Carbon Capture Science & Technology
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2024
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IF 10.4
Ming Jiang,Xintong Zhang,Mi Feng,Shijie Wang,Zhencai Zhang,Xiangping Zhang,Xingmei Lu,Fei Xu
Using CO 2 -derived dimethyl carbonate (DMC) instead of diphenyl carbonate (DPC) as a carbonyl source for synthesizing bio-based polycarbonates is a green and cost-effective route. However, the synthesis of high-performance polycarbonates via the DMC route remains challenging due to the poor reactivity and selectivity of DMC compared to DPC. Herein, we designed a series of highly active protic ionic liquid (PIL) catalysts for the synthesis of poly(isosorbide carbonate) (PIC) from DMC with ISB. The influences of the structures of anion and cation on the catalytic activity of PILs were systematically studied. Compared with the reported aprotic IL catalysts, the unique reactive hydrogen of the cation in PILs could form a strong hydrogen bond interaction with the carbonyl group of DMC, resulting in higher reactivity of the carbonyl carbon of DMC. Moreover, the nucleophilicity of the anion could be easily tuned by adjusting the p K a value, which effectively realized the balance of the reactivity difference between exo -OH and endo -OH in ISB. Among them, [DBUH][Im] showed the highest catalytic activity, and the weight-average molecular weight ( M w ) and glass transition temperature of PIC reached 55,700 g/mol and 160 °C, respectively. Combined with NMR analyses and DFT calculations, the mechanism that exhibited the synergetic catalytic effect of anion-cation for the polymerization of DMC and ISB was presented.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
·
IF 3.7
Zhaoyang Qi,Shiquan Zhong,Huiyun Su,Changshen Ye,Limei Ren,Ting Qiu,Jie Chen
ABSTRACT Dimethyl carbonate (DMC) is a crucial chemical raw material widely used in organic synthesis, lithium-ion battery electrolytes, and various other fields. The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol. However, the utilization of this catalyst presents several challenges during the process, including equipment corrosion, the generation of solid waste, susceptibility to deactivation, and complexities in separation and recovery. To address these limitations, a series of alkaline poly(ionic liquid)s, i.e. [DVBPIL][PHO], [DVCPIL][PHO], and [TBVPIL][PHO], with different cross-linking degrees and structures, were synthesized through the construction of cross-linked polymeric monomers and functionalization. These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics. Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC. It was discovered that the appropriate cross-linking degree and structure of the [DVCPIL][PHO] catalyst resulted in a DMC yield of up to 80.6%. Furthermore, this catalyst material exhibited good stability, maintaining its catalytic activity after repeated use five times without significant changes. The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Zhiqian Meng,Xiuyu Liu,Lin Zhou,Xinyi Wang,Qin Huang,Guoning Chen,Shuangfei Wang,Yan Jiang
The on-demand regulation of cell wall microstructures is crucial for developing wood as a functional building material for energy management and conversion. Here, a novel strategy based on reactive deep eutectic solvent is developed to one-step in situ fibrillate wood via disrupting the hydrogen bonding networks in cell walls and simultaneously carboxylating wood components, without significantly altering the native hierarchical structures of wood. Benefiting from its distinctive cell wall structure composed of individualized yet well-organized lignocellulose nanofibrils, in situ fibrillated wood exhibits a prominent mesoporous structure with a specific surface area of 81 m2/g. It represents a robust sponge material (5 MPa at 80% strain) with excellent durability. Due to the enhanced compressibility and charge polarization capacity, the in situ fibrillated wood (10 × 11 × 12 mm3) can generate a piezoelectric output voltage of up to 2 V under 221 kPa stress. The favorable microstructural characteristics render in situ fibrillated wood with highly thermal-insulating properties, high solar reflectivity, and mid-infrared emissivity, favoring outdoor passive cooling effects with a subambient temperature drop of 6 °C. Combining its controllable, durable, and eco-friendly attributes, our developed wood sponge represents a versatile structural material suitable for indoor/outdoor energy-saving applications.
