ADVANCED FUNCTIONAL MATERIALS
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2023
·Vol. 33
·期 12
·2210122
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IF 19
Yuyan Lai,Junsheng Yang,Linkun Cai,Mingxin Zhang,Xiaofeng He,Haitao Yu,Mu Li,Guo-Hong Ning,Panchao Yin
Porous liquids (PLs) have improved the understanding of the porous properties of matter; however, rational tuning of the viscosities and gas absorption properties of PLs lag far behind the explosive growth of PL applications. Herein, neat molecular PLs are constructed by grafting polymers onto the surface of 2 nm molecular nanocages with precisely tuned graft densities and molecular weights M w s. The flowability of the PLs showed a non-monotonic dependence on the M w of the polymers due to the interplay between the surface confinement effect and polymer chain entanglements, enabling optimization of their viscosities, similar to those of conventional liquids. The surface layer dynamics and gas absorption kinetics are quantified, correlation between the two properties is confirmed, and gas permeation process is regulated by surface layer dynamics. From the understanding of the structure–property relationship, the surface layer grafting densities are tuned to promote surface layer dynamics to achieve improved gas sorption performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Wei Zhou,Liang Xie,Yan Wang,Yani Ding,Xiaoxiao Meng,Fei Sun,Jihui Gao,Guangbo Zhao
Large-scale application of H 2 O 2 production through 2-electron oxygen reduction reaction (2eORR) greatly depends on the cost of electrode materials and configuration. In this work, engineered coal-derived oxygen-rich hierarchical activated coke (AC), which is low-cost and highly tunable in porosity and surface chemistry, was used as catalyst to fabricate gas diffusion electrodes (GDEs) for efficient H 2 O 2 production. Results showed that Fenton’s reagents treatment could significantly increase the contents of C O and –COOH on AC, leading to an increased hydrophilicity. However, the higher O contents do not necessarily enhance the selectivity of AC towards 2eORR (i.e., F-5-AC, F-10-AC), especially that F-20-AC exhibited a complete 4e pathway. GDEs were then fabricated with AC and oxidized AC as catalyst, key fabrication parameters including the PTFE binder and AC particle size, and operating parameters such as current intensity, electrolyte pH, and O 2 flow rate were optimized. Up to 747 mg/L H 2 O 2 were generated within 90 min. Results showed that oxidized AC exhibited a decreased H 2 O 2 yield, due to the flooding of GDEs caused by super-hydrophilicity property. Finally, DFT calculations were employed to reveal the synergistic effect of different O groups considering the fact of high O contents on AC.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Bin Huang,Kuan Li,Qi-Yu Ma,Tuan-Xiu Xiang,Rui-Xue Liang,Ya-Nan Gong,Bang-Jin Wang,Jun-Hui Zhang,Sheng-Ming Xie,Li-Ming Yuan
Metallacycles are a novel class of supramolecular materials with circular structures, internal cavities, and abundant host–guest chemical properties that have exhibited good application prospects in many fields. However, to the best of our knowledge, no research on the use of metallacycles as stationary phases for gas chromatographic (GC) separations has been published yet. In this work, we report for the first time the use of a homochiral metallacycle, [ZnCl2L]2, as a stationary phase for GC separations. [ZnCl2L]2 was synthesized by reaction of (S)-(1-isonicotinoylpyrrolidin-2-yl)methyl-isonicotinate (L) with ZnCl2 via coordination-driven self-assembly. The [ZnCl2L]2-coated column displayed an excellent separation performance not only of organic isomers but also of racemic compounds. Sixteen racemates (including alcohols, esters, amino acid derivatives, ethers, organic acids, and epoxides) and 21 isomeric compounds (including positional, structural, and cis/trans-isomers) were well separated on the [ZnCl2L]2-coated column. Impressively, some racemates were resolved with high resolution values (Rs), including 1,2-butanediol diacetate (Rs = 25.86), ethyl 3-hydroxybutyrate (Rs = 20.97), 1,3-butanediol diacetate (Rs = 18.09), and threonine derivative (Rs = 18.61). Compared with the commercial β-DEX 120 column for separation of the tested racemates, the [ZnCl2L]2-coated column exhibited good enantioseparation complementarity, enabling separation of some racemates that could not be separated, or were not well resolved, by the β-DEX 120 column. In addition, many organic mixtures, such as n-alkanes, alkylbenzenes, n-alcohols, and a Grob test mixture, were also well separated on the [ZnCl2L]2-coated column. The column also has good reproducibility and thermal stability on separation. This work not only reveals the great potential of metallacycles for GC separations but also opens up a new application of metallacycles in separation science.
