GREEN CHEMISTRY
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2025
·
IF 9.2
Xiaoqing Yang,Jinshan Zhao,JunFeng Zeng,Bihua Chen,Liang Tang,Jun Zhang,Akif Zeb,Zhiyong Li,Shiguo Zhang,Yan Zhang
Hyper-crosslinked porous ionic polymers (HCPIPs) are important materials for CO2 capture and catalytic conversion. In this work, we used ion exchange to combine the cross-linking-active tetraphenylborate anion (BPh4-) with a guanidine-based (Gua) ionic liquid (IL), forming a halogen-free IL ([Gua][BPh4]). Using different proportions of formaldehyde dimethyl acetal (FDA), we successfully constructed a series of halogen-free guanidine-functionalized HCPIPs (Gua-HCPIP-x) and achieved efficient CO2 capture and conversion. Specifically, Gua-HCPIP-4, which had rich porosity and a high specific surface achieved a CO2 adsorption capacity of up to 3.2 mmol g-1. Gua-HCPIP-x, with guanidine and BPh4- groups, exhibited higher efficiency and selectivity in the catalytic N-formylation reaction of CO2. Under mild conditions (3 bar, 80 °C), Gua-HCPIP-4 achieved a 94% yield in the CO2 N-formylation reaction and maintained catalytic activity after 5 cycles. This study provides new insights into enhancing the catalytic activity of the CO2 N-formylation reaction and offers practical guidance for synthesizing halogen-free HCPIPs.
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高影响因子
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Dongfeng Hong,Kejing Zhang,Mingshuo Yang,Ruijing Yang,Yusheng Xu,Qiudong Duan,Dacheng Zhou,Yongjin Li,Zhengwen Yang,Zhiguo Song,Yong Yang,Qi Wang,Jianbei Qiu
Photocatalytic conversion of CO 2 into valuable fuels is considered a promising approach for the development of sustainable and renewable energy sources. In this study, we utilized Mo-MOF as a precursor to obtain MoO 3 by pyrolytic derivatization and treated it to obtain MOF-MoO 3-x containing oxygen vacancies as a catalyst for the photocatalytic reduction of CO 2 to CO. MOF derivatization altered the morphology of the MoO 3 , which made the formation of oxygen vacancies easier and facilitated the separation of electron-hole pairs. Meanwhile, the increased specific surface area and the appearance of surface oxygen vacancies enhanced the CO 2 adsorption and activation capabilities of MOF-MoO 3-x . As a result, MOF-MoO 3-x demonstrated a significant enhances in the photoreduction activity of CO 2 . Its CO yield was 29.1 μmolg −1 h −1 , which was 3.7 times higher than that of MOF-MoO 3 and 2.4 times higher than that of H-MoO 3-x . This innovative strategy may provide a new avenue for improving the comprehensive performance of photocatalysts and developing renewable energy sources.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lijian Jin,Xueyan Hou,Lingxiao Zhan,Shangzhi Xie,Lina Gu,Hangqi Yang,Xin Wang,Xinfeng Qian,Jianchong Shen,Linjun Yang
In order to ameliorate the issues of corrosion and high regeneration energy associated with traditional biphasic solvents, a nonaqueous biphasic solvent has been proposed as a potential alternative. This study introduces Tetramethylethylenediamine (TMEDA) as a phase splitter within the Ethanolamine (MEA)/Dimethyl sulfoxide (DMSO) system, resulting in a novel nonaqueous biphasic solvent, TMEDA/MEA/DMSO. Compared with other screened phase splitters, the appropriate polar size and intermolecular interaction force of TMEDA are the key factors that make it comply with the screening of nonaqueous biphasic solvent. When the mass ratio of TMEDA/MEA/DMSO is maintained at 3:3:4, the CO 2 loading attains 0.54 mol (CO 2 )/mol (MEA), with the rich phase comprising 75 % of the total. 13 C NMR and FT-IR characteristics showed that the absorbent product is mainly in the form of MEACOO − /MEAH + . Absorption and phase separation mechanisms of absorbent elucidated by DFT calculations and molecular dynamics simulations. The limited opportunity for TMEDA to interact with MEA molecules emerges as the primary reason for its reduced involvement in the reaction, with the inclusion of TMEDA intensifying the aggregation of MEACOO − /MEAH + and triggering phase transition. In comparison to a 30 wt% MEA water-based absorbent, TMEDA/MEA/DMSO exhibits a 40 % reduction in regeneration energy (estimate) and possesses energy-saving attributes, rendering it a promising candidate for CO 2 capture.
