CHEMICAL ENGINEERING SCIENCE
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2023
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IF 4.7
Yanan Liu,Chengxiang Shi,Zhensheng Shen,Rui Yu,Lun Pan,Li Wang,Xiangwen Zhang,Ji-Jun Zou
It is significant to efficiently and feasibly produce high-performance jet fuel from renewable biomass. We reported here that lignin-derived phenolics can be alkylated by cellulose-derived cyclopentanol in a continuous-flow fixed-bed reactor packed with HUSY zeolite without the use of solvents. Under nitrogen pressure, the liquid-phase reaction was achieved. Among the investigated zeolites with different structures and SiO 2 /Al 2 O 3 , HUSY-150 exhibited excellent catalytic performance and stability. By adjusting reaction conditions, almost complete conversion of cyclopentanol was achieved, as well as high phenol conversion (∼70 %), and high polycyclic product selectivity (>95 %) over HUSY-150. Afterwards, we extended the range of feedstock from phenol to other phenolics (guaiacol, 2,6-dimethoxyphenol, and lignin oil surrogates), and even at a high LHSV (liquid hourly space velocity) of 36 mL/(g cat ·h), HUSY-150 maintained robust catalytic activity. This study demonstrates a feasible and effective method for producing high-performance jet fuel blends using lignocellulose-derived compounds.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
·
IF 8.4
Zhujun Ai,Xinmin Li,Rui Chen,Daobin Han,Huijie Bai,Shaoying Yan,Pengcheng Gu,Haiping Wu,Shijia Ding,Junman Chen,Hua Tang
DNA walkers have been widely used to build biosensing systems. However, their moving efficiency was limited, which has hindered practical applications. Here, we for the first time integrated localized CHA with nanoscale AuNPs scaffolds to achieve space double-confined catalytic hairpin assembly (SDCHA) for developing a fast three-dimensional DNA walker. Driven by spatially proximal displacement, the walker possessed a high walking speed, which was about 8 times, 9 times and 23 times faster than LCHA, CHA-AuNPs and conventional CHA, respectively. Moreover, the walking time was about 1.4–8.3 times shorter than most recently reported DNA walkers and space-confined strand displacement reactions. By further integrating it with magnetic probes and g-C 3 N 4 nanosheets , an ultrasensitive and enzyme-free homogeneous electrochemiluminescence (Ho-ECL) aptasensor was firstly constructed for sonic hedgehog (SHh) detection. Profiting from this tailored integration, the Ho-ECL aptasensor avoided multiple interferences from complex milieu as well as tedious procedures of electrode modifying and washing, showing good signal stability, repeatability and reliability. It was also proved to achieve ultrasensitive SHh detection with the detection limit as low as 13.5 fM, superior to previous research on SHh detection. This work might broaden ideas for the construction of fast DNA walkers and facile Ho-ECL bioanalytical methods for clinical diagnosis.
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ANALYST
·
2018
·Vol. 143
·期 8
·1881-1889
·
IF 3.864
Linlin Yang,Jun Zhao,Xinling Yu,Ruilong Zhang,Guangmei Han,Renyong Liu,Zhengjie Liu,Tingting Zhao,Ming-Yong Han,Zhongping Zhang
Hydrogen sulfide (H2S) is a key signaling molecule in the cytoprotection, vascular mediation and neurotransmission of living organisms. In-depth understanding of its production, trafficking, and transformation in cells is very important in the way H2S mediates cellular signal transductions and organism functions; it also motivates the development of H2S probes and imaging technologies. A fundamental challenge, however, is how to engineer probes with sensitivity and cellular penetrability that allow detection of spontaneous production of H2S in the entire cell space and live animals. Here, we report a rationally designed molecular switch capable of accessing all intracellular compartments, including the nucleus, lysosomes and mitochondria, for H2S detection. Our probe comprised three functional domains (H2S sensing, fluorescence, and biomembrane penetration), could enter almost all cell types readily, and exhibit a rapid and ultrasensitive response to H2S (≤120-fold fluorescence enhancement) for the dynamic mapping of spontaneously produced H2S as well as its distribution in the whole cell. In particular, the probe traversed blood/tissue/cell barriers to achieve mapping of endogenous H2S in metabolic organs of a live Danio rerio (zebrafish). These results open-up exciting opportunities to investigate H2S physiology and H2S-related diseases.
