JOURNAL OF MEMBRANE SCIENCE
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2025
·
IF 9
Han Zhang,Jiashuai Zhao,Yutong Wang,Ziting Zhu,Jiating Liu,Jian Lu,Fusheng Pan,Taotao Gao,Zhongyi Jiang
Covalent organic framework (COF)-based hybrid membranes have emerged as promising candidates for volatile organic compounds (VOCs) recovery. However, hybrid membranes with both high selectivity and permeability remain to be explored. Herein, a hierarchically structured COF (HCOF) with combined micro-, meso- and macropore was synthesized by Triformylphloroglucinol (Tp) and 2,5-diaminobenzoic acid (Pa-COOH) via NaCl templating, and subsequently employed as fillers to fabricate COF-based hybrid membranes. The abundant mesopores and macropores in HCOF provided fast mass transfer channels with reduced mass transfer resistance toward aromatics, thus enhancing the diffusion of VOCs in the hybrid membranes and exhibiting higher permeability. The optimal membrane with 2 wt% HCOF demonstrates a remarkable toluene permeability of 1.4 × 10 −6 mol μm m −2 s −1 Pa −1 along with a high toluene/N 2 selectivity of 589. The design of the hierarchical pore COF-based hybrid membrane in this study may inspire the development of advanced membrane structures for VOCs recovery.
研究领域:
材料科学
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化学工程
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膜技术
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分离科学
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环境科学
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DOI
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Jinpeng Liu,Chengcheng Hao,Huili Zhang,Hongyu Chen,Ling Zhang,Xiaodong Chen,Jianye Wang,Maohuai Wang,Shuxian Wei,Xiaoqing Lu,Zhaojie Wang,Siyuan Liu
Covalent organic frameworks (COFs) have become potential candidates for gas purification technology, especially in carbon capture and storage applications. By utilizing strategies such as pore structure design and functional modification, COFs have been developed to exhibit high selectivity and superior adsorption capacity for the effective capture and separation of CO2 from industrial waste gases. Notably, alkali metals exhibit strong interactions with the backbone of the COFs, which can enhance the CO2/N2 adsorption separation performance of these porous materials. This study details the synthesis of two-dimensional COF materials modified with acidic groups (TpPa-COOH and TpPa-SO3H) via mechanical grinding. Alkali metals such as Na, Li, and K were introduced into these groups through simple ion exchange reactions, thereby creating metal-modified COF materials. The impact of various alkali metals on the CO2/N2 adsorption separation performance of COF materials was investigated. Among the resulting products, lithiated TpPa-COOH showed the highest CO2 capture capacity of 2.65 mmol/g at 273 K and 1 bar. This may be due to the smaller atomic size of Li that offers larger adsorption space. Under the same conditions, the K-modified TpPa-SO3H exhibited the highest selectivity of 548, which surpasses most COFs reported in the literature. The superior performance was caused by the high polarization of the COF backbone triggered by the alkali metals. The inference was further confirmed by computational simulations. This work provides a facile method for the modification of porous materials with alkali metals to achieve superior gas separation performance.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Shichen Zeng,Xu Liang,Mingang Zhao,Yanxiong Ren,Hanze Ma,Ziting Zhu,Yuhan Wang,Shaoyu Wang,Junyi Zhao,Guangzhaoyao Yang,Xuerui Wang,Fusheng Pan,Guangwei He,Zhongyi Jiang
Covalent organic frameworks (COF) are deemed as disruptive membrane materials owing to their versatile functionalities, high stability and ordered nanochannels. However, the size mismatch between the COF intrinsic pore and gas molecules becomes a grand challenge when using COF membrane for carbon capture. Herein, we propose a new type of polymer-functionalized COF laminar membranes through grafting CO 2 -phlic polyethyleneimine (PEI) polymer onto carboxylic acid COF (cCOF) laminar membranes. The cCOF nanosheets with high density of carboxyl groups are prepared via modified single phase solution method and then assembled to fabricate membranes. Further, the cCOF membranes are functionalized with PEI using 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide/N-Hydroxysuccinimide (EDC/NHS) coupling chemistry. The introduction of abundant amino groups from PEI afford the affinity of membranes toward CO 2 . Meanwhile, the graft of the PEI polymers reduces the defects or pinholes on the membrane surface. As a result, the PEI functionalized cCOF membranes exhibit a high CO 2 permeance of 1004 GPU and a CO 2 /N 2 selectivity of 33.7, which reach the carbon capture target performance and show great prospect for treating real flue gas. Our approach of functionalizing cCOF membranes with tailored functionalities may inspire the design of molecule-selective COF membranes.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Cheng Liu,Qi Chen,Yueling Chen,Jimmy C. Yu,Jionghua Wu,Ling Wu
