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ChemSusChem

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https://www.readbyqxmd.com/read/28941193/discovery-of-open-cubane-core-structures-for-biomimetic-lnco3-or-4-water-oxidation-catalysts
#1
Sandra Luber, Mauro Schilling, Florian Hodel
Bio-mimetic catalysts such as {LnCo3(OR)4} (Ln = Er, Tm, OR = alkoxide) cubanes have recently been in the focus of research for artificial water oxidation processes. Previously the remarkable adaptability with respect to ligand shell, nuclear structure as well as protonation and oxidation states of those catalysts has been shown to be beneficial for the water oxidation process. We further explored the structural flexibility of those catalysts and present here a series of novel structures in which one metal center is pulled out of the cubane cage...
September 22, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28941070/non-aqueous-primary-li-air-flow-battery-and-optimization-of-its-cathode-through-experiments-and-modeling
#2
Byoungsu Kim, Kensuke Takechi, Sichao Ma, Sumit Verma, Shiqi Fu, Amit Desai, Ashtamurthy S Pawate, Fuminori Mizuno, Paul Kenis
We develop a primary Li-air battery with a flowing Li-ion free ionic liquid as the recyclable electrolyte, boosting power capability due to promoted superoxide diffusion and enhancing discharge capacity due to separately stored discharge products. Also we use experimental and computational tools to analyze cathode properties leading to a set of parameters that improve the discharge current density of the non-aqueous Li-air flow battery. We systematically modified the structure and configuration of the cathode gas diffusion layers (GDLs) by using different levels of hot-pressing and the presence or absence of a microporous layer (MPL)...
September 22, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28941209/bivo4-fern-architectures-a-competitive-anode-for-li-ion-batteries
#3
Deepak Dubal, Deepak Patil, Santosh Patil, N R Munirathnam, Pedro Gomez-Romero
The search of high-performance anode materials for Lithium-ion batteries (LIBs) is currently one of the most important tasks. Herein, we are introducing BiVO4 fern architectures as a new anode material for LIBs. The BiVO4 fern shows an excellent reversible capacity of 769 mAh/g (ultrahigh volumetric capacity of 3984 mAh/cm3) at 0.12 A/g with a great capacity retention. Later, a LIB full cell is assembled with BiVO4 ferns as anode and LiFePO4 (LFP, commercial) as cathode material. Notably, the device can achieve the capacity of 140 mAh/g at 1C rate that is 81 % of the capacity of cathode and maintained to 104 mAh/g at high C-rate of 8C, which makes BiVO4 a promising candidate as high-energy anode materials for LIBs...
September 21, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28941180/reactive-electrophilic-oi-species-evidenced-in-high-performance-ir-oxohydroxide-water-oxidation-electrocatalysts
#4
Cyriac Massué, Verena Pfeifer, Maurice Van Gastel, Johannes Noack, Gerardo Algara-Siller, Sebastien Cap, Robert Schlögl
Although quasi-amorphous Ir-oxohydroxides have repeatedly been identified as superior oxygen evolution reaction (OER) electrocatalysts, an exact description of the performance relevant species has so far remained a challenge. In this context, we report on the characterization of hydrothermally prepared IrIII/IV oxohydroxides exhibiting exceptional OER-performance. It was found that holes in the O2p states of IrIII/IV-oxohydroxides result in reactive OI--species identified by characteristic NEXAFS-features. A prototypical titration reaction based on CO as a probe molecule shows that these OI--species are highly susceptible to nucleophilic attack at room temperature...
September 21, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28940995/preparation-of-cobalt-based-electrodes-by-physical-vapor-deposition-on-various-nonconductive-substrates-for-electrocatalytic-water-oxidation
#5
Yizhen Wu, Le Wang, Mingxing Chen, Zhaoxia Jin, Wei Zhang, Rui Cao
Artificial photosynthesis requires efficient anodic electrode materials for water oxidation. We herein report the facial preparation of Co metal thin films through physical vapor deposition (PVD) on various nonconductive substrates, including regular and quartz glass, mica sheet, polyimide, and polyethylene terephthalate (PET). Subsequent surface electrochemical modification using cyclic voltammetry (CV) makes these films active for electrocatalytic water oxidation by reaching a current density of 10 mA cm-2 at a low overpotential of 330 mV in 1...
