Records |
Author |
Tong, J.; Fu, Y.; Domaretskiy, D.; Della Pia, F.; Dagar, P.; Powell, L.; Bahamon, D.; Huang, S.; Xin, B.; Costa Filho, R.N.; Vega, L.F.; Grigorieva, I.V.; Peeters, F.M.; Michaelides, A.; Lozada-Hidalgo, M. |
Title |
Control of proton transport and hydrogenation in double-gated graphene |
Type |
A1 Journal Article |
Year |
2024 |
Publication |
Nature |
Abbreviated Journal |
Nature |
Volume |
630 |
Issue |
8017 |
Pages |
619-624 |
Keywords |
A1 Journal Article; Condensed Matter Theory (CMT) ; |
Abstract |
The basal plane of graphene can function as a selective barrier that is permeable to protons but impermeable to all ions and gases, stimulating its use in applications such as membranes, catalysis and isotope separation. Protons can chemically adsorb on graphene and hydrogenate it, inducing a conductor–insulator transition that has been explored intensively in graphene electronic devices. However, both processes face energy barriersand various strategies have been proposed to accelerate proton transport, for example by introducing vacancies, incorporating catalytic metalsor chemically functionalizing the lattice. But these techniques can compromise other properties, such as ion selectivity or mechanical stability. Here we show that independent control of the electric field,<italic>E</italic>, at around 1 V nm<sup>−1</sup>, and charge-carrier density,<italic>n</italic>, at around 1 × 10<sup>14</sup> cm<sup>−2</sup>, in double-gated graphene allows the decoupling of proton transport from lattice hydrogenation and can thereby accelerate proton transport such that it approaches the limiting electrolyte current for our devices. Proton transport and hydrogenation can be driven selectively with precision and robustness, enabling proton-based logic and memory graphene devices that have on–off ratios spanning orders of magnitude. Our results show that field effects can accelerate and decouple electrochemical processes in double-gated 2D crystals and demonstrate the possibility of mapping such processes as a function of<italic>E</italic>and<italic>n</italic>, which is a new technique for the study of 2D electrode–electrolyte interfaces. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
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Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2024-06-20 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0028-0836 |
ISBN |
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Additional Links |
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Impact Factor |
64.8 |
Times cited |
|
Open Access |
|
Notes |
This work was supported by UKRI (EP/X017745: M.L.-H; EP/X035891: A.M.), the Directed Research Projects Program of the Research and Innovation Center for Graphene and 2D Materials at Khalifa University (RIC2D-D001: M.L.-H., L.F.V. and D.B.), The Royal Society (URF\R1\201515: M.L.-H.) and the European Research Council (101071937: A.M.). Part of this work was supported by the Flemish Science Foundation (FWO-Vl, G099219N). A.M. acknowledges access to the UK national high-performance computing service (ARCHER2). |
Approved |
Most recent IF: 64.8; 2024 IF: 40.137 |
Call Number |
CMT @ cmt @ |
Serial |
9247 |
Permanent link to this record |
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Author |
Huang, S.; Griffin, E.; Cai, J.; Xin, B.; Tong, J.; Fu, Y.; Kravets, V.; Peeters, F.M.; Lozada-Hidalgo, M. |
Title |
Gate-controlled suppression of light-driven proton transport through graphene electrodes |
Type |
A1 Journal article |
Year |
2023 |
Publication |
Nature communications |
Abbreviated Journal |
|
Volume |
14 |
Issue |
1 |
Pages |
6932-6937 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Recent experiments demonstrated that proton transport through graphene electrodes can be accelerated by over an order of magnitude with low intensity illumination. Here we show that this photo-effect can be suppressed for a tuneable fraction of the infra-red spectrum by applying a voltage bias. Using photocurrent measurements and Raman spectroscopy, we show that such fraction can be selected by tuning the Fermi energy of electrons in graphene with a bias, a phenomenon controlled by Pauli blocking of photo-excited electrons. These findings demonstrate a dependence between graphene's electronic and proton transport properties and provide fundamental insights into molecularly thin electrode-electrolyte interfaces and their interaction with light. Recent experiments have shown that proton transport through graphene electrodes can be promoted by light, but the understanding of this phenomenon remains unclear. Here, the authors report the electrical tunability of this photo-effect, showing a connection between graphene electronic and proton transport properties. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001094448600003 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2023-10-31 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2041-1723 |
