JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xiao-Lu Sun,Zan Liu,Zhi-Lin Cheng
This report introduced the facile synthesis of the carbon-nanofiber films reinforced by halloysite nanotubes (HNTs) via electrospinning. The HNTs-reinforced N-doped carbon-nanofiber films (PAN/HNTs-CNFs) possessed the higher strength and toughness while keeping the prospective adsorption capability for different sulfur compounds in oil due to the higher N doping content. The PAN/HNTs-CNFs were produced by firstly electrospinning for the HNTs-filled polyacrylonitrile (PAN) nanofiber films, followed by the high-temperature carbonization for the conversion of the polymer films into the carbon-nanofiber films with the N doping. The characterizations testified that the HNTs were capable of fulfilling the uniform and disordered dispersion in the carbon-nanofibers. For overcoming the toughness of the carbon-nanofiber film, the HNTs filling the obviously improved the mechanical performance of the carbon-nanofiber films by the pulling-out and bridging effect. Due to accessing the lipophilic and acid surface, abundant hierarchical pore structure and highly N-doping content, the PAN/HNTs-CNFs exhibited the remarkable adsorption performances for thiophene, benzothiophene, and dibenzothiophene (46.73 mg S/g, 38.4 mg S/g and 35.03 mg S/g for 800 ppm sulfur model oil), especially being suitable to the adsorption of thiophene. Furthermore, the study on the adsorption kinetics, equilibrium isotherms, and thermodynamics of thiophene over the PAN/HNTs-CNFs were conducted to discuss the adsorption mechanism.
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Environmental Science-Nano
·
2020
·Vol. 7
·期 10
·3007-3019
·
IF 7.683
Yingjie He,Lei Huang,Yixian Zhao,Weichun Yang,Taixu Hao,Bichao Wu,Haoyu Deng,Dun Wei,Haiying Wang,Jian Luo
Capacitive deionization (CDI) by Ag@C electrodes is a promising desalination technology for chlorine removal because there is no waste flow and no additional chemicals used during the removal and regeneration/cleaning processes. However, its efficacy and capacity are significantly limited by the low stability of Ag/C composites during the electrochemical process. In this study, we synthesized a new highly stable structure of Ag@C composites (named as Ag/N-CNP) through reductive adsorption of Ag+ by a polyaromatic amine followed by carbonization. We used in situ Raman spectroscopy, for the first time, to monitor in real-time the Cl− electrosorption/desorption process of Ag/N-CNP electrodes, which revealed that the stability of Ag@C electrodes was mainly controlled by the dissolution of Ag. The newly synthesized Ag–Nx structure stabilized Ag nanoparticles and uniformly distributed Ag species on the carbon matrix, which resulted in a high affinity for Cl− and significantly improved cyclic dechlorination performance. Results showed that the electrosorption capacity of the newly synthesized Ag/N-CNP electrodes could reach 75.3 mg g−1, substantially higher than that of traditional carbon electrodes. Moreover, such a capacity had almost no loss (only 1.4% loss) after 50 continuous treatment cycles and could still retain 76% after 100 cycles, demonstrating a highly reliable and cost-effective desalination performance significantly superior to that of previously reported Ag@C electrodes.
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Bioactive Materials
·
2020
·
IF 8.724
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.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
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
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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CHINESE JOURNAL OF POLYMER SCIENCE
·
2021
·Vol. 39
·期 6
·709-715
·
IF 3.603
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.
