CHEMICAL ENGINEERING JOURNAL
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2023
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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.
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Molecular Catalysis
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2023
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IF 4.6
Heshan Cai,Lin Fu,Hongyan Pan,Zaixin Yan,Teng Chen,Tianxiang Zhao
Microporous carbon materials are widely used in CO 2 adsorption because of their unique structure and excellent stability. In this work, N-doped porous carbon (NPC) with an ultramicroporous structure was prepared through the carbonization of an N-doped polymer and KOH at 600 °C, 700 °C, and 800 °C, respectively. The prepared NPC exhibited excellent CO 2 adsorption properties of up to 6.95 mmol· g −1 at 1 bar and 0 °C, and this value is considerably higher than that of the parent N-doped polymer. The excellent CO 2 adsorption performance is due to the well-defined ultramicroporous structure and high specific surface area of NPC. Moreover, these porous carbons can be combined with tetrabutylammonium bromide (TBAB) to fix CO 2 into various cyclic carbonates, with a yield of up to 99% without any solvent. Whether the cause is the adsorption or catalytic conversion of CO 2 , NPC-700 exhibits excellent stability and can be cycled multiple times without significant reduction in its performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Bingling Yuan,Guoxiong Zhan,Lei Xing,Yuchen Li,Zhoulan Huang,Zhen Chen,Lidong Wang,Junhua Li
Introduction of nanoparticles (NPs) in the solvent was treated an efficient route to enhance mass and heat transfer, therefore, it was a promising strategy to boost carbon dioxide (CO 2 ) absorption and desorption, especially for the biphasic solvent with weak absorption rate and low heat capacity. Herein, powder TiO 2 and SiO 2 with nanoscale was selected to prepare nanofluid for CO 2 capture, based on DMPA-NHD biphasic solvent. The stability of nanofluid and the effect of NPs on CO 2 absorption–desorption, phase-splitting was comprehensively explored in this work. Experimental results revealed that 0.06 wt% dosage of 30 nm TiO 2 presented excellent performance for CO 2 absorption. The liquid film resistance decreased by 11.8% after introducing NPs, therefore, the maximum mass transfer coefficient was 1.88 × 10 -10 mol·cm −2 ·s −1 ·Pa (at 30 °C), increasing by 30% than the blank. In addition, 0.06 wt% dosage of 50 nm SiO 2 leaded to significant promotion for CO 2 desorption, with the maximum desorption rate at 3.9 mmol/min, and the desorption energy consumption reduced by 9.5% compared with blank case. Importantly, introduction of NPs had no significant effect on the phase splitting behavior, according to the time-profile phase-splitting measurements. The advantage influence of NPs was well validated by current DEEA-AEEA and MEA-sulfolane biphasic solvent. Furthermore, the bench-scale CO 2 absorption and desorption evaluation revealed that the relative energy consumption was respectively reduced by 15.9% and 10.0%, after introduction of 50-Si-NPs and 30-Ti-NPs.
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CERAMICS INTERNATIONAL
·
2023
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IF 5.2
Yuan Tan,Jiangcheng Tang,Caichen Yang,Yunfeng Tian,Ziling Wang,Jian Pu,Bo Chi
The double perovskite (Pr 0.5 Ba 0.5 ) 1.8 Fe 1.8 Mn 0.2 O 5-δ decorated with in situ exsolved Fe nanoparticles (Fe@PBFM) was used as the cathode in a solid oxide electrolysis cell (SOEC) to convert CO 2 to CO and exhibited high efficiency and stability. This catalyst is synthesized from the simple perovskite (Pr 0.5 Ba 0.5 ) 0.9 Fe 0.9 Mn 0.1 O 3-δ (PBFM) by annealing it under an H 2 -N 2 atmosphere at 850 °C for 15 h. The cell fabricated with the Fe@PBFM cathode shows a higher current density of 1.6 A/cm 2 at 850 °C and 1.8 V than the cell with the unreduced PBFM. The increased current density can be attributed to the in situ exsolved Fe nanoparticles and generation of the Fe@PBFM double perovskite. Furthermore, the cell containing this active catalyst exhibits stable CO 2 electrolysis performance for 100 h at a stable voltage of 1.3 V, suggesting that Fe@PBFM is an attractive candidate as SOEC cathode for CO 2 electrolysis.
