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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Unravelling intercalation-regulated nanoconfinement for durably ultrafast sieving graphene oxide membranes

Jing Guo,Hongfei Bao,Yanqiu Zhang,Xi Shen,Jang-Kyo Kim,Jun Ma,Lu Shao

Graphene oxide (GO) membranes with unique sieving channels composing of galleries in stacked GO nanosheets , are promising for advanced separations towards environmental and energy remediation. Although GO membranes can be bridged by molecules to enhance the stability as well as separation capacity, the subtle alterations of GO stacking and the resulting changes of sieving channel structures induced by molecular intercalation failed to be delicately revealed. Herein, molecular intercalations are employed to generate spatial confinement on GO assembling and thus the structures of sieving channels are regulated. Moreover, different-sized intercalants are demonstrated display significant effects on GO stacking. Small-sized molecules facilitate in-plane orientation while large-sized molecules are inclined to inhibit the overlap, leading to a lower degree of alignment and a shorter transmembrane pathway and eventually a higher permeability. On this basis, the deliberately nanostructured GO membrane with both the superior robustness even under ultrasonication and an ultrafast water permeance surpassing 5 times than pristine GO membrane, is built by intercalation with optimal-sized molecules. This study provides the practical insights on realizing 2D GO material for cutting-edge separations.

研究领域: 环境科学 · 材料科学
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Journal of Energy Storage · 2024 · IF 8.9

Organic molecular intercalation regulated hydrated vanadate cathodes with improved electrochemical properties and fast kinetics for aqueous zinc-ion batteries

Chaoqun Yi,Linlin Chen,Chenqi Ping,Ruihan Zhang,Caifu Dong,Yaoguo Huang,Ming Wang,Yali Zhang

Due to the large hydrated zinc ion radius resulting from the stable solvation structure with six water molecules in electrolyte, the interlayer spacing of most vanadium-based materials fails to meet the requirements for efficient insertion and extraction of Zn 2+ . Therefore, it is crucial to optimize and reconstruct the V O layer structure in order to achieve rapid and stable zinc storage. In this paper, composites of phenylalanine methyl ester (PM) inserted hydrated V 2 O 5 (PMVO) are prepared using a one-step hydrothermal method. With the increase of PM insertion, the electrochemical properties initially exhibit enhancement followed by subsequent decline. Notably, PMVO-1.6 presents exceptional electrochemical performance, including a high capacity of 464 mAh g −1 at 0.1 A g −1 , excellent rate capability with 220 mAh g −1 at 7 A g −1 , and superior cycling stability with 97.5 % capacity retention after 1000 cycles at 4 A g −1 . The incorporation of PM not only serves as stable structural pillars, but also reduces the solubilization of vanadium, facilitates the diffusion kinetics of hydrated zinc ions, and enhances the surface pseudo-capacitance effect.

CAS / MDL: 7524-50-7
研究领域: 材料科学 · 电化学 · 能源存储
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Advanced Science · 2024 ·Vol. 11 ·期 23 ·2309171 · IF 14.3

Reversible Constrained Dissociation and Reassembly of MXene Films

Xuefeng Zhang,Xudong Liu,Qingqiang Liu,Yufa Feng,Si Qiu,Ting Wang,Huayu Xu,Hao Li,Liang Yin,Hui Kang,Zhimin Fan

Enabling materials to undergo reversible dynamic transformations akin to the behaviors of living organisms represents a critical challenge in the field of material assembly. The pursuit of such capabilities using conventional materials has largely been met with limited success. Herein, the discovery of reversible constrained dissociation and reconfiguration in MXene films, offering an effective solution to overcome this obstacle is reported. Specifically, MXene films permit rapid intercalation of water molecules between their distinctive layers, resulting in a significant expansion and exhibiting confined dissociation within constrained spaces. Meanwhile, the process of capillary compression driven by water evaporation reinstates the dissociated MXene film to its original compact state. Further, the adhesive properties emerging from the confined disassociation of MXene films can spontaneously induce fusion between separate films. Utilizing this attribute, complex structures of MXene films can be effortlessly foamed and interlayer porosity precisely controlled, using only water as the inducer. Additionally, a parallel phenomenon has been identified in graphene oxide films. This work not only provides fresh insights into the microscopic mechanisms of 2D materials such as MXene but also paves a transformative path for their macroscopic assembly applications in the future.