ISBN |
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Additional Links |
UA library record; WoS full record |
Impact Factor |
16.6 |
Times cited |
|
Open Access |
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Notes |
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Approved |
Most recent IF: 16.6; 2023 IF: 12.124 |
Call Number |
UA @ admin @ c:irua:201185 |
Serial |
9041 |
Permanent link to this record |
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Author |
Wahab, O.J.; Daviddi, E.; Xin, B.; Sun, P.Z.; Griffin, E.; Colburn, A.W.; Barry, D.; Yagmurcukardes, M.; Peeters, F.M.; Geim, A.K.; Lozada-Hidalgo, M.; Unwin, P.R. |
Title |
Proton transport through nanoscale corrugations in two-dimensional crystals |
Type |
A1 Journal article |
Year |
2023 |
Publication |
Nature |
Abbreviated Journal |
|
Volume |
620 |
Issue |
7975 |
Pages |
1-17 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Defect-free graphene is impermeable to all atoms(1-5) and ions(6,7) under ambient conditions. Experiments that can resolve gas flows of a few atoms per hour through micrometre-sized membranes found that monocrystalline graphene is completely impermeable to helium, the smallest atom(2,5). Such membranes were also shown to be impermeable to all ions, including the smallest one, lithium(6,7). By contrast, graphene was reported to be highly permeable to protons, nuclei of hydrogen atoms(8,9). There is no consensus, however, either on the mechanism behind the unexpectedly high proton permeability(10-14) or even on whether it requires defects in graphene's crystal lattice(6,8,15-17). Here, using high-resolution scanning electrochemical cell microscopy, we show that, although proton permeation through mechanically exfoliated monolayers of graphene and hexagonal boron nitride cannot be attributed to any structural defects, nanoscale non-flatness of two-dimensional membranes greatly facilitates proton transport. The spatial distribution of proton currents visualized by scanning electrochemical cell microscopy reveals marked inhomogeneities that are strongly correlated with nanoscale wrinkles and other features where strain is accumulated. Our results highlight nanoscale morphology as an important parameter enabling proton transport through two-dimensional crystals, mostly considered and modelled as flat, and indicate that strain and curvature can be used as additional degrees of freedom to control the proton permeability of two-dimensional materials. A study using high-resolution scanning electrochemical cell microscopy attributes proton permeation through defect-free graphene and hexagonal boron nitride to transport across areas of the structure that are under strain. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
001153630400007 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2023-08-23 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0028-0836; 1476-4687 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
64.8 |
Times cited |
17 |
Open Access |
|
Notes |
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Approved |
Most recent IF: 64.8; 2023 IF: 40.137 |
Call Number |
UA @ admin @ c:irua:203827 |
Serial |
9078 |
Permanent link to this record |
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Author |
Cai, J.; Griffin, E.; Guarochico-Moreira, V.; Barry, D.; Xin, B.; Huang, S.; Geim, A.K.; Peeters, F.M.; Lozada-Hidalgo, M. |
Title |
Photoaccelerated water dissociation across one-atom-thick electrodes |
Type |
A1 Journal article |
Year |
2022 |
Publication |
Nano letters |
Abbreviated Journal |
Nano Lett |
Volume |
22 |
Issue |
23 |
Pages |
