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Версия для печати | Главная > Центр > Научные советы > Научный совет по катализу > ... > 2012 год > № 64

№ 64

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  • Илья Иосифович МОИСЕЕВ
    — лауреат Демидовской премии
  • Сергей Степанович ИВАНЧЁВ
    К 80-летию со дня рождения
  • Евгений Зиновьевич ГОЛОСМАН
    К 75-летию со дня рождения
  • Симпозиум «Современные проблемы нанокатализа»
  • IX Международная конференция «Механизмы каталитических реакций»
  • II Всероссийская научная школа-конференция молодых ученых
    «Катализ: от науки к промышленности»
  • За рубежом
  • Приглашения на конференции



Илья Иосифович МОИСЕЕВ — лауреат Демидовской премии

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Сергей Степанович ИВАНЧЁВ
К 80-летию со дня рождения

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Евгений Зиновьевич ГОЛОСМАН
К 75-летию со дня рождения

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Симпозиум «Современные проблемы нанокатализа»

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IX Международная конференция «Механизмы каталитических реакций»

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II Всероссийская научная школа-конференция молодых ученых
«Катализ: от науки к промышленности»

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A Twist On Water Splitting

Photocatalysts: Nanosized crystal patchwork
generates hydrogen, raising alternative-energy hopes

By Mitch Jacoby

If water could be separated economically into oxygen and hydrogen, a clean-burning fuel, the world’s oceans would represent a free and virtually limitless feedstock for producing energy. A new strategy for designing light-activated catalysts that split water may help bring that alternative-energy goal a step closer to reality.

The interfaces between nanosized domains of α- and β-Ga2O3 mediate photocatalytic charge separation and water splitting.

Researchers in China have found that crystals of the semiconductor Ga2O3 that are composed of a patchwork of structurally distinct nanosized domains can split water photocatalytically (Angew. Chem. Int. Ed., DOI: 10.1002/anie.201207554). The study demonstrates that the interface between polymorphic crystal phases can play a key role in light-stimulated water splitting. The work may lead to photocatalysts that are more active than the relatively inefficient ones available today.

Photocatalysts split water by directing energy absorbed from light—often sunlight—to break water’s chemical bonds. The heart of the process is the light absorption event, which generates pairs of negatively charged electrons and positively charged holes (electron vacancies). The key to capitalizing on the energy absorbed from light is keeping the charges separated. Charge recombination can dissipate the absorbed energy before bonds are broken.

The standard strategy for maximizing charge separation in semiconductors calls for selectively doping the material to juxtapose positively (p-type) and negatively (n-type) charged regions. Researchers also make these types of interfaces, known as p-n junctions, by depositing two types of semiconductors side by side.

The new study, which was conducted by Xiang Wang, Can Li, and coworkers of the Dalian Institute of Chemical Physics, demonstrates an alternative way to keep charges separated. Rather than relying on p-n junctions to do the job, the Dalian team exploits the interfaces between structurally dissimilar nanosized domains of Ga2O3, which is known to crystallize in five polymorphic phases.

The researchers show that a simple heat treatment can be used to tailor the distribution of nanosized domains of Ga2O3’s so-called α and β phases. They further show that mixed α-β samples prepared by heating the starting material to roughly 600°C are up to seven times more catalytically active in splitting water than samples composed of either phase alone.

The University of Tokyo’s Kazunari Domen comments that although in this proof-of-concept study the overall activity of the Ga2O3 photocatalysts is not especially high, the strategy described here represents a new approach to boosting catalytic water-splitting efficiency. He adds that the method’s applicability may be limited, however, as a result of the relatively small number of materials known to exhibit similar kinds of polymorphs.

