Abstract:The crystal structure of Cu2(OH)(3)Cl has been determined using two natural samples with almost ideal stoichiometry. While one of the samples exhibits a twinned clinoatacamite structure, the other sample is characterized by the appearance of additional weak diffraction maxima at half integer positions of h and k. Structure refinement was carried out with the space group P1. The relationship between the triclinic phase, clinoatacamite, paratacamite and the herbertsmithite structure is discussed in terms of symm… Show more
“…There is a metastable polymorph to herbertsmithite known as kapellasite Colman et al, 2008;Malcherek and Schluter, 2007). The structure, though, is different, with no intersites (Fig.…”
“…It exists in at least four polymorphs (see Table I), although the fourth one (a low symmetry triclinic structure) has hardly been studied (Malcherek and Schluter, 2009). The least stable (and therefore the first to form during the corrosion of copper by sea water) is botallackite, which consists of distorted triangular copper layers with AA stacking (Hawthorne, 1985).…”
Section: A Botallackite Atacamite Clinoatacamitementioning
Quantum spin liquids form a novel class of matter where, despite the existence of strong exchange interactions, spins do not order down to the lowest measured temperature. Typically, these occur in lattices that act to frustrate the appearance of magnetism. In two dimensions, the classic example is the kagome lattice composed of corner sharing triangles. There are a variety of minerals whose transition metal ions form such a lattice. Hence, a number of them have been studied, and were then subsequently synthesized in order to obtain more pristine samples. Of particular note was the report in 2005 by Dan Nocera's group of the synthesis of herbertsmithite, composed of a lattice of copper ions sitting on a kagome lattice, which indeed does not order down to the lowest measured temperature despite the existence of a large exchange interaction of 17 meV. Over the past decade, this material has been extensively studied, yielding a number of intriguing surprises that have in turn motivated a resurgence of interest in the theoretical study of the spin 1 2 Heisenberg model on a kagome lattice. In this colloquium article, I will review these developments, and then discuss potential future directions, both experimental and theoretical, as well as the challenge of doping these materials with the hope that this could lead to the discovery of novel topological and superconducting phases.
“…There is a metastable polymorph to herbertsmithite known as kapellasite Colman et al, 2008;Malcherek and Schluter, 2007). The structure, though, is different, with no intersites (Fig.…”
“…It exists in at least four polymorphs (see Table I), although the fourth one (a low symmetry triclinic structure) has hardly been studied (Malcherek and Schluter, 2009). The least stable (and therefore the first to form during the corrosion of copper by sea water) is botallackite, which consists of distorted triangular copper layers with AA stacking (Hawthorne, 1985).…”
Section: A Botallackite Atacamite Clinoatacamitementioning
Quantum spin liquids form a novel class of matter where, despite the existence of strong exchange interactions, spins do not order down to the lowest measured temperature. Typically, these occur in lattices that act to frustrate the appearance of magnetism. In two dimensions, the classic example is the kagome lattice composed of corner sharing triangles. There are a variety of minerals whose transition metal ions form such a lattice. Hence, a number of them have been studied, and were then subsequently synthesized in order to obtain more pristine samples. Of particular note was the report in 2005 by Dan Nocera's group of the synthesis of herbertsmithite, composed of a lattice of copper ions sitting on a kagome lattice, which indeed does not order down to the lowest measured temperature despite the existence of a large exchange interaction of 17 meV. Over the past decade, this material has been extensively studied, yielding a number of intriguing surprises that have in turn motivated a resurgence of interest in the theoretical study of the spin 1 2 Heisenberg model on a kagome lattice. In this colloquium article, I will review these developments, and then discuss potential future directions, both experimental and theoretical, as well as the challenge of doping these materials with the hope that this could lead to the discovery of novel topological and superconducting phases.