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ChemistrySelect
·
2023
·Vol. 8
·期 37
·e202301015
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IF 2.1
Heming Zhang,Chan Meng,Qian Su,Li Dong,Wen Liu,Xiaokang Wang,Yunong Li,Weiguo Cheng
Graphical In this work, a series of halogen-free phosphonium ionic liquids (ILs) regulated by steric hindrance were designed and synthesized, for the catalytic synthesis of cyclic carbonates from CO 2 and epoxides, the effect of catalyst structures with different steric hindrance on catalytic activity was studied, and a plausible synergistic catalytic mechanism was proposed. The halogen-free bifunctional ILs proposed in this study provides a new insight on catalyst design and CO 2 utilization. In the cycloaddition reaction of carbon dioxide (CO 2 ) with epoxides, halogen catalysts lead to halogen loss and environmental pollution. It is necessary to design efficient and environmentally friendly catalysts. A series of halogen-free phosphonium ionic liquids (ILs) regulated by steric hindrance were designed and synthesized. It is further used as effective catalysts for the catalytic conversion of CO 2 into cyclic carbonates. The effect of different catalyst structures on catalytic activity has been investigated. Amino group has been shown to contribute to increased activity, and its location determines the degree of increased activity. Among them, [Bu 4 P] 2 [5-AMP] with meta-substitution showed the best catalytic activity, the conversion of propylene oxide (PO) was 96 % at the optimum conditions of 120 °C, 2 MPa and 3 h. Based on characterization analysis and DFT calculations, the interaction of ILs with CO 2 and PO were revealed. Finally, a plausible synergistic catalytic mechanism was proposed. The halogen-free, metal-free phosphonium ILs proposed in this paper provide a new insight on catalyst design and CO 2 utilization.
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CEMENT & CONCRETE COMPOSITES
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2023
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IF 10.5
Yuanyuan Shen,Long Jiang,Peiliang Shen,Ligang Peng,Chi-sun Poon,Fazhou Wang
A new eco-friendly carbonation coating with a photocatalytic function was developed using dicalcium silicate (C 2 S) and nano TiO 2 , aiming to remove air pollution and enhance the durability of concrete at the same time. The photocatalytic performance, mechanical properties, and durability of the carbonated coatings incorporating different additions of TiO 2 were evaluated, and the development of carbonation products and microstructure were investigated. The results show that the photocatalytic efficiency was increased linearly from 2518 μmol·m −2 ·h to 4392 μmol·m −2 ·h as the TiO 2 doping amount was increased from 1% to 8%. In addition, the composition and microstructure analysis indicated that TiO 2 not only improved the carbonation degree of C 2 S but also promoted the formation of metastable calcium carbonate, including aragonite, vaterite, and amorphous calcium carbonate, leading to a densified microstructure structure. At the same time, the improved carbonation process could capture up to 15.18% CO 2 by mass. As a result, the bonding strength was improved from 3.29 MPa to 4.69 MPa after incorporating 8% TiO 2 , which is much higher than the conventional cement-based coating. Furthermore, the microhardness of the coating increased from 150 HV to 178 HV.
