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Solid state voltammetry and sensors in solids and gases
This project explores the electrochemical reactivity of electron transfer donor/acceptors dissolved in and diffusing through solid and semi-solid, ionically conductive media. The emphasis is on developing voltammetric experiments that are quantitatively interpretable in terms of the mass transport and electron transfer rates and thermodynamic equilibria of the redox solutes, and to exploit such experiments to probe their chemical and electrochemical behavior in the solid media. Techniques for quantitative voltammetry in solids were essentially unknown prior to initiation of this DOE project. We mainly employ poly(ethers)s containing dissolved metal salts electrolytes ( polymer electrolytes''), as prototype solid and semi-solid solvents. During this award year we have (a) concluded a study of plasticization chemistry in poly (ether) polymer electrolytes, (b) made progress in devising techniques for measuring the rates of electron transfer reactions in solid and semi-solid poly (ether)s, (c) continued efforts to design and understand the behavior of microband electrodes of various widths (0.1 to 10 {mu}m) in voltammetry of redox solutes, and (d) initiated synthetic efforts to attach ethylene oxide chains of various lengths to redox solutes
Optimal path planning for nonholonomic robotics systems via parametric optimisation
Abstract. Motivated by the path planning problem for robotic systems this paper considers nonholonomic path planning on the Euclidean group of motions SE(n) which describes a rigid bodies path in n-dimensional Euclidean space. The problem is formulated as a constrained optimal kinematic control problem where the cost function to be minimised is a quadratic function of translational and angular velocity inputs. An application of the Maximum Principle of optimal control leads to a set of Hamiltonian vector field that define the necessary conditions for optimality and consequently the optimal velocity history of the trajectory. It is illustrated that the systems are always integrable when n = 2 and in some cases when n = 3. However, if they are not integrable in the most general form of the cost function they can be rendered integrable by considering special cases. This implies that it is possible to reduce the kinematic system to a class of curves defined analytically. If the optimal motions can be expressed analytically in closed form then the path planning problem is reduced to one of parameter optimisation where the parameters are optimised to match prescribed boundary conditions.This reduction procedure is illustrated for a simple wheeled robot with a sliding constraint and a conventional slender underwater vehicle whose velocity in the lateral directions are constrained due to viscous damping
Chemically modified electrodes: Recommended terminology and definitions (IUPAC Recommendations 1997)
Chemically modified electrodes (CMEs) comprise a relatively modern approach to electrode systems that finds utility in (1) a wide spectrum of basic electrochemical investigations, including the relationship of heterogeneous electron transfer and chemical reactivity to electrode surface chemistry, electrostatic phenomena at electrode surfaces, and electron and ionic transport phenomena in polymers, and (2) the design of electrochemical devices and systems for applications in chemical sensing, energy conversion and storage, molecular electronics, electrochromic displays, corrosion protection, and electro-organic syntheses. Compared with other electrode concepts in electrochemistry, the distinguishing feature of a CME is that a generally thin film of a selected chemical is bonded or coated onto the electrode surface to endow the electrode with the chemical, electrochemical, optical, electrical, transport, and other desirable properties of the film in a rational, chemically designed manner. In this report, we have attempted to identify and define the most widely used terminology in the growing field of CMEs and to recommend a particular term in cases where a multiplicity of terms has arisen over the past several years or where previously defined terms have taken on broadened meanings for the special cases of CMEs. It is expected that additional terms will be added to this lexicon in the future as new research directions evolve
Coexistence of ferro- and antiferromagnetic order in Mn-doped NiMnGa
Ni-Mn-Ga is interesting as a prototype of a magnetic shape-memory alloy
showing large magnetic field induced strains. We present here results for the
magnetic ordering of Mn-rich Ni-Mn-Ga alloys based on both experiments and
theory. Experimental trends for the composition dependence of the magnetization
are measured by a vibrating sample magnetometer (VSM) in magnetic fields of up
to several tesla and at low temperatures. The saturation magnetization has a
maximum near the stoichiometric composition and it decreases with increasing Mn
content. This unexpected behaviour is interpreted via first-principles
calculations within the density-functional theory. We show that extra Mn atoms
are antiferromagnetically aligned to the other moments, which explains the
dependence of the magnetization on composition. In addition, the effect of Mn
doping on the stabilization of the structural phases and on the magnetic
anisotropy energy is demonstrated.Comment: 4 pages, 3 figure
The complications of ‘hiring a hubby’: gender relations and the commoditisation of home maintenance in New Zealand