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EUROPEAN POLYMER JOURNAL
·
2023
·
IF 6
Xiaoxing Wang,Xinhong Cai,Xiaoqin Zhang,Jinggang Wang,Jin Zhu
A series of bio-based poly(ethylene-co-propylene furandicarboxylate) (PEPF) copolyesters with different compositions were synthesized from dimethyl-2,5-furandicarboxylate, ethylene glycol and 1,3-propanediol by transesterification and melting polycondensation. Their chemical structure, composition and sequence distribution were confirmed by 1 H NMR and 13 C NMR. The results of GPC showed that the obtained copolyesters had a high number average molecular weight between 25000 g/mol and 30900 g/mol. The thermal properties characterized by DSC showed that the T g increased with the mole fraction of EF from 64.4℃ for PEPF-23 to 83.2℃ for PEPF-84 as well as the samples displayed a high Young's modulus between 2800 and 3360 MPa and tensile strength between 56 and 89 MPa. Furthermore, the PEPF copolyesters exhibited excellent CO 2 , O 2 and H 2 O barrier properties compared with poly(ethylene terephthalate) with the BIFp of 8.7–10 times, 3.7–4.4 times and 1.5–1.6 times, respectively. The transparency of PEPFs was up to 89% by cutoff at 700 nm and had better solvent resistance. This work builds a bridge between poly(ethylene 2,5-furandicarboxylate) and poly(propylene 2,5-furandicarboxylate) and PEPFs owned excellent thermo-mechanical and gas barrier properties could be used in food packaging fields.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yue Sun,Sicheng Yuan,Ziheng Bai,Bin Liang,Dengyu Fu,Haodong Hu,Luchao Pei,Ruitao Wang,Yanji Zhu,Huaiyuan Wang
In the process of carbon capture, utilization and storage (CCUS), carbon dioxide is in long-term contact with metal pipelines and devices. Therefore, in the CCUS environment the corrosion of carbon dioxide to metals limits the service life. Herein we have explored the failure of epoxy (EP) coating in the CO 2 corrosion environment. Based on this, a unique g-C 3 N 4 -ESO-EP anti-corrosion coating suitable for CCUS conditions was prepared by using graphene-C 3 N 4 (g-C 3 N 4 ) nanosheet and epoxy silane oligomer (ESO) one-step method. The semiconductor g-C 3 N 4 prepared by the secondary thermal stripping method provides plentiful CO 2 adsorption sites and prevents the diffusion of corrosive ions (gathered state CO 2 , CO 3 2− , HCO 3 − , H + ) in the EP coating. The CO 2 gas permeability of g-C 3 N 4 -ESO-EP film (with thickness of 100 μm) is approximately 45.94% lower than that of EP film. After immersion in 1.0 M acid corrosion environment, the protection efficiency of g-C 3 N 4 -ESO-EP coating is 99.99%. After adding ESO, the “bridging effect” formed at the interface reduces the interface defects between the resin and the nano-sheet, and synergistically enhances the adhesion between the coating and the substrate. The g-C 3 N 4 -ESO-EP coating has passed the test of severe simulated CCUS corrosion environment (4 days in 3.0 MPa CO 2 and 3.5 wt% NaCl solution). The |Z| 0.01Hz value of g-C 3 N 4 -ESO-EP coating after immersion in 3.5 wt% NaCl solution for 120 days maintained 1.73 × 1011 O cm 2 , indicating the coating has long-term corrosion resistance. This work provides a new and simple method to improve the CO 2 resistance of EP coating and reveals the importance of functional composite coating for metal protection in CCUS process.
