INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
·
IF 4.229
Zhao Jiang,Xiang Gong,Bin Wang,Zhiqiang Wu,Tao Fang
Liquid organic hydrogen carrier (LOHC) is considered as a promising candidate for large-scale hydrogen storage. In this work, we found that Pt/TiO 2 catalysts exhibited better catalytic activity and selectivity compared to Pd/TiO 2 and commercial Pd/Al 2 O 3 catalysts in the dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NECZ) at 453 K. The catalytic activity of the noble metal catalysts followed the trend of Pt/TiO 2 > Pd/TiO 2 > Rh/TiO 2 > Au/TiO 2 > Ru/TiO 2 . Compared with the commercial Pd/Al 2 O 3 , Pt/TiO 2 greatly improved the selectivity and conversion rate, the reaction time was also shortened. In addition, kinetics calculation was carried out to obtain fundamental reaction parameters. It was found that the third step of 4H-NECZ dehydrogenation to NECZ was the rate-limiting step of the entire dehydrogenation reaction for all catalysts.
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ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Dongxing Tan,Jianling Zhang,Jinbiao Shi,Shaopeng Li,Bingxing Zhang,Xiuniang Tan,Fanyu Zhang,Lifei Liu,Dan Shao,Buxing Han
To develop photocatalysts with desirable compositions and structures for improving the efficiency and selectivity of CO2 conversion to CH4 under mild conditions is of great importance. Here, we design an effective photocatalyst of bimetal (Ag/Pd) nanoalloys supported on nitrogen-doped TiO2 nanosheet for CO2 conversion. Such a novel photocatalyst combines multiple advantages of abundant Ti3+ ions, oxygen vacancies, and substitutional nitrogen that are favorable for catalyzing CO2 reduction. It was found that CO2 could be efficiently transformed to CH4 under mild conditions, i.e., in aqueous solution and at atmospheric pressure and room temperature. The maximum production rate of CH4 can reach 79.0 μmol g–1 h–1. Moreover, the Ag/Pd bimetals supported on N-doped TiO2 nanosheet exhibit high selectivity to CH4. The as-synthesized photocatalyst can be well recycled for CO2 reduction.
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NANO
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2018
·
IF 1.1
Jing Liu,Xiao Li,Xin Gong,Taiping Qing,Peng Zhang,Bo Feng
The incorporation of dopant atoms alters the structure of MoS 2 , resulting in unique properties and practical applications. Herein, a facile and low-cost approach for producing N-doped molybdenum disulfide (N-MoS 2 ) was carried out using melamine and MoS 2 in a laboratory tube furnace at 400 ∘ C for 2 h. The N-MoS 2 fluorescent probe showed sensitive response to Hg 2 + in a wide concentration range of 0.4–10 μ M with a low limit of 28 nM. The practical applicability of detecting Hg 2 + in lake water samples may open a new way to evaluate Hg 2 + in wastewater.
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ACS Applied Energy Materials
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2018
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IF 0
Nan Jia,Qiaozhen Xu,Fengqi Zhao,Hong-Xu Gao,Jiaxin Song,Pei Chen,Zhongwei An,Xinbing Chen,Yu Chen
The electrochemical kinetics of oxygen reduction reaction (ORR) determines the energy conversion efficiency of fuel cells and metal–air batteries. Thus, developing efficient and low-cost electrocatalysts for the ORR has attracted mounting attention. Herein, a facile synthetic route is presented to achieve atomic dispersion of Fe–Nx species in N doped porous carbon nanocages, resulting in a single-atom ORR electrocatalyst. The obtained Fe/N codoped carbon nanocages exhibit a comparable half-wave potential (0.82 V) and higher limiting current density compared to the commercial Pt/C electrocatalyst. In addition, by using it as air electrode electrocatalyst, the assembled Zn–air battery device shows a specific capacity of 705 mAh g–1 at 5 mA cm–2 and a negligible voltage loss after continuous operation for 67 h. The superior performance of Fe/N codoped carbon nanocages is attributed to the porous structure and the synergetic effect of atomically dispersed Fe–Nx species and N doping.