CAS / MDL: 7664-39-3
研究领域: 材料科学 · 纳米技术
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Degradation and detoxification of propranolol by a molecular intercalation bismuth oxychloride semiconductor-organic framework

Runren Jiang,Guanghua Lu,Ranran Zhou,Tianjian Dang,Min Wang

In this work, the effects of different types of molecular intercalations on the morphology, photoelectrochemical performance, specific surface area and photocatalytic degradation propranolol (PRO) of BiOCl semiconductor-organic frameworks were studied by using different types of carbonate beverages (CBs) as solvents synthesized at room temperature. Interlayer organic molecules, as circuits of charge transmission can increase the strength of the electric field of the BiOCl layered structure and enhance the electronic coupling between layers. This, in turn, gives rise to narrowed bandgap energy and inhibited charge carrier recombination. Sugar (including fructose and glucose) molecules in the CB are helpful to insert into the BiOCl layer to make the thickness thinner, thus improving the specific surface area and light absorption capacity of BiOCl. Additionally, caramel molecules in CB can help broaden the light absorption and accelerate the charge transfer capacity of CB-BiOCl. The interaction of various molecules in the CB-BiOCl system significantly enhanced the photocatalytic degradation performance of PRO. Noticeably, twelve possible degradation intermediates were identified, and their toxicity decreased along with the degradation pathways. More importantly, the inhibiting effect of the degradation solution on zebrafish swimming activity weakened during the degradation process, indicating that the toxicity of the degradation solution gradually weakened. Furthermore, the mechanism of photocatalytic degradation of PRO with molecules as the circuit of charge transmission of the BiOCl semiconductor-organic framework was proposed.

研究领域: 环境科学 · 材料科学 · 生物学
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Small · 2024 · IF 13

Controllable Design of Metal-Organic Framework-Derived Vanadium Oxynitride for High-Capacity and Long-Cycle Aqueous Zn-Ion Batteries

Yuexin Liu,Jing Zhang,Yuan Liu,Mingcheng Zhang,Zhenghui Pan,Kefeng Cai

Introducing N atoms in vanadium oxides (VO x ) of aqueous Zn-ion batteries (ZIBs) can reduce their bandgap energy and enhance their electronic conductivity, thereby promoting the diffusion of Zn 2+ . The close-packed vanadium oxynitride (VON) generated often necessitates the intercalation of water molecules for restructuring, rendering it more conducive for zinc ion intercalation. However, its dense structure often causes structural strain and the formation of by-products during this process, resulting in decreased electrochemical performance. Herein, carbon-coated porous V 2 O 3 /VN nanosheets (p-VON@C) are constructed by annealing vanadium metal-organic framework in an ammonia-contained environment. The designed p-VON@C nanosheets are efficiently converted to low-crystalline hydrated N-doped VO x during subsequent activation while maintaining structural stability. This is because the V 2 O 3 /VN heterojunction and abundant oxygen vacancies in p-VON@C alleviate the structural strain during water molecule intercalation, and accelerate the intercalation rate. Carbon coating is beneficial to prevent p-VON@C from sliding or falling off during the activation and cycling process. Profiting from these advantages, the activated p-VON@C cathode delivers a high specific capacity of 518 mAh g −1 at 0.2 A g −1 and maintains a capacity retention rate of 80.9% after 2000 cycles at 10 A g −1 . This work provides a pathway to designing high-quality aqueous ZIB cathodes.

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

Small-molecule intercalation induces defective generation of bromine-doped bismuth oxychloride to enhance photocatalytic degradation and detoxification of tetracycline

Jianchao Liu,Yihao Qin,Guanghua Lu,Runren Jiang

Photocatalysts are one of the effective methods to degrade antibiotic contamination, but the efficiency is low and the toxicity is not well recognized. Deep lattice doping to induce defect generation is an effective way to improve the performance of photocatalysts. Here, defect-rich bromine-doped BiOCl-XBr photocatalysts were constructed with the help of small molecules inserted into the interlayer. The photocatalytic degradation performance of BiOCl-XBr was significantly enhanced, and its degradation rate was up to about 12 times that of BiOCl monomer. The main reasons for the stronger photocatalytic performance of BiOCl-XBr include Br doping to enhance visible light absorption, surface defects, and Bi valence changes to improve charge transport. The degradation of tetracycline (TC) produced more toxic intermediates, and the biotoxicity experiments also confirmed that the toxicity showed a trend of increasing and then decreasing, indicating that the more toxic intermediates were also mineralized during the degradation process. However, the mortality and hatching rate of zebrafish in the exposed group after degradation recovered but changed their activity pattern under light and dark conditions. This further warns us to focus on the toxicity changes after antibiotic degradation. Finally, based on the free radical analysis, the mechanism of photocatalytic degradation and detoxification of TC by BiOCl-XBr was proposed.

