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28 Dec 07:27

Piezoelectric Interlayer Enabling a Rechargeable Quasisolid‐State Sodium Battery at 0 °C

by Qing Ni, Yu Ding, Chengzhi Wang, Shiyin Bai, Kunkun Zhu, Yongjie Zhao, Lai Chen, Ning Li, Jingbo Li, Yuefeng Su, Haibo Jin
Piezoelectric Interlayer Enabling a Rechargeable Quasisolid-State Sodium Battery at 0 °C

A piezoelectric interlayer design between an Na3Zr2Si2PO12 solid electrolyte and sodium metal is demonstrated to solve the interfacial issues against low-temperature solid-state sodium batteries. A piezoelectric ZnO layer proves a favorable interlayer with matched modulus, high Na-adhesion, sufficient piezoelectricity to thoroughly reduce the interfacial resistance and promote a quasi-solid-state Na2MnFe(CN)6-based full cell operating at a harsh condition of 0 °C.


Abstract

Solid-state sodium (Na) batteries (SSNBs) hold great promise but suffer from several major issues, such as high interfacial resistance at the solid electrolyte/electrode interface and Na metal dendrite growth. To address these issues, a piezoelectric interlayer design for an Na3Zr2Si2PO12 (NZSP) solid electrolyte is proposed herein. Two typical piezoelectric films, AlN and ZnO, coated onto NZSP function as interlayers designed to generate a local stress-induced field for alleviating interfacial charge aggregation coupling stress concentration and promoting uniform Na plating. The results reveal that the interlayer (ZnO) with matched modulus, high Na-adhesion, and sufficient piezoelectricity can provide a favorable interphase. Low interfacial resistances of 91 and 239 Ω cm2 are achieved for the ZnO layer at 30 and 0 °C, respectively, which are notably lower than those for bare NZSP. Moreover, steady Na plating/stripping cycles are rendered over 850 and 4900 h at 0 and 30 °C, respectively. The superior anodic performance is further manifested in an Na2MnFe(CN)6-based full cell which delivers discharge capacities of 125 mA h g−1 over 1600 cycles at 30 °C and 90 mA h g−1 over 500 cycles at 0 °C. A new interlayer-design insight is clearly demonstrated for SSNBs breaking low-temperature limits.

04 Sep 04:22

Green synthesis of metal oxide nanostructures using naturally occurring compounds for energy, environmental, and bio-related applications

New J. Chem., 2019, 43,15846-15856
DOI: 10.1039/C9NJ03311D, Perspective
Brian Yuliarto, Ni Luh Wulan Septiani, Yusuf Valentino Kaneti, Muhammad Iqbal, Gilang Gumilar, Minjun Kim, Jongbeom Na, Kevin C.-W. Wu, Yusuke Yamauchi
This review summarizes the synthesis and functional applications of metal oxide nanostructures synthesized using plant-derived phytochemicals for energy, environmental, and biomedical applications.
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05 Jan 01:53

Correction for “Measurement of Hanatoxin-Induced Membrane Thinning with Lamellar X-ray Diffraction”

by Meng-Hsuan Hsieh, Yu-Shuan Shiau, Horng-Huei Liou, U-Ser Jeng, Ming-Tao Lee and Kuo-Long Lou
Langmuir
DOI: 10.1021/acs.langmuir.7b04276
04 Jan 06:49

Design of a porous cobalt sulfide nanosheet array on Ni foam from zeolitic imidazolate frameworks as an advanced electrode for supercapacitors

Nanoscale, 2018, 10,2735-2741
DOI: 10.1039/C7NR07931A, Paper
Xue Han, Kai Tao, Ding Wang, Lei Han
A porous Co9S8 nanosheet array on Ni foam can be realized via a facile 2D ZIF templated method.
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19 Jun 07:34

Nitrogen-doped graphene guided formation of monodisperse microspheres of LiFePO4 nanoplates as the positive electrode material of lithium-ion batteries

J. Mater. Chem. A, 2016, 4,12065-12072
DOI: 10.1039/C6TA03440C, Paper
Yingke Zhou, Jiming Lu, Chengji Deng, Hongxi Zhu, George Z. Chen, Shaowei Zhang, Xiaohui Tian
Three-dimensional porous composite microspheres of LiFePO4 and nitrogen-doped graphene have been synthesized by a solvothermal process coupled with subsequent calcination.
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01 Jun 13:20