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Arabian Journal of Chemistry
·
2023
·
IF 6
Panyang Guo,Jie Wang,Yunyan Tie,Xu Luo
In the marine high-pressure low-temperature environment, it is difficult to regulate the low-temperature rheology of the drilling fluid, and the spilled natural gas is easy to generate solid gas hydrate in the wellbore, causing problems such as wellbore blockage and increasing the risk of safe drilling operations. Although there are many researches on the invasion process of drilling fluid and the development of new hydrate inhibition, there is still a lack of research on the inhibition system suitable for drilling fluid. Therefore, this paper uses the self-developed hydrate formation evaluation experimental device to simulate and analyze the effect of inhibitors in reservoir environment and optimize the scheme of drilling fluid inhibition system. The results show that: (1) Through the improvement of the experimental device of water bath methane hydrate (MH) evaluation, the accuracy and parallel control of the equipment are enhanced, and the methane hydrate formed by sea water (SW) is less than that of distilled water (DW), and the structure of methane hydrate formed by distilled water is more compact. (2) Through the evaluation experiment of single inhibitor A3, PAC and CMC inhibition system, it was found that A3 had the best inhibition effect, and when the inhibitor concentration was 1.5 wt%, it had the best inhibition effect. (3) The influence of clay types on the formation of methane hydrate is also significantly different. Bentonite soil Red (BSR) has better inhibition performance than Bentonite soil Yellow (BSY), and its ' hut ' structure formed at low temperature is the reason for the formation of methane hydrate. (4) The inhibition ability of A3 inhibitor in BSY system and BSR system solution in general, the addition of KCl can play a strong synergistic inhibition ability with A3 in BSR system, and its electric field reduces the activation energy of water molecules as well as the consumption of free water is the reason to reduce the generation of methane hydrate.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Weinan Song,Mingxue Zhang,Weiguang Zhao,Qinglu Zhao,Hongshun Hao,Hai Lin,Wenyuan Gao,Shuang Yan
A modification approach is developed based on the idea of molecular imprinting technique to enhance the selective gas sensing performance of nanostructured SnO2 as gas sensors. The modification procedure, conducted on SnO2 microspheres as the porous substrate, involves in situ polymerization and calcination processes. A methanol-templated molecularly imprinted sample (cM-SnO2 MIP) was successfully synthesized via the modification procedure, which demonstrated great difference with its nonmodified counterpart (c-SnO2 MSs) in terms of both surface morphology and internal architecture. Gas sensing performance, including target gas response, selectivity, and dynamic sensing behavior, was investigated to validate the effectiveness of the imprinted cavities for methanol within cM-SnO2 MIPs. Compared to c-SnO2 MSs, the cM-SnO2 MIPs exhibited greatly enhanced methanol sensing selectivity and improved anti-interference ability by up to 2–10 times depending on the types of interference gases. Moreover, the predesigned target gas recognition capability of the molecularly imprinted sensors was proved by changing the template to ethanol and thus obtaining cE-SnO2 MIPs with excellent ethanol sensing selectivity as well as improved anti-interference ability. By constructing a sensor array, the excellent sensing selectivity of these nanostructured SnO2 microspheres was exploited to distinguish the chemically similar molecules, methanol and ethanol.
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Advanced Science
·
2022
·Vol. 9
·期 34
·2204519
·
IF 17.521
Tianci Huang,Yong Long,Zilong Dong,Qilin Hua,Jianan Niu,Xinhuan Dai,Jiangwen Wang,Junfeng Xiao,Junyi Zhai,Weiguo Hu
Aerogels have been attracting wide attentions in flexible/wearable electronics because of their light weight, excellent flexibility, and electrical conductivity. However, multifunctional aerogel-based flexible/wearable electronics for human physiological/motion monitoring, and energy harvest/supply for mobile electronics, have been seldom reported yet. In this study, a kind of hybrid aerogel (GO/CNT HA) based on graphene oxide (GO) and carboxylated multiwalled carbon nanotubes (CMWCNTs) is prepared which can not only used as piezoresistive sensors for human motion and physiological signal detections, but also as high performance triboelectric nanogenerator (TENG) coupled with both solid–solid and gas–solid contact electrifications (CE). The repeatedly loading–unloading tests with 20 000 cycles exhibit its high and ultrastable piezoresistive sensor performances. Moreover, when the obtained aerogel is used as the electrode of a TENG, high electric output performance is produced due to the synergistic effect of solid–solid, and gas–solid interface CEs (3D electrification: solid–solid interface CE between the two solid electrification layers; gas–solid interface CE between the inner surface of GO/CNT HA and the air filled in the aerogel pores). This kind of aerogel promises good applications for human physiological/motion monitoring and energy harvest/supply in flexible/wearable electronics such as piezoresistive sensors and flexible TENG.