Photocatalysis, which uses sunlight, N 2 and H 2 O to produce NH 3 , is a more sustainable approach to N 2 fixation than the Haber-Bosch process. However, its efficiency is severely limited by the difficulty of activating N N bonds. This work presents metal (M = Cu, Fe, V)-substituted MIL-125(Ti) (MIL-(MTi)) for photocatalytic N 2 fixation without using any sacrificial agents. Structural characterizations reveal that the active sites including oxygen vacancies (OV) and Ti 3+ species are formed by the resulting crystal distortion due to the partial substitution of Ti 4+ by other metal ions (Cu + , Fe 2+ , V 3+ ) in MIL-125(Ti). MIL-(CuTi) possesses a larger number of OV and Ti 3+ compared to MIL-(FeTi) and MIL-(VTi) due to the larger valence difference between Cu + and Ti 4+ . These active sites not only promote the adsorption and activation of N 2 and H 2 O, but also facilitate the photogenerated charge mobility. Photogenerated holes oxidize H 2 O to produce O 2 and H + . Photogenerated electrons reduce N 2 activated on Ti 3+ sites by combining with H + to form NH 4 + . Therefore, MIL-(CuTi) shows the highest NH 4 + production rate 46.5 µmol·h −1 ·g −1 , which is much higher than that (1.2 µmol·h −1 ·g −1 ) of the pristine MIL-125(Ti). This work provides a new insight into rational design for artificial N 2 fixation systems by the construction of the active site.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Zhang Lei,Cao Xueting,Xin Qingping,Ding Xiaoli,Jin Huimin,Chen Hao,Chu Qingquan,Du Yifei,Huang Wei,Zhang Ruihua,Bao Shiya,Zhang Yuzhong
In this study, a top-down etching method is used to obtain MXene nanosheets with an accordion-like structure, and the surface of the MXene nanosheets is functionalized with 3-aminopropyltriethoxysilane to obtain functionalized MXene nanosheets (f-MXene), which is combined into polyethylene oxide (PEO) copolymer matrix for fabricating mixed matrix membranes (MMMs). The f-MXene nanosheets enhance the CO 2 /N 2 separation performance of membranes in multiple ways. Firstly, the accordion-like structure of f-MXene increases the channel for rapid gas transport. Secondly, the two-dimensional sheet-shaped material has a high aspect ratio, which effectively weakens the interaction between polymer chains and inhibit crystallization. This increases free volume for molecular transport and helps improve gas permeability. Thirdly, the amino group can react reversibly with CO 2 , improving reaction selectivity, and facilitates CO 2 transport. Therefore, the PEO/f-MXene membrane exhibits excellent CO 2 permeability and CO 2 /N 2 selectivity. To explore more efficient separation technology, the membrane separation performance at low-temperature is investigated. At − 20 °C, the PEO/f-MXene-3% membrane has a CO 2 permeability of 47.8 Barrer and a CO 2 /N 2 selectivity of 280.9, which is 576.9% higher than that at 35 °C, exceeding the latest upper bound. Graphical
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FOOD RESEARCH INTERNATIONAL
·
2024
·
IF 7
Dongzhu Huang,Chenyi Sun,Yuhan Wu,Fangling Zheng,Qiqi Yang,Xinmeng Zhang,Qianying Dai,Xiaochun Wan,Qi Chen
This study aimed to investigate the effect of the combination of shaking and various anaerobic treatments on the aroma quality of gabaron oolong tea (GAOT) by chemical and sensory evaluation. The results showed that elevated anaerobic treatment harmed GAOT aroma, emphasizing undesirable attributes such as earthy, fatty, etc. A total of 85 volatiles were identified by gas chromatography-ion mobility spectrometry (GC-IMS), and the relationship between aroma attributes and volatiles were revealed by PLS regression projection and correlation network. Hexanal and octanal at inappropriate concentrations were main causes to the earthy attribute, while nonanal exhibited a potential masking effect against unpleasant attributes. Addition experiments and σ-τ plot analysis verified these associations. Furthermore, observing dynamic patterns of content changes of these three aldehydes in fresh leaves prior to tea thermal processing, providing references for future process optimization. These results provide a new direction for enhancing the quality of GAOT.