 

From Polyenes To Polycycles

Iridium-catalyzed reaction creates
valuable scaffolds enantioselectively

By Bethany Halford

A new protocol for preparing polycyclic compounds enantioselectively promises to make it easier to build these pharmaceutically relevant scaffolds (J. Am. Chem. Soc., DOI: 10.1021/ja310386m). The reaction, developed by Erick M. Carreira and coworkers at the Swiss Federal Institute of Technology, Zurich, uses an iridium-based catalyst and a zinc triflate promoter to coax the cascade reaction of polyenes (example shown). To begin the cascade, a racemic allylic alcohol within the polyene structure reacts with an iridium catalyst. This interaction appears to dictate the stereochemistry of the first cyclization. Subsequent cyclizations are effectively encoded in the first ring, the researchers believe. Using the protocol, Carreira and colleagues prepared nine polycyclic compounds—including heterocycles—in good yields, with enantiomeric excesses reaching 99%. “It is important to note that all the reactions are conducted at ambient temperature with commercial-grade solvents and reagents, making this cyclization protocol convenient to perform,” the chemists point out.

 

X-raying Catalysts In Action

Tomography method monitors changes
in chemically distinct nanoscale regions
of catalysts under reaction conditions

By Mitch Jacoby

Thanks to a specially designed reactor cell, researchers can now probe changes in the chemical composition, morphology, porosity, and other properties of individual 20-μm-sized catalyst particles as the particles mediate chemical reactions (Angew. Chem. Int. Ed., DOI: 10.1002/anie.201204930).

The study conducted by Joy C. Andrews of SLAC National Accelerator Laboratory; Bert M. Weckhuysen of Utrecht University, in the Netherlands; and coworkers demonstrates a procedure for exploiting high-energy X-ray microscopy to penetrate deeply into complex materials and resolve chemically distinct nanoscale regions within their bulk. Solid catalysts often undergo substantial changes—sometimes beneficial, sometimes detrimental—upon exposure to reactive chemicals at high temperature and pressure. Mapping those changes in three dimensions as they occur could lead to improved catalysts, but capturing the information remains challenging. To demonstrate the new method’s capabilities, the team probed a model Fischer-Tropsch C–C coupling catalyst as it was exposed to 10 atm of a mixture of H2 and CO at 350°C. The method pinpointed regions rich in Fe2O3, Fe2TiO5, Fe3O4, ZnO, and K2O and monitored the evolution of those regions over the course of several hours.

Chemical & Engineering News

 

Наиболее яркие статьи по катализу

Applied Catalysis A: General

Nanocatalysts for conversion of natural gas to liquid fuels and petrochemical feedstocks. Review article

M. Gharibi, F.T. Zangeneh, F. Yaripour, S. Sahebdelfar

http://www.sciencedirect.com/science/article/pii/S0926860X12004036

Fischer-Tropsch synthesis: Effect of Pd, Pt, Re, and Ru noble metal promoters on the activity and selectivity
of a 25%Co/Al2O3 catalyst

W. Ma, G. Jacobs, R.A. Keogh, D.B. Bukur, B.H. Davis

http://www.sciencedirect.com/science/article/pii/S0926860X12003183

 

Applied Catalysis B: Environmental

Mn-Fe/ZSM5 as a low-temperature SCR catalyst to remove NOx from diesel engine exhaust

Y.J. Kim, H.J. Kwon, I. Heo, I.S. Nam, B.K. Cho, J.W. Choung, M.S. Cha, G.K. Yeo

http://www.sciencedirect.com/science/article/pii/S0926337312002639

Improved visible light photocatalytic activity of TiO2 co-doped with vanadium and nitrogen

Jaiswal, R.; Patel, N.; Kothari, D.C.; Miotello, A.

http://www.sciencedirect.com/science/article/pii/S0926337312002974

 

Catalysis Today

The past, present and future of heterogeneous catalysis

I. Fechete, Y. Wang, J.C. Vedrine

http://www.sciencedirect.com/science/article/pii/S0920586112002751

Main technologies in biodiesel production: State of the art and future challenges. Review article

E. Santacesaria, G.M. Vicente, M. Di Serio, R. Tesser

http://www.sciencedirect.com/science/article/pii/S0920586112003446

 

Chemical Engineering Journal

Modified oil palm leaves adsorbent with enhanced hydrophobicity for crude oil removal

S.M. Sidik, A.A. Jalil, S. Triwahyono, S.H. Adam, M.A.H. Satar, B.H. Hameed

http://www.sciencedirect.com/science/article/pii/S1385894712008625

 

