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ChemSusChem

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https://www.readbyqxmd.com/read/28338295/insights-into-the-mechanism-of-a-covalently-linked-organic-dye-cobaloxime-catalyst-system-for-dye-sensitized-solar-fuel-devices
#1
Palas Baran Pati, Lei Zhang, Bertrand Philippe, Ricardo Fernández-Terán, Sareh Ahmadi, Lei Tian, Håkan Rensmo, Leif Hammarström, Haining Tian
A covalently-linked organic dye-cobaloxime catalyst system is developed by facile click reaction for mechanistic studies and application in dye sensitized solar fuel device based on mesoporous NiO. This system has been systematically investigated by photoelectrochemical measurements, density functional theory, time resolved fluorescence, transient absorption spectroscopy as well as photoelectron spectroscopy. The results show that irradiation of the dye-catalyst on NiO leads to ultrafast hole injection into NiO from the excited dye, followed by a fast electron transfer process to reduce the catalyst...
March 24, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28338286/stable-ni-particles-through-structural-reversibility-in-la-fe-ni-perovskite-type-metal-oxide-catalysts
#2
Patrick Steiger, Renaud Delmelle, Debora Foppiano, Lorenz Holzer, Andre Heel, Maarten Nachtegaal, Oliver Kröcher, Davide Ferri
Perovskite-type oxides have shown the ability to reversibly segregate precious metals from their structure. This reversible segregation behavior was explored for a commonly used catalyst metal, Ni, to prevent Ni sintering, which is observed on most catalyst support materials. TPR, XRD, XAS, electron microscopy and catalytic activity tests were used to follow the extent of reversible Ni segregation. LaFe1 xNixO3±δ (0 ≤ x ≤ 0.2) was synthesized using a citrate based solution process. After reduction at 600°C metallic Ni particles were displayed on the perovskite surfaces, which showed to be active towards the hydrogenation of CO2...
March 24, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28337857/wxc-c-nrgo-composite-derived-from-polyoxotungstate-conductive-polypyrrole-graphene-as-efficient-electrocatalyst-for-hydrogen-evolution-reaction
#3
Ya-Qian Lan, Xiao-Li Wang, Yu-Jia Tang, Wei Huang, Chun-Hui Liu, Long-Zhang Dong, Shun-Li Li
Efficient hydrogen evolution reaction (HER) from water through electrocatalysis using cost-effective materials is critical to realize the clean hydrogen production. Herein, with controlling the structure and composition of polyoxotungstate/conductive polypyrrole/graphene (PCG) precursor precisely and followed by the temperature-programmed reaction, we developed a highly active and stable catalyst WxC@C/NRGO. The composite presents splendid performance towards HER in acidic media, with a small onset overpotential of 24 mV vs...
March 23, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28334512/flow-pickering-emulsion-interfaces-enhance-catalysis-efficiency-and-selectivity-for-cyclization-of-citronellal
#4
Hengquan Yang, Huan Chen, Houbing Zou, Yajuan Hao
Cyclization of citronellal is a necessary intermediate step to produce the important flavor chemical (-)-menthol. We here demonstrate a continuous flow Pickering emulsion (FPE) strategy for selective cyclization of citronellal to (-)-isopulegol, using water droplets hosting heteropolyacid catalyst (HPA) to fill a column reactor. Owing to the large liquid-liquid interface and the excellent confinement capability of droplets toward HPA, the FPE system exhibits a catalysis efficiency much higher than those of batch systems (2~5 fold) and an excellent durability (two months)...
March 23, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28334500/efficient-and-stable-vacuum-free-processed-perovskite-solar-cells-enabled-by-a-robust-solution-processed-hole-transport-layer
#5
Chih-Yu Chang, Bo-Chou Tsai, Yu-Cheng Hsiao
In this work, efficient and stable vacuum-free processed perovskite solar cells (PeSCs) is demonstrated by employ solution-processed molybdenum tris-[1-(trifluoroethanoyl)-2-(trifluoromethyl)ethane-1,2-dithiolene] (Mo(tfd-COCF3)3)-doped poly(3,4-ethylenedioxythiophene) (PEDOT) film as hole transport layer (HTL). Our results indicate that the incorporation of Mo(tfd-COCF3)3 dopant can induce p-doping via the charge transfer from the highest occupied molecular orbital level of PEDOT host to the electron affinity of Mo(tfd-COCF3)3, leading to an increase in conductivity by more than three orders of magnitude...