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FUEL
·
2023
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IF 7.4
Qi Huang,Zhen Zhan,Yuanting Qiao,Xueting Pan,Shaojun Xu,Bien Tan,Chunfei Wu
Covalent triazine polymers, as large π conjugated, highly porous, nitrogen riched organic semiconductors, can play a key role in tackling the fuel energy crisis and global warming issues. However, their development in photocatalytic CO 2 reduction is still rare. More effective strategies to enhance CO 2 reduction activity need to be explored. Herein, different amounts of azobenzene pendants functionalized CTPs: Azo-CTP 0 , Azo-CTP 1 , Azo-mCTP 1 and Azo-CTP 2 , were fabricated for photocatalytic CO 2 reduction with Pd loaded. Among them, Azo-mCTP 1 displayed the highest CO 2 uptake capacity up to 48.2 cm 3 g −1 (2.15 mmol g −1 ) at 273 K, and the highest CH 4 evolution rate in the water system, with selectivity highly up to 97 %. Apart from that, the azobenzene functionalization of Azo-CTP 0 could significantly boost the CO 2 reduction efficiency by 4 times. Therefore, this study provides a potentially general approach for accurately modifying organic semiconductors to enhance photocatalytic performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xiaojing Cui,Yequn Liu,Wenjun Yan,Yanfeng Xue,Yangang Mei,Jiamei Li,Xiaoqing Gao,He Zhang,Shanhui Zhu,Yulan Niu,Tiansheng Deng
Suppressing reverse water-gas-shift (RWGS) reaction is high desirable but challenging and underdeveloped for Cu/ZnO catalysts, particularly for commercial Cu/ZnO/Al 2 O 3 catalysts. Different from the current methodologies to reduce RWGS reaction, we report a simply surface silylation method for efficiently minimizing RWGS reaction over a commercial Cu/ZnO/Al 2 O 3 catalyst. This method suppresses STY CO (Space-time yield) from 97.4 to 0.7 g CO ·kg cat −1 ·h −1 , improving STY MeOH from 20.2 to 39.9 g MeOH ·kg cat −1 ·h −1 and methanol selectivity from 15.1 to 92.9 mol%. The combination of characterization methods and density functional theory calculations provide insight into the suppressing mechanism of surface silylation on catalyst. A hydroxyl (on ZnO)-promoted RWGS reaction cycle is discovered, which can be efficiently inhibited by the consuming of hydroxyls via surface silyation. Our results provide a way to regulate RWGS reaction on Cu/ZnO-based catalysts and are expected to the further use of silylation strategy to tune the interconversion of CO and CO 2 via RWGS/WGS reaction on hydrogenation catalysts.
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AICHE JOURNAL
·
2023
·Vol. 70
·期 4
·e18349
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IF 3.7
Youluan Lu,Haonan Wu,Dongna Li,Yi Huang,Huijuan Guo,Tielin Wang,Lijuan Shi,Qun Yi
Porous frustrated Lewis pairs (FLPs) have been demonstrated as cutting-edge heterogeneous catalysts in acidic–basic catalysis, which, yet faces great challenges in synthesis. Herein, we propose a one-step de novo assembly strategy for constructing porous FLPs by capping monodentate ionic liquids (ILs) on metal clusters during the synthesis of metal–organic frameworks (MOFs). The capping of ILs makes adjacent metal sites on MOFs transforming to coordinatively-unsaturated metal Lewis acids, producing FLPs containing Lewis basic Cl − ions from ILs and metal sites. The distribution of ILs on the framework of MOFs endows the catalysts with large surface areas (up to 2125 m 2 g −1 ), open channels and good stability. The porous FLPs behave unprecedented activity for atmospheric CO 2 activation and coupling with epoxides (25–40°C, 1 bar, without cocatalyst). This de novo assembly strategy exhibits good universality for synthesizing porous FLPs from different kinds of ILs, paving a facile approach for designing high-efficiency acidic–basic catalysts.