“…Using Scherrer's equation 37 , we calculated the crystallite sizes to be approximately 18, 25 and 57 nm, for the Cu 2 (OH) 3 Cl {004} (ref. 38 ), Cu 2 O {111} (ref. 39 ) and Cu {111} (ref.…”
As energy demand continues to increase, so too do anthropogenic carbon emissions and global temperatures. Renewable energy sources such as solar, wind and hydroelectricity displace fossil fuel carbon emissions and continue to progress to wider deployment. However, long-term (seasonal) energy storage remains a challenge that must be addressed for renewables to meet a major fraction of global energy demand 1 . Carbon dioxide electroreduction to renewable fuels and feedstocks provides an energy storage solution to the seasonal variability of renewable energy sources 2 . When coupled with carbon capture technology, the carbon dioxide reduction reaction (CO 2 RR) offers a means to close the carbon cycle.CO 2 RR electrocatalysts lower energetic barriers to CO 2 reduction by stabilizing intermediates and transition states in the multistep electrochemical reduction process 3 . Copper reduces CO 2 to a wide range of hydrocarbon products such as methane, ethylene, ethanol and propanol 4 . Unfortunately, bulk copper is not selective among various carbon products, and it also suffers Faradaic efficiency (FE) losses to the competing hydrogen evolution reaction.Among possible products, C2+ hydrocarbons are highly sought in view of their commercial value. Ethylene, for example, is a precursor to the production of polyethylene, a major plastic. Selectively producing ethylene over methane circumvents costly paraffin-olefin separation 5 . Developing catalysts that work at ambient conditions to produce C2 selectively over C1 gaseous products will increase the relevance of renewable feedstocks in the chemical sector.Oxide-derived copper is one class of catalyst that has shown enhanced CO 2 RR activity and increased selectivity towards multi-carbon products [6][7][8] . The selectivity of these catalysts is dependent on structural morphology and copper oxidation state 9-17 . Electrochemical reduction of copper oxide catalyst films can lead to grain boundaries, undercoordinated sites and roughened surfaces that are hypothesized to be catalytically active sites 8,18 . Residual oxides, proposed to play a key role in catalysis, may exist after electrochemical reduction 7 . A recent report of oxygen plasma-activated oxide-derived copper catalysts achieved an ethylene FE of 60% at − 0.9 V versus reversible hydrogen electrode (RHE) 9 , with activity attributed to the presence of Cu + species. In situ hard X-ray absorption spectroscopy (hXAS) experiments have suggested stable Cu + species exist at highly negative CO 2 RR potentials of ~− 1.0 versus RHE 9 . However, the presence of Cu + species during CO 2 RR is still the subject of debate; 7,19 and in situ tracking of the copper oxidation state with time resolution during CO 2 RR has remained elusive.Morphological effects of copper nanostructures have a significant effect on the selectivity of CO 2 RR to multi-carbon products [20][21][22][23][24] . Copper catalysts with different morphologies have been synthesized through annealing, chemical treatments on thin films, colloidal synthesis and ...
“…For certain identifications, the crystal structures of collinsite, atacamite, and kröhnkite were refined starting from the atomic coordinates given by former authors (Brotherton et al, 1974;Hawthorne & Ferguson, 1975;Parise & Hyde, 1986;Yakubovich et al, 2003;Kolitsch & Fleck, 2005, 2006Zheng et al, 2005;Herwig & Hawthorne, 2006;Malcherek & Schlüter, 2009). The crystal structures compare well with those published by former authors.…”
Section: X-ray Experiments and Refinement Of The Crystal Structurementioning
O] based on single-crystal X-ray diffraction, electron microprobe, stable isotope analyses, and scanning electron microscope imaging. This is the first reported occurrence of kröhnkite in a cave environment. Atacamite represents the weathering product (in the presence of Lower-Cretaceous limestone-derived chlorine) of copper minerals washed into the cave from nearby ore bodies. Atacamite and kröhnkite have similar sources for copper and chlorine, whereas sodium probably originates from weathered Precambrian and Permian detrital rocks. Collinsite is believed to have precipitated from bat guano in a damp, nearneutral pH environment. The results show the following sequence of precipitation: ardealite-brushite-(gypsum)-atacamite-kröhnkite. This suggests that the observed mineral paragenesis is controlled by the neutralization potential of the host-rock mineralogy and the concentrations of Ca, Cl, Cu, and Na.Keywords: cave minerals, sulfates, phosphates, guano, stable isotopes, Cioclovina Cave, Romania Abstract:
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