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FOOD CHEMISTRY · 2021 · IF 7.514

Rational design of ultrahigh sensitive sunset yellow sensor based on 3D hierarchical porous graphitic carbon with sub-nanopores

Yajun Gao,Tingting Li,Tianyuan Zhang,Meiling Wang,Lu Gao,Zhenquan Yang,Zhanjun Yang

The content of sunset yellow (SY) in food must be strictly controlled, because its excessive intake may cause many adverse health effects. Herein, we proposed an ultrasensitive SY sensor by using hierarchical porous graphitic (HPG) carbon derived from polyaniline hydrogel. After a first step of polymerization, the HPG carbon was prepared through carbonization and further chemical activation. In particular, the activation process endowed the HPG carbon with a high content of optimized porous architecture (sub-nanoporous surface area accounts for more than 90% of microporous surface area), and thus providing a structural basis for high efficiency of SY pre-concentration on HPG carbon surface. Therefore, the proposed sensor showed record-high sensitivity (5285.7 A M −1 cm −2 ) and ultra-low detection limit (0.15 nM), which represents a performance improvement in SY sensing. Furthermore, the sensor displays excellent selectivity, reproducibility and stability, exhibiting a great perspective in ultrasensitive monitoring of SY in commercial products.

研究领域: 食品科学 · 材料科学 · 分析化学
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Covalent organic framework membrane with sub-nano pores for efficient desalination

Zhichao Li,Yu Zheng,Tianrun Gu,Xiangxuan Meng,Hui Wang,Kai Xu,Lijuan Cheng,Roni Kasher,Runnan Zhang,Zhongyi Jiang

Covalent organic frameworks (COFs) have emerged as advanced membrane materials for molecular separations, but it is rarely used for desalination due to the mismatch between the COFs pore size (1−5 nm) and the diameter of hydrated ions (<1 nm). Herein, we designed and fabricated an imide-linked TbTG COF membrane (COFM) with intrinsic sub-nano pores. The TbTG nanosheets were prepared by interfacial polymerization, and then self-assembled into COFMs on the porous PAN substrate. The sub-nano pore size (∼0.4 nm by simulation) conferred excellent size sieving capacity to the TbTG COFM with the molecular weight cut-off of only 180 Da, which was the lowest among COFMs ever reported. Moreover, the positive charge on the skeleton of TbTG COFM greatly fortified the Donnan effect. The TbTG COFM exhibits excellent salt rejections of 98.7% to Na 2 SO 4 , 99.1% to MgSO 4 , 99.5% to MgCl 2 and 93.3% to NaCl, respectively. The TbTG COFM also maintained high salt rejections under both high salt concentration up to 10000 ppm and high pH value of 9.4, showing great potential in seawater desalination applications.

研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Rapid synthesis of ultrathin covalent organic polymer membranes with subnanometer pores for efficient organic solvent nanofiltration

Jianghai Long,Xiansong Shi,Tong Ju,Xingyuan Wang,Zhe Zhang,Yong Wang

Covalent organic polymers (COPs) with abundant micropores are deemed as promising materials for building molecular separation membranes . In spite of this potential, fabricating COP separation membranes through an efficient and scalable method remains a significant challenge. Herein, we report a simple and efficient strategy for the synthesis of COP membranes with three-dimensionally interconnected micropores. Utilizing transition-metal nitrates as a catalyst, we achieve fast polymerization of amorphous COPs with relatively uniform micropores (0.7 nm in diameter). The rational design of organic-aqueous interface allows for the direct fabrication of robust COP membranes with an ultrathin thickness of ∼20 nm on porous polyacrylonitrile substrates. The resulting hydrophobic but pore-uniform frameworks in these membranes permit fast permeation of organic liquids with a notable molecular weight cutoff of 388 g mol −1 in ethanol. To demonstrate scalability, we show that our strategy can produce large-size COP membranes with a prominent area of 200 cm 2 , which exhibit performances similar to that of small membrane coupons. The present study offers a potentially scalable method for producing highly microporous COP membranes toward efficient molecular separation in organic liquids.

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

ZIF-8 derived carbon with confined sub-nanometer pores for electrochemically selective separation of chloride ions

Jie Qiao,Wenbiao Ma,Xiao Du,Xuli Ma,Zhong Liu,Jun Li,Guoqing Guan,Abuliti Abudula,Xiaogang Hao

Selective ion separation from aqueous solution is challenging and crucial for water purification. In this work, zeolitic imidazolate framework (ZIF-8) derived nano-porous carbon (NC-X-A) with confined sub-nanometer pores was synthesized by acid leaching and alkali activation after the carbonization of ZIF-8 precursor for the selective electrochemical separation of chloride ions (Cl − ). Here, the uptake capacity and selectivity of Cl − were improved by changing the carbonization temperature to tune the specific surface area and pore size. Based on the size confinement effect and the difference in free energies of dehydration, the obtained optimum carbon film, i.e., NC-1000-A coated electrode, exhibited separation factors of 1.384, 1.952 and 2.970 for Cl − /Br − , Cl − /F − and Cl − /SO 4 2− , respectively. It also showed fast uptake/release ability with an uptake equilibrium time less than 90 min. The Cl − uptake capacity reached to 64.06 mg g −1 and retained 99.7% of its initial value even after 1000 uptake/release cycles due to its porous structure with high specific surface area, good electrical conductivity and extra electric driving force during the ESIX process. Thus, it is expected that this kind of carbon film would be applied as a promising electroactive material for the selective separation of Cl − from wastewater.

