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INORGANICA CHIMICA ACTA · 2024 · IF 2.7

Highly efficient iodine capture from vapor and water using UiO-66-X: Effects of functional group modifications

Guang-Li Zhou,Bo-Wen Liu,Guang-Yu Cui,Wei Zhang,Ji-Min Yang

Radioactive iodine waste from the nuclear industry poses a critical threat to human health, and its effective capture has become an important research topic. In this study, modified UiO-66-X adsorbents (where X is ATA, BTA, or STA) were used to investigate the effects of the free functional groups in the UiO-66 skeleton on iodine capture in the vapor and solution states. The adsorption behavior revealed that the capture efficiency of UiO-66-ATA was substantially higher than that of UiO-66-BTA and UiO-66-STA because the electron-donating amino groups could enhance the I − I···π halogen bond interactions compared with the electron-withdrawing carboxyl and sulfonic acid groups. In addition, the pore volume of UiO-66-ATA was significantly higher than those of UiO-66-BTA and UiO-66-STA. In particular, the removal uptakes of UiO-66-ATA were 1108.1 mg/g (vapor phase) and 3601.9 mg/g (aqueous solution). This study is the first to investigate the effects of functional groups on the adsorption uptake of UiO-66 toward iodine. This efficient functional group modification strategy holds significant promise for the development of novel metal–organic framework adsorbents.

研究领域: 材料科学 · 环境科学 · 核能工程
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Vapor-phase polymerization of fibrous PEDOT on carbon fibers film for fast pseudocapacitive energy storage

Xiaoyan Zhu,Xiying Han,Rui Guo,Peng Yuan,Liqin Dang,Zonghuai Liu,Zhibin Lei

Poly(3,4-ethylenedioxythiophene) (PEDOT) has emerged as one of promising conductive polymers in energy storage devices. However, the conventional solution oxidative polymerization usually produces PEDOT with low conductivity and limited surface area. This work reports the preparation of highly conductive fibrous PEDOT by a vapor-phase polymerization initialized with Fe 2 O 3 nanosheets that are uniformly electrochemically deposited on the N-doped carbon nanofibers (CNFs) film. The incorporation of highly conductive PEDOT nanofibers expands the film and simultaneously increase the film conductivity by 80 times (103 S cm −1 ). Accordingly, an areal capacitance of 1926 mF cm −2 at 5 mA cm −2 with a PEDOT mass loading of 8.68 mg cm −2 has been achieved. Importantly, the fast pseudocapacitive charge storage mechanism afford the CNF-PEDOT a high-rate capability which retains 68% capacitance in 5–50 mA cm −2 . Especially, the CNF-PEDOT film electrode exhibits an outstanding stability with 87% capacitance retention after 10,000 consecutive charging and discharging cycles at 50 mA cm −2 . A CNF-PEDOT-based supercapacitor delivers an energy density of 97 μWh cm −2 at power density of 0.45 mW cm −2 , surpassing state-of-the-art PEDOT-based devices. This work will open a new avenue for preparing highly conductive PEDOT hybrid electrodes towards high-performance supercapacitors.

CAS / MDL: 126213-50-1 25014-41-9
研究领域: 材料科学 · 能源存储
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SYNTHETIC METALS · 2020 · IF 3.286

Controllable vapor phase polymerization of PEDOT films using imidazole as an inhibitor and their electrical and electrochromic properties

Wei Wang,Di Xu,Aibin Huang,Huihui Yuan,Junjie Xie,Xinyu Chen,Yunlong He,Tao Zhang,Hujiang Shen

PEDOT films were fabricated by vapor-phase polymerization (VPP) with different inhibitor contents in oxidant-containing solutions, and were characterized by X-ray diffraction, Raman spectroscopy, UV/vis transmittance spectra, atomic force microscopy, electrical conductivity and electrochromic measurements. The imidazole which serves as an inhibitor plays key roles on the polymerization reaction, and varying its content results in drastically different properties of the PEDOT films. In the imidazole/Fe(III) p -toluenesulfonate (Im/Fe) weight ratio range of 0∼0.25, the rate of polymerization can be significantly slowed down by increasing the Im/Fe ratio. The optimum Im/Fe ratio of 0.1 and polymerization time of 3 h results in PEDOT films with the highest conductivity on glass substrate (626 S/cm). Higher doping level is found in PEDOT films fabricated with the Im/Fe ratio above 0.1, causing low conductivity due to their loose morphology. The electrochromic properties of the films can be enhanced by prolonging the polymerization time to 3 h. It is found that the transmittance difference at 550 nm is above 10 % in PEDOT films fabricated with 3 h of polymerization. An electrochromic device is assembled and its coloring time is less than 3 s.