March 23, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28333410/pd-metalated-conjugated-nanoporous-polycarbazoles-for-additive-free-cyanation-of-aryl-halides-boosting-catalytic-efficiency-via-spatial-modulation
#6
Shunmin Ding, Chengcheng Tian, Xiang Zhu, Carter W Abney, Ziqi Tian, Bo Chen, Meijun Li, De-En Jiang, Ning Zhang, Sheng Dai
A novel spatial-modulation approach was developed to fabricate a new heterogeneous Pd-metalated nanoporous polymer for efficient and ligand-free cyanation of aryl halides. The resulting catalyst displays high activity in the synthesis of benzonitriles, including high product yield, excellent stability and recycle, and broad scope functional group tolerance.
March 23, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28332773/determination-of-conduction-and-valence-band-electronic-structure-of-latioxny-thin-film
#7
Markus Pichler, Jakub Szlachetko, Ivano Eligio Castelli, Nicola Marzari, Max Döbeli, Alexander Wokaun, Daniele Pergolesi, Thomas Lippert
The nitrogen substitution into the oxygen sites of several oxide materials leads to a reduction of the band gap to the visible light energy range, which makes these oxynitride semiconductors potential photocatalysts for efficient solar water splitting. Oxynitrides typically show a different crystal structure compare to the pristine oxide material. Since the band gap is correlated to both the chemical composition and the crystal structure, it is not trivial to distinguish what modifications of the electronic structure induced by the nitrogen substitution are related to compositional and/or structural effects...
March 23, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28332772/designing-highly-efficient-cui-photosensitizer-for-photocatalytic-h2-evolution-from-water
#8
Jaekwan Kim, Dong Ryeol Whang, Soo Young Park
A series of CuI photosensitizers was synthesized, characterized, and investigated for photocatalytic H2 evolution from water. The structure-property correlation was made for their catalytic activity and photophysical properties, which was further elaborated by DFT calculation. A novel CuI photosensitizer (Cu-TPAPhen) with triphenylamine-substituted phenanthroline ligand showed unprecedentedly high turnover number of 19,000 when tested in combination with triethylamine as a sacrificial reagent and colloidal Pt as a H2 evolution catalyst...
March 23, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28332296/electrochemistry-for-the-generation-of-renewable-chemicals-one-pot-electrochemical-deoxygenation-of-xylose-to-%C3%AE-valerolactone
#9
Olusola Oladele James, Waldemer Sauter, Uwe Schröder
In this study, we demonstrate the electrochemical conversion of xylose to δ-valerolactone via carbonyl intermediates. The conversion was achieved in aqueous media and at ambient conditions. This study also demonstrates that feedstocks for the use of electrochemistry for production of renewable chemicals and biofuels can be extended to primary carbohydrate molecules. This is the first report on a one-pot electrochemical deoxygenation of xylose to δ-valerolactone.
March 22, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28328085/an-efficient-and-reusable-embedded-ru-catalyst-for-the-hydrogenolysis-of-levulinic-acid-to-%C3%AE-valerolactone
#10
Zuojun Wei, Jiongtao Lou, Chuanmin Su, Dechao Guo, Yingxin Liu, Shuguang Deng
To achieve a higher activity and reusability of a Ru-based catalyst, Ru nanoparticles were embedded in N-doped mesoporous carbon through a hard-template method. The catalyst showed excellent catalytic performance (314 h(-1) turnover frequency) and recyclability (reusable five times with 3 % activity loss) for the hydrogenolysis of levulinic acid to γ-valerolactone. Compared with the mesoporous carbon without N-doping and conventional activated carbon, the introduction of N-dopant effectively improved the dispersion of Ru nanoparticles, decreased the average size of Ru nanoparticles to as small as 1...