September 21, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28940828/interface-manipulation-improving-plasmon-coupled-photoelectrochemical-water-splitting-on-%C3%AE-fe2o3-photoanodes
#6
Zhe Xu, Zhongwen Fan, Zhan Shi, Mengyu Li, Jianyong Feng, Lang Pei, Chenguang Zhou, Junkang Zhou, Lingxia Yang, Wenchao Li, Guangzhou Xu, Shicheng Yan, Zhigang Zou
Plasmon resonance effect of metal nanoparticles (NPs) offers a promising route to improve the solar energy conversion efficiency of semiconductors. Here, we found that the hot electrons generated by plasmon resonance effect of Au NPs tend to inject into the surface states instead of the conduction band of Fe2O3 photoanodes, then the severe surface recombination occurs. Such an electron transfer process seems to be independent on external applied potentials, but is sensitive to metal-semiconductor interface properties...
September 21, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28940717/imidazolium-ions-with-an-alcohol-substituent-for-enhanced-electrocatalytic-reduction-of-co2
#7
Xianbo Jin, Lin Zhang, Nian Wu, Jichen Zhang, Yang Hu, Zhiyong Wang, Lin Zhuang
Electrochemical reduction of CO2 to CO is attractive for carbon dioxide reduction, energy regeneration and storage. Imidazolium Ionic liquids (IMILs) are promising electrolyte catalysts for this important reaction. Herein we report functionalizing the imidazolium ion with a propanol substituent at the N site can significantly enhance the catalytic activity of IMILs, causing a positive shift of the onset potential for the CO2 reduction by about 90 mV in an acetonitrile electrolyte. Theoretical calculation indicated that the propanol hydroxyl could bridge a local hydrogen bonding chain as shortcut for proton transfer, leading to a dramatic decrease of the activation barrier for the IMIL-catalytic reduction of CO2...
September 20, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28929590/enhancing-photocurrent-generation-in-photosynthetic-reaction-center-based-photoelectrochemical-cells-with-biomimetic-dna-antenna
#8
Anne-Marie Carey, Haojie Zhang, Minghui Liu, Daiana Sharaf, Natalie Akram, Hao Yan, Su Lin, Neal Woodbury, Dong-Kyun Seo
3 to 4 times higher performance of biohybrid photoelectrochemical cells with photosynthetic reaction centers (RC) has been achieved by using a DNA-based biomimetic antenna. Synthetic dyes Cy3 and Cy5 were chosen and strategically placed in the anntena in such a way that they can collect additional light energy in the visible region of the solar spectrum and transfer it to RC through Förster resonance energy transfer (FRET). The antenna, a DNA templated multiple dye system, is attached to each Rhodobacter sphaeroides RC near the primary donor, P, to facilitate the energy transfer process...
September 19, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28926685/nir-absorbing-metal-free-organic-porphyrin-and-phthalocyanine-dyes-for-panchromatic-dscs
#9
Phillip Brogdon, Hammad Cheema, Jared Heath Delcamp
Dye-sensitized solar cells (DSCs) are a promising source of renewable energy. However, power conversion efficiency (PCE) of devices has been limited largely by the difficulty of producing electricity using photons from the near-infrared (NIR) spectral region. Metal-free organic sensitizers frequently employ strong electron donating or withdrawing moieties to tune the optical band gap to allow the absorption of lower energy wavelengths in charge transfer systems while porphyrins and phthalocyanines use substituents to shift the Soret and Q bands toward lower energy absorption...