研究领域: 材料科学 · 环境科学 · 化学工程
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Pore Size Control via Multiple-Site Alkylation to Homogenize Sub-Nanoporous Covalent Organic Frameworks for Efficient Sieving of Xenon/Krypton

Zhimin Jia,Zhaotong Yan,Jie Zhang,Yingdi Zou,Yue Qi,Xiaofeng Li,Yang Li,Xinghua Guo,Chuting Yang,Lijian Ma

Among various fission products generated in nuclear reactors, xenon and krypton are two important fission gases with high flow, diffusivity, and radioactivity. Moreover, xenon isolated from these products is an expensive industrial resource with wide applications in medicine and lighting, which makes the development of efficient methods for separation of xenon/krypton significant. However, it is usually difficult for xenon/krypton to be adsorbed by chemical adsorbents due to their inert gas properties, and sub-nanoporous adsorbents proven to be workable for the separation of xenon/krypton are still hard to prepare and regulate the pore size. Herein, we report two novel sub-nanoporous covalent organic frameworks (COFs), which were applied to the sieving of xenon/krypton for the first time. The sub-nanoporous COFs were synthesized via aldehyde–amine polycondensation reactions and the subsequent pore size regulation and homogenization process by using a facile, operational, and efficient multiple-site alkylation strategy. Impressively, the as-prepared sub-nanoporous COFs realized the efficient adsorption and sieving of xenon/krypton owing to their slightly larger pore sizes (∼7 Å) than the dynamic diameters of xenon/krypton and their larger pore volumes. The maximum adsorption capacity for xenon is up to 85.6 cm3/g, and the xenon/krypton selectivity can reach to 9.7. Moreover, the as-prepared COFs possess good γ-ray irradiation stability, which endows them with great potentials for the sieving of radioactive xenon/krypton in the practical application. The multiple-site alkylation strategy proposed in this study provides a valuable approach for the pore construction and control of the porous materials, especially the sub-nanoporous adsorption materials.

研究领域: 材料科学 · 核工程 · 化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Sub-nanopores enabling optimized ion storage performance of carbon cathodes for Zn-ion hybrid supercapacitors

Fulian Kang,Yang Li,Zhiyuan Zheng,Xinya Peng,Jianhua Rong,Liubing Dong

Aqueous Zn-ion hybrid supercapacitors (ZHSs) are attracting significant attention as a promising electrochemical energy storage system. However, carbon cathodes of ZHSs exhibit unsatisfactory ion storage performance due to the large size of hydrated Zn-ions ( e.g. , [Zn(H 2 O) 6 ] 2+ ), which encumbers compact ion arrangement and rapid ion transport at the carbon-electrolyte interfaces. Herein, a porous carbon material (HMFC) with abundant sub-nanopores is synthesized to optimize the ion storage performance of the carbon cathode in ZHSs , in which the sub-nanopores effectively promote the dehydration of hydrated Zn-ions and thus optimize the ion storage performance of the carbon cathode in ZHSs . A novel strategy is proposed to study the dehydration behaviors of hydrated Zn-ions in carbon cathodes, including quantitatively determining the desolvation activation energy of hydrated Zn-ions and in-situ monitoring active water content at the carbon-electrolyte interface. The sub-nanopores-induced desolvation effect is verified, and its coupling with large specific surface area and hierarchically porous structure endows the HMFC cathode with improved electrochemical performance, including a 53 % capacity increase compared to the carbon cathode counterpart without sub-nanopores, fast charge/discharge ability that can output 46.0 Wh/kg energy within only 4.4 s, and 98.2 % capacity retention over 20,000 charge/discharge cycles. This work provides new insights into the rational design of porous carbon cathode materials toward high-performance ZHSs.