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高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiangqian Guo,Chenhui Qiu,Zhiqiang Zhang,Jie Zhang,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction plays an important role in solving environmental issues and alleviating the energy crisis. However, it is still challenging to distribute the surface-active site on photocatalysts with efficient separation of carriers in rational. Herein, the Cu species loaded SrTiO 3 nanofiber was constructed through coaxial electrospinning which could realize the dispersion of the Cu site on the one-dimensional (1D) nanofiber structure. The 1D nanofiber with Cu site exhibited superior performance on photocatalytic CO 2 reduction based on the excellent ability of charge separation. The Cu 2 O and CuO were determined to be located on the surface of 1D SrTiO 3 nanofiber by the TEM and XPS. The work functions of SrTiO 3 , Cu 2 O, and CuO were calculated to be 5.26, 5.47, and 5.51 eV, respectively, suggesting that the carriers could transfer from SrTiO 3 nanofiber to the Cu species. The yield of CH 3 OH with the optimized 8%Cu-SrTiO 3 catalyst could reach 8.08 ± 0.03 µmol⋅g −1 ⋅h −1 . This work provided a coaxial electrospinning strategy to load the Cu species active site on the surface of 1D SrTiO 3 nanofiber for enhancing photoreduction CO 2 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zixuan Yu,Xiaohui Liu,Xiaoxiang Xu,Wenquan Tao,Zhuo Li,Boyu Li
How to improve the selectivity and stability while ensure the membrane permeability is a challenge of mixed matrix membranes (MMMs) for gas separation applications. We herein report an amine-functionalized COFs-based mixed-matrix membranes (MMMs) for CO 2 /N 2 separation, specifically COF-300-Amide/Pebax2533. This approach endeavors to concurrently enhance the selectivity of CO 2 /N 2 and stability while maintain the high permeability of CO 2 . The natural pore structure of amide-linked COFs significantly enhances the selectivity for CO 2 /N 2 separation, achieving a high permeability of 697.3 Barrer and superior CO 2 /N 2 selectivity up to 51.7. Furthermore, the highly crystalline nature and strong amide bonds of the amide-linked COFs greatly enhance membrane stability, as evidenced by an impressive anti-decomposition temperature of 390.2 °C and sustained performance over 28 days. The underlying interaction mechanisms of CO 2 adsorption and its diffusion mechanism of the COFs, along with their interfacial compatibility with the Pebax2533 matrix, were comprehensively quantified using GCMC, dcTSTs, and MD simulations. This pioneering study demonstrates that amide-linked COF-based MMMs possess remarkable potential for industrial CO 2 /N 2 separation applications, offering an innovative solution that combines high efficiency with long-term operational stability.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 8
·3364-3369
·
IF 2.7
Chunxia Li,Huimin Yu,Shaohong Guo,Jingchun Jia,Ying Chang,Meilin Jia,Jiang Wang
The photocatalytic reduction of carbon dioxide into high value-added chemical feedstock is significant for mitigation of the energy crisis and the greenhouse effect. Metal–organic frameworks (MOFs) possess broad application prospects in photocatalytic CO2 conversion due to the ability to adjust the metal types in metal cluster nodes. Herein, the CO2 photocatalytic performance of trimetallic Fe0.02Ni0.10–Cox–PCN-250 (x = 0.05, 0.10, 0.15, 0.20 mol) was investigated by adjusting the content of Co. Notably, the photocatalytic yields of Fe0.02Ni0.10–Cox–PCN-250 (x = 0.05, 0.10, 0.15, 0.20 mol) were higher than those of bimetallic Fe0.02Ni0.10–PCN-250 and Fe0.02Co0.10–PCN-250 irradiated by visible light. The optimum yield of CO was obtained by trimetallic Fe0.02Ni0.10–Co0.15–PCN-250, up to 299 μmol g−1 h−1. The enhanced yield of CO might be ascribed to the high CO2 adsorption capacity and photogenerated electron transfer after addition of a suitable amount of the third ion, Co. This study provides new insights by designing trimetallic catalysts to increase the efficiency of photocatalytic CO2 reduction.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jiepeng Zhao,Yifei Ma,Zhaomin Tong,Mei Wang,Liantuan Xiao,Suotang Jia,Xuyuan Chen