September 19, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28926196/a-strategy-for-simultaneous-synthesis-of-methallyl-alcohol-and-diethyl-acetal-with-sn-%C3%AE
#10
Wenda Hu, Yan Wan, Lili Zhu, Xiaojie Cheng, Shaolong Wan, Jingdong Lin, Yong Wang
Herein we report a strategy to simultaneously produce two important chemicals namely Methallyl alcohol (Mol) and diethyl acetal (Dal) from methacrolein (Mal) in ethanol solvent at low temperature with the use of Beta zeolites modified by tin (Sn-β catalysts). All Sn-β catalysts were prepared by the solid-state ion-exchange (SSIE) method, wherein the calcination step was conducted in different gas atmospheres. The one pre-calcined in Ar (Sn-β-Ar) diminishes the number of extra-framework Sn species and instead enables more Sn species exchanged into the framework as isolated tetrahedral Sn (IV), thus enhancing the catalytic activity of Meerwein-Ponndorf-Verley (MPV) reaction...
September 19, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28925025/ring-opening-polymerization-of-l-lactide-to-cyclic-poly-lactide-by-zeolitic-imidazole-framework-8-catalyst
#11
Zhixiong Luo, Somboon Chaemchuen, Kui Zhou, Francis Verpoort
The catalytic activity of ZIF-8 in the ring-opening polymerization of L-lactide without solvents or co-catalysts is presented for the first time. Two different synthetic strategies have been applied for synthesizing ZIF-8, either under solvothermal condition or by spray-drying procedure. Their catalytic activities are found to be correlating with the presence of open active sites in ZIF-8 structure. The structural defects which afford active acid and basic sites are supposed to cooperatively catalyze the reaction...
September 18, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28922576/anion-exchange-membranes-for-alkaline-fuel-cell-applications-the-effects-of-cations
#12
Zhe Sun, Bencai Lin, Feng Yan
Alkaline anion exchange membrane fuel cells (AEMFCs) are attracting great attention, because of their potential use of non-precious electrocatalysts. Anion exchange membrane (AEM) is one of the key components of AEMFCs. An ideal AEM should possess high hydroxide conductivity and sufficient long-term durability at elevated temperatures in high pH solutions. This review provides recent progresses of alkaline stability behavior of cations (including quaternary ammonium, imidazolium, guanidinium, pyridinium, tertiary sulfonium, phosphonium, benzimidazolium and pyrrolidinium) and their analogous AEMs, which have been investigated by both experimental studies and theoretical calculations...
September 18, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28922570/catalyst-stability-benchmarking-for-the-oxygen-evolution-reaction-the-importance-of-backing-electrode-material-and-dissolution-in-accelerated-aging-studies
#13
Simon Geiger, Olga Kasian, Andrea M Mingers, Shannon S Nicley, Ken Haenen, Karl J J Mayrhofer, Serhiy Cherevko
In searching for alternative oxygen evolution reaction (OER) catalysts for acidic water splitting, fast screening of materials intrinsic activity and stability in half-cell tests is of vital importance. It significantly accelerates the discovery of new promising materials without the need of time-consuming real cell analysis. In commonly employed tests, a conclusion on the catalyst stability is drawn solely on the basis of pure electrochemical information, e.g. by evaluating potential vs. time profiles. In this work we demonstrate important limitations of such approaches, which are related to the degradation of the backing electrode material...
September 18, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28921902/mechanistic-parameters-of-electrocatalytic-water-oxidation-on-limn2o4-in-comparison-to-natural-photosynthesis
#14
Lennart Köhler, Majid Ebrahimizadeh Abrishami, Vladimir Roddatis, Janis Geppert, Marcel Risch
Targeted improvement of the low efficiency of water oxidation during the oxygen evolution reaction (OER) is severely hindered by insufficient knowledge of the electrocatalytic mechanism on heterogeneous surfaces. We chose LiMn2O4 as a model system for mechanistic investigations as it shares the cubane structure with the active site of photosystem II and the valence of Mn3.5+ with the dark-stable S1 state in the mechanism of natural photosynthesis. The investigated LiMn2O4 nanoparticles are electrochemically stable in NaOH electrolytes and show respectable activity in any of the main metrics...
