CEMENT & CONCRETE COMPOSITES
·
2023
·
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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ChemistrySelect
·
2023
·Vol. 8
·期 37
·e202301015
·
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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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Huicong Zuo,Chunqiang Lu,Lei Jiang,Xianming Cheng,Zhiqiang Li,Yuelun Li,Danyang Li,Hua Wang,Kongzhai Li
Linz-Donawitz converter gas (LDG), an important by-product in the steel industry with CO (55–60 vol%) and CO 2 (15–20 vol%) as the main components, is usually used as fuel for heating or power generation, releasing massive of diluted CO 2 with the concentration lower than 15 % that is difficult to capture. Herein, we propose a method to produce pure H 2 via chemical looping water splitting by using LDG as reducing agent, which can easily concentrate CO 2 for capture. Fe 2 O 3 , one of the most environmentally friendly and low-cost oxides, was chosen as the oxygen carrier to perform this concept. It was found that the addition of small amounts of Ce 0.75 Zr 0.25 O 2 solid solution could strongly improve the activity of Fe 2 O 3 for CO conversion, especially at relatively low temperatures. Compared with pure Fe 2 O 3 , the CO conversion and H 2 yield were increased from 39.5 % and 0.34 mmol·g −1 to 100 % and 2.32 mmol·g −1 at 650 °C, respectively, after adding 5 wt% of Ce 0.75 Zr 0.25 O 2 . The strong interaction between the two oxides contributed to the enhanced performance via promoting CO adsorption and lattice oxygen releasing. Water splitting assisted by air oxidation could fully regenerate the reduced oxygen carrier, and the oxygen carrier was stable during the long-term chemical looping process, with the CO 2 capture rate at ca. 95.8 %. In situ DRIFTS results showed that CO 2 was produced through a direct reaction of lattice oxygen with CO, and the decomposition of carbonate species intermediate by adsorption of CO on the surface of oxygen carriers. This study gave full evidence that it was feasible for achieving H 2 generation and CO 2 capture in one step via chemical looping reforming of reducing exhaust gases (e.g., LDG) from industrial emissions.
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Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-15
·
IF 26.6
Li Minhan,Zhang Fangzhou,Kuang Min,Ma Yuanyuan,Liao Ting,Sun Ziqi,Luo Wei,Jiang Wan,Yang Jianping
Electrochemical reduction of CO 2 into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO 2 capture and utilization, resulting from their high catalytic activity and selectivity. The mobility and accessibility of active sites in Cu-based catalysts significantly hinder the development of efficient Cu-based catalysts for CO 2 electrochemical reduction reaction (CO 2 RR). Herein, a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride (g-C 3 N 4 ) as the active sites for CO 2 -to-CH 4 conversion in CO 2 RR. By regulating the coordination and density of Cu sites in g-C 3 N 4 , an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH 4 Faraday efficiency of 49.04% and produces the products with a high CH 4 /C 2 H 4 ratio over 9. This work provides the first experimental study on g-C 3 N 4 -supported single Cu atom catalyst for efficient CH 4 production from CO 2 RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO 2 RR by engineering Cu active sites in 2D materials with porous crystal structures.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Teng Lu,Zhaomin Li,Liping Du
This study explores the combined application of hydrophobic silica aerogels and SDS to enhance CO 2 storage capacity and oil recovery. Experimental data highlighted a marked increase in CO 2 solubility within silica aerogel-SDS nanofluids compared to brine and SDS solutions. Molecular dynamics simulations revealed CO 2 adsorption into nanopores. Silica aerogel nanoparticles extended CO 2 foam half-life by 6 % versus 62 % decline for sole SDS foam from 30 to 140 °C. Adjusting the SDS to nanoparticle ratio affects foam properties, with a ratio of 1.5 yielding optimal results. Core flooding experiments demonstrated a 75 % rise in CO 2 trapping efficiency using the nanofluids over SDS solutions. Two-dimensional tests showed aerogel-SDS foam surpassed SDS foam flooding by 12 % incremental oil recovery in upper layers, attributed to enhanced profile control. The combined agents present an effective approach for geological CO 2 storage and EOR optimization.
