CHEMICAL ENGINEERING JOURNAL
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2023
·
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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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Haitao Shi,Jiajia Yang,Zia Ahmad,Haijun Zhang,Jiping Chen
Solid amine materials have emerged as a class of adsorbent with promising potential for CO 2 capture from gas mixtures, such as biogas and flue gas. In this work, we developed a novel CO 2 capture material via co-grafting of polyethyleneimine (PEI) on mesocellular silica foam (MCF), and (3-glycidyloxypropyl)triethoxysilane (GPTES) was first used as a bridging medium. In the fabrication procedure of MCF@G-35.6 %PEI, a simple impregration of PEI in MCF modified with epoxy groups was conducted. In this procedure, the co-grafting of PEI was realized in terms of a portion of PEI (21.3 wt%) was anchored on the pore surface of MCF via the epoxy/amine reaction and the rest of PEI (14.3 wt%) could be stably attached to the pore surface of MCF via its interaction with anchored PEI. After systematic evaluation, the MCF@G-35.6 %PEI exhibited a maximum CO 2 adsorption capacity of 2.78 mmol/g at 50 °C and 50 %RH and fast adsorption kinetics with equilibrium time (break through from C/C 0 = 5 % to 95 %) is 22.85 min. Meanwhile, outstanding CO 2 adsorption capabilities within a wide temperature range of 30–90 °C and a large concentration range of 5–30 % vol. CO 2 were obtained by the use of MCF@G-35.6 %PEI. More importantly, the MCF@G-35.6 %PEI also exhibited an excellent long-term stability over 50 consecutive cycles. CO 2 adsorption kinetics of the sorbent was found to follow Avrami’s fractional order model and intraparticle diffusion model. Furthermore, temperature-programmed desorption was conducted to investigate the desorption kneitics and adsorption mechanism. All these findings demonstrate the great potential of MCF@G-35.6 %PEI for carbon capture and sequestration (CCS) technology.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Wenjun Zhang,Jian Liu,Zhong Jin
The electrochemical system based on water, CO2, and electricity is the key technology to realize the coexistence and combination of renewable energy and fossil energy, which can convert CO2 molecules into high-value-added products under mild and controlled conditions, thus achieving carbon neutrality. Designing efficient electrocatalysts to realize highly active, selective, and stable CO2RR has become one of the vital issues. Particularly, the nanostructure design and interface adjustment of electrocatalysts have been regarded as the key points for improving their catalytic performance. Herein, a tin dioxide hollow nanotube (SnO2 HNT) catalyst with a three-dimensional cross-linked network structure has been fabricated by electrospinning and rapid-heating calcination. The morphology and component structure of SnO2 HNTs were analyzed by a series of characterizations. The performance in electrocatalytic carbon dioxide reduction reaction (eCO2RR) was further tested. Owing to the hollow nanostructure, the catalyst possessed a large specific surface area and abundant active sites, which greatly accelerated mass transport and electron mobility. During eCO2RR, SnO2 HNTs achieved a peak faraday efficiency value of 87.4% for C1 products at −1.1 V vs RHE, which significantly suppressed the occurrence of hydrogen evolution side reactions. In addition, compared with the commercial SnO2 nanoparticles or partially reduced Sn/SnO2, the catalytic activity and selectivity of CO2-to-formate conversion significantly increased under the same potential, indicating that the optimization of electronic/geometric structure for high-yield metal oxides can effectively improve the comprehensive performance of eCO2RR.
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Catalysts
·
2023
·Vol. 13
·期 7
·1030
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IF 3.9
Siyi Jiang,Yujing Weng,Yangbin Ren,Shihang Meng,Xiaoman Li,Chao Huang,Yulong Zhang,Qi Sun
The chemical transformation of carbon dioxide (CO2) not only reduces the amount of carbon dioxide emitted into the Earth’s atmosphere by humans, but also produces carbon compounds that can be used as precursors for chemical and fuel production. Herein, a selective catalytic conversion of carbon dioxide to methanol is achieved by a bifunctional molybdenum disulfide catalyst (MoS2) with magnesium oxide and nickel and potassium promoters. Molybdenum disulfide prepared by the supercritical ethanol method has a large specific surface area and presents good catalytic performance with high methanol selectivity when loaded with potassium (K) and nickel (Ni) promoters. In addition, the catalysts were evaluated and it was founded that the addition of the K-promoter improved methanol selectivity. This research provides a new strategy for improved product selectivity and space–time yield (STY) of methanol in CO2hydrogenation.Keywords:CO2hydrogenation;molybdenum disulfide;methanol
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Hong Zhu,Yan Huang,Simi Li,Lingkui Zhao,Junfeng Zhang
The most promising approach to tackling the greenhouse gases is CO 2 capture and storage (CCS), and amine solid adsorbents are the most widely investigated materials. In this work, Zr species as an accelerator promote CO 2 adsorption of the Pentatethylenehexamine (PEHA)/sepiolite (SEP) adsorbents. The adsorption rate, CO 2 adsorption capacity, and amine efficiency were significantly improved under various conditions (temperature, gas flow, and CO 2 concentration) by the introduction of the optimal content of Zr, the optimal HSEP-Zr 0.13 -PEHA 0.5 -600 adsorbent exhibited 1.80 mmol/g at 60 °C. Adsorption experiments combine with characterization (TG, XPS, NH 3 -TPD, SEM and TEM) exhibited that the introduction of Zr species were high dispersion on sepiolite, and Zr-O bond was formed in the structure of sepiolite. The acidity of the sepiolite supporter was enhanced by Zr which is benefit for amine loading. Above all resulted in the regeneration and thermal stability of the adsorbent were improved together. The economic evaluation results demonstrated that the adsorbent with Zr species is low-cost for large-scale post-combustion CO 2 capture.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
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
·
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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ORGANOMETALLICS
·
2023
·
IF 2.8
Yanru Zhang,Jingjing Zhang,Ying Wang,Yang Li,Jun He,Yanyan Wang,Longbo Zhang,Zhenpeng Wang,Qingli Qian,Buxing Han
Synthesis of basic C2+ chemicals using CO2 and H2 is very promising. Herein, we present a protocol for the synthesis of different carboxylic acids by the reaction of ketones or aldehydes with CO2 and H2. The catalytic system consisted of the IrCl3 catalyst, LiI promoter, and acetic acid solvent. The yield can reach 52.9% based on the cyclohexanone substrate which can be derived from biomass. Various Cn ketones and aldehydes could be used as a substrate in the reaction, where the corresponding Cn+1 carboxylic acids were obtained. According to the mechanistic study, the reaction involved substrate conversion, reverse water–gas shift (RWGS) reaction, and carbonylation. This strategy provides an optional way of carboxylic acid production and CO2 utilization.