Engineering photocatalyst crystal facets and constructing heterojunctions are effective strategies to improve photocatalytic activity. The amino-modified titanium-based metal–organic framework (MOF) NH 2 -MIL-125(Ti) (NM) has drawn extensive attention as a photocatalyst by virtue of its high specific surface area, abundant pore structure, and narrow bandgap. However, its catalytic activity is hindered by fast electron-hole recombination and limited light absorption. This study synthesizes NM with engineered crystal facets and Co 3 O 4 @NH 2 -MIL-125(Ti) (C-NM) composites with varying Co 3 O 4 loadings using a facile hydrothermal method. The impact of heterojunctions and facet design on photocatalytic CO 2 reduction under visible light is also studied. Results show that the C-NM, with exposed {111} facets and optimal Co 3 O 4 loading, demonstrates superior photocatalytic CO and CH 4 production rates of 21.64 μmol h −1 g −1 and 3.99 μmol h −1 g −1 , 2.1 and 1.6 times higher than those of NM {001} , respectively. Experimental characterization and density functional theory (DFT) analyses attribute the improved photocatalytic activity to several mechanisms. First, crystal facet modulation can optimize the active sites and specific surface area of the photocatalysts. Second, by loading the narrow-bandgap Co 3 O 4 nanoparticles, bandgap of the C-NM photocatalyst is further reduced, thereby enhancing the absorption and utilization of visible light. Finally, the NM/Co 3 O 4 heterostructure minimizes electron-hole recombination, significantly boosting CO 2 reduction efficiency.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ming Chen,Huan Liu,Ying Wang,Zhiyong Zhong,Yu Zeng,Yuxin Jin,Daiqi Ye,Limin Chen
TiO 2 , ZrO 2 and a series of TiO 2 -ZrO 2 (TxZ1, x means the atomic ratio of Ti/Zr = 10, 5, 1, 0.2 and 0.1) composite oxide supports were prepared through co-precipitation, and then 3 wt% Co was loaded through wetness impregnation methods. The obtained 3 wt% Co/TiO 2 (3CT), 3 wt% Co/ZrO 2 (3CZ) and 3 wt% Co/TxZ1 (3CTxZ1) catalysts were evaluated for the oxidative ethane dehydrogenation reaction with CO 2 (CO 2 -ODHE) as a soft oxidant. 3CT1Z1 catalyst exhibits excellent catalytic properties, with C 2 H 4 yield, C 2 H 6 conversion and CO 2 conversion about 24.5 %, 33.8 % and 18.0 % at 650 °C, respectively. X-Ray Diffraction (XRD), in-situ Raman, UV–vis diffuse reflectance spectra (UV–vis DRS), H 2 temperature-programmed reduction (H 2 -TPR), Electron paramagnetic resonance (EPR) and quasi in-situ X-ray Photoelectron Spectroscopy (XPS) have been utilized to thoroughly characterize the investigated catalysts. The results revealed that 3CT1Z1 produced TiZrO 4 solid solution with more metal defect sites and oxygen vacancies (Ov), promoting the formation of Co 2+ -TiZrO 4 structure. Furthermore, the presence of Ov and Ti 3+ can facilitate the high dispersion and stabilization of Co 2+ , as well as suppressing the severe reduction of Co 2+ , leading to superior ethane oxidative dehydrogenation activity. Besides, less Co 0 is beneficial to ODHE reaction, because of its promotion effects for reverse water gas shift reaction ; however, more Co 0 results in dry reforming reaction (DRE). This work will shed new lights for the design and preparation of highly efficient catalysts for ethylene production.