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JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Li-Hao Xu,Yan Li,Shen-Hui Li,Ming-Yu Lv,Zhi-Ping Zhao
Expanding the metal–organic frameworks (MOFs) category using room-temperature colloidal chemistry route with regular crystal structure is challenging, but important for reducing energy consumption and realizing an economically viable application in industry. Herein, we developed a novel advanced copper terephthalate MOF (CuBDC) between graphene oxide (GO) layers using a simple space-confined growth strategy at room temperature. The inclusion of CuBDC@GO can realize high filler loadings while maintaining uniform dispersion throughout PDMS matrix. The paralled arranged CuBDC sheets created 1D inner vertical channels, along with the enlarged GO interlayer space for rapid molecule permeselective transport. The resultant mixed matrix membranes (MMMs) with 30 wt% CuBDC@GO loading improved the separation factor from 190.6 to 576.3, and simultaneously increased the total flux from 575.2 to 1357.4 g m -2 h -1 for separating 0.5 wt% butyl acetate at 40 °C. The transport mechanism was explained by adjusting the CuBDC content in composites to examine the significant increase in membrane permeability (from 12.5 to 58.3) and selectivity (from 0.7 to 2.0). Compared to alcohol or ketone, the larger size strip-like butyl acetate molecules are ideal for rapid transport through the CuBDC-supported 1D continuous inner channels, and effectively inhibit the movement of water molecules, ultimately resulting in the largest pervaporation performance improvement in butyl acetate/water separation. This CuBDC@GO prepared by a simple, green and room-temperature synthesis route can be widely applied to prepare defect-free membranes with excellent performance for sustainable applications. We also anticipate that this advanced space-confined growth strategy can be extended to various other MOFs and applications.
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Polymers
·
2022
·Vol. 14
·期 2
·322
·
IF 4.967
Hong Qi,Qingshan Shi,Yuhai Qian,Yueming Li,Jingjun Xu,Caihong Xu,Zheng Zhang,Xiaobao Xie
In this work, the atomic oxygen (AO) erosion-resistance effect and mechanism of the Perhydropolysilazane (PHPS) coating were investigated from the perspective of element distribution in the depth direction. The results revealed that the coating demonstrated good adhesion and intrinsic AO erosion-resistance, which was attributed to the composition gradient formed in the coating. Moreover, the oxygen ratio of the SiOx on top layer of the coating could be elevated during AO exposure, strengthening the Ar ion etching durability of the coating. According to these results, an AO erosion-resistance mechanism model of the PHPS-derived SiOx coating was finally obtained.Keywords:PHPS;silica coating;atomic oxygen;erosion-corrosion;resistance mechanism
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Huayu Wu,Nuo Xu,Zhouheng Jiang,Anyu Zheng,Qiaofang Shi,Rongguan Lv,Lubin Ni,Guowang Diao,Ming Chen
Necklace-box structural FeS 2 /WS 2 carbon nano-composite fibers (NB FeS 2 /WS 2 -CNFs) are fabricated by electrospinning-sulfuration-hydrothermal process. NB FeS 2 /WS 2 -CNFs exhibit the spatial confined structure, which is able to restrain volume expansion effectively in the process of Na + intercalation/deintercalation and improve the cycling stability and rate performance. NB FeS 2 /WS 2 -CNFs exhibit remarkable initial coulombic efficiency (ICE = 87.0%) and stable long cycle (~422.6 mA h g −1 at 0.5 A g −1 after 500 cycles) for sodium storage capability. The heterojunction interface between FeS 2 and WS 2 can alleviate the damage of the micro-crystal plane and enhance electrochemical kinetic process. The structure evolution and mechanism of sodium storage are explored by ex-situ methods, which further confirm the spatial and interface confinement effect distinctly. In addition, the electrochemical kinetic properties of lithium-ion batteries (LIBs), sodium-ion batteries (SIBs) and potassium-ion batteries (PIBs) are compared, thereby revealing the energy storage mechanism and different ion migration modes of the three batteries. This work provides a guide for the synthesis of bimetallic compounds based on the spatial confinement and heterojunction interface confined strategy that efficiently improves energy storage performance of electrode material.