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Solar RRL
·
2024
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IF 6
Meijuan Ding,Mei Li,Jingzhi Wang,Zhiliang Jin
Herein, the application of graphdiyne (GDY) in photocatalytic splitting of water and hydrogen evolution is explored. In this article, GDY is prepared by ball milling using calcium carbide as raw material, and it is compounded with phosphating Mo–metal-organic frameworks (MOFs), to explore the photocatalytic hydrogen evolution performance and hydrogen evolution mechanism of composite catalysts. In the results, it is shown that the P–Mo–MOFs (PMF)/G-25 composite photocatalyst has the best hydrogen evolution activity, and the hydrogen evolution rate is highest at pH = 9, reaching 1668.5 μmol g −1 h −1 . Through the four-cycle hydrogen evolution cycle stability test, the PMF/G-25 composites still has good hydrogen evolution stability. It is shown that the combination of phosphating Mo–MOFs and GDY can enhance the hydrogen evolution activity and has excellent hydrogen evolution performance. In the Mott–Schottky test, it is found that PMF and GDY are n-type semiconductors. The conduction and valence values are −0.56 and 1.10 eV for GDY, and −0.68 and 0.97 eV for PMF, respectively. The mechanism of photocatalytic hydrogen evolution is analyzed, and it is speculated that S-Scheme heterojunction is formed between PMF and GDY to further promote photocatalytic hydrogen evolution.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Ling Yu,Hui Gao,Nan Zhang,Xian-Ming Zhang
Proton-conducting materials have gained popularity owing to their extensive applications in biologic/chemical sensors, supercapacitors, proton sieving, and proton-exchange-membrane fuel cells. To date, the most commercially used polymer membrane has been the Nafion series that exhibits conductivity exceeding 0.1 S cm −1 , however, this series is expensive, has poor dimensional stability, and requires a complex synthesis process. The key criterion for selecting Nafion alternatives is to achieve the systematic integration of high proton conductivity with high stability through a simple and efficient approach. In this study, we used an aliovalent metal substitution strategy to design serial metal–organic frameworks (MOFs), including tetragonal T -Cd-BTC (CH 3 NH 2 CH 3 ) 2 [Cd(BTC)](H 2 O) and quasi-cubic quasi- C -In-BTC (C 4 H 7 N 2 )[In(BTC)] and Im@quasi- C -In-BTC (C 3 H 5 N 2 ) 2 [In(BTC)] frameworks, with 2-methylimidazolium and imidazolium cations as templates, respectively. Because of the aliovalent substitution of In(III) for Cd(II), both the metal–oxygen bond strength and unit cell symmetry gradually increased, resulting in an increase in the thermal stability of quasi- C -In-BTC and Im@quasi- C -In-BTC at temperatures of up to 700 K. Compared with in situ loaded 2-methylimidazolium quasi- C -In-BTC , Im@quasi- C -In-BTC prepared by incorporating the imidazolium cation into the pores of activated quasi- C -In-BTC exhibited a higher proton conductivity of 7.1 × 10 −2 S cm −1 at 338 K and 95 % relative humidity. Thus, Im@quasi- C -In-BTC demonstrated real-life application. This result was confirmed by integrating Im@quasi- C -In-BTC with a poly(vinyl pyrrolidone)-poly(vinylidene fluoride) polymer matrix. Density functional theory simulations indicated that Im@quasi- C -In-BTC was strongly acidic and had high water–adsorption capacities, which contributed to extensive hydrogen-bond networks and strong host–guest interactions, in accordance with the experimental finding.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 12
·7178-7186
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IF 10.7
Haiyuan Li,Dingxin Liu
In photocatalysis, catalysts are crucial for effective charge transfer and separation. Using Mo-MOF and CdCo-MOF as precursors, we have designed an effective Cd0.76Cd0.17Mo0.07S (Ethy-CCMS) photocatalyst. We compared the performance of samples prepared in different environments and found that the rod-shaped Ethy-CCMS prepared in an alkaline environment provided by ethylenediamine exhibited the highest photocatalytic hydrogen production activity with an efficiency of 30.14 mmol g−1 h−1, which was 32.2 times higher than that of the CdS prepared under aqueous solution conditions. The solid solution formed can accelerate the separation of photogenerated electrons and avoid the formation of high oxidation power h+ compared to CdS alone. In addition, adding Mo and Co enables these three metals to form bonds with S. The shared S-bond improves the stability of the material and significantly mitigates the photocorrosion phenomenon. This study investigates the role of sulfides derived from Mo-MOF and CdCo-MOF as sustainable and promising co-catalyst candidates to enhance the photocatalytic performance of CdS-based composites.
