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LANGMUIR · 2020 · IF 3.557

N-Doping Carbon-Nanotube Membrane Electrodes Derived from Covalent Organic Frameworks for Efficient Capacitive Deionization

Li Ren,Jiemei Zhou,Sen Xiong,Yong Wang

Capacitive deionization (CDI) is an energy-efficient and environmentally friendly electrochemical desalination technology which has attracted increasing attention in recent years. Electrodes are crucial to the performance of CDI processes, and utilizing a carbon-nanotubes (CNTs) membrane to fabricate electrodes is an attractive solution for advanced CDI processes. However, the strong hydrophobicity and low electrosorption capacity limit applications of CNTs membranes in CDI. To solve this problem, we introduce crystalline porous covalent organic frameworks (COFs) into CNTs membranes to fabricate N-doping carbon-nanotubes membrane electrodes (NCMEs). After solvothermal growth and carbonization, CNTs membranes are successfully coated with imine-based COFs and turned into integrated NCMEs. Comparing with the CNTs membranes, the NCMEs exhibit an ∼2.3 times higher electrosorption capacity and superior reusability. This study not only confirms that COFs can be used as high-quality carbon sources but also provides a new strategy to fabricate high-performance CDI electrodes.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Bioactive Materials · 2020 · IF 8.724

Synergistic anti-inflammatory and osteogenic n-HA/resveratrol/chitosan composite microspheres for osteoporotic bone regeneration

Limei Li,Mali Yu,Yao Li,Qing Li,Hongcai Yang,Meng Zheng,Yi Han,Di Lu,Sheng Lu,Li Gui

The development of functional materials for osteoporosis is ultimately required for bone remodeling. However, grafts were accompanied by increasing pro-inflammatory cytokines that impaired bone formation. In this work, nano-hydroxyapatite (n-HA)/resveratrol (Res)/chitosan (CS) composite microspheres were designed to create a beneficial microenvironment and help improve the osteogenesis by local sustained release of Res. Study of in vitro release confirmed the feasibility of n-HA/Res/CS microspheres for controlled Res release. Notably, microspheres had anti-inflammatory activity evidenced by the decreased expression of pro-inflammatory cytokines TNF-α, IL-1β and iNOS in RAW264.7 cells in a dose dependent manner. Further, enhanced adhesion and proliferation of BMSCs seeded onto microspheres demonstrated that composite microspheres were conducive to cell growth. The ability to enhance osteo-differentiation was supported by up-regulation of Runx2, ALP, Col-1 and OCN, and substantial mineralization in osteogenic medium. When implanted into bone defects in the osteoporotic rat femoral condyles, enhanced entochondrostosis and bone regeneration suggested that the n-HA/Res/CS composite microspheres were more favorable for impaired fracture healing. The results indicated that optimized n-HA/Res/CS composite microspheres could serve as promising multifunctional fillers for osteoporotic bone defect/fracture treatment.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Ultrasmall Mo2C in N-doped carbon material from bimetallic ZnMo-MOF for efficient hydrogen evolution

Yuanyuan Guo,Qi Huang,Junyang Ding,Li Zhong,Ting-Ting Li,Yue Hu,Jinjie Qian,Shaoming Huang

The exploration and development of cost-effective and highly stable electrocatalysts with the highest possible energy efficiency remain a constant pursuit in the catalyst design and synthesis for electrocatalytic hydrogen evolution reaction (HER). In this work, a convenient approach is proposed to synthesize a type of ultrafine Mo 2 C nanoparticles in average sizes of 3–4 nm embedded in hierarchically porous N-doped carbon material calcined from bimetallic ZnMo-MI (MI = 2-methylimidazole) is obtained at 1000 °C, denoted as ZnMo-MI-1000 . First of all, the crystalline hybrid metal-organic framework of ZnMo-MI is fabricated from zeolitic imidazolate framework of Zn-MI precursors via solvothermal reaction, in which the conversion from Zn-MI to ZnMo-MI occurs gradually over time. After calcination , the as-obtained ZnMo-MI-1000 sample shows a satisfying HER performance with the small overpotential of 83.0 mV in 0.5 M H 2 SO 4 and 100.1 mV in 1.0 M KOH to reach a current density of 10 mA cm −2 , which is attributed to ultrasmall Mo 2 C, Mo and N-doped graphitic carbon matrix. The multiporous network of ZnMo-MI-1000 can provide continuous mass transportation with a minimal diffusion resistance that produce effective electrocatalytic kinetics in both acidic and alkaline media , which is utilized as a highly active and durable nonprecious metal electrocatalyst for HER.

