1. Copper Nanoparticles for Printed Electronics: Routes Towards Achieving Oxidation Stability
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  4. Copper Nanoparticles for Printed Electronics: Routes Towards Achieving Oxidation Stability

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The ancestors of the Ciboney migrated from the mainland of South America, with the earliest sites dated to 5, BP. When Columbus arrived they were the dominant culture in Cuba, having an estimated population of , Other towns soon followed, including San Cristobal de la Habana , founded in , which later became the capital. Gonzalo Perez de Angulo was appointed governor of Cuba. He arrived in Santiago, Cuba on 4 November and immediately declared the liberty of all natives. But what was most important was that the colony developed as an urbanized society that primarily supported the Spanish colonial empire. By the midth century, its colonists held 50, slaves, compared to 60, in Barbados ; , in Virginia , both British colonies; and , in French Saint-Domingue , which had large-scale sugar cane plantations. Spain's alliance with the French pitched them into direct conflict with the British, and in a British expedition of five warships and 4, troops set out from Portsmouth to capture Cuba. The British arrived on 6 June, and by August had Havana under siege. The British immediately opened up trade with their North American and Caribbean colonies, causing a rapid transformation of Cuban society.

Kaki, M. Karuna, S. Sarada, C. Kumar, and R. Swamy and U. Picheansoonthon and V. Jerawong, Thai Pharmaceutical Textbook No. Tadtong, C. Puengseangdee, S. Prasertthanawut, and T. Yang, X. Zhang, S. Yang, and W. Wei and T. Kiyohara, C. Ichino, Y. Kawamura, T. Nagai, N. Sato, and H. Yoon, I. Je, X. Cui et al. Miyazawa, Y. Okuno, S. Nakamura, and H. Park, H.

Copper Nanoparticles for Printed Electronics: Routes Towards Achieving Oxidation Stability

Yoon, and D. Yang, K. Kinoshita, K. Koyama et al. Yu, Y. Qi, G. Luo, H. Duan, and J. Jeong, J. Choi, Z. Lou, X. Jiang, and S. Folin and V. View at Google Scholar B. Mayur, S. Sandesh, S. Shruti, and S. View at Google Scholar K. Yamazaki, A.

Journal of Botany

Hashimoto, Y. Kokusenya, T. Miyamoto, and T. View at Google Scholar R. Re, N.

Pellegrini, A. Proteggente, A. Pannala, M. Yang, and C. Tewtrakul and A.

Surarit, C. Jansom, N. Lerdvuthisopon, S. Kongkham, and P. Sarker, L. Nahar, and Y. Iloki-Assanga, L.

Lara-Espinoza et al. Munin and F. Murugan and T. Bhau, B. Borah, R. Ahmed et al. Tang, M. Li, S. The diatom species Ditylum brightwellii, however, has been reported to be growth-inhibited across a large range of pCu thresholds from as low as 8. Dinoflagellates Figure 4C As with the previous functional types, Brand et al. They found this group to be generally more sensitive than coccolithophores, but less so than cyanobacteria.

Several Peridinium, Prorocentrum, and Thoracosphaera species displayed completely suppressed growth around pCu Prior to this, Schenck documented complete inhibition of Gonyaulax tamarensis at pCu 11, and Pistocchi et al.

Anderson and Morel , however, found that pCu 9. We cannot know if cell division ceased with motility. In Gymnodinium sp. To our knowledge, there are no published accounts of dinoflagellate responses to Cu addition in situ that can be discussed in terms of pCu.

As a group, dinoflagellates have received the least attention of the four taxonomic groups discussed here. Coccolithophores Figure 4D Coccolithophores display intermediate sensitivity to elevated pCu relative to cyanobacterial and diatom species. Coccolith morphology and volume in E. The largest sample of isolates tested to date are reported in Echeveste et al. We calculate an average pCu of 8. Similarly, we calculate a pCu of 9. In situ observation and incubations involving coccolithophores are few; on the west coast of Norway, Muller et al.