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ENERGY & FUELS
·
2023
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IF 5.3
Tongxin Li,Xuefei An,Jiaqi Chen,Long Fan,Dong Fu
CO2 capture and storage (CCS) from point sources is an important part of CO2 emission reduction technologies. In particular, adsorbents with high capacity and selectivity are needed to reduce the cost of CCS technologies. Herein, we report the controlled synthesis of N-doped carbon materials, which exhibit high CO2/N2 selectivity and CO2 adsorption capacity. Specifically, cellulose-based nitrogen-doped carbon aerogels (CNCAs) were prepared using cellulose as a precursor and dissolving it in the mixed solution of NaOH and urea, followed by hydrothermal polymerization, freeze-drying, carbonization and activation. During the experiment, the effects of NaOH and urea on the formation and microstructure of carbon aerogels (CAs) were tested, and the impacts of carbonization/activation temperature on the pore structure, nitrogen content, microcrystalline structure and CO2 adsorption performance were further investigated. Impressively, for a simulated flue gas with a composition of 15% vol of CO2 and 85% vol of N2, the CNCA-750 adsorbent prepared in this work showed excellent adsorption and separation performance for CO2. The adsorption capacity can reach 3.65 mmol CO2/g and that selectivity can reach 19.69. Compared with other absorbents, it has excellent water resistance, high chemical stability, low cost and lower adsorption heat. Comprehensively, CNCAs have great prospects in the ultralow emission of industrial flue gas.
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Journal of CO2 Utilization
·
2023
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IF 7.7
Zhongzheng Zhang,Lina Zhang,Qiang Gao,Nannan Sun,Wei Wei
Nitrogen (N)-doped microporous hollow carbon spheres were prepared by facilely nanocasting spherical SiO 2 with N-containing melamine phenolic resin through a simple in-situ polymerization process. Through regulating the dosage of melamine, N content in microporous hollow carbons could be easily tuned to an unprecedented level of 49.2 wt%. Additionally, in order to address the common problem of relatively poor structural porosity of N-doped carbons, especially after incorporating vast N into carbon frameworks in reported literature, a comprehensive strategy including optimizing carbonization temperature and performing further activation by CO 2 and KOH were explored, and their effects on material textural properties and CO 2 capacity were systematically studied. Although this strategy did not completely avoid the N loss during activation of carbon materials, it sharply promoted the textural properties of carbon materials at the expenses of partial N and efficiently produced a series of highly microporous carbon materials, still with abundant N species (11.5 ∼ 29.9 wt%) and large structural porosity (330 ∼ 1263 m 2 /g). More importantly, these N-doped microporous hollow carbons, when used for CO 2 capture, showed superior CO 2 capacities of 3.00 mmol/g (25 °C and 1 bar) and 1.05 mmol/g (40 °C and 0.1 bar), exceptionally robust cyclic stability, and low regeneration energy of 2.75 GJ/ton CO 2 , which is much lower than aqueous amine-based absorbents and comparable to amine-supported adsorbents. Thus, these outstanding adsorption performances make the N-doped microporous hollow carbon spheres prepared in this study more promising for energy-effective CO 2 capture from dilute gas streams.
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APPLIED CATALYSIS A-GENERAL
·
2023
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IF 5.5
Taoning Lei,Qi Dang,Tong Wu,Yun Wu,Jingyi Yu
Electrochemical reduction of CO 2 enables a flexible and efficient way of converting CO 2 into diverse products. Cu 2 O is regarded as a crucial species for electrocatalytically transforming CO 2 to methanol while facing challenges such as the deactivation of the catalyst and low selectivity of desired products. Therefore, the modification of Cu 2 O and the improvement of its catalytic activity needs to be addressed. Herein, we reported a novel synthesis of Cu 2 O nanocubes (Cu 2 O-cube) using the wet chemical method and demonstrated a Faradaic efficiency of 29.1 % for methanol. We found Cu 2 O (100) facet was responsible and beneficial to improve methanol production . The performance degradation at different potentials due to the deactivation of Cu 2 O-cube were revealed from the changes of surface morphologies by scanning electron microscope (SEM). The electrocatalytic activity of Cu 2 O-cube was further enhanced by embedding Cu 2 O-cube into ZnO nanowires (ZnO@Cu 2 O-cube) through drop-drying, leading to a Faradaic efficiency of 38.9 % towards methanol at − 0.45 V vs. RHE. For parallel comparison, an alternative binding form of ZnO and Cu 2 O was investigated through stacking Cu 2 O film onto ZnO nanowires (ZnO@Cu 2 O-film) through electrodeposition . The results elucidated that the existence of ZnO tended to suppress the production of ethanol and the binding site of ZnO-Cu 2 O could improve the selectivity of methanol.
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