[In Depth] Why humans are the high-energy apes

by Ann Gibbons
We may not be raring to go on a Monday morning, but humans are the Energizer Bunnies of the primate world. That's the conclusion of a new study that for the first time measures precisely how many calories humans and apes burn each day. Compared with chimpanzees and other apes, our revved-up internal engines burn calories 27% faster, according to a paper in Nature this week. This higher metabolic rate equips us to quickly fuel energy-hungry brain cells, paving the way for our bigger brains. And lest we run out of gas when food is short, the study also found that humans are fatter than other primates, giving us energy stores to draw on in lean times. Author: Ann Gibbons
05 Mar 07:25

[Report] Selective conversion of syngas to light olefins

by Feng Jiao
Although considerable progress has been made in direct synthesis gas (syngas) conversion to light olefins (C2=–C4=) via Fischer-Tropsch synthesis (FTS), the wide product distribution remains a challenge, with a theoretical limit of only 58% for C2–C4 hydrocarbons. We present a process that reaches C2=–C4= selectivity as high as 80% and C2–C4 94% at carbon monoxide (CO) conversion of 17%. This is enabled by a bifunctional catalyst affording two types of active sites with complementary properties. The partially reduced oxide surface (ZnCrOx) activates CO and H2, and C−C coupling is subsequently manipulated within the confined acidic pores of zeolites. No obvious deactivation is observed within 110 hours. Furthermore, this composite catalyst and the process may allow use of coal- and biomass-derived syngas with a low H2/CO ratio. Authors: Feng Jiao, Jinjing Li, Xiulian Pan, Jianping Xiao, Haobo Li, Hao Ma, Mingming Wei, Yang Pan, Zhongyue Zhou, Mingrun Li, Shu Miao, Jian Li, Yifeng Zhu, Dong Xiao, Ting He, Junhao Yang, Fei Qi, Qiang Fu, Xinhe Bao
23 Feb 04:02

Core–Shell Nanocomposites Based on Gold Nanoparticle@Zinc–Iron-Embedded Porous Carbons Derived from Metal–Organic Frameworks as Efficient Dual Catalysts for Oxygen Reduction and Hydrogen Evolution Reactions

by Jia Lu, Weijia Zhou, Likai Wang, Jin Jia, Yunting Ke, Linjing Yang, Kai Zhou, Xiaojun Liu, Zhenghua Tang, Ligui Li and Shaowei Chen

TOC Graphic

ACS Catalysis
DOI: 10.1021/acscatal.5b02302
15 Feb 13:56

N2O decomposition on CoOx, CuOx, FeOx or MnOx supported on ZrO2: The effect of zirconia doping with sulfates or K+ on catalytic activity

Publication date: 15 June 2016
Source:Applied Catalysis B: Environmental, Volume 187
Author(s): Daniela Pietrogiacomi, Maria Cristina Campa, Lea Roberta Carbone, Simonetta Tuti, Manlio Occhiuzzi
Zirconia doped with sulfates or K+ were prepared by impregnation with (NH4)2SO4, or KNO3 aqueous solutions. MeOx/ZrO2 and MeOx/doped-ZrO2 catalysts (Me=Co, Cu, Fe or Mn) were prepared by wet impregnation of zirconia and doped-zirconia supports. The effect of doping on MeOx properties was studied by XRD, UV–vis DRS, H2-TPR and FTIR and the influence of doping on the catalytic activity for N2O decomposition was investigated under ideal conditions (N2O in He) and under real reaction conditions (addition of NO, O2, and water vapour to the reactant mixture). Characterization results indicated that all samples contained mainly dispersed Men+ species interacting with the support. In MeOx/sulfated-ZrO2 the doping with electron-withdrawing sulfates stabilized the Men+ oxidation state. In CoOx/K-ZrO2 samples the doping with electron-releasing K+ increased the poly-nuclear CoOx reducibility. FTIR characterization suggested that the electron-donor capacity of Co2+ site had the order CoOx/sulfated-ZrO2 <CoOx/ZrO2 <CoOx/K-ZrO2. Catalytic results showed that dispersed Men+ are the active site for N2O decomposition on MeOx/ZrO2. The “twin peak pattern” of catalytic activity versus tmi d-electron number suggests that formation and stability of the intermediate Me(n+1)+O- surface complex, requiring the mobility of Men+ oxidation state, are key factors for activity. Because the electron-withdrawing sulfates lowered the electron-donor capacity of tmi, hindering the formation of Me(n+1)+O-, the effect of sulfate-doping was to decrease the deN2O activity in MeOx/sulfated-ZrO2. Conversely, because the electron-releasing potassium cation increased electron-donor capacity of Co2+, yielding an easier formation of the intermediate surface complex, the effect of K-doping was to increase the deN2O activity in CoOx/K-ZrO2. From an applied viewpoint, cobalt supported on ZrO2 and K-doped ZrO2 systems, that were affected by reversible inhibitory effect in real reaction conditions, are interesting catalysts for N2O abatement and for simultaneous abatement of N2O and NO with hydrocarbons.