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ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Wanfeng Wang,Panqing Yang,Yanling Guo,Haoran Ji,Fang Liang
Four phenylurea herbicides (PUHs) were assessed for degradation and transformation into N-nitrosodimethylamine (NDMA) under three oxidation conditions (chlorine (Cl 2 ), chlorine dioxide (ClO 2 ), and ozone (O 3 )) from an aqueous solution. Removal ratios correlated with the numbers of halogen elements contained in PUHs (isoproturon (0) > chlorotoluron (1 Cl) > diuron (2 Cl) > fluometuron (3 F) ), and the degradation efficiencies of oxidants from fastest to slowest were: O 3 , ClO 2 , and Cl 2 . NDMA can be generated directly from the ozonation of PUHs. Further, compared with chloramination alone, ozonation prominently promoted NDMA formation potential (NDMA-FP) during post-chloramination, and NDMA-FPs increased approximately 23–68 times than those during ozonation only at 2.5 mg/L O 3 over 10 min; molar yields of NDMA from highest to lowest were 11.1% (isoproturon), 1.17% (chlorotoluron), 1.0% (diuron), and 0.73% (fluometuron). The PUH degradation kinetics data during ozonation agreed with the pseudo-first-order model. The rate constant k obs were 0.31 × 10 −3 –19.8 × 10 −3 s −1 . The k obs and removal ratios of PUHs during ozonation partially scaled with the mass, LogK ow , and Henry’s constants of PUHs. Comparisons of measured NDMA-FPs with calculated NDMA-FPs from residual PUH after oxidation showed that the intermediates produced during ozonation facilitated NDMA-FPs; this contribution was also observed for chlorotoluron and isoproturon during ClO 2 oxidation. Examination of reaction mechanisms revealed that tertiary amine ozonation, N-dealkylation, hydroxylation, the cleavage of N–C bonds, ammonification , and nitrification occurred during the ozonation of PUHs, and the dimethylamine (DMA) functional groups could be decomposed directly and transformed into NDMA via the formation of the intermediate unsymmetrical dimethylhydrazine . NDMA is also formed from the reaction between DMA and phenylamino-compounds. Clarifying primary degradation products of PUHs and transformation pathways of NDMA during oxidation processes is useful to optimize treatment processes for water supplies.
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JOURNAL OF POWER SOURCES
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2020
·
IF 8.247
Yuan Wang,Hanzhi Wang,Tian C. Zhang,Shaojun Yuan,Bin Liang
A novel hierarchical porous carbon derived from poly(p-phenylenediamine) incorporated with reduced graphene oxide (rGO) is prepared for CO 2 capture and supercapacitors . In this synthesis, chemically in-situ oxidative polymerization and KOH chemical activation are employed with the controllable introduction of GO (GO/Polyphenylenediamine = 0–2 wt%). The obtained carbon material (APG-1%) with high surface area (860.4 m 2 g −1 ) and rich N content (7.91 wt%) exhibits excellent CO 2 capture ability (4.65 mmol g −1 at 298 K, 5 bar) and good electrochemical performance as a supercapacitor electrode with 158.5 F g −1 in 6 M KOH at a current density of 1 A g −1 . Even at a high current density of 10 A g −1 , a capacity of 115.2 F g −1 is still maintained. The rational addition of rGO provides an effective strategy of simultaneous improvement of CO 2 adsorption and capacitive performance.