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ELECTROCHIMICA ACTA
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2018
·
IF 5.116
Chao Li,Jing Xue,Ao Huang,Jing Ma,Fangzhu Qing,Aijun Zhou,Zhihong Wang,Yuehui Wang,Jingze Li
Owing to the unique redox reaction and the relative low molar mass of the repeating unit, poly(N-vinylcarbazole) (PVK) was selected as an advanced organic cathode for potassium-ion-based dual-ion battery (PDIB) with the K foil anode and KPF 6 -based electrolyte. The operation mechanism of this PDIB is that PF 6 − anions are migrated from the electrolyte and incorporated into PVK cathode via the attraction to the positively charged N atom of carbazole ligand, and then are released into the electrolyte in the subsequent discharge process; simultaneously, K + cations are reversibly stored/removed in/from the anode during charging/discharging. It shows a high median operation potential of 4.05 V vs. K + /K and can achieve a high specific capacity of 117 mAh g −1 at 20 mA g −1 , which is close to its theoretical value of 138 mAh g −1 . More impressively, even at the highest current density of 2000 mA g −1 for 500 cycles, a high average specific capacity of 61 mAh g −1 can still be obtained with capacity rentation of 55%.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Qijie Mo,Wenbiao Zhang,Liuqing He,Xiang Yu,Qingsheng Gao
Exploring noble-metal-free electrocatalysts for hydrogen evolution reaction (HER) is the key issue in hydrogen economy blueprint. Herein, bimetallic Ni 2-x Co x P supported by N-doped carbon nanofibers (denoted as Ni 2-x Co x P/N-C NFs) are developed via electrospinning followed by pyrolysis under an inert flow. The space confinement by in-situ formed N-doped carbon matrix produces ultrafine Ni 2-x Co x P with abundant active-sites. More importantly, the engineering on Ni 2-x Co x P solid-solution-alloys can vary electronic configuration and consequently optimize hydrogen binding on electrocatalyst surface, accomplishing prominent HER activity in a wide pH range. The optimal Ni 2-x Co x P/N-C NFs afford low overpotentials ( η 10 ) of 100, 130 and 110 mV to reach a current density of -10 mA cm −2 in 0.5 M H 2 SO 4 , 1.0 KOH and 1.0 M PBS (phosphate buffer saline), respectively, performing among the best of noble-metal-free electrocatalysts. With a good functionality for oxygen evolution ( η 10 = 280 mV), such composite further delivers a high efficiency for overall water splitting, featuring a comparable cell voltage (1.56 V @ 10 mA cm −2 ) to a commercial IrO 2 /C − Pt/C couple, and remarkably better stability. Identifying electrocatalysis relying on solid-solution alloys, this work will inspire the exploration of cost-efficient electrocatalysts and the new understanding on catalytic mechanisms.
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MOLECULES
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2018
·Vol. 23
·期 7
·1521
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IF 3.098
Xiangmin Song,Chunjuan Liu,Peiqi Chen,Hao Zhang,Ranfeng Sun
Natural products are an important source of pesticide discovery. A series ofN-amino-maleimide derivatives containing hydrazone group were designed and synthesized based on the structure of linderone and methyllinderone which were isolated fromLindera erythrocarpaMakino. According to the bioassay results, compounds2and3showed 60% inhibition against mosquito (Culex pipiens pallens) at 0.25 µg·mL−1. Furthermore, the results of antifungal tests indicated that most compounds exhibited much better antifungal activities against fourteen phytopathogenic fungi than linderone and methyllinderone and some compounds exhibited better antifungal activities than commercial fungicides (carbendazim and chlorothalonil) at 50 µg·mL−1. In particular, compound12exhibited broad-spectrum fungicidal activity (>50% inhibitory activities against 11 phytopathogenic fungi) and compounds12and14displayed 60.6% and 47.9% inhibitory activity againstRhizoctonia cerealisat 12.5 µg·mL−1respectively. Furthermore, compound17was synthesized, which lacks N-substituent at maleimide and its poor antifungal activity againstSclerotinia sclerotiorumandRhizoctonia cerealisat 50 µg·mL−1showed that the backbone structure ofN-amino-maleimide derivatives containing hydrazone group was important to the antifungal activity.Keywords:maleimide;linderone;methyllinderone;antifungal activity
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ACS Applied Bio Materials
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2018
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IF 0
Jianjun Luo,Xing Zhang,Jeremiah Ong’achwa Machuki,Chengbai Dai,Yang Li,Kaijin Guo,Fenglei Gao
Composite biomaterials with hierarchical structures have emerged as new approaches for bone-tissue engineering. In this study, a biomimetic, osteoconductive tricomposite scaffold made of N-doped graphene–hydroxyapatite (NG–HA) hybrids blended with an agarose (AG) matrix was prepared via a facile hydrothermal/cross-linking/freeze-drying method. The structure and composition of AG/NG–HA were examined by scanning electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, Fourier transform infrared, Raman spectroscopy, and thermogravimetric analysis. The as-prepared scaffolds showed hierarchical pore architecture and an organic–inorganic composition, which simulated the composition and structure of natural bone tissue. The effect of AG/NG–HA on bone mesenchymal stem cells (MSCs) osteoblast proliferation, differentiation, and mineralization was tested in vitro. The expression of osteogenic-related genes was determined by real-time polymerase chain reaction. Our results showed that the introduction of N-graphene into the hybrid scaffold significantly improved its mechanical properties, an effect that promoted the proliferation and viability of MSCs. Moreover, the scaffolds triggered selective differentiation of MSCs to osteogenic lineage while conferring good cell adhesion, enhanced alkaline phosphatase activity, and mineralization. A distal femoral condyle critical size defect in rabbits was used as a platform to confirm the effect of AG/NG–HA on bone regeneration in vivo. Our experiments show that the AG/NG–HA hybrid scaffolds provided a favorable environment for new bone formation. The results presented in this study suggest that the AG/NG–HA hybrid scaffolds have potential in bone-tissue regeneration engineering.