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CERAMICS INTERNATIONAL
·
2023
·
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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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.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Hao Tang,Zi Ang Chen,Muchen Wu,Shunbo Li,Ziran Ye,Mingjia Zhi
Tuning the size of Au nanoparticles is always an interesting task when constructing Au/semiconductor heterojunctions for surface plasmon resonance-enhanced photocatalysis. In particular, the size of Au nanoparticles in the newly emerging “plasmonic aerogel” photocatalyst concept could approach the size of the semiconductor phase. This work provides an alternative route to realize the size tuning of Au nanoparticles in Au-CeO 2 composite aerogels to some extent, within the framework of the well-established epoxide addition sol–gel method. The size tuning is achieved by exploiting the multi-functionalities of a mixed organic acid additive containing a thiol group in the gelation step. The obtained aerogel photocatalysts are composed of a porous backbone of interconnected CeO 2 nanoparticles and Au nanoparticles, and the size of Au nanoparticles ranges from ∼30 nm to sub-10 nm, while the size of CeO 2 remains at ∼15–10 nm. The surface plasmon resonance peak position and intensity contributed by the Au nanoparticles then vary accordingly. Photocatalytic CO 2 reduction at the gas–solid interface is chosen as a model reaction to study the effect of Au nanoparticle size on the photocatalytic activity of composite aerogel photocatalysts. The addition of Au nanoparticles undoubtedly enhances the overall activity of the CeO 2 aerogel photocatalyst, while the degree of enhancement (in terms of total charge consumption) and product selectivity (CH 4 or CO) are different and correlated with the size of the Au nanoparticles. The best performance can be achieved in a composite in which the Au sizes are the smallest.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 46
·e54671
·
IF 3
Zonglin He,Zhenhong Huang,Jiahui Chen,Ansheng Chen,Jiaoyan Ai,Lina Song,Baohua Liu
Poly (propylene carbonate) diol (PPCD) is one of the most attractive CO 2 copolymers. PPCD-based polyurethane has excellent mechanical properties and hydrophilicity, and is widely used in various fields. However, poor alkali resistance limits the application of PPCD-based polyurethane in wet-type artificial leather (WPL). In order to solve this problem, polyurethane solution (PUS) for wet-type artificial leather was prepared by using PPCD and polytetramethylene ether glycol (PTMG) as soft segments. The chemical structure, viscosity, molecular weight and distribution, physical and mechanical properties, thermal properties and dynamic mechanical thermal properties of PUS were characterized. The changes of the physical and mechanical properties of PUS films and surface morphology of WPLs after soaking in 10 wt% NaOH solution at room temperature for 24 h were studied, so as to evaluate the alkali resistance of polyurethane. The retention of tensile strength and tearing strength of PUS films modified by PTMG increased from 80% to 96% and from 89% to 100%, respectively. The scanning electron microscopy results showed that appropriate PTMG was beneficial to the formation of microporous structure for CO 2 -based polyurethane leather. The leather without PTMG showed agglomeration phenomenon, the micropores were not obvious, and the changes were obvious after soaking in alkali solution. After being modified by PTMG, the morphology of leather after soaking in alkali solution was basically unchanged. Polyurethane leather prepared with PTMG and PPCD as soft segments has excellent alkali resistance. These results suggest that PPCD could be a potential artificial leather material.
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Biomass Conversion and Biorefinery
·
2023
·
IF 4
Chen Jun Xiu,Li Jin Hao,Bao Agula
The development of porous carbon materials with high CO 2 adsorption capacity is crucial for addressing the current issues of industrial air pollution and global warming. In this study, B/N codoped porous carbon materials were prepared via a combined strategy involving the use of a self-sacrificing template in conjunction with potassium hydroxide activation; moreover, g-C 3 N 4 was used as the N source and boric acid was used as the B source. The pore structure and surface chemistry were investigated in detail using different techniques such as X-ray diffraction, scanning electron microscopy, N 2 adsorption and desorption, transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. Results showed that the prepared material exhibited the highest specific surface area (2278 m 2 /g) and pore volume (1.00 cm 3 /g) when the ratio of B/N sources was 1:0.5; moreover, its CO 2 adsorption value (3.26 mmol/g) was higher than those of most codoped adsorbents.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
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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Molecular Catalysis
·
2023
·
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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