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141.
The thermolytic molecular precursor method was used to introduce site-isolated Ti(IV) and Ta(V) centers onto the surface of a mesoporous SBA15 support. The resulting surface SiOH, TiOH, and TaOH sites were modified with a series of (N,N-dimethylamino)trialkylsilanes, Me2NSiMe2R (where R = Me, n Bu, or n Oc). Compared to the unmodified catalysts, the surface-modified catalysts are more active in the epoxidation of cyclohexene with H2O2 and exhibit a markedly greater selectivity for cyclohexene oxide (up to 58% for Ti(IV) and greater than 95% for Ta(V)). In situ spectroscopies were used to probe this phenomenon, and it was determined that a siloxy-capped Ti(IV) or Ta(V) site is essential to achieve the high epoxide selectivity. 相似文献
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144.
Yanfang Wu Danielle Bennett Richard D. Tilley John Justin Gooding 《Advanced materials (Deerfield Beach, Fla.)》2020,32(18):1904339
Single molecule measurements are revolutionizing the understanding of the stochastics of behavior of single molecules. There is a common theme referred to as a near-field approach, in how many single molecule measurements are being performed in assays. The term near field is used because the measurement volume is typically very small such that a single molecule, or a single molecule binding pair, within that volume is of an appreciable concentration. The next development in detection will be performing many single molecule measurements at one time such that single molecule measurements can be used as the basis for quantitative analysis. There have already been some notable developments in this direction. Again, all have a common theme in that nanoparticles are used to create many near-field volumes that can be measured simultaneously. Herein, the coupled developments in nanoparticles and measurement strategies that allow nanoparticles to be the backbone of the next generation of sensing technologies are discussed. 相似文献
145.
S. David Tilley Marcel Schreier João Azevedo Morgan Stefik Michael Graetzel 《Advanced functional materials》2014,24(3):303-311
Photocathodes based on cuprous oxide (Cu2O) are promising materials for large scale and widespread solar fuel generation due to the abundance of copper, suitable bandgap, and favorable band alignments for reducing water and carbon dioxide. A protective overlayer is required to stabilize the Cu2O in aqueous media under illumination, and the interface between this overlayer and the catalyst nanoparticles was previously identified as a key source of instability. Here, the properties of the protective titanium dioxide overlayer of composite cuprous oxide photocathodes are further investigated, as well as an oxide‐based hydrogen evolution catalyst, ruthenium oxide (RuO2). The RuO2‐catalyzed photoelectrodes exhibit much improved stability versus platinum nanoparticles, with 94% stability after 8 h of light‐chopping chronoamperometry. Faradaic efficiencies of ～100% are obtained as determined by measurement of the evolved hydrogen gas. The sustained photocurrents of close to 5 mA cm?2 obtained with this electrode during the chronoamperometry measurement (at 0 V vs. the reversible hydrogen electrode, pH 5, and simulated 1 sun illumination) would correspond to greater than 6% solar‐to‐hydrogen conversion efficiency in a tandem photoelectrochemical cell, where the bias is provided by a photovoltaic device such as a dye‐sensitized solar cell. 相似文献
146.
Ludmilla Steier Isaac Herraiz‐Cardona Sixto Gimenez Francisco Fabregat‐Santiago Juan Bisquert S. David Tilley Michael Grätzel 《Advanced functional materials》2014,24(48):7681-7688
Recent research on photoanodes for photoelectrochemical water splitting has introduced the concept of under‐ and overlayers for the activation of ultrathin hematite films. Their effects on the photocatalytic behavior were clearly shown; however, the mechanism is thus far not fully understood. Herein, the contribution of each layer is analyzed by means of electrochemical impedance spectroscopy, with the aim of obtaining a general understanding of surface and interface modifications and their influence on the hematite photoanode performance. This study shows that doping of the hematite from the underlayer and surface passivation from annealing treatments and an overlayer are key parameters to consider for the design of more efficient iron oxide electrodes. Understanding the contribution of these layers, a new design for ultrathin hematite films employing a combination of a gallium oxide overlayer with thin niobium oxide and silicon oxide underlayers is shown to achieve a photocurrent onset potential for the photoelectrochemical oxidation of water more negative than 750 mV versus the reversible hydrogen electrode (RHE) at pH 13.6, utilizing Co‐Pi as a water oxidation catalyst. It is demonstrated that multilayer hematite thin film photoanodes are a strategy to reduce the overpotential for this material, thereby facilitating more efficient tandem cells. 相似文献
147.
Hausi A. Müller Mehmet A. Orgun Scott R. Tilley James S. Uhl 《Journal of Software: Evolution and Process》1993,5(4):181-204
Reverse-engineering is the process of extracting system abstractions and design information out of existing software systems. This process involves the identification of software artefacts in a particular subject system, the exploration of how these artefacts interact with one another, and their aggregation to form more abstract system representations that facilitate program understanding. This paper describes our approach to creating higher-level abstract representations of a subject system, which involves the identification of related components and dependencies, the construction of layered subsystem structures, and the computation of exact interfaces among subsystems. We show how top-down decompositions of a subject system can be (re)constructed via bottom-up subsystem composition. This process involves identifying groups of building blocks (e.g., variables, procedures, modules, and subsystems) using composition operations based on software engineering principles such as low coupling and high cohesion. The result is an architecture of layered subsystem structures. The structures are manipulated and recorded using the Rigi system, which consists of a distributed graph editor and a parsing system with a central repository. The editor provides graph filters and clustering operations to build and explore subsystem hierarchies interactively. The paper concludes with a detailed, step-by-step analysis of a 30-module software system using Rigi. 相似文献