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JOURNAL OF FLUORESCENCE
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2024
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IF 2.6
Dai Zhengyuan,Liu Hao,Sun Xuyuan,Wang Ying,Fan Jie,Li Li,Ding Yaping
Using o-phenylenediamine as carbon source and phytic acid as phosphorus source, two P-rich carbon quantum dots RCDs and BCDs were synthesized successfully by changing the reaction temperature and time of hydrothermal method. It was found that RCDs with red emission could realize sensitive detection of 2-methylimidazole, and 2-methylimidazole had no obvious quenching effect on BCDs with blue emission, which made RCDs a sensitive, quick and selective fluorescence sensor for 2-methylimidazole detection. Under the optimal experimental conditions, the fluorescence intensity of RCDs decreased with the increasing of 2-methylimidazole concentration. The detection of 2-methylimidazole concentration by the carbon quantum dots sensor showed a good linear relationship in the range of 5 ~ 110 µM, and the low detection limit was 0.61 µM (S/N = 3). The sensor is able to detect 2-methylimidazole in lake water, enabling the application of real samples. The results show that this work provides a simple fluorescence method to detect 2-methylimidazole in water.
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Carbon Capture Science & Technology
·
2025
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IF 10.5
Dudu Li,Zhifang He,Ying Chen,Zelong Xu,Zibo Yang,Hao Zhang,Zhihua Qiao
Carbon nanotubes (CNTs), known for their elevated specific surface area, exemplary mechanical properties and thermal stability, are regarded as optimal reinforcing fillers for the fabrication of mixed matrix membranes (MMMs). In this study, self-supported MMMs were prepared using melted zeolitic imidazolate framework (ZIF), denoted ZIF-62 glass, as the continuous phase and multi-walled CNTs (MWCNTs) particles as the dispersed phase. The resulting membranes were thoroughly characterized, and the effect of different incorporation amounts of MWCNTs on the gas separation performance was investigated. It is noteworthy that at an incorporation amount of 4 wt. % MWCNTs, the ideal selectivity of prepared self-supported ( a g ZIF-62) 0.96 (MWCNTs) 0.04 MMM for CO 2 /N 2 and CH 4 /N 2 was 31.2 and 8.6 respectively, exceeding the 2019 Robeson upper bound. The results demonstrated that MWCNTs have excellent gas transport properties and significantly enhance the separation performance. Furthermore, the self-supported ( a g ZIF-62) 0.96 (MWCNTs) 0.04 MMM also exhibited excellent mechanical properties and pressure resistance, making them highly promising candidates for advanced gas separation applications. This study not only highlights the effectiveness of MWCNTs as functional fillers in MMMs but also presents a novel approach for designing high-performance gas separation membranes.
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Materials Horizons
·
2025
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IF 10.7
Linlin Zhao,Meiyu Hu,Xiaohang Yin,Hao Yang,Liyun Zhu,Pingyuan Sun,Xiya Wang,Songwei Ai,Yonghui Zheng,Genjie Li,Tingting Yang,Xuerui Chen,Jingyu Zhang
Effectively alleviating cerebral ischemia-reperfusion (I/R) injury is challenging despite medical advances. Prompt restoration of blood flow after ischemic stroke causes secondary damage to brain tissue, triggers neuroinflammation and overproduces reactive oxygen species (ROS). MiRNA regulates genes involved in neuron apoptosis and neuroinflammation, thus exhibiting potential in ameliorating cerebral I/R injury. However, as miRNA is vulnerable to degradation, its effective delivery poses obstacles to clinical applications. Inspired by therapeutic potential of miR-210 inhibitors in ischemic stroke-induced neuroinflammation, we constructed a multifunctional nanosystem composed of ceria nanozymes and zeolitic imidazolate framework-90 (ZIF-90) nanoparticles to deliver miR-210 inhibitors to treat cerebral I/R injury. Attributed to proton sponge effect of ZIF-90, this nanosystem allows for lysosome escape of miR-210 inhibitors to protect their intracellular bioactivity, while integration of ZIF-90 and ceria nanozymes utilizes multi-enzyme cascade activities to constrain lipid peroxidation and reduce oxidative damage in brain tissues of mice with middle cerebral artery occlusion (MCAO). After crossing the blood-brain barrier, miR-210 inhibitors target TET2 to suppress pro-inflammatory cytokines, finally inhibiting neuroinflammation. More than uncertain stability and efficacy of direct TET2 protein administration, delivery of miR-210 inhibitors by multifunctional nanosystems engendered neuroprotection, indicating their potential for protein replacement therapy against cerebral I/R injury.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wei Liu,Heng Zhang,Zhe Zhang,Yali Ji,Tiantian Xu,Xusheng Li,Jiao Chen,Mengyao She,Ping Liu,Shengyong Zhang,Jian-Li Li
