them, Cs 4 Mn 0.7 Cu 0.3 Sb 2 Cl 12 microcrystals have the best photocatalytic performance, and the yields of CO and CH 4 are 503.86 and 68.35 µmol g −1 , respectively, after 3 h irradiation, which are the highest among pure phase perovskites reported so far. In addition, in situ Fourier transform infrared (FT-IR) spectroscopy and electron spin resonance (ESR) spectroscopy are used to explore the mechanism of the photocatalytic reaction. The results highlight the potential of this class of materials for photocatalytic reduction reactions.
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PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2023
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IF 5.5
Yifu Wang,Bin Yang,Biao Gao,Longtai Li,Yu Zhou,Yaping Zhang,Tatsumi Ishihara,Limin Guo
The efficient catalytic hydrogenation of CO 2 to methanol is a promising route for CO 2 emission mitigation and utilization. Recently, the Co-In based materials as one of the excellent alternative catalysts for CO 2 hydrogenation to methanol have received intense attention. Herein, we developed new and efficient Co-In based catalysts (the composite of Co 3 InC 0.75 and In 2 O 3 ) by Prussian Blue analogues (PBA) pyrolysis . And a series of Co 3 InC 0.75 -In 2 O 3 composites with tunable proportion of Co 3 InC 0.75 and In 2 O 3 has been prepared. The experimental results demonstrate the Co 3 InC 0.75 -In 2 O 3 catalysts have high catalytic CO 2 hydrogenation performance into methanol, reaching a methanol yield up to 0.62 g MeOH g cat −1 h −1 at 300 °C, 5 MPa, 24000 cm 3 STP g cat −1 h −1 , and H 2 /CO 2 = 3:1, the high reaction stability and air resistance. The synergetic effects between Co 3 InC 0.75 and In 2 O 3 for the enhanced methanol production were confirmed by a series of characterizations, and a positive correlation between methanol production activity and the fraction of Co 3 InC 0.75 /In 2 O 3 was well established.
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ENERGY & FUELS
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2023
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IF 5.3
Linghan Xia,Mengchen Wu,Yimeng Li,Hongyan Guo,Yonghong Cheng,Guodong Meng
As one of the most consensus goals around the world, reduction of carbon emissions has attracted huge attention from academic and industry communities for developing renewable energy sources and carbon capture techniques. Nonthermal equilibrium plasma catalysis has been proven to be a very promising way for CO2 conversion into high-value-added products; however, the synergistic catalytic mechanism between the plasma and various catalysts remains a challenge. In this work, we designed a reactor of atmospheric pressure glow discharge (APGD) plasma jet coupled with V2O5/TiO2 nanocomposite catalysts and studied the influence of V2O5 mass fraction, catalyst pretreatment, and reaction plasma parameters on the CO2 dissociation performance. Results showed that the designed reactor could introduce high-density plasma to the downstream area and maintain lower gas temperature, allowing the collaboration between APGD and the V2O5/TiO2 catalyst. The XRD analysis indicated that the solid solution phase TiVO4 could be formed in catalysts by V2O5 doping and reach a maximal content at a mass fraction of 30%, which determined the most excellent redox ability of the catalyst. The pretreatment of the as-prepared catalyst by Ar dielectric barrier discharge (DBD) plasma increased the oxygen vacancy density of the catalyst, thereby raising the conversion rate by 18.43%. Moreover, the transition regime between laminar and turbulent states was found to be the optimal configuration for CO2 dissociation. The reaction pathway was proposed for CO2 dissociation synergistically catalyzed by an APGD plasma jet and V2O5/TiO2. Ultimately, the maximum conversion of 14.88% and energy efficiency of 40.45% were simultaneously achieved, which were superior to the results of most atmospheric pressure plasmas. This work opens an avenue to develop plasma technology for sustainable CO2 utilization.
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ENERGY & FUELS
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2023
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IF 5.3
Xianhang Jin,Enze Ren,Min Zheng,Xiurong He,Yun Yang
A CO2 phase change absorbent (CPCA) is of interest because it has the potential to reduce energy consumption for CO2 capture. Controllable phase separation behavior was expected in the development and application of a CPCA. In this study, the effects of CO2 loading under different activators and physical solvents on the phase separation behavior of an activated methyldiethanolamine (MDEA)-based CPCA were investigated. By adjustment of the CO2 loading, controllable phase separation behavior was achieved and the absorbent comprising an activator with more −NH– groups and a physical solvent with low ET(30) was favored to exhibit phase separation. Of special interest was that, with the increasing of CO2 loading, phase behaviors, from the liquid phase to solid–liquid phase and then to the liquid phase, were observed for CPCA comprising MDEA/piperazine (PZ)/N-methyl-2-pyrrolidone (NMP), which was different from all of the other known CPCAs. The solid compound was identified as PZ carbamate by X-ray diffraction (XRD), Fourier transform infrared (FTIR), and elemental analysis, and the liquid-phase samples were detected by 13C nuclear magnetic resonance (NMR). The phase change mechanism of this special phenomenon was proposed.