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LANGMUIR
·
2020
·
IF 3.557
Guangjian Peng,Yiheng Sun,Guijing Dou,Yahao Hu,Weifeng Jiang,Taihua Zhang
Accurate evaluation of the shell elastic modulus of microcapsules is of great significance to understanding their performance during production, processing, and applications. In this work, microcompression was employed to investigate the elastic behaviors of a single microcapsule. It was modeled as a microsphere with a core–shell structure compressed between two rigid plates. Based on the assumption that the contact pressure between the microsphere and plates obeys parabolic distribution, a microcompression method derived from the Reissner’s theory and the modified Hertz contact theory was established to evaluate the shell elastic modulus. Applications were carried out on poly(methylmethacrylate) (PMMA) microcapsules containing n-octadecane. The average elastic modulus of PMMA shells measured by the proposed microcompression method agrees well with that of the bulk PMMA sample. Furthermore, the elastic modulus of PMMA shells was found to have size dependence on the diameter of the microcapsules. Finally, finite element models combined with the newly proposed method were constructed to accurately predict the microcompression behaviors of microcapsules with different sizes.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Xiaoying Zhai,Weiguo Lin,Jinkai Liu,Xu Chen,Junfeng Yong,Wensheng Yang
The development of earth-abundant electrocatalysts to replace noble metal for oxygen reduction reaction (ORR) has attracts tremendous interest. In this work, Fe, N-codoped porous carbon-embedded Fe 3 C nanoparticles (Fe 3 C/Fe, N-PCR) is fabricated from petroleum vacuum residue via a simple template-assisted and subsequent doping-assisted calcination method. The unique hybrid material shows great features: abundant active sites including pyridinic N, Fe N, and Fe 3 C nanoparticles, a relatively large surface area (509.3 m 2 g − 1 ) and 3D interconnected hierarchical porous structure. The Fe 3 C/Fe, N-PCR as an electrocatalyst exhibits remarkable ORR catalytic activity in alkaline medium, with a high onset potential of 1.02 V and half-wave potential of 0.86 V, which surpass commercial Pt/C (20 wt%) by ca. 30 and 20 mV, respectively. Moreover, Fe 3 C/Fe, N-PCR has outstanding long-term stability and tolerance to methanol poisoning, outperforming Pt/C. Combining with the exciting performance, abundant and cheap raw material, and facile synthetic method, Fe 3 C/Fe, N-PCR catalyst has promising future in ORR. This study also provides a new approach for high value utilization of petroleum vacuum residue.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Yang Hui,Chen Yingxi,Wang Chunbao,Wang Guangjin
Because of low-cost, marvelous activity and excellent stability characteristics, nonprecious metal carbide-based catalysts are promising candidates for hydrogen evolution reaction (HER). However, inferior specific surface area and undesirable catalytic activity of pure phase carbides greatly impedes their industrialization process. Herein, ultrafine Mo 2 C nanoparticles embedded in N-doped carbon nanosheet has been synthesized by a facile strategy. High viscosity of guar gum alleviates the aggregation of nanocrystals by providing space-confinement effect; besides, NaCl plays two roles: (1) hard template directing the formation of carbon nanosheet; (2) molten salt adjusting the nucleation and growth process of Mo 2 C to ensure the formation of ultra-small Mo 2 C nanoparticles. Two-dimensional sheet-like carbon accelerates the electron transfer , and rich heterojunction between ultrafine Mo 2 C and N-doped carbon facilitates boosting the HER catalytic activity. The prepared Mo 2 C/NCS with optimized composition exhibit excellent electrocatalytic activity and stability both in acidic (189 mV at a current density of 10 mV/cm 2 with a Tafel slope of 61.2 mV/dec) and alkaline medium (142 mV at a current density of 10 mV/cm 2 with a Tafel slope of 56.1 mV/dec). This work may provide insight for developing economic and high-efficient catalysts for water splitting.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Xiaobin Zhou,Mengke Wang,Junyang Chen,Xiaolei Xie,Xingguang Su
Single atom nanozymes are the artificial enzymes with enzyme-like activity, which have attracted a great deal attention in recent years due to their unique merits such as remarkable stability, excellent atom utilization and low cost. Herein, a convenient and sensitive colorimetric strategy was developed for the sensing of galactose based on Fe–N–C single-atom nanozyme (Fe-SAzyme). The Fe-SAzyme was prepared through “isolation-pyrolysis” method that exhibited intrinsic peroxidase mimicking activity, which can quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce blue-colored oxTMB in the presence of hydrogen peroxide (H 2 O 2 ). Galactose can be oxidized by galactose oxidase (Gal Ox) to generate H 2 O 2 , and Fe-SAzyme can be utilized for quantitative colorimetric detection of galactose. A good linearity between absorbance and the galactose concentration in the range of 50–500 μM was obtained with a detection limit of (LOD) 10 μM. The Fe-SAzyme based colorimetric strategy offered a rapid, convenient and economic way for galactose quantification detection, which could be used as an alternative method for galactosemia diagnosis.
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