研究领域: 材料科学 · 电化学 · 能源存储
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DESALINATION · 2025 · IF 9.8

Electric-field-induced ultrafast and selective ZIF-8 filling in graphene membrane pores for precision dye desalination

Jialu Li,Zhonghao Xu,Yangdong He,Sheng Shi,Sihan Ye,Liyun Zhang,Lan Ma,Jian Zhen Ou,Hao Yu

Integrating metal-organic-frameworks (MOFs) into graphene oxide (GO) membranes offers a pathway toward stable and highly selective nanofiltration, yet conventional blending or precursor-diffusion-driven in situ growth compromise structural integrity and is prohibitively slow (∼36 h). Here, we report an electric-field-driven strategy that induces electrophoretic migration of Zn 2+ and 2-methylimidazole precursors, enabling ultrafast (<60 s) synthesis of ZIF-8 within the internal pores of ethylenediamine (EDA)-crosslinked GO-based membranes intercalated by arched graphene (WG). Growth is directed preferentially into high-permeability channels, sequentially plugging dominant and subdominant pores at a rate 2160 times faster than diffusion. This selective pore filling suppresses ZIF-8 overgrowth and minimizes structural disruption, while enhancing rejection performance. The resulting membrane exhibits exceptional dye rejection of 87.11 % (MB), 99.45 % (EBT), 97.39 % (CV), 99.21 % (CR), and 99.37 % (TB), surpassing pristine GO (36.90–91.07 %) and slightly outperforming diffusion-grown counterparts. Meanwhile, the intrinsic 0.7 nm pores of ZIF-8 permit nearly complete salt permeation (rejection <2.73 %), yielding practical dye/salt selectivity >8. Amine-functionalized ZIF-8 further promotes crosslinking, imparting remarkable stability: wet/dry interlayer spacing variation <1 Å and strong resistance to acid/base exposure, hydraulic flushing, and ultrasonication. This electric-field-guided, sub-nanopore engineering strategy thus establishes a generalizable platform for precision separation membranes using diverse substrates and porous framework.

CAS / MDL: 10034-96-5 7722-84-1
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Ion-Selective Micropipette Sensor for In Vivo Monitoring of Sodium Ion with Crown Ether-Encapsulated Metal–Organic Framework Subnanopores

Jiahao Liu,Jiahao Lu,Wenliang Ji,Guangwen Lu,Jiao Wang,Tingyan Ye,Yisha Jiang,Juanjuan Zheng,Ping Yu,Nannan Liu,Yanan Jiang,Lanqun Mao

In vivo sensing of the dynamics of ions with high selectivity is essential for gaining molecular insights into numerous physiological and pathological processes. In this work, we report an ion-selective micropipette sensor (ISMS) through the integration of functional crown ether-encapsulated metal–organic frameworks (MOFs) synthesized in situ within the micropipette tip. The ISMS features distinctive sodium ion (Na+) conduction and high selectivity toward Na+ sensing. The selectivity is attributed to the synergistic effects of subnanoconfined space and the specific coordination of 18-crown-6 toward potassium ions (K+), which largely increase the steric hindrance and transport resistance for K+ to pass through the ISMS. Furthermore, the ISMS exhibits high stability and sensitivity, facilitating real-time monitoring of Na+ dynamics in the living rat brain during spreading of the depression events process. In light of the diversity of crown ethers and MOFs, we believe this study paves the way for a nanofluidic platform for in vivo sensing and neuromorphic electrochemical sensing.

研究领域: 生物医学工程 · 神经科学 · 分析化学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Artificial bi-functional layers promoting Zn2+ desolvation and homogeneous deposition for reversible zinc metal anodes

Jiahao Chen,Miao He,Anjun Hu,Mengjiao Liu,Chuan Zhao,Bo Zhou,Runjing Li,Zhongfu Yan,Yu Pan,Yining Fan,Jing Liu,Liujun Cao,Jianping Long

Rechargeable aqueous zinc-ion hybrid supercapacitors (ZHSs) are drawing extensive attention because of their cost-effectiveness and diminished safety hazards. Nevertheless, large-scale application of ZHSs has been hindered by the severe side reactions and rampant dendrites growth on the surface of Zn metal anodes. Herein, we propose a three-dimensional organic–inorganic composite frame material as an artificial bi-functional layer coated on the zinc foil, featuring nitrogenous functional groups with zincophilicity (abbreviated as NCFM@Zn). The nitrogen (N) site's strong adsorption capacity and synergistic effect of the sub-nanopore size promote rapid desolvation of zinc ions and reduce side reactions, while also prolonging galvanized nucleation's Sand's time and allowing for even nucleation. Moreover, the uniform distribution of N on the layer results in homogeneous zinc ions flux and supports consistent zinc plating while inhibiting dendrites generation. As a result of this unique artificial bi-functional layer, symmetric Zn cells can survive 2500 h at 2.5 mA cm −2 . High-areal-capacity zinc||activated carbon hybrid supercapacitors also demonstrate 20,000 cycles at high Coulombic efficiency, thus highlighting the utter convenience and potential of this strategy for modifying rechargeable metal hybrid supercapacitor surfaces.

CAS / MDL: 693-98-1
研究领域: 材料科学 · 电化学 · 储能 · 超级电容器
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