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Xiuli Wang,Abudurexiti Rehman,Rong-mei Kong,Yuanyuan Cheng,Xiaoxia Tian,Maosheng Liang,Lingdong Zhang,Lian Xia,Fengli Qu
Facile and sensitive determination of formaldehyde (FA) in indoor environments still remains challenging. Herein, a fluorescent probe, termed PHN@MOF, was synthesized by embedding the fluorescent molecule of N-propyl-4-hydrazine-naphthalimide (PHN) into a metal–organic framework (MOF) for sensitive and visual monitoring of FA. The hydrazine group of PHN acts as the specific reaction group with FA based on the condensation reaction. The host of MOF (UiO-66-NH2) offers the surrounding confinement space required for the reaction. Owing to the enrichment effect and molecular sieve selection of UiO-66-NH2 to FA, PHN@MOF, compared with free PHN, exhibits very high sensitivity and selectivity based on space confinement-induced sensitivity enhancement (SCISE). Moreover, the fluorescence of UiO-66-NH2 offers a reference signal for FA detection. Using this ratiometric fluorescent PHN@MOF probe, a colorimetric gel plate and test paper were developed and used to visually monitor FA in air.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Wei Cheng,Yumei Peng,Yi Wang,Weidong Jiang,Yan Long,Guangyin Fan
Hydrogen evolution from ammonia borane (AB) hydrolysis is of great importance considering the ever-increasing demand for green and sustainable energy. However, the development of a facile and efficient strategy to construct high-performance catalysts remains a grand challenge. Herein, we report an amino-group and space-confinement assisted strategy to fabricate Rh nanoparticles (NPs) using amino-functionalized metal-organic-frameworks (UiO-66-NH 2 ) as a NP matrix (Rh/UiO-66-NH 2 ). Owing to the coordination effect of amino-group and space-confinement of UiO-66-NH 2 , small and well-distributed Rh NPs with a diameter of 3.38 nm are successfully achieved, which can be served as efficient catalysts for AB hydrolysis at room temperature . The maximum turnover frequency of 876.7 min −1 is obtained by using the Rh/UiO-66-NH 2 with an optimal Rh loading of 4.38 wt% and AB concentration of 0.2 M at 25 °C, outperforming most of the previously developed Rh-based catalysts. The catalyst is also stable in repetitive cycles for five times. The high performance of this catalyst must be ascribed to the structural properties of UiO-66-NH 2 , which enable the formation of small and well-dispersed Rh NPs with abundant accessible active sites. This study provides a simple and efficient method to significantly enhance the catalytic performance of Rh for AB hydrolysis.
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Science Bulletin
·
2025
·
IF 21.1
Duo Pan,Ziyuan Han,Junting Lei,Yutao Niu,Hu Liu,Sunmi Shin,Chuntai Liu,Zhanhu Guo
With the rapid progress of aerospace frontier engineering, the extreme space thermal environment has brought severe challenges to astronauts’ space suits, putting forward higher requirements for thermal protection materials. On this basis, a unique core-shell structured hexagonal boron nitride (h-BN)/silicon dioxide (SiO 2 ) nanofiber membrane (HS) was prepared using the coaxial electrospinning method, of which both the thermal insulation SiO 2 nanofiber cortex and the passive radiation cooling (PRC) h-BN nanofiber core make it a promising dual-effect thermal management material. Especially, when the amount of h-BN is 0.9 g, the resultant HS (HS 0.9 ) exhibits astonishing low thermal conductivity of 0.026 W m −1 K −1 and high reflectivity and emissivity of exceeding 90% over an extremely wide range. The expected dual-effect thermal management performance enables the HS to have an ideal cooling effect under both high sunlight intensity and strong light radiation. In addition, HS also shows excellent flame retardant performance arising from the excellent high-temperature stability of h-BN and SiO 2 . What is more, the tensile strength of HS 0.9 was also significantly increased from 0.42 to 7.2 MPa by encapsulating polyimide through vacuum filtration. Therefore, the research results of this work provide innovative highlights for high-temperature protection in daily life and even extreme space environments.