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CHEMICAL PAPERS
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2023
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IF 2.2
Liu Wenqiang,Li Jiangxin,Xie Yuheng,Wang Yajuan,Zhang Juan
Dimethyl carbonate (DMC) is widely used and nontoxic and can replace more dangerous materials such as dimethyl sulfate or methyl chloride. Spherical particle catalysts (PILs-XSS) were synthesized by suspension polymerization, which was characterized by SEM–EDS, FT-IR, TG, and BET-BJH. The characterization results showed that PILs-XSS had a specific core structure, a certain pore size (14.3 nm), and surface area size (71.5m 2 /g) and remained stable at 293.4 °C. The catalyst performance was evaluated by a one-pot synthesis of dimethyl carbonate. The process conditions were optimized in detail. The optimal reaction conditions were as follows: the dosage of PILs-XSS was 2.5 wt %, the CO 2 pressure was 1.5 MPa, the reaction temperature was 100 °C, the reaction time was 4 h, the molar ratio of methanol to propylene oxide (PO) was 3: 1, and the dosage of cocatalyst Na 2 CO 3 was 3 wt %. Under the optimum conditions, the conversion of PO was up to 98.8% and the yield of DMC reached 53.7%. In addition, the combined catalyst PILs-Na 2 CO 3 was easily recovered by filtration in the reaction system. After five times of repeated use, the activity and the shape of the catalyst were almost unchanged, which meant that the catalyst had amazing mechanical strength. This study found that the transesterification catalyst Na 2 CO 3 not only had good transesterification efficiency but also promoted the reaction of CO 2 . Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Keran Lv,Rui Tu,Lihui Xiao,Wei Wei,Yuchun Xu,Guoqing Ren,Rong Huang,Weiqiao Deng,Tie Yu
A mechano-catalysis approach is introduced into “heterogeneously catalyzed gas phase reaction” with continuous gas flow, and Ruthenium (Ru) doped Nickel (Ni) milling balls (Ru/Ni) serve as CO 2 methanation catalyst. Under mechanical vibration conditions, Ru/Ni presented a state-of-the-art TOF CH4 of 15995.6 h −1 and higher CH 4 selectivity (>95%) at 340 ∼ 390 ℃. Compared with conventional Ru-Ni/Al 2 O 3 catalyst, Ru/Ni also exhibited intact Ru-Ni structure without deactivation and coke formation over 200 hrs. The surface and spatial distribution of Ru species on Ni substrate were studied by XRD, SEM, XPS, TOF-SIMS and XANES . In situ DRIFTs were also conducted to examine the reaction intermediates and boosting impact of Ru species on hydrogenation ability, and the advantages of mechanical vibration reactor for CO 2 methanation are proposed finally. This work pioneers a new idea for low energy consumption and high efficiency CO 2 hydrogenation.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
You Wang,Zhongke Dai,Jiajia Wang,Du Zhang,Fa Zhou,Jiawei Li,Jianhan Huang
Combining inorganic semiconductors with covalent organic frameworks (COFs) to construct excellent hybrid materials is a promising strategy for solar-driven CO 2 reduction, but how to modulate the charge migration to achieve optimal catalytic efficiency remains a great challenge. Herein, we successfully fabricated well-defined core–shell structured HBWO@Br-COFs hybrid materials using the nano-flowered Bi 2 WO 6 (HBWO) as the core and the triazine-based imine-functionalized Br-COF as the shell. The electrostatic attraction between HBWO and Br-COF leads to the formation of C-O covalent bond and a tight and stable interface. Impressively, the Scheme-II heterojunction was favorably formed at the interfacial layer between the core and the shell, and they provided a stable platform for the rapid transfer of the photogenerated charge and efficient separation of the electron-hole pairs, resulting in excellent photocatalytic CO 2 reduction. The resultant HBWO@Br-COF-2 exhibited high CO yield rate of 19.9 μmol·g −1 ·h −1 , about 3.4 times higher than HBWO (5.8 μmol·g −1 ·h −1 ) and 2.6 times greater than Br-COF (7.53 μmol·g −1 ·h −1 ), respectively. This work provides helpful ideas for the optional design and facile fabrication of the novel inorganic–organic hybrid materials for photocatalytic CO 2 reduction.
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ACS ES&T Engineering
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2023
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IF 7.1
Peng Chen,Yun Wang,Jiazhen Liao,Yi Liang,Qingqing Ye,Yi Wang,Zhongwei Jiang,Chunhui Shan,Wendong Zhang,Fan Dong
The dissociation of H2O molecules plays an important role in producing protons for promoting hydrogenation reduction of CO2. Therefore, developing excellent photocatalysts to promote the dissociation of H2O molecules and reveal the effect mechanism is the key research direction to enhance CO2 reduction efficiency. In this work, we synthesized BiSbO4 with oxygen vacancies (OVs) to investigate the photocatalytic mechanism of CO2 conversion and H2O dissociation. Experimental results indicate that the introduction of OVs into BiSbO4 can enhance the absorption capacity of light, narrowing band gaps and impeding the recombination of photogenerated carriers. Importantly, the existence of OVs in BiSbO4 can promote the adsorption and activation of H2O molecules via the stronger covalent interaction, which facilitates the dissociation of H2O molecules to generate more protons and lowers the energy barriers of •COOH to improve the efficiency of CO2 reduction. This study reinforces our understanding of the principle of photocatalytic CO2 reduction and the important role of H2O dissociation in photocatalytic CO2 conversion.
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