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Materials Advances · 2020 ·Vol. 2 ·期 2 ·692-699 · IF 0

Tailored N-doped porous carbons via a MOF assembly process for high-performance CO2 uptake

Fangyuan Gai,Dongying Zhu,Yunhuan Wu,Xiaogang Zhao,Changhai Liang,Zhenguo Liu,Yunling Liu,Tonghua Wang

Striking a balance between the nitrogen content and pore texture of N-containing metal–organic framework (MOF)-derived carbon is a considerable challenge for high-performance CO2 capture. The high-temperature pyrolysis and activation facilitated well-developed pore structures but resulted in serious nitrogen loss of MOFs. In this work, we developed MOF (ZIF-8)-derived N-doped porous carbons (NPCs) by integrating ZIF-8 with pomelo peel via a co-carbonization and activation process to construct a high-performance CO2 adsorbent. The pomelo peel can effectively prevent the nitrogen loss from the ZIF-8 backbone via pre-melting and polymerization and simultaneously offer the ideal porosity and BET surface area during the co-carbonization and activation process. By tuning the ZIF-8 loading capacity and the activation temperature, the sample NPC-800-4 prepared at 800 °C possessed both ultrahigh surface area (∼1967 m2 g−1) and high N content (∼13.15 wt%). Particularly, the CO2 capacity of NPC-800-4 reached 5.51 mmol g−1 at 25 °C and 9.01 mmol g−1 at 0 °C under 1 bar due to its relatively high content of pyrrolic-N (N5 ∼ 61.2%) and pyridinic-N (N6 ∼ 16.5%), as well as the proper pore size distribution (0.64 nm). In addition, the TPD measurement and CO2 adsorption energy (Qst) of NPC-800-4 also suggested the high desorption activation temperature and energy, indicating a strong binding capacity toward CO2. Moreover, NPC-800-4 exhibited almost constant CO2 uptake in 8 consecutive adsorption–desorption cycles, indicating that the sample with great stability and recyclability would be easily adapted and recycled from industries. This co-carbonization and activation strategy to assembly MOFs with biomass would pave the way for enhancing CO2 capture of MOF-derived carbons.

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JOURNAL OF MOLECULAR LIQUIDS · 2020 · IF 5.065

Microstructures of the Gemini surfactant microemulsion system 14-4-14/1-propanol/n-heptane/water

Xiaoxing Lu,Shaoxia Xie,Jian Kuang,Hujun Xie

A comprehensive experimental investigation on the microstructures of microemulsion constructed with Gemini surfactant has been carried out. The structural transition of the microemulsion system, 14-4-14/1-propanol/ n -heptane/water, from water-in-oil (W/O) to bi-continuous (B.C.) has been characterized by electrical conductivity and cyclic voltammetry . Being a typically percolative system, spherical nanodroplets are observed in the W/O system, while interlinks of water and oil continuous phases are observed in the middle phase, as confirmed by cryo-TEM. Most importantly, the role of water is clearly revealed. Increasing the water content results in size enhancement as well as improvement of micropolarity and diffusion behavior. Results of DSC measurements suggest that free water dominates only at high total water content. The unfrozen water which is not detected by DSC takes a considerable amount in the W/O system at low total water content, while the interphasal water reaches over 50% of total water in the middle phase system.

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APPLIED CATALYSIS A-GENERAL · 2020 · IF 5.006

Electron utilization efficiency of ZVI core activating PMS enhanced by C-N/g-C3N4 shell

Wenyan Wang,Yunlan Xu,Dengjie Zhong,Nianbing Zhong

Removal of complexation metal from plating effluents is always a problem. In this work, a core-shell structure zero-valent iron@nitrogen/graphite carbon nitride doped carbon (ZVI@C-N/g-C 3 N 4 ) composite was prepared and used to activate peroxymonsulfate (PMS) to treat complexation nickel simulated wastewater. Compared with ZVI, ZVI@C-N/g-C 3 N 4 significantly enhanced the efficiency and repeatability of PMS activation. For 45 min treatment, the removal efficiency of 50 ppm Ni-EDTA and Ni-citrate simulated wastewater reached 95.8 % and 100 %, respectively. The excellent performance of ZVI@C-N/g-C 3 N 4 is attributed to that the amino groups of nitrogen in C-N/g-C 3 N 4 shell can regulate the transmission rate of electrons released from ZVI core by adjusting the transmission rate of H + , so as to improve the electron utilization efficiency of PMS activation.

