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Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode
Understanding the oxygen reduction reaction at fuel cell cathodes requires information on adsorbed oxygenated species. Sanchez Casalongue et al. report in situidentification of oxygenated intermediates at cathodes and establish a correlation between the cathode potential and the surface speciation.
- Hernan Sanchez Casalongue
- , Sarp Kaya
- & Hirohito Ogasawara
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Pits confined in ultrathin cerium(IV) oxide for studying catalytic centers in carbon monoxide oxidation
Catalytic carbon monoxide oxidation is an industrially important process. Here, the authors show that ultrathin cerium(IV) oxide with surface confined pits provides an ideal platform for investigating and optimizing the role of local atomic structure on carbon monoxide adsorption and oxygen activation.
- Yongfu Sun
- , Qinghua Liu
- & Yi Xie
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Chitosan confinement enhances hydrogen photogeneration from a mimic of the diiron subsite of [FeFe]-hydrogenase
Naturally occurring hydrogenase enzymes are capable of efficient hydrogen production but low stability and high cost limits their industrial use. Here, the authors show that chitosan encapsulation improves the catalytic efficiency of a mimic of the diiron subsite of the H-cluster of [FeFe]-hydrogenase.
- Jing-Xin Jian
- , Qiang Liu
- & Li-Zhu Wu
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Capsule-controlled selectivity of a rhodium hydroformylation catalyst
The selectivity and activity of enzymes is largely attributed to the well-defined cavities around their active sites, defined by the secondary coordination sphere. Here, the authors show that similar strategies may be applied to tune the selectivity of synthetic rhodium hydroformylation catalysts.
- Vladica Bocokić
- , Ayfer Kalkan
- & Joost N. H. Reek
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Hydrodefluorination of carbon–fluorine bonds by the synergistic action of a ruthenium–palladium catalyst
Selective hydrodefluoridization is important as an industrial reaction and in the disposal of chlorofluorocarbons. Here, the authors prepare a heterodimetallic ruthenium–palladium complex, which is active in the hydrodefluorination of aromatic and aliphatic molecules under mild reaction conditions.
- Sara Sabater
- , Jose A. Mata
- & Eduardo Peris
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Cobalt phosphate-modified barium-doped tantalum nitride nanorod photoanode with 1.5% solar energy conversion efficiency
The search for efficient photoanodes for water oxidation is ongoing. Here, the authors investigate the effect of barium doping on a tantalum nitride nanostructured photoanode, and report a solar energy conversion efficiency of 1.5% in the presence of a cobalt phosphate co-catalyst.
- Yanbo Li
- , Li Zhang
- & Kazunari Domen
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Ordered macroporous platinum electrode and enhanced mass transfer in fuel cells using inverse opal structure
Inverse opal structures are desirable for fuel cell electrodes, but application of such structures in polymer electrolyte membrane fuel cells is yet to be realised. Kimet al.report fabrication of a platinum catalyst layer with an inverse opal structure, and show improved fuel cell performance.
- Ok-Hee Kim
- , Yong-Hun Cho
- & Yung-Eun Sung
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Cadmium iodide-mediated allenylation of terminal alkynes with ketones
The allenylation of terminal alkynes is a convenient route to allenes from simple starting materials, though previously limited to formaldehyde and aldehyde substrates. Here a method enabling the use of ketones is reported, giving easy access to trisubstituted allenes.
- Xinjun Tang
- , Can Zhu
- & Shengming Ma
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Directing reaction pathways by catalyst active-site selection using self-assembled monolayers
Control of active sites of heterogeneous catalysts can lead to enhanced product selectivity. Here, the authors use self-assembled alkanethiolate monolayers with varying surface densities to tune the selectivity of hydrogenation and hydrodeoxygenation of furfural on supported palladium catalysts.
- Simon H. Pang
- , Carolyn A. Schoenbaum
- & J. Will Medlin
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A copper-phyllosilicate core-sheath nanoreactor for carbon–oxygen hydrogenolysis reactions
Nanoscale copper catalysts are useful for the selective hydrogenation of carbon–oxygen bonds, although they may be deactivated under harsh conditions. Here the authors report the enhanced activity and stability of core-sheath copper-phyllosilicate nanoreactors due to electronic and morphological effects.
- Hairong Yue
- , Yujun Zhao
- & Jinlong Gong
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Trinuclear zinc complexes for biologically relevant μ3-oxoanion binding and carbon dioxide fixation
Molecular models of the biologically relevant oxoanion-bridged trinuclear zinc cluster found in numerous enzymatic active sites are desirable. Cao et al. report the synthesis of a trinuclear zinc scaffold, pre-organized to capture oxoanions, and its ability to catalytically convert CO2to carbonates in solution.