9566-9570 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Recent experiments demonstrated that interfacial water dissociation (H2O ⇆ H+ + OH-) could be accelerated exponentially by an electric field applied to graphene electrodes, a phenomenon related to the Wien effect. Here we report an order-of-magnitude acceleration of the interfacial water dissociation reaction under visible-light illumination. This process is accompanied by spatial separation of protons and hydroxide ions across one-atom-thick graphene and enhanced by strong interfacial electric fields. The found photoeffect is attributed to the combination of graphene's perfect selectivity with respect to protons, which prevents proton-hydroxide recombination, and to proton transport acceleration by the Wien effect, which occurs in synchrony with the water dissociation reaction. Our findings provide fundamental insights into ion dynamics near atomically thin proton-selective interfaces and suggest that strong interfacial fields can enhance and tune very fast ionic processes, which is of relevance for applications in photocatalysis and designing reconfigurable materials. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000892112200001 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2022-11-30 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
1530-6984 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
10.8 |
Times cited |
3 |
Open Access |
OpenAccess |
Notes |
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Approved |
Most recent IF: 10.8 |
Call Number |
UA @ admin @ c:irua:192759 |
Serial |
7330 |
Permanent link to this record |
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Author |
Cai, J.; Griffin, E.; Guarochico-Moreira, V.H.; Barry, D.; Xin, B.; Yagmurcukardes, M.; Zhang, S.; Geim, A.K.; Peeters, F.M.; Lozada-Hidalgo, M. |
Title |
Wien effect in interfacial water dissociation through proton-permeable graphene electrodes |
Type |
A1 Journal article |
Year |
2022 |
Publication |
Nature communications |
Abbreviated Journal |
Nat Commun |
Volume |
13 |
Issue |
1 |
Pages |
5776-5777 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Strong electric fields can accelerate molecular dissociation reactions. The phenomenon known as the Wien effect was previously observed using high-voltage electrolysis cells that produced fields of about 10(7) V m(-1), sufficient to accelerate the dissociation of weakly bound molecules (e.g., organics and weak electrolytes). The observation of the Wien effect for the common case of water dissociation (H2O reversible arrow H+ + OH-) has remained elusive. Here we study the dissociation of interfacial water adjacent to proton-permeable graphene electrodes and observe strong acceleration of the reaction in fields reaching above 10(8) V m(-1). The use of graphene electrodes allows measuring the proton currents arising exclusively from the dissociation of interfacial water, while the electric field driving the reaction is monitored through the carrier density induced in graphene by the same field. The observed exponential increase in proton currents is in quantitative agreement with Onsager's theory. Our results also demonstrate that graphene electrodes can be valuable for the investigation of various interfacial phenomena involving proton transport. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000862552600012 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2022-10-01 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
16.6 |
Times cited |
14 |
Open Access |
OpenAccess |
Notes |
|
Approved |
Most recent IF: 16.6 |
Call Number |
UA @ admin @ c:irua:191575 |
Serial |
7228 |
Permanent link to this record |
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Author |
Sun, P.Z.; Yagmurcukardes, M.; Zhang, R.; Kuang, W.J.; Lozada-Hidalgo, M.; Liu, B.L.; Cheng, H.-M.; Wang, F.C.; Peeters, F.M.; Grigorieva, I.V.; Geim, A.K. |
Title |
Exponentially selective molecular sieving through angstrom pores |
Type |
A1 Journal article |
Year |
2021 |
Publication |
Nature Communications |
Abbreviated Journal |
Nat Commun |
Volume |
12 |
Issue |
1 |
Pages |
7170 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Two-dimensional crystals with angstrom-scale pores are widely considered as candidates for a next generation of molecular separation technologies aiming to provide extreme, exponentially large selectivity combined with high flow rates. No such pores have been demonstrated experimentally. Here we study gas transport through individual graphene pores created by low intensity exposure to low kV electrons. Helium and hydrogen permeate easily through these pores whereas larger species such as xenon and methane are practically blocked. Permeating gases experience activation barriers that increase quadratically with molecules' kinetic diameter, and the effective diameter of the created pores is estimated as similar to 2 angstroms, about one missing carbon ring. Our work reveals stringent conditions for achieving the long sought-after exponential selectivity using porous two-dimensional membranes and suggests limits on their possible performance. Two-dimensional membranes with angstrom-sized pores are predicted to combine high permeability with exceptional selectivity, but experimental demonstration has been challenging. Here the authors realize angstrom-sized pores in monolayer graphene and demonstrate gas transport with activation barriers increasing quadratically with the molecular kinetic diameter. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000728562700016 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2021-12-09 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