CAS / MDL: 70693-62-8
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Stepwise carbonization of nanocellulose to N-doped carbons with structural transformation and enhanced peroxymonosulfate activation

Jianan Yu,Zhiliang Zhu,Hua Zhang,Yanling Qiu,Daqiang Yin,Yi Cheng,Shaobin Wang

Metal-free nanocarbons with versatile structural dimensions and unique properties are promising materials for remediation of polluted environment. In this work, a 3-dimensional (3D) interconnected porous N-doped carbon (CN-3) was synthesized by stepwise pyrolysis of dicyandiamide and nanocellulose, and a solid-state-growth and rolling-up mechanism was proposed for the stepwise transformation from stacking layered structures (melem and g-C 3 N 4 ) into CN-3 with 3D interconnected network nano-architectures. It was found that the functional carbons obtained at varying annealing temperature presented different activities in peroxymonosulfate (PMS) activation for endocrine-disrupting chemical (estrone) oxidation, showing temperature-dependent mechanisms from radical-dominated reaction to nonradical oxidation. CN-3 presented 100% estrone removal in 10 min, much higher than the layered carbons. In addition, CN-3 exhibited satisfactory stability during the catalytic reactions. Characterizations indicated that persistent free radicals on the layered carbons tended to induce radical reaction while graphitic structure and N in derived 3D carbons are more responsible for nonradical reaction. This work provides new insights to the relationship between the carbon structural transformation and catalytic PMS activation to induce different oxidative pathways, which facilitate the generation of a highly active and stable carbon-based catalytic system for organic degradation.

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ANALYST · 2020 ·Vol. 146 ·期 1 ·207-212 · IF 3.978

Fe–N/C single-atom nanozyme-based colorimetric sensor array for discriminating multiple biological antioxidants

Wenjie Jing,Xiangkun Cui,Fanbo Kong,Wei Wei,Yunchao Li,Louzhen Fan,Xiaohong Li

Identifying the species and concentrations of antioxidants is really important because antioxidants play important roles in various biological processes and numerous diseases. Compared with an individual sensor detecting a single antioxidant with limited specificity, a sensor array could simultaneously identify various antioxidants, in which 3–5 types of nanomaterials with peroxidase-like activity are absolutely necessary. Herein, as a single-atom nanozyme, Fe–N/C with oxidase-mimicking activity was applied to construct a triple-channel colorimetric sensor array: (1) Fe–N/C catalytically oxidized three substrates 3,3′,5,5′-tetramethylbenzidine (TMB), 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS) and o-phenylenediamine (OPD) to produce blue oxidized TMB (oxTMB), green oxidized ABTS (oxABTS) and yellow oxidized OPD (oxOPD), respectively; (2) with oxTMB, oxABTS and oxOPD as three sensing channels, a colorimetric sensor array was constructed for simultaneously discriminating glutathione (GSH), L-cysteine (L-Cys), ascorbic acid (AA), uric acid (UA), and melatonin (MT), even quantifying concentrations (with GSH as a model analyst). The performance of the sensor array was validated through accurately identifying 15 blind samples containing GSH, L-Cys, AA, UA and MT in buffer solution and human serum samples, and also in binary and ternary mixtures. This work proved that fabricating a single nanozyme-based sensor array was a simplified and reliable strategy for simultaneously probing multiple antioxidants.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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ACS Applied Polymer Materials · 2021 · IF 4.089

n-Type Semiconductive Polymer and Poly(vinylidene fluoride-trifluoroethylene-chlorotrifluoroethylene) Blends for Energy Storage Applications

Rui Qiao,Haoran Xu,Shaonan Chen,Sheng Chen,Hang Luo,Dou Zhang

Dielectric polymers play a vital role in modern electronic and electrical application because of easy processing, light weight, and high breakdown strength. A high dielectric constant (εr) and breakdown strength cannot be satisfied simultaneously in the dielectric homopolymers. Via combining the merits of different polymers, the dielectric polymer blending method is a feasible option to address this issue. In this paper, n-type semiconductive polymer poly(1,6,7,12-tetra-chlorinated perylene-N-2-aminoethyl acrylate-N′-dodecylamine-3,4,9,10-tetracarboxylic bisimide) (PPDI) and relaxor ferroelectric polymer poly(vinylidene fluoride-trifluoroethylene-chlorotrifluoroethylene) (PVTC) were utilized to prepare the dielectric polymer blends because PPDI had the characteristic of binding electrons and PVTC possessed a high εr. A series of polymer blends with different weight ratios of PPDI were fabricated to investigate the loading effect of an n-type semiconductive polymer on the dielectric and energy storage properties of PPDI/PVTC blends. The experimental results showed that, when the loading was below 3 wt %, the εr of polymer blends increased from 25 to 33 at 102 Hz with the increasing content of polymer PPDI and then decreased from 33 to 7 with the increasing concentration from 3 to 40 wt %. The dielectric behavior of polymer blends was related to the dispersion of organic fillers and interface polarization. Additionally, a low dielectric loss was found in all polymer blending films. A maximal discharge energy density of 4.42 J/cm–3 was achieved in the 4.5 wt % PPDI/PVTC blending film at 200 kV/mm–1. The finding presents an innovative idea to synthesize high-performance all-organic dielectric materials.