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高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 22
·4062
·
IF 5.719
Bo Zhang,Shuai Zhang,Yi Xia,Pingping Yu,Yin Xu,Yue Dong,Qufu Wei,Jing Wang
Optical excitation is widely acknowledged as one of the most effective means of balancing sensor responses and response/recovery properties at room temperature (RT, 25 °C). Moreover, noble metals have been proven to be suitable as photosensitizers for optical excitation. Localized surface plasmon resonance (LSPR) determines the liberalization of quasi-free electrons in noble metals under light irradiation, and numerous injected electrons in semiconductors will greatly promote the generation of chemisorbed oxygen, thus elevating the sensor response. In this study, pure SnO2and Au/SnO2nanowires (NWs) were successfully synthesized through the electrospinning method and validated using XRD, EDS, HRTEM, and XPS. Although a Schottky barrier led to a much higher initial resistance of the Au/SnO2composite compared with pure SnO2at RT in the dark, the photoinduced resistance of the Au/SnO2composite became lower than that of pure SnO2under UV irradiation with the same intensity, which confirmed the effect of LSPR. Furthermore, when used as sensing materials, a detailed comparison between the sensing properties of pure SnO2and Au/SnO2composite toward NO2in the dark and under UV irradiation highlighted the crucial role of the LSPR effects. In particular, the response of Au/SnO2NWs toward 5 ppm NO2could reach 65 at RT under UV irradiation, and the response/recovery time was only 82/42 s, which far exceeded those under Au modification-only or optical excitation-only. Finally, the gas-sensing mechanism corresponding to the change in sensor performance in each case was systematically proposed.Keywords:Au-loaded;UV irradiation;synergistic effect;NO2;gas sensor
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MATERIALS & DESIGN
·
2022
·
IF 9.417
Haifeng Zhang,Yang Liu,Xueya Xu,Ting Meng,Gangwen Fu,Yong Gao,Jie Pu,Yuxuan Wang
In the past decade, single-atom and nanocluster catalysts have emerged as promising materials for high efficiency electrocatalysis, while geometric morphologies and electronic properties of the supporting substrates dramatically affect the overall electrocatalytic performances. We have constructed highly oriented nitrogen-doped carbon nanotubes on carbon cloth (V-CNTs/CC) and demonstrated it can serve as superior substrate for Pt nanoclusters that are typical electrocatalysts for hydrogen evolution reactions. Compared with Pt@CNTs/CC, the Pt@V-CNTs/CC has significantly improved electron transport and charge transfer efficiency, as well as gas diffusion capability, leading to excellent catalytic activity and stability. The V-CNTs/CC designed in this work can serve as general support for various single-atom or nanocluster catalysts for high-performance electrocatalysis.
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JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Chunhui Wang,Shuangshuang Zhao,Wei Shen,Xiaoming Xi,Lishan Yang,Lixiong Bai,Yahui Yang,Chenghuan Huang,Jian Zhu,Youyuan Zhou,Yitai Qian,Zhongliang Tian,Yanqing Lai,Liqiang Xu
Layered high-temperature LiCoO 2 (HT-LiCoO 2 ), a mature commercial cathode for 3C electronic devices, has been unable to satisfy the new and ever-growing battery demands due to its high price and the structural instability at high temperature or high voltage conditions. The practical strategies mainly conclude introducing even dopants and functional modifications to LiCoO 2 crystals, but lacking explorations on the precise-control of non-equilibrium intermediates and preferred crystal planes during the solid-solid-gas (SSG) synthesis process. Here, the structure-optimal HT-LiCoO 2 micro-bricks are synthesized via coherent pyrolysis followed by a SSG reaction from Co–Al-mixed oxalate precursors, forming layered phase, ideal crystal morphology and uniformly distributed Al-dopants. In particular, we observe both of the phase progression and morphology evolution during the synthesis process of LiCo 1-x Al x O 2 micro-bricks. Integrating the superiorities of the nanosized intermediates and Al-doping regulation, smaller crystalline size and less salt-rock defects are realized in the target cathodes, ultimately achieving promoted Li + diffusion kinetic and electrochemical stability. Combined with the theory calculation, the optimized LiCo 1-x Al x O 2 with possible ion channels and the dopant-affected band gap have been simulated. These insights can help to guide the SSG synthesis of layered cathode materials with preferential orientations, precise doping and tailored phase compositions .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Shujun Sun,Jun Zhang,Changdong Sheng,Hui Zhong
A novel Na2SiO3/Fenton system was employed for NO removal from coal-fired flue gas in a bubble reactor. The NO removal efficiency of this system could reach 94.36% when the flue gas residence time was 3 s. The hydrolysis reaction of Na2SiO3 produced OH-, which made the solution alkaline, and the formation of iron-based colloids in the alkaline environment effectively catalyzed the generation of free radicals from H2O2, O2•– radicals, which was the main reason for the increase of NO removal efficiency. The reaction of H2O2 catalyzed by iron-based colloids increased the solution pH, which could not only further improve the NO removal efficiency but also enhance the useless decomposition of H2O2. Na2SiO3 could buffer the solution pH, which weakened the ineffective decomposition of H2O2 and prolonged the effective denitrification time. The X-ray diffraction and ion chromatography analysis showed that NO was finally converted to NO3– and NO2–.
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