研究领域:
食品科学
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茶叶加工学
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化学分析
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Chunzheng Wu,Jingyuan Lin,Zhuojiong Xie,Xuan Kai,Xiao Yu,Zhenyu Yan,Jinwei Fang,Shanliang Chen,Jianzhong Guo,Wei Wang,Fengping Peng
Temperature fluctuations caused by sunlight represent a form of low-quality thermal energy that is generally insufficient for driving chemical reactions. Here, we designed a ZnO–MXene (Ti3C2) heterostructure catalyst, which can harvest solar near-infrared (NIR) energy to drive the sluggish ammonia production reaction using water and N2 as the feedstock. Our research confirmed that ammonia was produced through a pyroelectric process, rather than a photocatalytic process. The ZnO–MXene heterostructure with ∼20 wt% of Ti3C2 exhibited a 6.5-fold improvement in activity compared to bare ZnO. The Ti3C2 not only harvests NIR energy to heat up the pyroelectric ZnO, but also traps the pyro electrons from ZnO and co-catalyzes the reduction of N2 to ammonia. This work offers a novel strategy for ammonia production utilizing the abundant solar NIR energy under ambient conditions.
研究领域:
材料科学
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催化化学
·
能源利用
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DOI
高影响因子
Nano Energy
·
2020
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IF 16.602
Zhenqing Zhao,Changhyeok Choi,Song Hong,Huidong Shen,Chao Yan,Justus Masa,Yousung Jung,Jieshan Qiu,Zhenyu Sun
Solar N 2 fixation under visible light offers a promising method toward sustainable NH 3 production at benign conditions. However, it still remains a formidable challenge to activate and cleave N N bonds and promote the separation and transport of electrons and holes during photocatalysis . To address these issues, the discovery and design of high-performance and robust photocatalysts is imperative. Here, we report the defect engineering of two-dimensional oxidized Sb nanosheets to activate intrinsically inactive Sb for efficient visible light-driven N 2 reduction to NH 3 . Impressively, the Sb nanosheets rich in Sb and oxygen vacancies afford a remarkable NH 3 formation rate of up to 388.5 μg NH3 h −1 g cat. −1 without cocatalyst in visible light, 8 times higher than that for bulk Sb and also significantly outperforming many previously reported photocatalysts. The defective Sb nanosheets exhibit excellent stability after five successive reaction cycles. Further density functional theory calculations reveal a considerably strong interaction between N 2 and defects on the surface and edge of Sb nanosheets , which facilitates the formation of *NNH (N 2 + (H + + e - ) → *NNH, where * denotes an adsorption site), thus promoting photocatalytic N 2 reduction. This finding opens a novel avenue to enhancing N 2 photofixation over inherently inactive surfaces by synergistically engineering defect sites.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Hao Du,Changzhu Yang,Wenhong Pu,Lingyu Zeng,Jianyu Gong
Electrochemical reduction of N2 reaction (NRR) into NH3 promises a sustainable and environmentally friendly technology at ambient temperature. However, high energy barrier and the competition with the hydrogen evolution reaction result in poor NH3 yield and low faradaic efficiency (FE) of NRR. Herein, the FeS2 catalyst was synthesized via a one-step hydrothermal method for NRR. In the N2-saturated Na2SO4 electrolyte, this catalyst exhibited superior catalytic performance to achieve a high NH3 yield (37.2 μg h–1 mgcat.–1) and FE (11.2%) with high stability and selectivity at −0.5 V versus the reversible hydrogen electrode, outperforming other NRR catalysts. According to experimental results, a preferable associative distal pathway was proposed. Density functional theory calculations revealed that the NRR process can proceed preferably on Fe atoms instead of S atoms, and the conversion of *NH2 to *NH3 was the potential-determining step with an energy barrier of 0.45 eV. Therefore, this work offers a new avenue to prepare high-efficiency and highly selective transition-metal-based catalysts for NRR under ambient conditions.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
