JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Ruoxing Liao,Yumin Guo,Liqiu Yang,Haoli Zhou,Wanqin Jin
Membrane technology , a successful technology for separating gases such as CO 2 /CH 4 mixture, has attracted much attention because of its low energy consumption, and membrane performance is an important factor affecting its industrial application. Herein, the solvent-induced microstructure of a polyimide membrane was employed to enhance its CO2/CH4 separation performance. The effect of solvents on the membrane structure and gas separation performance was investigated by using different solvents (such as tetrahydrofuran, N,N-dimethylacetamide) to dissolve a newly synthesized polyimide polymer, which was fabricated into a membrane. Various characterization methods, such as positron annihilation lifetime spectroscopy (PALs) and X-ray diffractometry (XRD), were conducted to reveal changes in the microstructure of membranes prepared with different solvents. The interaction of solvents with groups of polymer backbones was also analyzed for the explanation of the effect of solvents on the membrane performance for the separation of different gas pairs, such as CO2/CH4 mixture. The results showed that a membrane with optimal separation performance was obtained by optimizing the solvent composition, which exceeded the 2018 mixed-gas CO2/CH4 upper bound. The induced effect of solvents on the polymer membrane structure provides a new research path for the optimization of polymer membranes to enhance separation performance.
研究领域:
材料科学
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化学工程
·
气体分离技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guanhua Liu,Lirong Wang,Lihang Yan,Hao Zhao,Yaoxuan Li,Liya Zhou,Ying He,Li Ma,Yunting Liu,Jing Gao,Yanjun Jiang
Enzymatic reduction of CO 2 into high-value chemicals has become an emerging technology attributed to its high selectivity and catalytic efficiency under mild conditions. While, the low solubility of CO 2 at room temperature, the expensive cofactors and the poor stability of free enzyme limit the application potential. To solve these problems, we used organic microcapsules together with MOF to protect formate dehydrogenase (FDH) by encapsulation and carbonic anhydrase (CA) by covalent bond with high CO 2 capture ability to construct a dual-enzyme microreactor. Besides, the additional mesopores of the microreactor can ensure the efficient internal diffusion of the substrate and product. Electron mediator was used to enhance electrocatalytic NADH regeneration to efficiently reduce CO 2 to formate in the enzyme electrocatalysis system. After optimization, the highest yield of formate in the electrocatalytic CO 2 reduction system by the dual enzyme microreactor was 2.917 mM with a generation rate of 1.296 × 10 4 μmol g cat -1 h −1 , which was 8.9 times higher than free enzyme.
研究领域:
化学工程
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生物催化
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电化学
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环境科学
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产品关联
DOI
高影响因子
FUEL
·
2020
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IF 5.578
Run-Ping Ye,Lin Liao,Tomas Ramirez Reina,Jiaxu Liu,Durgaiah Chevella,Yonggang Jin,Maohong Fan,Jian Liu
The CO 2 methanation is an important process in coal-to-gas, power-to-gas and CO 2 removal for spacecraft. Recently, metal-organic framework (MOF) derivatives have been demonstrated as high-performance catalysts for CO 2 upgrading processes. However, due to the high costs and low stability of MOF derivatives, it still remains challenge for the development of alternative synthesis methods avoiding MOF precursors. In this work, we present the sol-gel method for loading Ni-MOF to silica support in two-steps. Upon modifying the procedure, a more simplified one-step sol-gel method has been developed. Furthermore, the obtained Ni/SiO 2 catalyst still exhibits great catalytic performance with a CO 2 conversion of 77.2% and considerable CH 4 selectivity of ~100% during a stability test for 52 h under a low temperature of 310 °C and high GHSV of 20,000 mL·g −1 ·h −1 . Therefore, this work provides a ground-breaking direct strategy for loading MOF derived catalysts, and might shed a light on the preparation of highly dispersed Ni/SiO 2 catalyst.