研究领域: 环境科学 · 材料科学 · 生物学
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Advanced Materials Technologies · 2022 ·Vol. 7 ·期 12 ·2200158 · IF 8.856

Intercalation of Small Organic Molecules into Ti3C2Tx MXene Cathodes for Flexible High-Volume-Capacitance Zn-Ion Microsupercapacitor

Weijia Liu,La Li,Chuqiao Hu,Di Chen,Guozhen Shen

The delamination of 2D Ti 3 C 2 T x MXene endows the injection of various ions and small organic molecules into its layers, thus leading to a tunable distance between layers and adjustable electrochemical properties. A suitable selection of intercalators needs to be considered according to the relevant metal-ion-based energy storage device because of the different radii of metal ions such as Li + , Na + , Mg 2+ Zn 2+ , etc. Herein, the intercalation of N , N -dimethylacetamide (DMAC), acetonitrile (ACN), dimethyl sulfoxide (DMSO), LiCl (H 2 O) into Ti 3 C 2 T x cathodes and their electrochemical performance comparisons by fabricating Zn-ion microsupercapacitors (MSCs) is reported. Studies found that an increased calculated interlayer space of 3.42, 7.47, 7.79, 8.3 Å is obtained for the H 2 O, DMSO, ACN, DMAC intercalated Ti 3 C 2 T x cathodes, and a decreased calculated binding energy of −0.03, −0.78, −1.91, and −3.06 eV is obtained for the Ti 3 C 2 T x -H 2 O, Ti 3 C 2 T x -DMSO, Ti 3 C 2 T x -ACN, and Ti 3 C 2 T x -DMAC, respectively. The highest interlayer space, lowest binding energy, and amide groups make the DMAC intercalated Ti 3 C 2 T x - based MSC exhibit volumetric capacitance of 1873 F cm −3 at a scan rate of 5 mV s −1 , much higher than 1103 F cm −3 for Ti 3 C 2 T x -H 2 O, 1313 F cm −3 for Ti 3 C 2 T x -ACN, 544 F cm −3 for Ti 3 C 2 T x -DMSO. The superior flexibility that results in invariable capacitance under 5000 bending cycles, together with the lighting test of the fabricated MSC, demonstrates its application in the wearable integrated system.

研究领域: 材料科学 · 能源存储 · 电化学
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Advanced Materials Technologies · 2022 ·Vol. 8 ·期 5 ·2201465 · IF 8.856

Single-Crystalline Layered Metal-Halide Perovskite Microwires with Intercalated Molecules for Ultraviolet Photodetectors

Rudai Zhao,Ting Zhang,Shiheng Wang,Lutong Guo,Zhenkun Gu,Yiqiang Zhang,Yanlin Song

Intercalation regulation is a special way to tune the photophysical properties of perovskite without changing the organic cations. Here, it is found that dimethyl sulfoxide can be effectively intercalated into synthesized (OHC 6 H 5 CH 2 CH 2 NH 3 ) 2 PbBr 4 perovskite through hydrogen bonds between organic spacer layers and solvent molecules. The new intercalated perovskite can be stored for more than two months under a relative humidity of about 60% at room temperature without encapsulation. The single crystal microwire array device based on this special structure presents photoelectric response of a light on/off ratio of 400 under 365 nm irradiation at 3 V. The device has a low dark current of 10 −13 A. Moreover, the inserted solvent molecules can be removed from the perovskite or reinserted into the perovskite under different processing conditions. The results show the potential to regulate the optoelectronic properties of perovskites by reversibly binding intercalated molecules with perovskites.

CAS / MDL: 10031-22-8
研究领域: 材料科学 · 光学工程
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