Processes
·
2023
·Vol. 12
·期 1
·64
·
IF 3.5
Zehui Zhao,Guangmin Ren,Xiangchao Meng,Zizhen Li
In order to achieve efficient photocatalytic N2reduction activity for ammonia synthesis, a photochemical strategy was used in this work. UiO-66 was prepared through the solvothermal method and further loaded with Au nanoparticles (Au NPs) onto the UiO-66 (Zr) framework. The experimental results verified that there were metal–support interactions between Au NPs and UiO-66; this could facilitate charge transfer among Au NPs and UiO-66, which was beneficial to enhance the photocatalytic activity. The best N2fixation effect of Au/UiO-66 with a loading of 1.5 wt% was tested, with a photocatalytic yield of ammonia of 66.28 μmol g−1h−1while maintaining good stability. The present work provides a novel approach to enhancing photocatalytic N2fixation activity by loading NPs onto UiO-66.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Naiyun Liu,Ruqiang Wu,Yixian Liu,Yunliang Liu,Peiji Deng,Yaxi Li,Yongchao Du,Yuanyuan Cheng,Zechao Zhuang,Zhenhui Kang,Haitao Li
Electrochemical nitrogen reduction reaction (NRR) is a promising method for ammonia synthesis under ambient conditions. However, the NRR performance is limited to an extremely strong N≡N bond in N2 and the competing hydrogen evolution reaction. Introducing oxygen vacancies (OVs) has been considered as a forceful means to accelerate the sluggish NRR reaction kinetics. Herein, we reported the design of Fe-doped NiMoO4 catalysts for NRR. Fe doping can increase the amount of OVs in the catalyst and contribute to lattice strain enhancement, thereby leading to the improvement of the electron transport rate and catalytic active for NRR. In 0.1 M Na2SO4 solution, the 5% Fe-NiMoO4 catalyst achieves a NH3 yield rate of 15.36 μg h–1 mgcat.–1 and a Faradaic efficiency of 26.85% under −0.5 V versus RHE. Furthermore, the 5% Fe-NiMoO4 catalyst exhibits excellent stability (up to 13 h) during the reaction.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xuan Tang,Yugao Wang,Mengni Wei,Xueqin Zhang,Ye Li,Xiaomin Li,Jinping Li,Jiangfeng Yang
Reduction of zeolite crystal size from the micron scale to the nanoscale leads to a significant increase in specific surface area, favoring mass-transfer pathways. Here, we have prepared nanoscale (ca. 30–80 nm) IM-5@100 zeolite (IMF type) by a facile strategy of regulating the amount of Al source in the starting gel, and have investigated its CH 4 /N 2 adsorption and separation properties. We found that on decreasing the amount of Al source, the crystal size of the product changed significantly, decreasing from strips of length about 1 μm to irregular nanocrystals. Compared with micron-sized IM-5@50, the mesopore volume of IM-5@100 was increased fourfold from 0.12 cm 3 /g to 0.49 cm 3 /g, its external surface area was increased from 38 m 2 /g to 118 m 2 /g, and its DFT pore size distribution based on N 2 adsorption/desorption showed a mesopore distribution in the range 5–10 nm. Adsorption kinetics tests showed that nano-IM-5@100 can achieve adsorption equilibrium more swiftly and exhibits better mass-transfer performance. Moreover, IM-5@100 showed good adsorption capacity for CH 4 (17.8 cm 3 /g) and high IAST selectivity (4.7) for CH 4 /N 2 (50:50, v/v). Breakthrough experiments have indicated that IM-5@100 permits efficient practical separation of CH 4 /N 2 .
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高影响因子
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