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CATALYSIS LETTERS · 2022 ·Vol. 153 ·期 11 ·3383-3391 · IF 2.936

The Efficient CO2 Fixation Catalyzed by Fe-Based Catalyst for Synthesizing Benzimidazoles

Zhang Luping,Tu Xuewei,Han Weihang,Chen Liangchen,Chen Yutong,Zheng Hui

As the main resource of greenhouse gas, CO 2 needs to be fixed into different chemicals to relieve the environmental problem. Fe-based catalyst and g-C 3 N 4 have received extensive attention due to their easy preparation, low cost, and environmental friendliness. Herein, a heterogeneous catalyst system consisting of rich-electron g-C 3 N 4 and strong electron-withdrawing groups Fe-complex [Fe(bpy)(CO) 2 (Cl) 2 ] was developed, which could promote electron transfer and enhance the electronic interaction for fixing CO 2 . o -phenylenediamine substrates with different electron-donating/withdrawing groups were employed to fix CO 2 into high-valued heterocycle benzimidazoles. The optimum reaction conditions were examined by orthogonal experiments. A series of benzimidazole derivatives were synthesized with yield up to 98%, which indicated the catalyst had the ability of fixing CO 2 . This catalyst provides a new pathway for fixing CO 2 into valuable benzimidazole derivatives. Graphical Abstract

研究领域: 化学 · 环境科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Enhanced photocatalytic CO2 reduction to CH4 by Mn2O3/MgTi2O5 nanocomposite

Yaru Shen,Jiasheng Cai,Xin Huang,Yi Zheng,Yu Shao

Photocatalysis is a green technology which could sustainably convert CO 2 into value-added chemicals by using solar energy. Under xenon light irradiation, Mn 2 O 3 /MgTi 2 O 5 nanocomposites synthesized by two-step hydrothermal method greatly increase photocatalytic activity of CO 2 reduction. The optimal yield 420.53 μmol g −1 h −1 for CH 4 is achieved at a ratio 1:10 (W/W) of Mn 2 O 3 to MgTi 2 O 5 , with selectivity of 98.1 %, i.e., 4 and 33 times larger than those of individual MgTi 2 O 5 and Mn 2 O 3 , respectively. The superior photocatalytic performance is attributed to the formation of S-type heterojunction, valence change of Mn 3+ /Mn 4+ , and the bridging effect of Mg migration, which facilitates the separation and transfer of photogenerated electrons and holes. Mn 2 O 3 /MgTi 2 O 5 constructs an efficient redox photocatalytic system composed of a light trapping component (Mn 2 O 3 ), electron transport channel (Mg penetrating Mn 2 O 3 ), mutually separated reduction center (MgTi 2 O 5 ) and oxidation center (Mn 2 O 3 ). The potential Mn 2 O 3 /MgTi 2 O 5 photocatalyst for CO 2 reduction provides new insights to design novel efficient photocatalyst composites akin to biological photosynthesis.

CAS / MDL: 69-72-7
研究领域: 材料科学 · 环境科学
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MACROMOLECULAR RAPID COMMUNICATIONS · 2022 ·Vol. 43 ·期 20 ·2200341 · IF 5.006

Chemically Recyclable CO2-Based Solid Polyesters with Facile Property Tunability

Yongjia Lou,Jialin Xu,Luyan Xu,Zhuo Chen,Bo-Lin Lin

Synthesizing chemically recyclable solid polymeric materials is a significant strategy to potentially achieve carbon neutral production of new polymers and alleviate plastic pollution, especially when the synthesis is based on CO 2 and inexpensive co-feedstocks available in large scales. Additionally, polymeric materials should have high enough molecular weight to exhibit distinguished properties from low molar mass polymers to serve for a broader range of application scenarios. However, up to now, strategies for developing solid-state CO 2 -based chemically recyclable polyesters with both high molecular weight and facile property tunability are still unprecedented. Herein, a brand-new synthetic route is developed to synthesize chemically recyclable CO 2 -based solid polyesters with high molecular weight ( M n up to 587.7 kg mol −1 ) and narrow dispersity ( Đ < 1.2), which should further broaden the potential application scenarios of new CO 2 -based polyesters. Additionally, complete monomer recovery from poly( δLH 2 ) material is also achieved. The preserved terminal alkene groups allow facile property tuning of the polyesters via photo-initiated thiol-ene click reactions, enabling more potential utilities and further functionalizations.