研究领域:
化学工程
·
催化材料
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2019
·Vol. 30
·期 8
·7950-7962
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IF 2.195
Hu Bingbing,Guo Qiang,Wang Kang,Wang Xitao
In this paper, a series of indium oxides were prepared by calcining the In(OH) 3 precursors, which were synthesized by hydrothermal method using the mixed solution of ethylenediamine (En) and water as a solvent. The morphologies, particle sizes, pore structure, crystallinity and surface defect concentration of these photocatalysts were adjusted by varying the ratio of En to water during the preparation of In(OH) 3 precursors. The results revealed that In 2 O 3 photocatalysts obtained from the precursor prepared in En containing solvent exhibited much higher photocatalytic activities for CO 2 reduction with H 2 O when compared to that derived from the precursor prepared in pure water. This result can be ascribed to several reasons as following. Firstly, the En addition with a suitable amount can improve the crystallinity of In 2 O 3 and decrease the surface defect concentration, which obviously depressed the recombination of photogenerated electrons and holes. Also, the addition of En during the preparation of precursor can decrease the particle size, increase specific surface area and pore structure, resulting into the increase of active sites. Finally, the band gap of In 2 O 3 can be slightly narrowed after the addition of En, resulting in enhanced light absorption in the visible region. When the ratio of ethylenediamine to water is 1:1, the as-prepared In 2 O 3 possessing the largest specific surface area and pore volume, enhanced light absorption ability and higher hole–electron separation efficiency, exhibited the highest photocatalytic activity. Under visible light irradiation, the H 2 , CO and CH 4 production rates of 5.3, 8.3 and 27.2 µmol/g cat /h can be achieved, respectively.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Science China-Materials
·
2025
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IF 7.4
Huang Fuxia,Liu Yifei,Wang Feng,Liu Ya,Guo Liejin
BiOI materials show significant potential for photocatalytic CO 2 reduction, but their limited CO 2 activation and poor charge carrier properties hinder conversion efficiency. In this study, we engineered BiOI-based photocatalysts with abundant crystal defects to enhance performance. X-ray diffraction (XRD), Raman spectroscopy, and high-resolution transmission electron microscopy (HRTEM) revealed lattice distortions and twin crystals in BiOI-LD and BiOI-TC. Ultraviolet-visible spectroscopy, micropore and chemisorption analyses, and photoluminescence spectroscopy demonstrated that crystal defects improved light absorption, CO 2 adsorption, charge transfer efficiency, and carrier lifetime. Electron paramagnetic resonance (EPR) spectroscopy showed increased superoxide radical generation in BiOI-TC, suggesting higher reactivity. Consequently, BiOI achieved a CH 3 CH 2 OH generation rate of 6.2 µmol g −1 h −1 with 100% selectivity. Key intermediates (*CO, *COCO, *CHO, *CH 2 ) for CH 3 CH 2 OH production were identified, and C 2 H 6 formation in BiOI-LD was linked to the generation of *CH 3 .
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Rui Yang,Xiaozhong Zheng,Hao Fu,Xinyue Cao,Yangguang Hu,Yiyin Huang
Graphical Cu 7 S 4 /Cu nanoflowers with strong CO 2 adsorption and abundant boundaries were developed by a facile thermal reduction, which underwent in situ dynamic restructuring during ECR to generate highly active S-doped Cu 2 O/Cu hybrid catalyst. Thermodynamic and experimental analysis revealed that the optimized adsorption of the HCOO * intermediate on S−Cu 2 O/Cu was regulated and surface H was suppressed by S-doping. The high activity for CO 2 -to-HCOOH attributed to the strengthen CO 2 adsorption, abundant boundaries at Cu 2 O/Cu interfaces, and the regulation of adsorption energy by S-doping Optimized catalytic properties and reactant adsorption energy played a crucial role in promoting CO 2 electrocatalysis. Herein, Cu 7 S 4 /Cu underwent in situ dynamic restructuring to generate S−Cu 2 O/Cu hybrid catalyst for effective electrochemical CO 2 reduction to formate that outperformed Cu 2 O/Cu and Cu 7 S 4 . Thermodynamic and in situ Raman spectra revealed that the optimized adsorption of the HCOO* intermediate on S−Cu 2 O/Cu was regulated and the H 2 pathway (surface H) was suppressed by S-doping. Meanwhile, Cu 7 S 4 /Cu nanoflowers created abundant boundaries for ECR and strengthened the CO 2 adsorption by inducing Cu. These findings provide a new perspective on synthetic methods for various electrocatalytic reduction processes.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Lixin Song,Guobin Liu,Zhenping Qu
CO 2 hydrogenation to methanol and/or dimethyl ether (DME) holds promise for mitigating greenhouse gas effects and addressing energy scarcity. However, the relationship between product selectivity and the collective nature of the catalysts remains ambiguous due to the intricate reaction network. Here, a series of Cu/Zn x Al y O z catalysts with different surface properties have been engineered by manipulating the Zn/Al ratio to achieve product controllability for CO 2 hydrogenation. The results unveil the pivotal role of the H 2 dissociation capability in governing CO 2 conversion, which is regulated by the concentration of Cu 0 species. Furthermore, the number of surface hydroxyl groups, the proportion of moderately strong basic sites and moderately strong acidic sites show desirable linear correlations with the selectivity of CO, CH 3 OH, and DME, respectively. Importantly, the ZnAl 2 O 4 -Al 2 O 3 or Cu-ZnAl 2 O 4 -Al 2 O 3 interface notably enhances moderately strong acidic sites, aiding methanol dehydration to DME. This work offers a comprehensive guide to the rational design of catalysts for oriented product synthesis from CO 2 hydrogenation.