2041-1723 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
12.124 |
Times cited |
28 |
Open Access |
OpenAccess |
Notes |
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Approved |
Most recent IF: 12.124 |
Call Number |
UA @ admin @ c:irua:184840 |
Serial |
6989 |
Permanent link to this record |
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Author |
Zou, Y.-C.; Mogg, L.; Clark, N.; Bacaksiz, C.; Milanovic, S.; Sreepal, V.; Hao, G.-P.; Wang, Y.-C.; Hopkinson, D.G.; Gorbachev, R.; Shaw, S.; Novoselov, K.S.; Raveendran-Nair, R.; Peeters, F.M.; Lozada-Hidalgo, M.; Haigh, S.J. |
Title |
Ion exchange in atomically thin clays and micas |
Type |
A1 Journal article |
Year |
2021 |
Publication |
Nature Materials |
Abbreviated Journal |
Nat Mater |
Volume |
20 |
Issue |
12 |
Pages |
1677-1682 |
Keywords |
A1 Journal article; Condensed Matter Theory (CMT) |
Abstract |
The physical properties of clays and micas can be controlled by exchanging ions in the crystal lattice. Atomically thin materials can have superior properties in a range of membrane applications, yet the ion-exchange process itself remains largely unexplored in few-layer crystals. Here we use atomic-resolution scanning transmission electron microscopy to study the dynamics of ion exchange and reveal individual ion binding sites in atomically thin and artificially restacked clays and micas. We find that the ion diffusion coefficient for the interlayer space of atomically thin samples is up to 10(4) times larger than in bulk crystals and approaches its value in free water. Samples where no bulk exchange is expected display fast exchange at restacked interfaces, where the exchanged ions arrange in islands with dimensions controlled by the moire superlattice dimensions. We attribute the fast ion diffusion to enhanced interlayer expandability resulting from weaker interlayer binding forces in both atomically thin and restacked materials. This work provides atomic scale insights into ion diffusion in highly confined spaces and suggests strategies to design exfoliated clay membranes with enhanced performance. Layered clays are of interest for membranes and many other applications but their ion-exchange dynamics remain unexplored in atomically thin materials. Here, using electron microscopy, it is found that the ion diffusion for few-layer two-dimensional clays approaches that of free water and that superlattice cation islands can form in twisted and restacked materials. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000689664000001 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2021-09-21 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
1476-1122; 1476-4660 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
39.737 |
Times cited |
2 |
Open Access |
OpenAccess |
Notes |
|
Approved |
Most recent IF: 39.737 |
Call Number |
UA @ admin @ c:irua:181691 |
Serial |
6999 |
Permanent link to this record |
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Author |
Griffin, E.; Mogg, L.; Hao, G.-P.; Kalon, G.; Bacaksiz, C.; Lopez-Polin, G.; Zhou, T.Y.; Guarochico, V.; Cai, J.; Neumann, C.; Winter, A.; Mohn, M.; Lee, J.H.; Lin, J.; Kaiser, U.; Grigorieva, I., V; Suenaga, K.; Ozyilmaz, B.; Cheng, H.-M.; Ren, W.; Turchanin, A.; Peeters, F.M.; Geim, A.K.; Lozada-Hidalgo, M. |
Title |
Proton and Li-Ion permeation through graphene with eight-atom-ring defects |
Type |
A1 Journal article |
Year |
2020 |
Publication |
Acs Nano |
Abbreviated Journal |
Acs Nano |
Volume |
14 |
Issue |
6 |
Pages |