March 22, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28326678/rational-engineering-of-bodipy-bridged-trisindole-derivatives-for-solar-cell-applications
#11
Nicolas Leclerc, Ibrahim Bulut, Quentin Huaulmé, Antoine Mirloup, Patricia Chávez, Sadiara Fall, Anne Hébraud, Stéphane Méry, Benoit Heinrich, Thomas Heiser, Patrick Lévêque
Boron dipyrromethene (Bodipy) are known to be efficient photon harvesting chromophores. However, their study as active materials in bulk heterojunction (BHJ) solar cells is still scarce. In this paper, we developed new synthetic ways to design original Bodipy-based dumbbell-shape molecules, including a first 2,3,5,6-tetravinyl aromatic Bodipy molecule. We demonstrated that high fill factors can be obtained in BHJ solar cells when blended with a fullerene derivative, leading to a new Bodipy-based record power conversion efficiency of 5...
March 21, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28322516/metal-organic-framework-templated-catalyst-synergy-in-multiple-sites-for-catalytic-co2-fixation
#12
Hai-Long Jiang, Meili Ding, Si Chen, Xiao-Qin Liu, Lin-Bing Sun, Junling Lu
The types and quantities of active sites play critical roles in catalysis. Herein, ZnO nanoparticles encapsulated N-doped porous carbon has been rationally prepared by the pyrolysis of a metal-organic framework (MOF) followed by moderate oxidation treatment. The resultant catalyst exhibits excellent activity, selectivity and recyclability in the CO2 cycloaddtion reactions with epoxides, due to the synergy of multiple sites inherited from the MOF and generated by the oxidation process.
March 21, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28322007/one-electron-initiated-two-electron-oxidation-of-water-by-aluminum-porphyrins-with-earth-s-most-abundant-metal-ion
#13
Fazalurahman Kuttassery, Siby Mathew, Shogo Sagawa, Sebastian Nybin Remello, Arun Thomas, Daisuke Yamamoto, Satomi Onuki, Yu Nabetani, Hiroshi Tachibana, Haruo Inoue
We report here a new molecular catalyst for efficient water splitting, aluminum porphyrins (tetra-methylpyridiniumylporphyrinatealuminum: AlTMPyP), containing the Earth's most abundant metal as the central ion. One-electron oxidation of the aluminum porphyrin initiates the two-electron oxidation of water to form hydrogen peroxide as the primary reaction product with the lowest known overpotential (97 mV). The aluminum-peroxo complex was clearly detected by a cold-spray ionization mass-spectrometry in HRMS mode and the structure of the intermediate was further confirmed using laser-Raman spectroscopy, indicating the hydroperoxy complex of AlTMPyP to be the key intermediate in the reaction...
March 20, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28318144/eco-efficient-synthesis-of-highly-porous-coco3-anodes-for-li-and-na-storage-using-supercritical-co2-precursors
#14
Hui-Ying Li, Chuan-Ming Tseng, Cheng-Hsien Yang, Tai-Chou Lee, Ching-Yuan Su, Chien-Te Hsieh, Jeng-Kuei Chang
An eco-efficient synthesis route of high-performance carbonate anodes for Li+ and Na+ batteries is developed. With supercritical CO2 (SCCO2) as the precursor, which has gas-like diffusivity, extremely low viscosity, and near-zero surface tension, CoCO3 particles are uniformly formed and tightly connected on graphene nanosheets (GNSs). This synthesis can be conducted at 50 °C, which is considerably lower than the temperature required for conventional preparation methods, minimizing energy consumption. The obtained CoCO3 particles (~20 nm in diameter), which have a unique interpenetrating porous structure, can increase the number of electroactive sites, promote electrolyte accessibility, shorten ion diffusion length, and readily accommodate the strain generated upon charging/discharging...
March 20, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28318143/designing-squaraines-to-control-charge-injection-and-recombination-processes-in-nio-based-dye-sensitized-solar-cells
#15
Oliver Langmar, Davide Saccone, Anna Amat, Simona Fantacci, Guido Viscardi, Claudia Barolo, Ruben Costa, Dirk Michael Guldi
Herein, the synthesis of a novel family of squaraines (SQ) and their application in p-type dye-sensitized solar cells (DSSC) is presented. In particular, two sets of SQs were designed. The SQs have been characterized by using a joint theoretical, photophysical and electrochemical approach. Importantly, the presence of different central groups forces them into a frozen cis (dicyanovinyl group) or a trans (oxygen group) conformation. Based on the latter, the current work enables the direct comparison between cis and trans isomers, as well as the impact of a different number of anchors...