Journal of Catalysis

CO hydrogenation to methanol on Cu-Ni catalysts: Theory and experiment

F. Studt, F. Abild-Pedersen, Q. Wu, A.D. Jensen, B. Temel, J.D. Grunwaldt, J.K. Norskov

http://www.sciencedirect.com/science/article/pii/S0021951712001765

 

ChemCatChem

Simultaneous Generation of Mesoxalic Acid and Electricity from Glycerol on a Gold Anode Catalyst
in Anion-Exchange Membrane Fuel Cells

Le Xin, Zhiyong Zhang, Zhichao Wang, Wenzhen Li

http://onlinelibrary.wiley.com/doi/10.1002/cctc.201200017/full

 

ChemSusChem

An Intermolecular Heterobimetallic system for Photocatalytic Water Reduction

Sven Hansen, Marcus Klahn, Torsten Beweries, Uwe Rosenthal

http://onlinelibrary.wiley.com/doi/10.1002/cssc.201100794/full

 

Advanced Synthesis & Catalysis

Catalytic Asymmetric Epoxidation of 2-Cyclopentenones

Carl A. Busacca, Daniel R. Fandrick, Jinhua J. Song, Chris H. Senanayake

http://onlinelibrary.wiley.com/doi/10.1002/adsc.201200072/full

 

Angewandte Chemie International Edition

Electronic Modulation of a Copper/Zinc Oxide Catalyst by a Heterojunction for Selective Hydrogenation
of Carbon Dioxide to Methanol

Fenglin Liao, Ziyan Zeng, Clive Eley, Qin Lu, Xinlin Hong, Shik Chi Edman Tsang

http://onlinelibrary.wiley.com/doi/10.1002/anie.201200903/full

 

Applied Organometallic Chemistry

Mixed metal MgO–ZrO2 nanoparticle-catalyzed O-tert-Boc protection of alcohols and phenols under solvent-free conditions

Manoj B. Gawande, Sharad N. Shelke, Paula S. Branco, Anuj Rathi and Rajesh K. Pandey

http://onlinelibrary.wiley.com/doi/10.1002/aoc.2846/full

 

Chemical Engineering and Technology

Testing of a Ni-Al2O3 Catalyst for Methane Steam Reforming Using Different Reaction Systems

N. de Miguel, J. Manzanedo, P. L. Arias

http://onlinelibrary.wiley.com/doi/10.1002/ceat.201100348/pdf

 

Asia-Pacific Journal of Chemical Engineering

Application of clean technologies using electrochemistry in ionic liquids

A.P. Doherty, L. Diaconu, E. Marley, P. L. Spedding, R. Barhdadi, M. Troupel

http://onlinelibrary.wiley.com/doi/10.1002/apj.529/pdf

 

Chemistry – A European Journal

Bimetallic Catalysis using Transition and Group 11 Metals: An Emerging Tool for C-C Coupling and Other Reactions

M. H. Pérez-Temprano, J. A. Casares, P. Espinet

http://onlinelibrary.wiley.com/doi/10.1002/chem.201102888/full

 

Journal of Chemical Technology and Biotechnology

Heterogeneously catalyzing C-C coupling reactions with precious metal nanoparticles

Simon K. Beaumont

http://onlinelibrary.wiley.com/doi/10.1002/jctb.3748/full

 

Helvetica Chimica Acta

Substrate Range of the Titanium TADDOLate Catalyzed Asymmetric Fluorination of Activated Carbonyl Compounds

Andreas Bertogg, Lukas Hintermann, Dominique P. Huber, Mauro Perseghini, Maria Sanna, Antonio Togni

http://onlinelibrary.wiley.com/doi/10.1002/hlca.201100375/pdf

 

Macromolecular Reaction Engineering

Effect of Hydrogen and External Donor on Propylene Polymerization Kinetics with a 4th-Generation Ziegler-Natta Catalyst

Ahmad Alshaiban, João B. P. Soares

http://onlinelibrary.wiley.com/doi/10.1002/mren.201200002/full

 