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JOURNAL OF MATERIALS SCIENCE
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2018
·Vol. 54
·期 6
·4589-4600
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IF 2.993
Tan Jiabin,He Xiaobo,Yin Fengxiang,Liang Xin,Chen Biaohua,Li Guoru,Yin Huaqiang
In this study, a β-Mo 2 C/N, P-co-doped carbon (NPC) catalyst with a porous structure of β-Mo 2 C nanoparticles loading on NPC matrix was prepared by vacuum-rotary evaporation and followed by a facile pyrolysis process for hydrogen evolution reaction (HER). The porous structure is beneficial for exposing more active sites and the mass transfer during the HER. In addition, the carbon matrixes with the highly doped N and P heteroatoms also provide their positive contributions to its high catalytic activity for HER. Owing to the advantages mentioned above, the optimized catalyst shows a small overpotential of 181 mV for driving a cathodic current density of 10 mA cm −2 , a low Tafel slope of 65.3 mV dec −1 and a high exchange current density of 1.5 × 10 −2 mA cm −2 during HER processes in acid electrolyte. The excellent performance of the β-Mo 2 C/NPC makes it a great potential candidate as the HER electrocatalyst.
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Frontiers of Chemical Science and Engineering
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2018
·Vol. 12
·期 3
·346-357
·
IF 2.643
Zhang Chao,Lu Chenbao,Bi Shuai,Hou Yang,Zhang Fan,Cai Ming,He Yafei,Paasch Silvia,Feng Xinliang,Brunner Eike,Zhuang Xiaodong
Porous polymers have been recently recognized as one of the most important precursors for fabrication of heteroatom-doped porous carbons due to the intrinsic porous structure, easy available heteroatom-containing monomers and versatile polymerization methods. However, the heteroatom elements in as-produced porous carbons are quite relied on monomers. So far, the manipulating of heteroatom in porous polymer derived porous carbons are still very rare and challenge. In this work, a sulfur-enriched porous polymer, which was prepared from a diacetylene-linked porous polymer, was used as precursor to prepare S-doped and/or N-doped porous carbons under nitrogen and/or ammonia atmospheres. Remarkably, S content can sharply decrease from 36.3% to 0.05% after ammonia treatment. The N content and specific surface area of as-fabricated porous carbons can reach up to 1.32% and 1508 m 2 ∙g –1 , respectively. As the electrode materials for electrical double-layer capacitors, as-fabricated porous carbons exhibit high specific capacitance of up to 431.6 F∙g –1 at 5 mV∙s –1 and excellent cycling stability of 99.74% capacitance retention after 3000 cycles at 100 mV∙s –1 . Furthermore, as the electrochemical catalysts for oxygen reduction reaction, as-fabricated porous carbons presented ultralow half-wave-potential of 0.78 V versus RHE. This work not only offers a new strategy for manipulating S and N doping features for the porous carbons derived from S-containing porous polymers, but also paves the way for the structureperformance interrelationship study of heteroatoms codoped porous carbon for energy applications.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2018
·Vol. 165
·期 7
·H348
·
IF 3.662
Le Wang,Hangjia Shen,Sanshuang Gao,Xamxikamar Mamat,Guangzhi Hu
As an excellent catalyst toward hydrogen peroxide reduction, Fe-based nanomaterial like Fe-N-C configuration is promising candidate to be used for H2O2 sensing. In this work, a novel N-doped mesoporous carbon by atomically dispersed Fe-N dopant composite modified electrode (Fe/NOMC) was prepared by hard template approach and then fabricated non-enzymatic sensor was used for H2O2 determination. The morphology and property of Fe/NOMC composite were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX), small angle X-ray diffraction (XRD) spectrum and nitrogen-sorption measurement, respectively. The electrochemical sensing performance of the Fe/NOMC composite modified glassy carbon electrode (GCE) was studied by cyclic voltammetry and chronoamperometry methods. An excellent performance toward hydrogen peroxide reduction was achieved in a wide range of 8–23000 μM, with limitation of detection (LOD) about 5 μM and a correlation coefficient of 0.998, as well as a short response time (2 s) and good selectivity.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2018
·
IF 3.649
Yujing Chen,Chuang Li,Xiao Chen,Yan Liu,Changhai Liang
Highly crystallized ZSM-23 zeolite samples were synthesized by employing the dual structure directing agents pyrrolidine (PY) and isopropylamine (IPA). The existence of two types of structure directing agents widened the synthesis composition ratio range and speeded up the crystallization. The samples obtained showed larger micropore surface areas and volumes compared with the products synthesized with single SDA. It was found that the use of the dual-structure directing agent had no effect on the total acidity but altered the acid site distribution where more weak and medium acidic sites were exposed and was found to be more suitable for n-hexadecane hydroisomerization. The bifunctional catalysts prepared from the supports using the dual-structure directing agent showed excellent catalytic performance under certain reaction conditions. It was noteworthy that Pt/PI-200 (Pt supported on the dual-structure directing agent with a SiO 2 /Al 2 O 3 ratio of 200) showed a constant selectivity to iso-hexadecane ca. 69% with contact time of 0.75 min and longer.
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