Graphical abstract

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14 Feb 06:33

In situ synthesis of In2S3@MIL-125(Ti) core–shell microparticle for the removal of tetracycline from wastewater by integrated adsorption and visible-light-driven photocatalysis

Publication date: 5 June 2016
Source:Applied Catalysis B: Environmental, Volume 186
Author(s): Hou Wang, Xingzhong Yuan, Yan Wu, Guangming Zeng, Haoran Dong, Xiaohong Chen, Lijian Leng, Zhibin Wu, Lijuan Peng
Metal-organic frameworks (MOFs) have been attracted considerable attention in the field of energy generation and environmental remediation. In this article, a novel core–shell In2S3@MIL-125(Ti) (MLS) photocatalytic adsorbent was successfully prepared by a facile solvothermal method. The as-obtained materials were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, N2 adsorption–desorption isotherm, X-ray photoelectron spectroscopy, UV–vis diffuse reflection spectroscopy and zeta potentials. It is indicated that the hybrids consisted of MIL-125(Ti) as the core and three-dimensional In2S3 sheets network as the shell has high surface area, mesoporous structure, and improved electronegativity and visible-light absorption. The MLS exhibited excellent adsorption performance for the removal of tetracycline (TC) from water. The adsorption process is sensitive to the solution pH, ionic strength and initial TC concentration. The Langmuir isotherm and pseudo-second-order mode could well describe the adsorption process and adsorption kinetics. The adsorption mechanism is mainly responsible for surface complexation, π–π interactions, hydrogen bonding and electrostatic interactions. Further, in TC degradation experiments under visible light exposure in presence of core–shell MLS, the optimal additive content of MIL-125(Ti) in synthesis process was 0.1g, and the corresponding photodegradation efficiency for TC was 63.3%, which was higher than that of pure In2S3 and pure MIL-125(Ti). The improved photocatalytic performance was mainly ascribed to the opened porous structure, effective transfer of photo-generated carriers, Ti3+–Ti4+ intervalence electron transfer and the synergistic effect between MIL-125(Ti) and In2S3. The degradation by-products of TC molecules were monitored by three-dimensional excitation-emission matrix fluorescence spectroscopy. Parts of TC molecules were mineralized into CO2 and H2O. The core–shell MLS composites also revealed good performance for the removal of TC from real wastewater including medical wastewater, municipal wastewater and river water. Therefore, the novel hybrids may be used as promising photocatalytic adsorbent for wastewater purification.

Graphical abstract

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18 Nov 05:38

[Association Affairs] Gordon Research Conferences

This issue of Science includes the program of the 2016 AAAS Annual Meeting. 2016 “Session I” Meetings will be held between January 9 and March 25 in Ventura, CA and Galveston, TX in the United States, and internationally in the Tuscany region of Italy. A PDF of the program as it appears in this issue is available here; for more information on the meeting (including registration forms and information on accommodations), please visit www.grc.org.
20 Aug 03:04

3D Mesoporous Graphene: CVD Self-Assembly on Porous Oxide Templates and Applications in High-Stable Li-S Batteries

by Jia-Le Shi, Cheng Tang, Hong-Jie Peng, Lin Zhu, Xin-Bing Cheng, Jia-Qi Huang, Wancheng Zhu, Qiang Zhang

A nanostructured carbon with high specific surface area (SSA), tunable pore structure, superior electrical conductivity, mechanically robust framework, and high chemical stability is an important requirement for electrochemical energy storage. Porous graphene fabricated by chemical activation and liquid etching has a high surface area but very limited volume of electrochemically accessible mesopores. Herein, an effective strategy of in situ formation of hierarchically mesoporous oxide templates with small pores induced by Kirkendall diffusion and large pores attributed to evaporation of deliberately introduced volatile metal is proposed for chemical vapor deposition assembly of porous graphene frameworks (PGFs). The PGFs inherit the hierarchical mesoporous structure of the templates. A high SSA of 1448 m2 g−1, 91.6% of which is contributed by mesopores, and a mesopore volume of 2.40 cm3 g−1 are attained for PGFs serving as reservoirs of ions or active materials in electrochemical energy storage applications. When the PGFs are applied in lithium-sulfur batteries, a very high sulfur utilization of 71% and a very low fading rate of ≈0.04% per cycle after the second cycle are achieved at a current rate of 1.0 C. This work provides a general strategy for the rational construction of mesoporous structures induced by a volatile metal, with a view toward the design of hierarchical nanomaterials for advanced energy storage.