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2020
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IF 5.825
Junhui Liu,Guanghui Zhang,Xiao Jiang,Junhu Wang,Chunshan Song,Xinwen Guo
Iron-based catalysts have been widely used to synthesize value-added hydrocarbons through CO 2 hydrogenation. Fe carbide, Fe 5 C 2 , was proposed as the active phase responsible for C C coupling during the chain growth. However, the reaction mechanism over iron-based catalysts is still under debate due to the presence of multiple phases of Fe species. In this work, Fe 5 C 2 and K-modified Fe 5 C 2 were prepared and used to study the relationship between the Fe phase, catalytic performance and reaction pathways. CH 4 and CO selectivities of 46.1 C-mol% and 2.8 C-mol% were obtained on Fe 5 C 2 at a CO 2 conversion of 49.8 %, with the main hydrocarbon products being alkanes. With the addition of the promoter K, the C 2 -C 4 = selectivity increased to above 38.0 C-mol%, and the selectivity to C 5+ hydrocarbons increased to 23.9 C-mol% at a similar CO 2 conversion. CH 4 and C 2+ hydrocarbons formed through the CO 2 →CO→hydrocarbons (indirect) route over K-modified Fe 5 C 2 , whereas the direct hydrogenation route occurred on unmodified Fe 5 C 2 in addition to the indirect route of CO 2 to CO to hydrocarbons through Fischer-Tropsch synthesis (FTS) processes. This work offers insights in direct CO 2 hydrogenation over Fe 5 C 2 and Fe 3 O 4 -Fe 5 C 2 catalysts, which advances the understanding of the functions of active phases and reaction pathways of CO 2 hydrogenation over iron-based catalysts.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2019
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IF 3.073
Suresh Mutyala,Madhavi Jonnalagadda,Harisekhar Mitta,Raveendra Gundeboyina
MIL-101 (Cr) was synthesized by a hydrothermal method and used as support to prepare a series of polyethylenimine (PEI) incorporated MIL-101 (Cr) by wet impregnation method. All characterization results revealed that the structure of MIL-101 (Cr) was well-maintained by the incorporation of polyethylenimine and confirmed the presence of PEI within MIL-101 (Cr). The CO 2 adsorption studies were carried out in a fixed bed reactor from 30 to 90 °C, 1 bar. The adsorption of CO 2 has been increased by the incorporation of PEI. It was due to the chemical interaction between the NH 2 and CO 2 groups to form a carbamate. The high CO 2 adsorption capacity 3.81 mmol g −1 was shown by 70 wt% PEI loaded MIL-101 (Cr) at 75 °C, 1 bar, because of more number of NH 2 groups and a high number of CO 2 molecules diffusion. Its adsorption capacity was 4.7 times higher than the adsorption capacity of MIL-101 (Cr) (0.80 mmol g −1 ). Moreover, in moisture condition, CO 2 adsorption capacity was increased to 4.4 mmol g −1 by the formation of ammonium bicarbonate and showed good adsorption stability throughout each adsorption-desorption cycle. The Avrami adsorption kinetic model was well fitted with experimental breakthrough CO 2 adsorption data of MIL-101 (Cr)-PEI-70. It suggested that the adsorption of CO 2 on PEI incorporated material was chemical adsorption.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
RSC Advances
·
2023
·Vol. 13
·期 25
·17362-17369
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IF 3.9
Zhe Zhang,Fanhao Kong,Bizhen Yuan,Yinnian Liao,Xiue Ren,Yu Hou