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APPLIED CATALYSIS A-GENERAL
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2023
·
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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MOLECULES
·
2023
·Vol. 28
·期 17
·6276
·
IF 4.6
Yanxi Li,Yuhua Bai,Zhuozheng Wang,Qihan Gong,Mengchen Li,Yawen Bo,Hua Xu,Guiyuan Jiang,Kebin Chi
Developing metal–organic framework (MOF) adsorbents with excellent performance and robust stability is of critical importance to reduce CO2emissions yet challenging. Herein, a robust ultra-microporous MOF, Cu(bpfb)(bdc), with mixed ligands of N, N′-(1,4-phenylene)diisonicotinamide (bpfb), and 1,4-dicarboxybenzene (bdc) was delicately constructed. Structurally, this material possesses double-interpenetrated frameworks formed by two staggered, independent frameworks, resulting in two types of narrow ultra-micropores of 3.4 × 5.0 and 4.2 × 12.8 Å2, respectively. The above structural properties make its highly selective separation at 273~298 K with a CO2capacity of 71.0~86.2 mg/g. Its adsorption heat over CO2and IAST selectivity were calculated to be 27 kJ/mol and 52.2, respectively. Remarkably, cyclic breakthrough experiments corroborate its impressive performance in CO2/N2separation in not only dry but also 75% RH humid conditions. Molecular simulation reveals that C-H···OCO2in the pores plays a pivotal role in the high selectivity of CO2adsorption. These results point out the huge potential application of this material for CO2/N2separation.Keywords:metal–organic frameworks;ultra-microporous;robust;breakthrough;CO2capture
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Jiachen Sun,Néstor Guijarro,Peihang Li,Udayabhaskararao Thumu,Jun-Ho Yum,Kevin Sivula,Zhiming M. Wang
One of the promising methods to solve the current energy and environment issues is photoelectrochemical (PEC) water splitting and CO2 reduction reaction. Chalcopyrite copper indium gallium sulfide (CIGS) and CuIn0.3Ga0.7S2 nanocrystal thin films have been considered photovoltaic materials, and here, we demonstrated their potential to reduce CO2 into CO. A modified solution process affords to decrease the number of surface ligands, which triggers an increase in the crystal size and an improved reproducibility in performance and output current. After depositing gold nanoparticles on the surface of CIGS, the Faradic efficiency related to the CO2-to-CO conversion can reach 12.93% in aqueous electrolytes and 25% in nonaqueous electrolytes. Further investigation points out that in the range of applied potential between −0.1 and −0.2 V vs a reversible hydrogen electrode (RHE), the CIGS photocathode appears to display a stable photocurrent density for 1 h, but when applying a higher applied bias, such as of −0.3 V vs RHE, the degradation of the current is significant. Additionally, we found that coupling catalysts to the CIGS increases the selectivity toward CO and minimizes the competitive hydrogen evolution reaction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Feifei You,Yunan Zhou,Danyang Li,Hao Zhang,Dawei Gao,Xiaohong Ma,Rui Hao,Juzhe Liu
Photoreduction of CO 2 to value-added chemicals and fuels is an attractive solution to alleviate environmental problems and energy crisis at the same time. However, engineering efficient photocatalysts with high activity and product selectivity is still challenging. Herein, we achieved three-dimensional (3D) spatial configuration design at micro-scale and heterogeneous interface construction at nano-scale on a SnS 2 /SnO 2 composite, which featured hierarchical flower-like morphology consisted of nanosheets and type-II semiconductor structure . It behaved excellent selectivity and impressive photocatalytic CO 2 -to-CO performance with a yielding rate of 60.85 μmol g -1 h −1 , roughly 3 times higher than that of SnS 2 and was in the front rank of this kind catalysts under 300 W Xe lamp illumination without using any sensitizers or noble metals . The enhanced catalytic capability could be attributed to the elaborately built structure with suitable energetic position that afforded effective separation and migration of photo-generated electron/hole pairs as well as enhanced light caption and absorption. Meanwhile, main reactive intermediates (e.g., CO 2 – and *COOH) were captured by in-situ Fourier transform infrared spectroscopy (FTIR), suggesting a fluent catalytic pathway on the SnS 2 /SnO 2 platform. This work provides a new scheme to build advanced catalysts based on multiscale design and rational phase assembling.
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