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Porous graphene frameworks (PGFs) are fabricated on hierarchically mesoporous oxide templates with small pores induced by Kirkendall diffusion and large pores attributed to evaporation of a deliberately introduced volatile metal. A high specific surface area of 1448 m2 g−1 and large mesopore volume of 2.40 cm3 g−1 are attained for PGFs serving as reservoirs of ions or active materials in lithium-sulfur batteries.

17 Jul 00:27

Highly efficient polymer solar cells cast from non-halogenated xylene/anisaldehyde solution

Energy Environ. Sci., 2015, 8,2744-2752
DOI: 10.1039/C5EE01917F, Paper
Christian Sprau, Felix Buss, Michael Wagner, Dominik Landerer, Manuel Koppitz, Alexander Schulz, Daniel Bahro, Wilhelm Schabel, Philip Scharfer, Alexander Colsmann
Several high performance polymer:fullerene bulk-heterojunctions are deposited from non-halogenated xylene/anisaldehyde solution, yielding power conversion efficiencies up to 9.5%.
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11 May 12:42

Selective Hydrogenation of Furfural to Furfuryl Alcohol in the Presence of a Recyclable Cobalt/SBA-15 Catalyst

by Maïté Audemar, Carmen Ciotonea, Karine De Oliveira Vigier, Sébastien Royer, Adrian Ungureanu, Brindusa Dragoi, Emil Dumitriu, François Jérôme

Abstract

The hydrogenation of furfural to furfuryl alcohol was performed in the presence of a Co/SBA-15 catalyst. High selectivity (96 %) at a conversion higher than 95 % is reported over this catalytic system. As the conversion of furfural to furfuryl alcohol occurs over metallic Co sites, the effect of reduction temperature, H2 pressure, and reaction temperature were studied. Optimum reaction conditions were: 150 °C, 1.5 h, 2.0 MPa of H2. The catalyst was recyclable, and furfuryl alcohol was recovered with a purity higher than 90 %. The effect of the solvent concentration was also studied. With a minimum of 50 wt % of solvent, the selectivity to furfuryl alcohol and the conversion of furfural remained high (both over 80 %). Likewise, the activity of the catalyst is maintained even in pure furfural, which confirms the real potential of the proposed catalytic system. This catalyst was also used in the hydrogenation of levulinic acid to produce γ-valerolactone selectively.

Thumbnail image of graphical abstract

The fast and the furfural: Furfuryl alcohol is produced from furfural with a yield of 88 % in the presence of a recyclable and stable Co/SBA-15 catalyst at 150 °C under H2 pressure in ethanol. This catalyst is also active and selective in the hydrogenation of levulinic acid to γ-valerolactone.

11 Dec 16:01

Synthesis and structure of 8-tetrahydrofuronium and 8-tetrahydropyronium derivatives of iron bis(dicarbollide)(-I) and their ring cleavage reactions. Design of novel ferracarborane ligands and nucleoside conjugates

Dalton Trans., 2014, Accepted Manuscript
DOI: 10.1039/C4DT03015J, Paper
Irina Lobanova, Irina Kosenko, Julia Laskova, Ivan Ananyev, Anna Druzina, Ivan Godovikov, Vladimir I Bregadze, Shicheng Qi, Zbigniew Jan Lesnikowski, Andrey Semioshkin
8-Tetrahydrofuronium and 8-tetrahydropyronium derivatives of iron bis(dicarbollide)(-I) were synthesized. Their reactions of ring cleavage by MeOH, N3-, amines and 1,2-bis(diphenylphosphino)ethane were investigated. 8-Tetrahydrofuronium iron bis(dicarbollide)(-I) was found to be more...
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07 Dec 12:18

Polymer supported ZIF-8 membranes prepared via an interfacial synthesis method

Chem. Commun., 2015, 51,918-920
DOI: 10.1039/C4CC06699E, Communication
Yanbo Li, Lik H. Wee, Alexander Volodin, Johan A. Martens, Ivo F. J. Vankelecom
Polyethersulfone supported continuous ZIF-8 membranes were prepared via an interfacial synthesis method. These membranes showed excellent performance in the nanofiltration range.
The content of this RSS Feed (c) The Royal Society of Chemistry