Hoffmann et al. Meng et al. Discussion This systematic review highlights that most studies on Cu toxicity in marine phytoplankton do not facilitate discussion in terms of pCu. As such, the dominant trend yielded by efforts to describe Cu toxicity between diverse phytoplankton, as that presented here, remains the taxonomic partitioning reported in Brand et al.

There exists large variability within these groupings and even between replicated studies, however. We found no further trends in Cu toxicity from the perspectives of microalgal biogeography, finer taxonomic division e.

Qualitative observations gathered through this review are plentiful Supplementary Table 1 , and many of these studies support the taxonomic trend presented by Brand et al.

Suggested Considerations for Future Work Our literature survey highlighted issues confounding comparability among Cu ecotoxicology studies. Here we briefly discuss some considerations and suggestions to obtain high-quality data and improve replicability in Cu toxicity investigations with regard to three broad issues.

We recommend this be read before any attempt to investigate Cu toxicity in photosynthetic microalgae. Of the 99 studies which could not be compared here, 60 were excluded from our quantitative comparison because they were conducted in natural seawater without synthetic chelating agent addition.

Therefore, accounting for trace metal speciation is the most overlooked consideration in Cu toxicity investigations, and we stress once more that it is imperative to a replicable study. This discrepancy was likely due to accumulation of organic metabolite exudates in the batch cultures, which has been addressed before Saifullah, ; Lombardi and Vieira, ; Wiramanaden et al.

Their data reinforce that trace metal ecophysiology results obtained using batch cultures should be viewed with caution, particularly when cell densities greatly exceed environmental levels Vasseur et al. Lower cell densities, in conjunction with semi-continuous or similar culturing methods, reduce accumulation of organic exudates, changes in pH, and required nutrient amendments, all of which may confound observations and replicability.

Macronutrient and Micronutrient Availability Should be Considered Nitrogen and phosphorus availability altered Cu sensitivity in Ditylum brightwellii, Thalassiosira pseudonana, and Phaeodactylum tricornutum Rijstenbil and Wijnholds, ; Rijstenbil et al.

Likewise, the availability of other trace metals can ameliorate Cu toxicity. Increases in dissolved zinc and manganese reduced sensitivity to added Cu in situ Braek et al. Alternatively, Cu toxicity was exacerbated by increases in cadmium, zinc, and lead Bartlett and Rabe, ; Khan and Saifullah, , , and Cu availability alters Fe-quotas and uptake in various isolates and even heterogeneous field populations Peers et al.

The relatively short timescale of Cu toxicity experiments allows for many experimental treatments. We recommend that nutrient interactions be considered and ideally tested in experimental design. Cu Toxicity in C. In the latter strain, however, decreases in cell volume were only achieved when Fe and phosphorus were co-limiting. Thus, the Cu: C assimilation ratios measured in phytoplankton communities sampled along Line P may be higher than those determined in laboratory studies. Just before dawn on each sampling day, four 60 mL TMC polycarbonate bottles were rinsed and filled with sample water and spiked with kBq of H 14 CO 3 -.

Bottles were incubated at in situ light and temperature for 24 h in the on-deck incubators. After the incubation, the volume of each bottle was recorded and the contents were gently filtered onto 25 mm GFF filters. The filters were then immersed in scintillation cocktail and archived until they could be analyzed in the laboratory. Mixed layer seawater density was highest at P26 Mixed layer depths ranged two-fold 15—31 m , and were deepest farthest offshore P16 and P26 Table 1.

Mixed layer nitrate concentrations were below detection 0. However, they were elevated at P16 5. Phosphate and silicic acid concentrations were not limiting across the transect.