CAS / MDL: 51364-51-3 865-33-8
研究领域: 材料科学 · 化学工程 · 环境科学
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LUMINESCENCE · 2017 ·Vol. 32 ·期 8 ·1448-1455 · IF 1.509

A tricorn-rhodamine fluorescent chemosensor for detection of Co2+ ions

Jing Li,Shuhua Han

A novel chemosensor TrisRh based on tris(2-aminoethyl)amine and rhodamine 6G is designed and synthesized as a fluorescence turn-on probe for Co 2+ ions that is paramagnetic with a property of quenching fluorescence. Rhodamine spirolactam forms are nonfluorescent, whereas, ring-opening of corresponding spirocyclic induced by Co 2+ results in strong fluorescence emission. Upon the addition of Co 2+ ions, TrisRh can display significant enhancements in absorbance and fluorescence intensity as well as evident colorific transformation, which can be perceived by the naked eye. The association stoichiometry of TrisRh to Co 2+ ions was inferred to be 1:1 through Job's plot and electrospray ionization mass spectrometry analysis. The binding model was speculated from Fourier transform infrared spectra and 1 H–nuclear magnetic resonance technologies. Significantly, the limit of detection was determined to be as low as 1.22 nmol. Furthermore, TrisRh can exhibit robust anti-jamming ability against other interference metal ions.

CAS / MDL: 107-22-2
研究领域: 分析化学 · 生物化学
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CATALYSIS TODAY · 2022 · IF 6.562

Development of soluble UiO-66 to improve photocatalytic CO2 reduction

Li Tan,Yanru Li,Qian Lv,Yuyan Gan,Yuan Fang,Yu Tang,Lizhi Wu,Yuanxing Fang

The conversion of CO 2 to valuable chemicals by photocatalysis has attracted widespread interesting. Owing to the linear structure of CO 2 molecule with strong C O bond, the surface reaction is considered as one of the main issues to restrict the conversion efficiency. Herein, soluble UiO-66 has been developed as co-catalyst to enhance the photocatalytic performance for CO 2 reduction. The soluble UiO-66 has presented the performance ca. 1.5 higher than the insoluble version, yielding 30.6 µmol/h for CO 2 to CO conversion by using 5.0 mg sample. This improvement can be attributed to the preserved framework by soluble UiO-66. Therefore, the chemisorption of CO 2 molecules can be improved, boosting the reduction reaction for CO production. This research provides a new path for a rational design of metal-organic framework (MOF) for photoredox catalysis, meanwhile inspiring advanced application of MOF catalysis with the soluble manner.

研究领域: 化学 · 材料科学 · 环境科学
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2023 · IF 5.7

CO2 capture based on Al2O3 ceramic membrane with hydrophobic modification

Hongming Fu,Kaili Xue,Jihao Yang,Zhaohao Li,Heng Zhang,Dan Gao,Haiping Chen

In this paper, Al 2 O 3 ceramic membrane is modified to hydrophobicity by grafting 1 H,1 H,2 H,2 H-perfluorodecyltriethoxysilane. And its properties are characterized in detail. CO 2 capture performance of ceramic membrane is investigated by experiments. Results show that wetting resistance after modification is significantly improved, and contact angle increases from the initial 49.8–130.9°. However, hydrophobic modification has no significant effect on the crystalline phase, surface morphology and pore size distribution of the ceramic membrane. With ethanolamine (MEA) as absorbent, CO 2 mass transfer rate and capture efficiency using modified hydrophobic ceramic membrane are 46.6 × 10 −3 mol/(m 2 ·s) and 98.0%, showing significantly increase compared to the original membrane. After 72 h immersion in MEA solution, quality of ceramic membrane does not change significantly. And there is almost no change in average pore size. We believe this study will provide a reference for the industrial application for CO 2 capture by gas-liquid membrane contactor with ceramic membrane.