September 18, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28921891/enhanced-formation-of-c1-products-in-the-electroreduction-of-co2-by-adding-a-carbon-dioxide-adsorption-component-to-a-gas-diffusion-layer-type-catalytic-electrode
#15
Bhanu Chandra Marepally, Claudio Ampelli, Chiara Genovese, Tapish Saboo, Siglinda Perathoner, Florian M Wisser, Laurent Veyre, Jérôme Canivet, Elsje Alessandra Quadrelli, Gabriele Centi
The addition of a CO2 adsorption component (substituted imidazolate-based SIM-1 crystals) to a gas diffusion layer (GDL) type catalytic electrode allows to enhance the activity and especially the selectivity to >C1 carbon chain products (ethanol, acetone and isopropanol) of a Pt-based electrocatalyst that is not able to form products of CO2 reduction involving C-C bond formation under conventional (liquid-phase) conditions. This indicates that the increase of the CO2 effective concentration at the electrode active surface is the factor controlling the formation of >C1 products rather than only the intrinsic properties of the electrocatalyst...
September 18, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28921874/polaronic-charge-carrier-lattice-interaction-in-lead-halide-perovskites
#16
Christoph Wolf, Young-Hoon Kim, Himchan Cho, Tae-Woo Lee
Almost ten years after the renaissance of the popular perovskite-type semiconductors based on lead-salts with general formula AMX3 (A=organic or inorganic cation, M=divalent metal, X=halide), many facets of photophysics continue to puzzle researchers. In this review, we shed some light on the low mobilities of charge carriers in lead-halide perovskites with special focus on the lattice properties at non-zero temperature. The polar and soft lattice leads to pronounced electron-phonon coupling, limiting carrier mobility and retarding recombination...
September 18, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28921879/natural-and-artificial-mn4ca-cluster-for-water-splitting-reaction
#17
Chunxi Zhang, Changhui Chen, Yanxi Li, Guoqing Zhao, Ruoqing Yao
The oxygen-evolving center (OEC) in photosystem II (PSII) is a unique biological catalyst that splits water into electrons, protons and O2 by using solar energy. Recent crystallographic studies have revealed that the structure of the OEC is an asymmetric Mn4Ca-cluster, which provides a blueprint to develop man-made water-splitting catalysts in artificial photosynthesis. Although it is a great challenge to mimic the whole structure and function of the OEC in the laboratory, significant advances have recently been achieved...
September 17, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28921883/stupendous-role-of-co-sensitizers-in-dye-sensitized-solar-cells
#18
Lingamallu Giribabu, Vamsi Krishna Narra, Venkata Suman Krishna Jonnadula, Mrinalini Madoori, Prasanthkumar Seelam
Co-sensitization in dye sensitized solar cells (DSSCs) received significant attention for improving the efficiency and stability of renewable energy resources. In this context, ruthenium metal and porphyrin dyes based DSSCs achieved increment in power conversion efficiency (PCE) from 8 - 11% to 11-14% after addition of additives, co-adsorbents and co-sensitizers by reducing the aggregation and charge recombination. Among the three supporting materials, co-sensitizers played major role to enhance the performance and stability of DSSCs which assist in commercialization...
September 16, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28915345/chemoselective-and-catalyst-free-o-borylation-of-silanols-a-facile-access-to-borasiloxanes
#19
Krzysztof Kuciński, Grzegorz Hreczycho
This paper demonstrates, for the first time, a highly chemoselective synthesis of various borasiloxanes from hydroboranes and silanols which was achieved through a catalyst-free dehydrogenative coupling at room temperature. This green protocol, which uses easily accessible reagents, allows for the obtaining of borasiloxanes under air atmosphere and solvent-free conditions.
September 15, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28914497/fuel-production-from-seawater-and-fuel-cells-using-seawater
#20
Shunichi Fukuzumi, Yong-Min Lee, Wonwoo Nam
Seawater is the most abundant resource on our planet and fuel production from seawater has the remarkable merit that it would not compete with growing demands of pure water. This review focuses on the production of fuels from seawater and their direct use in fuel cells. Electrolysis of seawater under appropriate conditions affords hydrogen and dioxygen with 100% Faradaic efficiency without oxidation of chloride ion. Photoelectrocatalytic production of hydrogen from seawater provides promising way to produce hydrogen with low cost and high efficiency...
September 15, 2017: ChemSusChem
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