- Xiao Liu
- , Pingwu Du
- & Rui Cao
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| Open AccessStable platinum nanoclusters on genomic DNA–graphene oxide with a high oxygen reduction reaction activity
Platinum nanoclusters are well-known catalysts for the oxygen reduction reaction, although the performance of clusters smaller than 2 nm is poorly studied. Here, the authors report 1.4 nm platinum clusters supported on DNA–graphene oxide composites and demonstrate promising electrochemical activity and stability.
- Jitendra N. Tiwari
- , Krishna Nath
- & Kwang S. Kim
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Nitrate formation from atmospheric nitrogen and oxygen photocatalysed by nano-sized titanium dioxide
Nitrate pollutants are known to contribute to a variety of environmental problems. Here, the authors suggest that nano-sized titanium dioxide, as used in numerous surface coatings, may catalyse the formation of nitrate via the photochemical reaction of atmospheric nitrogen and oxygen.
- Shi-Jie Yuan
- , Jie-Jie Chen
- & Han-Qing Yu
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Probing the nature of gold–carbon bonding in gold–alkynyl complexes
Fundamental understanding of gold–carbon bonding in homogeneous catalysts is vital for improved catalyst design, although spectroscopic information is limited. Here, the authors probe the bonding in gold–alkyne complexes using a combination of photoelectron spectroscopy and ab initiocalculations.
- Hong-Tao Liu
- , Xiao-Gen Xiong
- & Lai-Sheng Wang
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Chemical synthesis of lactic acid from cellulose catalysed by lead(II) ions in water
The direct transformation of cellulose into high-value chemicals is a key process in the establishment of biomass-derived chemical production. Here, the authors present the lead(II)-catalysed conversion of cellulose into lactic acid via a cascade reaction, which proceeds in water under mild conditions.
- Yanliang Wang
- , Weiping Deng
- & Huilin Wan
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| Open AccessCapture and conversion of CO2 at ambient conditions by a conjugated microporous polymer
Conjugated microporous polymers are highly flexible materials that may be used for gas storage and catalysis applications. Here, the authors report metal-functionalized conjugated microporous polymers capable of both capturing CO2and functioning as a heterogeneous catalyst in its conversion to propylene carbonate.
- Yong Xie
- , Ting-Ting Wang
- & Wei-Qiao Deng
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Codoping titanium dioxide nanowires with tungsten and carbon for enhanced photoelectrochemical performance
Titanium dioxide nanowires are used as photoanodes in photoelectrochemical water splitting. Here Zheng et al. demonstrate that doping these nanowires with tungsten and carbon atom pairs considerably enhances their performance.
- In Sun Cho
- , Chi Hwan Lee
- & Xiaolin Zheng
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Solvent-free aerobic oxidation of hydrocarbons and alcohols with Pd@N-doped carbon from glucose
The development of efficient catalysts for the aerobic oxidation of hydrocarbons to high-value chemicals is industrially important. Here, the authors show that palladium nanoparticles loaded on porous nitrogen-doped carbon are highly active catalysts under laboratory and industrially relevant conditions.
- Pengfei Zhang
- , Yutong Gong
- & Yong Wang
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Spatial separation of photogenerated electrons and holes among {010} and {110} crystal facets of BiVO4
Charge separation determines the efficiency of semiconductor-based photocatalysts. Here Li et al. show that, in BiVO4, photogenerated electrons and holes accumulate on different crystal facets and the targeted deposition of cocatalysts increases the efficiency of photocatalytic water oxidation.
- Rengui Li
- , Fuxiang Zhang
- & Can Li
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Probing the catalytic activity of porous graphene oxide and the origin of this behaviour
Graphene oxide has been proposed as an alternative to precious metals for the catalysis of aerobic oxidative reactions; however, high catalyst loadings are needed. Here a simple base and acid treatment is shown to enhance its catalytic activity for the oxidative coupling of amines under ambient conditions.
- Chenliang Su
- , Muge Acik
- & Kian Ping Loh
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Iron-catalysed transformation of molecular dinitrogen into silylamine under ambient conditions
The transition metal-catalysed reduction of nitrogen, vital for the production of fertilizer, usually requires expensive molybdenum catalysts. Here, Yuki et al.describe the iron-catalysed reduction of nitrogen under ambient conditions and propose a reaction pathway supported by DFT calculations.
- Masahiro Yuki
- , Hiromasa Tanaka
- & Yoshiaki Nishibayashi
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Non-syngas direct steam reforming of methanol to hydrogen and carbon dioxide at low temperature
Proton exchange membrane fuel cells are good potential power sources for mobile devices but require very pure H2 production at low temperatures. Yu et al. report the use of a CuZnGaOx catalyst capable of producing CO-free H2from methanol via a non-syngas direct steam-reforming route at 150–200 °C.