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At P3, a broad fluorescence peak was present from 5 to 30 m depth Figure 2. Total dissolved Cu concentrations ranged between 1. Dissolved Cu was highest near the coast at P3 2. Mixed layer [Cu] d decreased along the transect toward P20 1. Dissolved ligand concentrations were highest at P3 The average [L]: The [L]: Figure 3. Salinity was sampled at 5 m using the ship's internal seawater pumping system, while the Cu concentration and speciation samples were from the shallowest depths sampled along the transect 7—10 m; Table 2.

Total [chl a ] varied more than fold along Line P varied between 0. The 0. Cyanobacteria and picoeukaryote abundance varied between 0. They were most abundant at P3 and tended to be more prevalent at deeper depths at all stations e. Table 4. Biomass and rate parameters measured at each sampling depth along Line P.

Table 5. Size-fractionated Cu: C assimilation ratios 24 h , short-term Cu uptake rates 2 h , long-term Cu uptake rates 24 h , and the short-term: Total bacterial abundance between stations P4 and P26 varied between 0. Volumetric and cell-normalized rates of bacterial productivity varied between 0.

Both volumetric and carbon-normalized rates of bacterial productivity were fastest at P16 and P Bacterial abundance and productivity were within the range previously reported for summer months along Line P 0. The concomitant sampling of total dissolved Cu, Cu speciation, and various measures of biological biomass and productivity allow us to determine how Cu might influence microorganisms along Line P.

There were a number of statistically significant correlations along the transect for p -values, see Table 6. Table 6. Statistically significant Pearson correlations of biomass, productivity, Cu uptake, and chemical parameters measured along Line P in August Figure 4.

C assimilation ratios ranged between 0. The average Cu: Short-term Cu uptake rates are in excess of long-term uptake rates due to either cellular efflux or remineralization by micrograzers Semeniuk et al. The ratio of short-term: LT ratios ranged between 2.

The ST: LT ratios were more variable for the 0. The two highest ST: LT values in the 0. Without these outliers, the average ST: LT ratios for all size fractions were consistently lower at P26 2. We present some of the first measurements of dissolved Cu in the northeast subarctic Pacific Ocean. Total dissolved Cu varied 1.

These values are similar to surface water [Cu] d previously measured along Line P 1. The elevated [Cu] d at P3 7 and 12 m depth and at 10 m depth at P4 may be due to their closer proximity to terrestrial and shelf sources of Cu.

Upwelling begins at these stations by March, due to Ekman pumping as the California and Alaska currents bifurcate along the British Columbia coast Thomson, ; Foreman et al. Intermediate waters — m off the coast of Washington are enriched in Cu 2—3 nM relative to surface waters Jones and Murray, Upwelling of these waters could account for the observed enrichment of [Cu] d at P3 and P4.

Surface water [Cu] d at P26 2. Total dissolved Cu at P26 was also higher than [Cu] d at P16 1. Dissolved Fe in the mixed layer was also significantly higher at P26 0. Recent dissolved lead Pb isotope data along Line P indicate that the source of dissolved Pb in the upper 75 m at P26 is from Asian dust sources McAlister, At stations P4 through P20, North American dust sources were the dominant sources of metals to surface waters McAlister, Thus, the higher Fe and Cu concentrations at P26 compared to P16 could be due to atmospheric dust deposition from Asia.

It is also possible that transport of coastal waters via mesoscale eddies Johnson et al. However, satellite altimetry anomalies demonstrate that there was not an eddy at P26 during the time of sampling Figure 5. Though it is difficult to distinguish between atmospheric and isopycnal transport of Cu to P26 with our data, sporadic atmospheric dust deposition events have been previously linked to primary productivity increases at P26 Bishop et al.

These data suggest that a recent atmospheric dust deposition event may have occurred at P26 shortly before our arrival. Figure 5. Satellite derived sea surface height anomalies cm along the Line P transect for August 8, Strong Cu binding ligands were present across the transect at all sampling depths, and were always in excess of the total dissolved Cu concentrations, resulting in sparingly low inorganic Cu concentrations.