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PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2017
·Vol. 135
·期 5
·45765
·
IF 1.86
Leiqing Hu,Jun Cheng,Yannan Li,Jianzhong Liu,Junhu Zhou,Kefa Cen
To optimize the CO 2 permeation and CO 2 /H 2 separation performance of hollow fiber-supported polydimethylsiloxane (PDMS) membranes, the effect of the viscosity of the PDMS coating solution on surface morphologies, thickness of PDMS layer, and solution intrusion into surface pores of hollow fiber supports was investigated. Increases in both stirring time and standing time could increase the viscosity of the PDMS solution. The PDMS layer thickness increased when the coating solution viscosity increased, whereas the surface roughness of the PDMS layer markedly decreased and then slightly changed. Moreover, when the stirring time of the PDMS coating solution was 9 min and the standing time was increased from 2 min to 25 min, the CO 2 permeance first decreased, then increased to ∼2250 GPU probably due to the decreased intrusion depth, and finally decreased because of the substantially increased thickness of the PDMS layer. However, the CO 2 /H 2 selectivity increased to 3.4 with an increase in coating solution viscosity. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 45765.
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CELLULOSE
·
2017
·Vol. 25
·期 1
·205-216
·
IF 3.417
Xu Qinqin,Song Longchu,Zhang Lihua,Hu Gang,Chen Qin,Liu Enhui,Liu Yu,Zheng Qiang,Xie Haibo,Li Nanwen
The reversible reaction of the hydroxyl groups in cellulose with CO 2 in the presence of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) results in a rapid and effective derivative dissolution of cellulose in DMSO, by which a series of cellulose acetate propionate (CAP) and cellulose acetate butyrate (CAB) with various degrees of substitution (DS) were synthesized controllably without adding external catalysts. Wherein DBU not only achieves the dissolution of cellulose, but also acts as an efficient organocatalyst for the subsequent cellulose derivatization. The DS of CAB and CAP can be tuned by changing the feed molar ratio of propionic (butyric) anhydride/acetic anhydride and the reaction temperature. The structural and thermal properties of the products were characterized by several analytical techniques including NMR, FT-IR, and TGA. The CO 2 /DBU/DMSO dissolution system provides a new platform for controllable synthesis of mixed cellulose esters with high efficiency under mild conditions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Fei Lv,Lang He,Xue Bai,Du Wang,Yan Zhao
Efficient charge transfer and effective separation of photo-generated charge carriers are crucial factors in photocatalysis . In this study, we present the design of a composite photocatalyst consisting of cobalt and bismuth (CoBi) bimetallic nanoparticles incorporated into a honeycomb nitrogen-doped graphitic carbon ( N -GC) matrix. The ultra-thin porous N -GC matrix exhibits excellent electrical conductivity , a high number of active sites, and enables efficient absorption and multiple reflection of incident light. The CoBi bimetal- N -GC interface establishes a self-driven charge transport channel that effectively suppresses the backflow of photogenerated electrons, leading to prolonged separation of photo-generated carriers and a significant improvement in photocatalytic activity . The CoBi@ N -GC catalyst showcases outstanding performance, producing CH 4 and CO at rates of 36.07 μmol·g −1 ·h −1 and 44.09 μmol·g −1 ·h −1 respectively, confirming its superior photocatalytic capabilities.
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PubMed
高影响因子
CRYSTENGCOMM
·
2025
·
IF 2.6
Ming-Li Ma,Le-Chen Zheng,Rui Li,Yabo Xie
MOF@COF heterostructures featuring abundant porosity, designable structures and efficient separation of photogenerated charge carriers are enthusiastically embraced as promising candidates for the capture and conversion of CO2. Nonetheless, the laborious synthesis procedures involving energy-consuming protection and degassing steps severely impede their widespread application. In this study, a concentration-acid co-regulation strategy was developed to synthesize highly efficient MOF@COF composites in atmospheric air, obviating the need for vacuum, inert gases, and/or repeated freezing. With reduced supersaturation of the synthesis mixtures and intensified competitive coordination from acid modulators, the crystallization of COFs was strategically confined to the exterior surfaces of MOFs, fostering intimate contact to facilitate the interphase electron transfer. The synthesized MOF@COF heterostructures thereby exhibited radically enhanced CO2RR performances, yielding ca. 2.5 times more CO than the original deficiently-contacted composite. Moreover, the versatility of the synthesis strategy was validated using altered MOF and COF structures, shedding light on the significance of crystallization regulation in fabricating advantageous heterostructures. These findings are poised to effectively propel the development and practical implementation of MOF@COF composites.
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