- Kai Man Kerry Yu
- , Weiyi Tong
- & Shik Chi Edman Tsang
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Scalable organocatalytic asymmetric Strecker reactions catalysed by a chiral cyanide generator
The Strecker synthesis is an established method for the production of α-amino acids. Here, a scalable catalytic asymmetric Strecker reaction is reported that allows one-pot synthesis of enantiomerically pure α-amino acids.
- Hailong Yan
- , Joong Suk Oh
- & Choong Eui Song
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Spectroscopic observation of iodosylarene metalloporphyrin adducts and manganese(V)-oxo porphyrin species in a cytochrome P450 analogue
Metalloporphyrin compounds are studied as models of cytochrome P450, which is capable of catalysing oxidative reactions. Here, reaction conditions are varied to allow spectroscopic observation of oxidant-metalloporphyrin adducts and metal-oxo intermediates, which may elucidate reaction mechanisms.
- Mian Guo
- , Hang Dong
- & Aiwen Lei
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| Open AccessSn-Beta zeolites with borate salts catalyse the epimerization of carbohydrates via an intramolecular carbon shift
Epimerization of carbohydrates to rare sugars yields products that have potential applications as anti-viral drugs or chiral building blocks. Here, Sn-Beta zeolite in the presence of sodium tetraborate is shown to catalyze the selective epimerization of aldoses in aqueous media.
- William R. Gunther
- , Yuran Wang
- & Yuriy Román-Leshkov
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Highly stable Pt monolayer on PdAu nanoparticle electrocatalysts for the oxygen reduction reaction
Platinum is used as a cathode in fuel cells but undergoes dissolution during potential changes, hindering commercial application in electric vehicles. Sasakiet al.report a new class of stable electrocatalysts that consist of platinum monolayers on palladium–gold alloy nanoparticles.
- Kotaro Sasaki
- , Hideo Naohara
- & Radoslav R. Adzic
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A non-syn-gas catalytic route to methanol production
Methanol is an important industrial chemical and liquid fuel, and is usually produced by the syn-gas route from natural gas. Wuet al. develop a new catalytic process that directly converts ethylene glycol, derived from biomass or fossil fuels, to methanol in hydrogen using a Pd/Fe2O3co-precipitated catalyst.
- Cheng-Tar Wu
- , Kai Man Kerry Yu
- & Shik Chi Edman Tsang
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Unsupported boron–carbon σ-coordination to platinum as an isolable snapshot of σ-bond activation
σ-Complexes of transition metals are key intermediates in metal-mediated bond activation, but have traditionally been isolable only when chelating or when one of the participating atoms is hydrogen. Here, a complex is isolated with an unsupported borirene ligand bound not through the unsaturated C=C bond, but exclusively via a B–C single bond.
- Holger Braunschweig
- , Peter Brenner
- & Alfredo Vargas
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Review Article |
The biology and chemistry of high-valent iron–oxo and iron–nitrido complexes
High-valent iron–oxo and –nitrido complexes are intermediates in the catalytic cycles of various metalloenzymes that activate dioxygen and dinitrogen. Hohenbergeret al. review the advances in the chemistry of model high-valent iron–oxo and –nitrido systems and relate them to our understanding of related enzymes.
- Johannes Hohenberger
- , Kallol Ray
- & Karsten Meyer
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| Open AccessTandem synthesis of alternating polyesters from renewable resources
Biomass-derived monomers are a renewable resource for the production of polymers. Robertet al. develop an auto-tandem catalytic transformation for the synthesis of aliphatic polyesters—'activated' monomers are prepared from dicarboxylic acids, which can be copolymerized with epoxides.
- Carine Robert
- , Frédéric de Montigny
- & Christophe M. Thomas
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Direct stereoselective α-arylation of unmodified enals using an organocatalytic cross-coupling-like reaction
Cross-coupling reactions are widely used for creating new carbon–carbon bonds in chemical syntheses. Using the cross-coupling concept, Wang and colleagues present an organocatalytic strategy for the direct and stereoselective α-arylation of enals that occurs under mild conditions.
- Xixi Song
- , Aiguo Song
- & Wei Wang
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Iron-based cathode catalyst with enhanced power density in polymer electrolyte membrane fuel cells
Replacing platinum in polymer-electrolyte-membrane fuel cells with iron-based catalysts could provide low-cost power generators, but often leads to low power densities. Here, a new iron-based cathode catalyst is developed with enhanced power density, volumetric activity and mass-transport properties.
- Eric Proietti
- , Frédéric Jaouen
- & Jean-Pol Dodelet
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Organocatalytic enantioselective β-functionalization of aldehydes by oxidation of enamines and their application in cascade reactions
The transformation of iminium ions to enamines has been used extensively in organocatalysis, but conversion of enamines to iminium species has not been exploited. In this study, oxidative enamine catalysis allows the conversion of enamines to iminium ions and the direct asymmetric β-functionalization of simple aldehydes.
- Shi-Lei Zhang
- , He-Xin Xie
- & Wei Wang