Macromolecular Chemistry and Physics

Poly(ε-caprolactone) by Combined Ring-Opening Polymerization and Polycondensation

Hans R. Kricheldorf, Steffen M. Weidner, Felix Scheliga, Mohammed Lahcini

http://onlinelibrary.wiley.com/doi/10.1002/macp.201200061/full

 

Israel Journal of Chemistry

Asymmetric Autocatalysis Triggered by Chiral Crystals Formed from Achiral Compounds and Chiral Isotopomers

Tsuneomi Kawasaki, Kenso Soai

http://onlinelibrary.wiley.com/doi/10.1002/ijch.201100155/full

 

Chinese Journal of Chemistry

Friedel-Crafts Alkylation of Indoles with Nitroalkenes Catalyzed by Zn(II)-Thiourea Complex

Ningning Wan, Yonghai Hui, Zhengfeng Xie, Jide Wang

http://onlinelibrary.wiley.com/doi/10.1002/cjoc.201180480/pdf

 

Journal of the Chinese Chemical Society

Control of Catalytic Activity Via Porosity, Chemical Composition, and Morphology of Nanostructured Porous
Manganese Oxide Materials

Chun-Hu Chen, Steven L. Suib

http://onlinelibrary.wiley.com/doi/10.1002/jccs.201100699/pdf

 

WIRES: Computational Molecular Science

A refinement of everyday thinking: the energetic span model for kinetic assessment of catalytic cycles

Sebastian Kozuch

http://onlinelibrary.wiley.com/doi/10.1002/wcms.1100/full

 

Zeitschrift für anorganische und allgemeine Chemie

Synthesis of a Water-Stable 2, 4-Bis(trifluoromethyl)phenyl-Substituted Phosphonous Acid Palladium Complex
and its Catalytic Activity in Cross-Coupling Reactions

Boris Kurscheid, Hans-Georg Stammler, Beate Neumann, Berthold Hoge

http://onlinelibrary.wiley.com/doi/10.1002/zaac.201100344/full

 

The Chemical Record

Design of Molecular Catalysts for Achievement of High Turnover Number in Homogeneous Hydrogenation

Noriyoshi Arai, Takeshi Ohkuma

http://onlinelibrary.wiley.com/doi/10.1002/tcr.201100019/full

 

European Journal of Organic Chemistry

Biocatalytic Approaches to the Henry (Nitroaldol) Reaction

Sinéad E. Milner, Thomas S. Moody, Anita R. Maguire

http://onlinelibrary.wiley.com/doi/10.1002/ejoc.201101840/full

 

European Journal of Inorganic Chemistry

Cooperative Catalysis with First-Row Late Transition Metals

Jarl Ivar van der Vlugt

http://onlinelibrary.wiley.com/doi/10.1002/ejic.201100752/full

 

ChemPhysChem

The Role of Effective Mass of Carrier in the Photocatalytic Behavior of Silver Halide-Based Ag@AgX (X=Cl, Br, I):
A Theoretical Study

Xiangchao Ma, Ying Dai, Meng Guo, Baibiao Huang

http://onlinelibrary.wiley.com/doi/10.1002/cphc.201200159/full

 

Aiche Journal

Multiscale modeling for emergent behavior, complexity, and combinatorial explosion

Dionisios G. Vlachos

http://onlinelibrary.wiley.com/doi/10.1002/aic.13803/full

 

The Canadian Journal of Chemical Engineering

Evolving applications of zeolite molecular sieves

Christopher C. H. Lin, K. Amy Dambrowitz, Steven M. Kuznicki

http://onlinelibrary.wiley.com/doi/10.1002/cjce.20667/pdf

 

Journal of Peptide Science

Peptides as asymmetric catalysts and templates for the controlled formation of Ag nanoparticles

Helma Wennemers

http://onlinelibrary.wiley.com/doi/10.1002/psc.2422/full

 

Chemie Ingenieur Technik

New Catalysts for the Hydrogenation of Glucose to Sorbitol

Reinhard Geyer, Peter Kraak, Axel Pachulski, Rainer Schödel

http://onlinelibrary.wiley.com/doi/10.1002/cite.201100108/pdf

 


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