March 20, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28317341/metal-doping-for-enhancing-the-photoelectrochemical-behavior-of-lafeo3-photocathodes
#16
María Isabel Díez-García, Roberto Gómez
The development of tandem devices for water photosplitting requires finding photocathodic materials based on earth-abundant elements and showing long-term stability in aqueous electrolytes. Ternary metal oxides seem to be a viable option, among which perovskites stand out. In this context, transparent and compact LaFeO3 thin film electrodes have been prepared by sol-gel, both undoped and doped with metals (M) such as magnesium or zinc. Pristine electrodes support the development of cathodic photocurrents in 0...
March 20, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28317277/nasicon-bi2o3-composite-electrolyte-for-all-solid-state-lithium-batteries-low-temperature-fabrication-and-conductivity-enhancement
#17
Sang-Don Lee, Kyu-Nam Jung, Hyeongil Kim, Hyun-Seop Shin, Seung-Wan Song, Min-Sik Park, Jong-Won Lee
All-solid-state lithium batteries offer notable advantages over conventional Li-ion batteries with liquid electrolytes in terms of energy density, stability, and safety. To realize this technology, it is critical to develop highly reliable solid-state inorganic electrolytes with high ionic conductivities and acceptable processability. Li1+xAlxTi2-x(PO4)3 (LATP) with a NASICON (Na superionic conductor)-like structure is regarded as a potential solid electrolyte, owing to its high "bulk" conductivity (~10-3 S cm-1) and excellent stability against air and moisture...
March 20, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28317268/enhanced-surface-charge-transport-and-stability-of-cds-1d-zr-fe2o3-nanorod-arrays-with-al2o3-passivation-layer-for-photoelectrochemical-solar-hydrogen-generation
#18
Jum Suk Jang, Mahadeo A Mahadik, Arunprabaharan Subramanian, Min Cho, Hee-Suk Chung
CdS sensitized 1D Zr:Fe2O3 nanorod arrays have been synthesized on fluorine-doped tin oxide substrates via a two-step hydrothermal method. The photoelectrochemical results demonstrate that the current density (4.2 mA.cm-2 at 0 V (vs. Ag/AgCl) recorded under illumination for the CdS/1D Zr:Fe2O3 photoanodes is 2.8 time higher than the bare 1D Zr:Fe2O3. The extended absorbance spectrum, the reduced recombination, and the effective transport of photogenerated holes in CdS to the electrolyte facilitate enhancement in photoelectrochemical performance...
March 20, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28303687/design-principles-for-covalent-organic-frameworks-in-energy-storage-applications
#19
Sampath B Alahakoon, Christina M Thompson, Gino Occhialini, Ronald Alexander Smaldone
Covalent organic frameworks (COFs) are an exciting class of microporous materials that have been explored as energy storage materials for more than a decade. This review will discusses the efforts to develop these materials for applications in gas and electrical power storage. This review will also discuss some of the design strategies for developing the gas sorption properties of COFs and mechanistic studies on their formation.
March 16, 2017: ChemSusChem
https://www.readbyqxmd.com/read/28301085/operando-soft-x-ray-absorption-spectroscopic-study-on-a-solid-oxide-fuel-cell-cathode-during-electrochemical-oxygen-reduction
#20
Takashi Nakamura, Ryo Oike, Yuta Kimura, Yusuke Tamenori, Tatsuya Kawada, Koji Amezawa
Operando soft X-ray absorption spectroscopic technique, which could analyze electronic structures of the electrode materials at elevated temperature and controlled atmosphere under electrochemical polarization, was established and its availability was demonstrated by investigating electronic structural changes of an La2NiO4+d dense film electrode during electrochemical oxygen reduction reaction. Clear O K-edge and Ni L-edge X-ray absorption spectra could be obtained below 773 K in fully atmospheric pressure of 100 ppm O2-He, 0...
March 16, 2017: ChemSusChem
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