CAS / MDL: 126213-50-1 288-32-4
研究领域: 材料科学 · 化学工程
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Nanomaterials · 2019 ·Vol. 9 ·期 12 ·1688 · IF 4.034

Ni-Based Catalyst Derived from NiAl Layered Double Hydroxide for Vapor Phase Catalytic Exchange between Hydrogen and Water

Xiaoyu Hu,Peilong Li,Xin Zhang,Bin Yu,Chao Lv,Ning Zeng,Junhong Luo,Zhi Zhang,Jiangfeng Song,Yong Liu

A high-efficient and low-cost catalyst on hydrogen isotope separation between hydrogen and water is an essential factor in industrial application for heavy water production and water detritiation. In past studies, Pt-based catalysts were developed but not practical for commercial use due to their high cost for vapor phase catalytic exchange (VPCE), while for impregnated nickel catalysts with a lower cost the problems of agglomeration and low Ni utilization existed. Therefore, to solve these problems, in-situ grown Ni-based catalysts (NiAl-LDO) derived from a layered double hydroxide (LDH) precursor were fabricated and first applied in VPCE in this work. Compared with traditional impregnated Ni-based catalysts, NiAl-LDO catalysts own a unique layered structure, homogeneous dispersed metallic phase, higher specific surface area as well as stronger metal-support interactions to prevent active metal from agglomerating. These advantages are beneficial for exposing more active sites to improve dynamic contacts between H2and HDO in a catalyst surface and can bring excellent catalytic activity under a reaction temperature of lower than 400 °C. Additionally, we found that the dissociative chemisorption of HDO and H2occurs not only in Ni (111) but also in NiO species where chemisorbed H(ads), D(ads), OH(ads) and OD(ads) are formed. The results highlight that both of the Ni2+species and Ni0species possess catalytic activities for VPCE process.Keywords:vapor phase catalytic exchange;layered double oxides;Ni catalyst;water detritiation

研究领域: 化学工程 · 核化学与化工
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CARBOHYDRATE POLYMERS · 2022 · IF 10.723

A universal construction of robust interface between 2D conductive polymer and cellulose for textile supercapacitor

Jun Wan,Rong Hu,Junfeng Li,Shiyun Mi,Jinglin Xian,Zhiheng Xiao,Ziyang Liu,Aojie Mei,Siqi Xu,Mingzhao Fan,Huiyu Jiang,Qian Zhang,Huihong Liu,Weilin Xu

Conductive polymer (CP) fabric is considered as the ideal electrode for flexible energy storage due to its light weight, good flexibility and high energy storage properties. However, the conventional polymer-coated cellulose fiber synthesized by liquid-phase oxidation polymerization always forms disordered assembly of polymer particles on fiber, which endures poor mechanical stability. Here, we report a two-dimensional (2D) CP based fabric electrode realized by a salt-template assisted vapor-phase polymerization method, which achieves robust coating of 2D CP on various cellulose fibers. Typically, the prepared 2D polypyrrole@cotton electrode displays a high specific capacitance (902.6 mF cm −2 ) and good cycling stability (86.5% capacitance retention after 12,000 cycles). The capacitance of flexible symmetrical device retains at more than 90% when it is bent to 180° after 1000 bending cycles. This work provides a new strategy for the robust interface between functional materials and cellulose fibers, and has great potential for commercial mass production.

CAS / MDL: 109-97-7 9002-89-5
研究领域: 材料科学 · 能源存储
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JOURNAL OF SOLID STATE CHEMISTRY · 2024 · IF 3.2

The effective adsorption separation of n-hexane/3-methylpentane by Vapor-Phase linker exchange of Zeolitic-Imidazolate Framework ZIF-8