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Small
·
2024
·
IF 13
Xinyu Wang,Lei Yang,Huanyu Liang,Chunliu Zhu,Jing Shi,Jingyi Wu,Jingwei Chen,Weiqian Tian,Yue Zhu,Huanlei Wang
The poor cycling stability and rate performance of transition metal selenides (TMSs) are caused by their intrinsic low conductivity and poor structural stability, which hinders their application in potassium-ion batteries (PIBs). To address this issue, encapsulating TMSs within carbon nanoshells is considered a viable strategy. However, due to the lack and uncontrollability of internal void space, this structure cannot effectively mitigate the volume expansion induced by large K + , resulting in unsatisfactory electrochemical performance. Herein, peanut-shaped FeSe 2 @carbon yolk-shell capsules are prepared by modulation of the internal space. The active FeSe 2 is encapsulated within a robust carbon shell and an optimal void space is retained between them. The outer carbon shell promotes electronic conductivity and avoids FeSe 2 aggregation, while the internal void mitigates volume expansion and effectively ensures the structural integrity of the electrode. Consequently, the FeSe 2 @carbon anode demonstrates exceptional rate performance (242 mAh g −1 at 10 A g −1 ) and long cycling stability (350 mAh g −1 after 500 cycles at 1 A g −1 ). Furthermore, the effect of internal space modulation on electrochemical properties is elucidated. Meanwhile, ex situ characterizations elucidate the K + storage mechanism. This work provides effective guidance for the design and the internal space modulation of advanced TMSs yolk-shell structures.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Danqing Shen,Xueping Chen,Gaohui Lu,Ruonan Shi,Jianming Pan
Monodispersed magnetic sorbents (MMSs) display great potential for adsorptive removal of pollutants, but the conventional methods cannot meet requirements of scalable, time-saving, and energy-efficient fabrication. In this work, space-confined synthesis of nitrilotriacetic acid immobilized magnetic sorbents (NAIMSs-E) in aqueous continuous phase of high internal phase emulsions (HIPEs) was conducted, and as-prepared high quality sorbents (sensitive response to magnetic field, abundant affinity groups, uniform shell size, and stable structure) were applied for removing bivalent cadmium (Cd 2+ ) from aqueous solutions. 2-(Bis-carboxymethyl-amino)-6-{3-[2-(3,4-dihydroxy-phenyl)-ethylcarbamoyl]-propionylamino}-hexanoic acid was firstly synthesized as a robust anchor and a functional modifier onto magnetic Fe 3 O 4 . The effects of synthesis conditions to the morphology and structure were studied, and the forming mechanism based on emulsion nano-reactor was demonstrated. NAIMSs-E are expected to possess fast equilibrium rate, and approximately 90% of the maximum adsorption capacity is achieved within 60 min. The maximum uptake amounts are 49.98 mg g −1 , 80.58 mg g −1 , 176.4 mg g −1 at 288 K, 298 K, and 308 K, respectively, and the monolayer chemisorption based on sharing and transferring of electrons is the main rate-limiting step. Moreover, NAIMSs-E have excellent regeneration and specific affinity towards Cd 2+ , even for actual water samples. In addition, the spontaneous, endothermic, and entropy increased adsorption process is also confirmed. Therefore, this work not only presents a new clue to fabricate MMSs via simple emulsion nano-reactor, but also provides a novel platform for Cd 2+ removal.
研究领域:
环境科学
·
材料科学
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JOURNAL OF CHROMATOGRAPHY A
·
2026
·
IF 4
Yehong Han,Juntao Wang,Weihua Liu,Pengfei Li,Meiting Zhang,Xuhui Jin,Zhi Wang
A low-cost, battery-free cold assisted SPME device with 40 min cooling was developed. • It demonstrated a higher extraction efficiency for volatiles than conventional SPME. • The efficient cooling enables 30%–44% improvement in PCNs extraction via CA-SPME. • The CA-SPME-GC–MS/MS method achieves enrichment up to 4299 for eight PCNs. • It was successfully applied to the determination of PCNs in drinking water samples. A cold-assisted headspace solid-phase microextraction (CA-HS-SPME) method combined with gas chromatography–mass spectrometry (GC–MS) was developed for the determination of eight polychlorinated naphthalene (PCN) congeners in water sample. In the CA-HS-SPME setup, frozen gel served as the refrigerant and copper tube as the thermal conductor to cool the polydimethylsiloxane (PDMS) fiber during extraction, thereby enhancing extraction efficiency. The main experimental variables affecting the extraction performance, including temperature, extraction time, and salt concentration, were systematically optimized. Under the optimized conditions, the method exhibited good linearity over the range of 0.1/0.5/1–500 pg/mL, with the correlation coefficient ( r ) values ≥ 0.9962. The enrichment factors for the PCNs ranged from 955 to 4299, while the limits of detection and quantification were 0.02–0.28 pg/mL and 0.07–0.92 pg/mL, respectively. The intra-day and inter-day precisions (n = 6), expressed as the relative standard deviations, were 10.8%–16.3% and 12.2%–17.8%, respectively. The recoveries obtained from fortified water samples ranged from 90.7% to 117.8%. The proposed method is sensitive, simple, solvent-free, and provides an effective approach for the determination of trace PCNs in water. Download: Download high-res image (169KB) Download: Download full-size image
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