Solar-driven photocatalytic CO 2 -to-CH 4 conversion represents a promising strategy to mitigate the energy and climate crisis. However, it is still challenging to achieve efficient CO 2 conversion due to the difficulties of CO 2 activation, sluggish kinetics of water oxidation half-reaction and high cost of sacrificial agents in conventional reaction systems. Herein, by precisely integrating bimetallic sulfide with functionalized UiO-66 to construct a Cu 0.1 Zn 0.9 S/Bim-UiO-66 S-scheme heterojunction photocatalyst, which innovatively accomplished complete CO 2 methanation and benzimidazole synthesis in one redox cycle. Experimental results reveal that the optimized photocatalyst exhibited an exceptional CH 4 production rate of 35.2 μmol h −1 g −1 (selectivity of 100 %) and 92 % benzimidazole conversion under simulated solar irradiation. Mechanistic studies demonstrate that the S-scheme heterojunction significantly enhances photogenerated charge carrier separation efficiency through the establishment of a built-in electric field, while preserving the strongest redox potentials of the two semiconductors. Remarkably, the benzimidazole synthesis process replaced conventional H 2 O oxidation, proving beneficial for CO 2 -to-CH 4 conversion. This work provides new insights into designing high-performance photocatalysts for CO 2 conversion and the synthesis of fine chemicals.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wensheng Wei,Yuxin Wang,Guangwen Xu,Jinggang Zhao,Lei Shi
In this work, a series of multifunctional integrated heterogeneous catalysts (PS-[EIMBr-COO] 2 M, M = Fe 2+ , Co 2+ , Ni 2+ and Zn 2+ ) with abundant active sites and a dynamic swing-active architecture were successfully constructed, which were applied in catalytic cycloaddition of CO 2 and propylene oxide (PO) for efficient propylene carbonate (PC) preparation. The PS-[EIMBr-COO] 2 Co catalyst demonstrated the best catalytic activity with a 98.92 % conversion of PO, a 99.00 % selectivity towards PC, and a TOF value of 120.75 h −1 at 110 °C. The characterization techniques and theoretical simulation revealed that the excellent catalytic performance of the PS-[EIMBr-COO] 2 Co catalyst was attributed to the synergistic effect of the Lewis acid center, imidazolinium groups (Lewis base), Br − ions (nucleophilic site), and swing-active structure. The synergistic effect between active sites reduced the reaction energy barrier of the rate-determining step, and the swing-active structure in catalyst was believed to improve the contact efficiency between the active site and the reaction substrate. The synthesized PS-[EIMBr-COO] 2 Co catalyst was structurally stable and maintained its initial catalytic ability after seven cycles. Moreover, the PS-[EIMBr-COO] 2 Co catalyst shows good substrate universality for the cycloaddition reactions of epoxides. The catalyst construction strategy of functional integration and flexible active structure has high universality for cycloaddition catalyst design, and has important guiding significance for rational design of efficient heterogeneous catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Qinghai Long,Yutao Bai,Anteng Dai,Huajie Qiu,Xuanang Fu,Xiaoyun Chen,Chao Liu,Waseem Hayat,Bihong Lv,Guohua Jing,Zuoming Zhou
In this study, 2-dibutylaminoethanol imidazole ([DBAE][Im]) was developed as a novel ionic liquid for energy-efficient CO₂ capture to address key challenges, such as high energy consumption and elevated regeneration temperatures, associated with conventional amine-based absorbents. The self-extractable behavior of [DBAE][Im] facilitated reversible liquid–liquid phase separation during CO₂ absorption and desorption. The CO 2 absorption loading of the [DBAE][Im] solution (0.5 mol·L −1 ) reached 0.82 mol·mol −1 at 313.15 K, and the regeneration efficiency remained high at 87 % even after five consecutive regeneration cycles at 371.15 K. The reaction and self-extraction mechanisms were determined using carbon nuclear magnetic resonance spectroscopy and quantum chemical calculations. These analyses revealed that the significant polarity difference and weak hydrogen bonding between [DBAE][Im] and water (H₂O) induced a phase transition before CO 2 absorption. During absorption, CO 2 reacted with [DBAE][Im] to form carbamate/bicarbonate (HCO₃ − /CO₃ 2− ) species, which resulted in a homogeneous solution due to the decreased polarity of CO₂ products and the strong hydrogen bonds formed between the products and H₂O. Following thermal desorption, [DBAE][Im] separated into the upper phase, restoring its high polarity and reducing intermolecular hydrogen bonding with H₂O. Owing to its self-extraction capability, the regeneration rate of [DBAE][Im] improved significantly at 371.15 K, while the regeneration heat duty was reduced by 47 % compared to monoethanolamine. The results demonstrate that the novel aqueous [DBAE][Im] absorbent offers substantial energy savings for CO₂ capture, presenting a promising approach for advancing carbon capture technologies.
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