CAS / MDL: 156028-26-1
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CHINESE JOURNAL OF POLYMER SCIENCE · 2021 ·Vol. 39 ·期 6 ·709-715 · IF 3.603

Isoselective Ring-opening Polymerization of Racemic Lactide Catalyzed by N-heterocyclic Olefin/(Thio)urea Organocatalysts

Wang Zhen-Yu,Xu Guang-Qiang,Zhou Li,Lv Cheng-Dong,Yang Ru-Lin,Dong Bing-Zhe,Wang Qing-Gang

The isoselective ring-opening polymerization of racemic lactide was achieved by combining N -heterocyclic olefin (NHO) with mono(thio)ureas or bis(thio)ureas as catalytic systems. The polymerization process shows high stereoselectivity, controllability and reactivity, delivering multi-block isotactic polylactides with high chain-end fidelity and narrow molecular weight distributions. The enhancement of catalytic performance was observed in the following order: bisthiourea (DTU) < monothiourea (TU) < bisurea (DU) < urea (U). The highest P m (probability of forming a meso dyad) = 0.91 was observed at −70 °C when using NHO/U1 catalytic system and the high stereoselectivity was attributed to chain-end control mechanism.

CAS / MDL: 108-91-8 21436-03-3
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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Positively charged poly (N-vinyl imidazole) gel-filled loose nanofiltration membranes: Performances and modelling analysis

Liang Cheng,Mengxiao Zhang,Chuanjie Fang,Weilin Feng,Liping Zhu,Youyi Xu

Loose nanofiltration (NF) membrane with pore radius approaching 1 nm and positive charges can be valuable alternative to commercial available negatively charged polyamide NF membrane in specific applications, such as removal of hardness and heavy metal ions and selective separation of dyes/salts mixture. In this work, positively charged poly( N -vinyl imidazole) (PVI) gel-filled loose NF membranes were developed by asymmetric gel-filling upon an asymmetric ultrafiltration (UF) support via UV-initiated surface grafting polymerization and post-quaternization. Compared to the polyamide NF membranes, these membranes displayed a comparable salt rejection ability due to their stronger Donnan exclusion effect. A rigorous three-parameter transport model (TPM) considering steric, Donnan and dielectric exclusion on ions partitioning via effective pore radius ( r p ), membrane charge density ( X d ) and averaged pore dielectric constant ( ε p ), was used to analyze the membrane parameters. Then the gel conformation model (GM) treating confined gel as semi-dilute polymer solution with a characteristic correlation length ( ξ ) was applied to analyze these gel composites. The results suggest that the gel polymer volume fraction ( φ ) is decisive in the gel mesh size (viewed as membrane pore size) and gel permeability. Surface porosity of the asymmetric UF base is a limiting factor in membrane permeability. The joint modelling analysis can clarify the membrane structure-properties relationship, performance limits and potentials of the gel-filled NF membrane and hence facilitate structure design and optimization.

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CATALYSIS LETTERS · 2020 ·Vol. 151 ·期 6 ·1728-1737 · IF 2.482

Exploring N-Containing Compound Catalyst for H2S Selective Oxidation: Case Study of TaON and Ta3N5

Huang Huiting,Shen Lijuan,Yang Shuai,Hu Wenjian,Zhang Lili,Feng Jianyong,Jiang Lilong,Yu Tao,Li Zhaosheng,Zou Zhigang

Abstract In addition to traditional metal oxides, N-containing compound would become efficient catalyst for H 2 S selective oxidation. TaON and Ta 3 N 5 , taking as examples, with porous structure are able to selectively oxidize H 2 S into sulfur. TaON exhibits ca. 99% H 2 S conversion and ca. 89% sulfur selectivity at 250 ℃, while Ta 3 N 5 exhibits near complete H 2 S conversion (~ 100%) and 86% sulfur selectivity at 250 ℃. TaON of lower N content shows higher sulfur selectivity (~ 90–100%) above 130 ℃, compared with that (~ 86–95%) over Ta 3 N 5 . Whereas, Ta 3 N 5 of higher N content demonstrates higher H 2 S conversion (~ 30–40%) below 160 ℃, compared with that (~ 6–30%) over TaON. Temperature programmed desorption results show that Ta 3 N 5 owns larger amount of acid sites and weaker basic sites than TaON. Over Ta 3 N 5 , the reactant molecules could dissociatively adsorb on acid sites more frequently and could be easier to move across the weaker basic sites, thus increasing probability for reaction at low temperature. Manipulating both cations and anions in N-containing compound can alter surface property for optimization of selective H 2 S oxidation. Graphic Abstract

CAS / MDL: 1314-61-0
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