研究领域: 材料科学 · 环境工程
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY · 2024 · IF 5.9

Electron-rich Ni2+ in Ni3S2 boosting electrocatalytic CO2 reduction to formate and syngas

Maomao Liu,Guizeng Liang,Ningce Zhang,Tao Li,Lipeng Diao,Ping Lu,Xiaoliang Zhao,Daohao Li,Dongjiang Yang

Rationally constructed new catalyst can promote carbon dioxide reduction reaction (CO 2 RR) to valuable carbonaceous fuels such as formate and CO, providing a promising strategy for low CO 2 emissions. Herein, the synthesized Ni 3 S 2 @C as a highly efficient electro-catalyst exhibits remarkable selectivity for formate with 73.9% faradaic efficiency (FE) at −0.7 V vs. RHE. At high applied potential, it shows a high syngas evolution with CO/H 2 ratios (0.54–3.15) that are suitable for typical downstream thermochemical reactions . The experimental and theoretical analyses demonstrate that the electron-rich Ni 2+ in Ni 3 S 2 enhances the adsorption behavior of ∗ OCHO intermediate, reduces the energy barrier of the formation of intermediates, and improves the selectivity of the formate product. Attenuated total reflection surface-enhanced infrared absorption spectra conducted in situ show that ∗ OCHO intermediate is more likely to be generated and adsorbed on Ni 3 S 2 , enhancing the selectivity and activity of the formate product.

CAS / MDL: 9005-38-3
研究领域: 电化学 · 催化材料 · 可再生能源
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ACS Omega · 2020 · IF 2.87

Optimization of CO2 Adsorption on Solid-Supported Amines and Thermal Regeneration Mode Comparison

Yangyang Guo,Lei Luo,Yang Zheng,Tingyu Zhu

For improving the CO2 adsorption capacity of solid-supported amines, five commercial porous supports have been selected and impregnated with tetraethylenepentamine (TEPA), and their CO2 adsorption performances have been evaluated using a fixed-bed reactor coupled with mass spectrometry. For solid-supported amines, CO2 adsorption capacities coincide with the texture characterization of the adsorbent supports (mesoporous alumina, montmorillonite, silica gel, porous resin, MCM-41 molecular sieve), and the optimum TEPA loading amount is mainly affected by the pore volume. The mesoporous supports were found to be more conducive to uniform loading of organic amine, with more than 370 mg/g CO2 adsorbed per unit TEPA. Other components in flue gas, especially H2O, favor CO2 adsorption on solid-supported amines. SO2 inhibited the CO2 adsorption, which was mainly attributable to the strong and irreversible binding of SO2 on some amine sites. NO had little effect on CO2 adsorption. Thermal stabilities of solid-supported amines have been tested based on thermogravimetry curves, and the main weight loss peak for TEPA appears at 513 K for solid-supported amines. Linear and step regeneration modes have been compared, revealing that the temperature for step regeneration is 37 K lower than that for the linear regeneration mode. Moreover, the desorption peak area for the step regeneration mode is 20% higher than that for the linear regeneration mode, indicating that the step regeneration mode can be used in practical applications, to reduce energy consumption during regeneration.

研究领域: 化学工程 · 环境科学
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Fabrication of cellulose nanofibrils/UiO-66-NH2 composite membrane for CO2/N2 separation

Xiong-Fei Zhang,Yi Feng,Zhongguo Wang,Mingmin Jia,Jianfeng Yao

Incorporating metal-organic frameworks into cellulose matrix to prepare composite membranes is promising in gas-separation applications. In this study, UiO-66-NH 2 (Zr-based MOF) nanoparticles are wrapped into the densely packed cellulose nanofibrils (CNF-COOH) via a facile vacuum filtration process. The existence of acid-base interactions and electrostatic forces between UiO-66-NH 2 and CNF-COOH renders ideal interfacial morphology. Results show that UiO-66-NH 2 is cross-linked by -COOH groups and well-dispersed in the CNF matrix. The porous UiO-66-NH 2 strengthens the diffusion process of CO 2 molecules, thus elevating the permeation flux and separation factor simultaneously. The optimum separation performance is achieved over CM-1 membrane with a CO 2 permeability of 139 Barrer and a CO 2 /N 2 selectivity ratio of 46.