Solar-driven CO2 reduction into fuels and sustainable energy has attracted increasing attention around the world. However, the photoreduction efficiency remains low due to the low efficiency of separation of electron–hole pairs and high thermal stability of CO2. In this work, we prepared a CdO decorated CdS nanorod for visible light driven CO2 reduction. The introduction of CdO facilitates the photoinduced charge carrier separation and transfer and acts as an active site for adsorption and activation of CO2 molecules. Compared with pristine CdS, CdO/CdS exhibits a nearly 5-fold higher CO generation rate (1.26 mmol g−1 h−1). In situ FT-IR experiments indicated that CO2 reduction on CdO/CdS may follow a COOH* pathway. This study reports the pivotal effect of CdO on photogenerated carrier transfer in photocatalysis and on CO2 adsorption, which provides a facile way to enhance photocatalytic efficiency.
研究领域:
材料科学
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环境科学
·
化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
·
IF 6.1
Wei Rong,Meili Ding,Pan Ma,Suyu Kong,Jianfeng Yao
Accumulation of atmospheric CO 2 poses a serious threat to the global environment, but there is still a lack of effective CO 2 catalytic conversion under mild conditions. Herein, multifunctional ZnO/N-doped porous carbon materials, ZNPC-X, were fabricated by pyrolysis of available pine pollen with melamine and zinc chloride . The optimized ZNPC-600 produced at 600 °C can work as an efficient photothermal catalyst towards CO 2 cycloaddition conversion with a high catalytic yield of 99% under mild conditions (0.3 W/cm 2 , 1 bar). Moreover, ZNPC-600 shows excellent recyclability after ten cycles and desirable performance even under simulated flue gas and after moisture treatment. Absorption spectra and time-dependent infrared images unveil that the intrinsically broad light absorption and high photothermal conversion efficiency are the major reasons for the high activity of ZNPC-600. Besides, photogenerated electrons can be transferred to CO 2 and activate it, while photogenerated holes can be used as Lewis acid to facilitate the ring opening of epoxides. In addition, the hierarchical pore structure and the synergy between ZnO and pyridine N also play a role in the mass transfer and activation of epoxides and CO 2 , respectively. This work provides a low-cost and facile solution to obtain catalysts derived from biomass for promoting CO 2 conversion.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Carbon Letters
·
2023
·Vol. 33
·期 5
·1395-1406
·
IF 4.5
Chen Zhangjing,Li Liangliang,Cheng Gang
Photocatalytic CO 2 reduction is a promising approach for reducing CO 2 emissions and achieving the goal of carbon neutrality. In this work, selectively coupling Cu(OH) 2 and CuO with amine-modified brookite TiO 2 (NH 2 –B–TiO 2 ) has been achieved by a simple precipitation method. The results show that CuO is better than Cu(OH) 2 as a co-catalyst to enhance the CO 2 photoreduction capability of NH 2 –B–TiO 2 . The highest rates of CO 2 conversion to CH 4 and CO of NH 2 –B–TiO 2 –CuO composite reach 6.05 and 3.25 μmol h −1 g −1 , respectively, which is higher than 8 times the yield of CH 4 of NH 2 –B–TiO 2 . It is proposed that the NH 2 –B–TiO 2 –CuO composite offers an effective charge transfer through the formation of a p–n junction between NH 2 –B–TiO 2 and CuO interfaces, while in the NH 2 –B–TiO 2 –Cu(OH) 2 composite, the Cu(OH) 2 dominantly serves as an electron sink to capture photo-induced electrons, promoting photo-induced carrier separation. This work provides an ingenious synthetic method for selectively anchoring Cu(OH) 2 and CuO on semiconductors with different charge transfer routes for an efficient CO 2 photoreduction. Graphical abstract
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）