Le Chen,An Xie,Nan Zhang,Jianjun Yin,Qun Chen,Mingyang He,Zhihui Zhang

Zeolitic-Imidazolate Framework 8 (ZIF-8), a porous crystalline absorbent, could be synthesized from the coordination reaction of zinc ions and 2-methylimidazole (2-mIM). ZIF-8 has a large specific surface area and a high adsorption capacity for n -hexane ( n HEX). However, ZIF-8 suffers from low selectivity for both linear and mono-chain alkanes. Therefore, ZIF-8 was modified through 2-mIM ligand being partly replaced by 2-nitroimidazole (2-nIM) through Vapor-Phase post-synthesis modification. The modified materials were denoted as ZIF-8-2-nIM-X (X = 24h, 48h, 72h). ZIF-8-2-nIM-X has a higher specific surface area and better thermal stability than ZIF-8. Further thermodynamic and kinetic calculations show that the affinity of hexane isomers on ZIF-8-2-nIM-X is spontaneous physical adsorption combined with an exothermic process. In contrast, kinetic studies show that the adsorption of hexane isomers on ZIF-8-2-nIM-X is a pseudo-second-order kinetic model. The batch and dynamic adsorption and separation properties of ZIF-8-2-nIM-X for hexane isomers were studied. The results of the one-component vapor adsorption equilibrium experiment show that ZIF-8-2-nIM-72h has the best adsorption separation coefficient at 293 K. The adsorption capacity of n HEX and 3-methylpentane (3MP) were 211.63 mg/g and 33.91 mg/g, respectively. Compared with ZIF-8 (selectivity coefficient: 1.08), the adsorption selectivity coefficient of the modified material is greatly improved. The adsorption selectivity coefficient of n HEX/3MP is 6.24 (ZIF-8-2-nIM-72h).

研究领域: 材料科学 · 物理化学
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Materials Today Energy · 2022 · IF 9.257

Incorporating highly dispersed alumina in PEO-based solid electrolytes by vapor phase infiltration for all-solid-state lithium metal batteries

Yue Zhang,Wenda Bao,Haoyuan Li,Lianqi Zhao,Beili Yi,Haojie Zhao,Yuqing Zuo,Longxing Su,Xincan Cai,Lingyu Liu,Jin Xie

Solid-state lithium-metal batteries with composite polymer electrolytes are promising for next-generation energy-storage devices. Typical synthesis strategies of preparing inorganic-polymer composite mainly focused on physical mixing of inorganic fillers with polymer or surface coating of inorganic thin films on polymer, which are hard to suppress Li-dendrite penetration. Here, we demonstrate the bulk and interface properties of powdery poly (ethylene oxide) can be modified simultaneously with highly dispersed alumina using a vapor phase infiltration (VPI) approach. The chemically synthesized alumina with under-coordinated aluminum sites shows strong interaction with PEO, and therefore highly dispersed in the polymer matrix as well as on the surface of the polymer. On the lithium metal anode side, it reduces the interfacial resistance and allows Li|Li symmetric battery to cycle more than 1400 h under 0.2 mAh/cm 2 . On the cathode side, it increases the electrochemical stability window of PEO up to 4.25V without compromising the charge transfer kinetics. The result shows the promise of using VPI as a facile one-step method to tune the properties of the polymer on a large scale for battery applications.

研究领域: 材料科学 · 电化学
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RSC Advances · 2016 ·Vol. 6 ·期 110 ·108217-108228 · IF 3.289

In situ synthesis of molybdenum oxide@N-doped carbon from biomass for selective vapor phase hydrodeoxygenation of lignin-derived phenols under H2 atmosphere

Lujiang Xu,Zheng Han,Ying Zhang,Yao Fu

The vapor phase hydrodeoxygenation (HDO) of lignin-derived phenols under H2 atmosphere has great significance for producing high-quality fuels and commodity chemicals. Herein, we reported a simple, green method to prepare molybdenum oxide@N-doped carbon (MoOx@NC) via in situ pyrolysis of molybdenum precursor preloaded cellulose and demonstrated its catalytic performance for vapor phase HDO of lignin-derived phenols. When the pyrolysis temperature was at 600 °C, the catalyst (MoOx@NC-600) exhibited the best catalytic performance in vapor phase HDO of guaiacol. Through systematically investigating the parameters, such as: reaction temperature, WHSV, residence time, and concentration, the optimal reaction conditions for vapor phase HDO of guaiacol were 450 °C and 1 h−1 with atmospheric H2. The concentration of the feed was 20% in mesitylene, and the residence time was about 3.3 s. The carbon yield of aromatic hydrocarbons was 83.3%, with 65.7% benzene, 15.5% toluene and 2.1% alkylbenzenes. In addition, other lignin-derived phenols were also investigated and desired results were achieved with the MoOx@NC-600 catalyst. Furthermore, MoOx@NC-600 showed good stability due to the N-doped carbon formed on the surface of the MoOx particles. The catalysts were characterized using elemental analysis, AAS, BET, XRD, XPS, TEM, and EDS mapping. The high catalytic performance of MoOx@NC-600 toward lignin-derived phenols HDO can be attributed to the synergistic effect of the carbon supports and Mo5+ (molybdenum oxynitrides), Moδ+ (Mo2N) and Mo4+ on the surface of the MoOx particles.