CAS / MDL: 10026-11-6
研究领域: 材料科学 · 环境科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

S-scheme heterojunction Cu-porphyrin/TiO2 nanosheets with highly efficient photocatalytic reduction of CO2 in ambient air

Feng Yue,Mengke Shi,Cong Li,Yang Meng,Shuo Zhang,Lan Wang,Yali Song,Jun Li,Hongzhong Zhang

Directly capturing CO 2 in ambient air and converting it into value-added fuels using photocatalysis is a potentially valuable technology. In this study, Cu-porphyrin (tetrakis-carboxyphenyl porphyrin copper, CuTCPP) was innovatively anchored on the surface of TiO 2 (titanium dioxide) nanosheets to form an S-scheme heterojunction. Based on this, a photocatalytic reaction system for stably converting CO 2 in ambient air into value-added fuels at the gas–solid interface was constructed without addition of sacrificial agents and alkaline liquids. Under the illumination of visible light and sunlight, the evolution rate of CO is 56 μmol·g −1 ·h −1 and 73 μmol·g −1 ·h −1 , respectively, with a potential CO 2 conversion rate of 35.8 % and 50.4 %. The enhanced of photocatalytic performance is attributed to the introduction of CuTCPP, which provides additional active sites, significantly improves capture capacity of CO 2 and the utilization of electrons. Additionally, the formation of S-scheme heterojunction expands the redox range and improves the separation efficiency of photo-generated charges.

CAS / MDL: 1317-70-0 5593-70-4
研究领域: 光催化 · 材料科学 · 环境科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Zeolitic imidazolate frameworks-based porous liquids with low viscosity for CO2 and toluene uptakes

Xiaoqian Li,Dechao Wang,Zhongjie He,Fangfang Su,Nan Zhang,Yangyang Xin,Hongni Wang,Xiaolu Tian,Yaping Zheng,Dongdong Yao,Mingtao Li

Porous liquids (PLs) as a novel class of materials combine the permanent porosity of microporous solids, the rapid mass transfer of liquids, and fluidity, thus exhibiting extraordinary promise for gas capture and separation. However, the practical application of PLs was severely restricted by their undesirable relative high viscosity and melting temperature. In this work, the symmetric dicationic ionic liquids [C 6 BIm 2 ][NTf 2 ] 2 was synthesized as a steric hindrance solvent to construct a type of low viscosity zeolitic imidazolate frameworks (ZIFs)-based PLs. Specifically, the ZIF-67-PLs-2 ( i.e. , ZIF-67 loading of 2.0% in PLs) presented a low viscosity with 543.4 mPa·S at 25 °C, which was about 20 times lower than that of type III PLs reported previously. Meanwhile, ZIF-67-PLs showed long-term stability even over 180 days and broke the fluidity limitation down to −64 °C, broadening the work conditions. Moreover, ZIF-67-PLs-10 ( i.e. , ZIF-67 loading of 10.0% in PLs) achieved 55 times CO 2 and 7 times toluene adsorption capacity more than those of the corresponding pure DILs, respectively. Remarkably, the fascinating features of ZIF-67-PLs including lower viscosity, wide liquid range and higher adsorption pave a new way for the optimal design of novel PLs towards gas uptake and separation.

研究领域: 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Nanostructured AlOOH – A promising catalyst to reduce energy consumption for amine-based CO2 capture

Cong Jiang,Maohong Fan,Ge Gao,Wufeng Jiang,Xiaoshan Li,Cong Luo,Liqi Zhang,Fan Wu

In order to alleviate the intensive energy demand of amine-based post-combustion carbon capture technology, metal oxyhydroxide AlOOH of nanoscale was synthesized through the hydrothermal method and applied to accelerate the CO 2 desorption rate and reduce the regeneration heat duty of aqueous monoethanolamine (MEA) solution for the first time. Results showed that the use of AlOOH could accelerate the desorption rate by up to 560% and increase the desorption amount by 251%. By comparing the performance between AlOOH and Al 2 O 3 , it can be found that the presence of extra hydroxyl groups is 20.6% more efficient in catalyzing CO 2 desorption. According to a simplified heat transfer model created in this work, AlOOH could reduce the heat duty by 17% with only 0.1 wt% loading, which exhibited the highest performance cost ratio among related literature. In addition, the cyclic stability of AlOOH was confirmed through various characterization methods, including XRD, FT-IR, SEM, and N 2 adsorption–desorption. More importantly, a possible catalytic mechanism of AlOOH was discussed and proved where it could change reaction pathways in different CO 2 loading regions. This work reveals a promising research direction towards cost-efficient and high-performance metal oxyhydroxide catalysts in the catalytic amine regeneration field to approach the net-zero carbon emission goal.

研究领域: 材料科学 · 环境工程 · 化学工程
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