Compared to previous studies Buck et al. The ligand concentration range 6. Thus, the concentrations reported here are higher than those reported for just the strong ligand class by other groups, using a different analytical window 2—4 nM; e.

Copper Nanoparticles for Printed Electronics: Routes Towards Achieving Oxidation Stability

Although the provenance and structure of the strong Cu-binding ligands in the open ocean is unknown, there are a number of possible sources and candidate compounds.

Since [L] was not correlated with cyanobacteria abundance, heterotrophic bacteria may produce the majority of these strong Cu binding ligands.

Similar to [Cu] d , [L] was highest near the fresher coastal surface waters and decreased toward the open ocean. The higher [L]: Ligands in marine sediment porewaters, though weaker than in surface waters, can exceed nM concentrations and can diffuse into the overlying bottom water Skrabal et al.

As intermediate waters pass over the shelf sediments during upwelling, they may become enriched in weaker Cu binding ligands. Humic substances are electrochemically active, and their peaks were observed in the coastal stations data not shown.

Inorganic Cu concentrations varied five-fold 19—94 fM with a corresponding pCu range of However, the C: Few direct measurements of cellular Cu quotas—defined as the intracellular ratio of Cu normalized to organic C e.

Similar to standard 24 h oceanographic incubation assays e. C assimilation ratios presented here and in our previous study Semeniuk et al. Thus, while the accumulation of cellular 67 Cu and 14 C may vary diurnally, the ratio of the incorporation of each tracer after 24 h will represent a pseudo-steady state Cu: C assimilation ratio, as long as the added tracers are at equilibrium see Section Cu Uptake Rates, Cu: Assuming similar environmental conditions, our ratios should be comparable to other field and laboratory estimates of Cu: C quotas of phytoplankton isolates and mixed assemblages.

Table 7. Particulate Cu: C ratios in natural phytoplankton communities and laboratory strains grown under Cu-limiting and toxic conditions. There were two major differences between the experimental set-up in this study and our previous study.

First, in our previous study, the 67 Cu tracer was allowed to equilibrate with the in situ ligands for 30 min, while we chose a 2 h equilibration time here. Stronger Cu-binding ligands will have a faster forward reaction rate constant than weaker ligands due to competition with calcium see Section Cu Uptake Rates, Cu: Thus, we could expect the 67 Cu tracer to be rapidly bound to the strong ligand pool first, and more of the 67 Cu tracer would equilibrate with the weaker ligand pool with a longer equilibration time.

Since Cu bound to weaker organic ligands is more bioavailable than Cu bound to stronger ligands Semeniuk et al. Second, in our previous study, water was collected in the mid to late afternoon, spiked with 67 Cu and 14 C, and allowed to incubate for 24 h. In the present study, we spiked the water with the isotopes just before dawn. Thus, cells spent a greater proportion in the light near the start of the incubation than in our previous study.

A greater amount of fixed 14 C would have been available for respiration during the night than in our previous study. Freshly fixed organic 14 C can be respired within hours after initially fixed Halsey et al. C assimilation ratios as observed in the present study. Both methodological differences may have caused the higher Cu: C assimilation ratios here.

Thus, the tracer equilibration time appears to play a more important role, and future work should compare the effect of 67 Cu equilibration times with the in situ ligands on the measured Cu: C assimilation ratios. The size fractionated Cu: C assimilation ratios reported here 0.

In addition, independent measurements of cellular Cu quotas in natural phytoplankton communities compare well with our Cu: Average cellular Cu: These data suggest that the Cu: C ratios determined here using 67 Cu and 14 C approximate in situ values. Further work comparing 67 Cu and SXRF methods on the same samples would greatly benefit the veracity of both methods. Geochemical estimates of the Cu: P ratio of The range of these ratios 0. However, the average Cu: C ratios reported here and for single cells reported by Twining et al.