CAS / MDL: 97-53-0 103-65-1
研究领域: 化学工程 · 催化材料
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MACROMOLECULAR RAPID COMMUNICATIONS · 2022 ·Vol. 43 ·期 20 ·2200347 · IF 5.006

Re-Stickable Yarn Supercapacitors with Vaper Phase Polymerized Multi-Layered Polypyrrole Electrodes for Smart Garments

Chen Zhao,Tao Wan,Wenxiong Yuan,Zhaoqiang Zheng,Xiaoteng Jia,Kewei Shu,Lei Feng,Yonggang Min

Yarn supercapacitors have attracted significant attention for wearable energy storage due to their ability to be directly integrated with garments. Conducting polymer polypyrrole (PPy) based yarn supercapacitors show limited cycling stability because of the huge volume changes during the charge–discharge processes. In addition, laundering may cause damage to such yarn supercapacitors. Here, the fabrication of PPy-based re-stickable yarn supercapacitors is reported with good cycling stability by employing vapor phase polymerization (VPP) and water-soluble polyethylene oxide (PEO) film as the adhesive layer. VPP duration and cycle are controlled to achieve multi-layered PPy electrodes. The assembled yarn supercapacitors show a good cycling stability with capacitance retention of 79.1% after 5000 charge–discharge cycles. The energy stored in the yarn supercapacitor is sufficient to power a photodetector. After gluing the yarn supercapacitors onto a PEO film, the devices can be stunk on and peeled off the garment to avoid the mechanical stresses during the washing process. Three yarn supercapacitors connected in parallel on PEO film show negative changes in electrochemical performance after 5 sticking-peeling cycles. This work provides a facile way to fabricate PPy-based re-stickable energy storage devices with high cycling stability for smart garments.

CAS / MDL: 109-97-7
研究领域: 材料科学 · 能源存储 · 纺织工程
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CRYSTAL GROWTH & DESIGN · 2014 · IF 4.558

Hollow SAPO-34 Cubes with Hierarchically Organized Internal Structure

Jie Gong,Fei Tong,Xiaobo Ji,Changfeng Zeng,Chongqing Wang,Yinong Lv,Lixiong Zhang

We herein report novel hollow SAPO-34 cubes with a hierarchical internal structure. They are prepared from dry gels containing gelatin by a vapor-phase transport method. Microscopic characterization reveals that the cubes are constructed by symmetrically packed four two-top-point truncated octahedrons encapsulated by dense crystalline shells, exhibiting a structure-in-structure formation. The cubes show either +-shaped or the butterfly like X-shaped black spots on their faces under light. Investigation of the formation process of the hollow SAPO-34 cubes demonstrates a surface to core crystal growth route, which has not been found in vapor-phase transport synthesis of zeolites. A possible formation mechanism is proposed.

研究领域: 材料科学 · 化学工程
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Inorganic Chemistry Frontiers · 2021 ·Vol. 8 ·期 23 ·5016-5023 · IF 6.569

A binary all-nanoporous composite membrane constructed via vapor phase transformation for high-permeance gas separation

Mengqi Bu,Yang Feng,Qingxun Li,Yiran Wang,Shou Feng,Kai Zhang,Yujie Jiang,Lili Fan,Zixi Kang,Daofeng Sun

Metal–organic framework (MOF) membranes with an ultra-small pore size (<4 Å) have shown great prospects in the highly selective separation of small gas molecules such as hydrogen, but their narrow channels may result in a low gas permeance. To improve the gas permeance of ultra-microporous MOF membranes, a stable covalent organic framework (COF) with large and uniform pores is doped to construct a binary COF/MOF all-nanoporous composite (ANC) membrane, equivalent to reducing the effective membrane thickness but avoiding the challenging ultra-thin membrane preparation. The COF synthesized by ball milling is combined with a metal gel to form a precursor membrane, which was then transformed to a COF/MOF ANC membrane by treatment with the MOF ligand vapor. A very small amount of solvent has been applied, offering an environmentally-friendly preparation process. Compared with the pristine MOF membrane, the COF/MOF ANC membranes possess a highly improved gas permeance from 22 GPU to 551 GPU with a slight sacrifice of selectivity; this introduces a new strategy to optimize the separation performance of MOF membranes.

CAS / MDL: 109-86-4
研究领域: 材料科学 · 化学工程
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