This paper examines the commoditization of traditionally male domestic tasks through interviews with handymen who own franchises in the company ‘Hire a Hubby’ in New Zealand and homeowners who have paid for home repair tasks to be done. Discussions of the commoditization of traditionally female tasks in the home have revealed the emotional conflicts of paying others to care as well as the exploitative and degrading conditions that often arise when work takes place behind closed doors. By examining the working conditions and relationships involved when traditionally male tasks are paid for, this paper raises important questions about the valuing of reproductive labour and the production of gendered identities. The paper argues that while working conditions and rates of pay for ‘hubbies’ are better than those for people undertaking commoditized forms of traditionally female domestic labour, the negotiation of this work is still complex and implicated in gendered relations and identities. Working on the home was described by interviewees as an expression of care for family and a performance of the ‘right’ way to be a ‘Kiwi bloke’ and a father. Paying others to do this labour can imply a failure in a duty of care and in the performance of masculinity
Geochemical analysis of bulk marine sediment by Inductively Coupled Plasma–Atomic Emission Spectroscopy on board the JOIDES Resolution
Geochemical analyses on board the JOIDES Resolution have been enhanced with the addition of a Jobin-Yvon Ultrace inductively coupled plasma-atomic emission spectrometer (ICP-AES) as an upgrade from the previous X-ray fluorescence facility. During Leg 199, we sought to both challenge and utilize the capabilities of the ICP-AES in order to provide an extensive bulk-sediment geochemical database during the cruise. These near real-time analyses were then used to help characterize the recovered sedimentary sequences, calculate mass accumulation rates of the different sedimentary components, and assist with cruise and postcruise sampling requests. The general procedures, sample preparation techniques, and basic protocol for ICP-AES analyses on board ship are outlined by Murray et al. (2000) in Ocean Drilling Program Tech Note, 29. We expand on those concepts and offer suggestions for ICP-AES methodology, calibration by standard reference materials, data reduction procedures, and challenges that are specific to the analysis of bulk-sediment samples. During Leg 199, we employed an extensive bulk-sediment analytical program of ~600 samples of varying lithologies, thereby providing several opportunities for refinement of techniques. We also discuss some difficulties and challenges that were faced and suggest how to alleviate such occurrences for sedimentary chemical analyses during future legs
Nucleation of Al3Zr and Al3Sc in aluminum alloys: from kinetic Monte Carlo simulations to classical theory
Zr and Sc precipitate in aluminum alloys to form the compounds Al3Zr and
Al3Sc which for low supersaturations of the solid solution have the L12
structure. The aim of the present study is to model at an atomic scale this
kinetics of precipitation and to build a mesoscopic model based on classical
nucleation theory so as to extend the field of supersaturations and annealing
times that can be simulated. We use some ab-initio calculations and
experimental data to fit an Ising model describing thermodynamics of the Al-Zr
and Al-Sc systems. Kinetic behavior is described by means of an atom-vacancy
exchange mechanism. This allows us to simulate with a kinetic Monte Carlo
algorithm kinetics of precipitation of Al3Zr and Al3Sc. These kinetics are then
used to test the classical nucleation theory. In this purpose, we deduce from
our atomic model an isotropic interface free energy which is consistent with
the one deduced from experimental kinetics and a nucleation free energy. We
test di erent mean-field approximations (Bragg-Williams approximation as well
as Cluster Variation Method) for these parameters. The classical nucleation
theory is coherent with the kinetic Monte Carlo simulations only when CVM is
used: it manages to reproduce the cluster size distribution in the metastable
solid solution and its evolution as well as the steady-state nucleation rate.
We also find that the capillary approximation used in the classical nucleation
theory works surprisingly well when compared to a direct calculation of the
free energy of formation for small L12 clusters.Comment: submitted to Physical Review B (2004
Political Corporate Social Responsibility: Reviewing Theories and Setting New Agendas
There has been rising interest in political corporate social responsibility (political CSR), defined as activities where CSR has an intended or unintended political impact, or where intended or unintended political impacts on CSR exist. Based on a survey and content analysis of 146 peer-reviewed academic articles from 18 journals over the 14-year period 2000–2013, this paper systematically reviews the existing applications of general theories (such as legitimacy theory, the resource-based view and Habermasian political theory) within the political CSR literature.The survey indicates that the political CSR field is dominated by institutional theory and stakeholder theory, but future theory development needs to go beyond these theories in order to address a number of critical gaps. This review specifically points to several avenues for future political CSR research with regard to the individual level of analysis, domain integration and political CSR in multinational enterprises. The paper ends with a call for a new theory-informed and pluralist research agenda on political CSR to integrate different perspectives and re-examine the role of the state
Milagrito: a TeV air-shower array
Milagrito, a large, covered water-Cherenkov detector, was the world's first
air-shower-particle detector sensitive to cosmic gamma rays below 1 TeV. It
served as a prototype for the Milagro detector and operated from February 1997
to May 1998. This paper gives a description of Milagrito, a summary of the
operating experience, and early results that demonstrate the capabilities of
this technique.Comment: 38 pages including 24 figure
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