Interestingly, the Cu: Thus, diatoms may be primarily responsible for removing Cu from the mixed layer. Thus, the estimates of cellular Cu uptake rates across the transect are slightly faster than would be predicted using laboratory data. The difference between the laboratory and field estimates could be due to phytoplankton community composition structure and experimental designs e. Some phytoplankton have higher Cu demands during Fe limitation Peers et al.

Oceanic phytoplankton strains have higher basal metabolic Cu requirements compared to coastal strains, and may reflect an increased reliance on Cu in waters with chronically low Fe Peers and Price, ; Annett et al.

The somewhat elevated Fe concentrations measured at P26, possibly caused by an Fe-input event see Section Distribution of Total Dissolved Cu in Line P Surface Waters , provide an opportunity to test whether natural Fe-enrichment can influence the Cu physiology of marine phytoplankton.

Compared to P26 where the community was clearly Fe-limited, the Cu: Furthermore, the differences between Cu: These data indicate that there may be an interaction between Fe and Cu metabolism in indigenous phytoplankton communities, and that larger phytoplankton in HNLC regions may have a greater dependence on Cu availability.

Thus, we hypothesized that Cu: Laboratory studies of isolated marine phytoplankton strains have demonstrated that organically complexed Cu is bioavailable Hudson, ; Quigg et al. In situ Cu ligand complexes were also bioavailable to marine phytoplankton surveyed at P26 in Semeniuk et al. Despite this, Cu uptake rates or Cu: C assimilation ratios were not correlated with [Cu] d. Since phytoplankton Cu quotas and steady-state Cu uptake rates can vary by an order of magnitude among taxa grown in identical Cu concentrations Ho et al.

Similar to our previous studies of Cu uptake rates at P26 Semeniuk et al. We hypothesized that cellular efflux or remineralization by micrograzers may account for this. Thus, Cu cycling between dissolved and particulate phases in surface waters may be rapid compared to the export of particulate Cu from surface waters.

C drawdown ratio in surface waters along Line P using this slope 1. The calculated range, 1. Timothy et al. Using a middle value for the net Cu: Integrated over a 20 m summer mixed layer depth, this corresponds to an estimated net loss of Cu from the mixed layer of 1—1.

The surface residence time is much longer than other bioactive metals, such as Fe 6— days; Bergquist and Boyle, ; Ellwood et al.

Assuming that the source and loss terms in the surface mixed layer are at steady state, this indicates that a Cu atom in the surface ocean would exchange between dissolved and particulate phases 22— times before being exported. Copper enters phytoplankton through either a high- or low-affinity Cu transport system Guo et al. Thus, if intracellular Cu increases above the cell's metabolic demand due to non-specific uptake, it will have to be effluxed or detoxified intracellularly.

Copper efflux has also been documented in marine prokaryotic and eukaryotic phytoplankton Foster, ; Hall et al. In addition, micrograzing and bacterial remineralization might mediate fast exchange of Cu between the dissolved and the particulate pools, as recently shown for Ni and Zn Twining et al. Therefore, fast biological Cu uptake and efflux, as wells as efficient micrograzing and bacterial remineralization of Cu in surface waters might have significant impacts on the cycling of Cu in the sea.

The experimental design was carried out by DS and MM. All authors contributed to data interpretation, and the manuscript was primarily written by DS.

The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest. Anderson, D. Copper sensitivity of Gonyaulax tamarensis. Annett, A. The effects of Cu and Fe availability on the growth and Cu: C ratios of marine diatoms.

Barwell-Clarke, J. Google Scholar. Bergquist, B. Dissolved iron in the tropical and subtropical Atlantic Ocean. Cycle 20, GB Bishop, J. Robotic observations of dust storm enhancement of carbon biomass in the North Pacific.

Science , — Biswas, H. Copper addition helps alleviate iron stress in a coastal diatom: Booth, B. Size classes and major taxonomic groups of phytoplankton at two locations in the subarctic Pacific Ocean in May and August, Temporal variation in the structure of autotrophic and heterotrophic communities in the subarctic Pacific.


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