7280-7286 |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Defect-free graphene is impermeable to gases and liquids but highly permeable to thermal protons. Atomic-scale defects such as vacancies, grain boundaries, and Stone-Wales defects are predicted to enhance graphene's proton permeability and may even allow small ions through, whereas larger species such as gas molecules should remain blocked. These expectations have so far remained untested in experiment. Here, we show that atomically thin carbon films with a high density of atomic-scale defects continue blocking all molecular transport, but their proton permeability becomes similar to 1000 times higher than that of defect-free graphene. Lithium ions can also permeate through such disordered graphene. The enhanced proton and ion permeability is attributed to a high density of eight-carbon-atom rings. The latter pose approximately twice lower energy barriers for incoming protons compared to that of the six-atom rings of graphene and a relatively low barrier of similar to 0.6 eV for Li ions. Our findings suggest that disordered graphene could be of interest as membranes and protective barriers in various Li-ion and hydrogen technologies. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000543744100086 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2020-05-19 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
1936-0851 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
17.1 |
Times cited |
53 |
Open Access |
|
Notes |
; The work was supported by the Lloyd's Register Foundation, EPSRC-EP/N010345/1, the European Research Council, the Graphene Flagship, the Deutsche Forschungsgemeinschaft project TRR 234 “CataLight” (Project B7, Grant No. 364549901), and the research infrastructure Grant No. INST 275/25 7-1 FUGG. E.G. and L.M. acknowledge the EPSRC NowNANO programme for funding. ; |
Approved |
Most recent IF: 17.1; 2020 IF: 13.942 |
Call Number |
UA @ admin @ c:irua:170708 |
Serial |
6586 |
Permanent link to this record |
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Author |
Mogg, L.; Hao, G.-P.; Zhang, S.; Bacaksiz, C.; Zou, Y.; Haigh, S.J.; Peeters, F.M.; Geim, A.K.; Lozada-Hidalgo, M. |
Title |
Atomically thin micas as proton-conducting membranes |
Type |
A1 Journal article |
Year |
2019 |
Publication |
Nature nanotechnology |
Abbreviated Journal |
Nat Nanotechnol |
Volume |
14 |
Issue |
10 |
Pages |
962-+ |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Monolayers of graphene and hexagonal boron nitride (hBN) are highly permeable to thermal protons1,2. For thicker two-dimensional (2D) materials, proton conductivity diminishes exponentially, so that, for example, monolayer MoS2 that is just three atoms thick is completely impermeable to protons1. This seemed to suggest that only one-atom-thick crystals could be used as proton-conducting membranes. Here, we show that few-layer micas that are rather thick on the atomic scale become excellent proton conductors if native cations are ion-exchanged for protons. Their areal conductivity exceeds that of graphene and hBN by one to two orders of magnitude. Importantly, ion-exchanged 2D micas exhibit this high conductivity inside the infamous gap for proton-conducting materials3, which extends from ∼100 °C to 500 °C. Areal conductivity of proton-exchanged monolayer micas can reach above 100 S cm−2 at 500 °C, well above the current requirements for the industry roadmap4. We attribute the fast proton permeation to ~5-Å-wide tubular channels that perforate micas’ crystal structure, which, after ion exchange, contain only hydroxyl groups inside. Our work indicates that there could be other 2D crystals5 with similar nanometre-scale channels, which could help close the materials gap in proton-conducting applications. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000488977100016 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2019-09-02 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1748-3387; 1748-3395 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
38.986 |
Times cited |
44 |
Open Access |
|
Notes |
; The work was supported by the Lloyd's Register Foundation, the Engineering and Physical Sciences Research Council (EPSRC)-EP/N010345/1, EP/M010619/1 and EP/ P009050/1, the European Research Council, the Graphene Flagship and the Royal Society. M.L.-H. acknowledges a Leverhulme Early Career Fellowship, G.-P.H. acknowledges a Marie Curie International Incoming Fellowship, and L.M. acknowledges the EPSRC NOWNano programme for funding. Y.Z. acknowledges the assistance of Eric Prestat in TEM specimen preparation. Computational resources were provided by the TUBITAK ULAKBIM High Performance and Grid Computing Center (TR-Grid e-Infrastructure). ; |
Approved |
Most recent IF: 38.986 |
Call Number |
UA @ admin @ c:irua:163589 |
Serial |
5407 |
Permanent link to this record |
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Author |
Hu, S.; Gopinadhan, K.; Rakowski, A.; Neek-Amal, M.; Heine, T.; Grigorieva, I.V.; Haigh, S.J.; Peeters, F.M.; Geim, A.K.; Lozada-Hidalgo, M. |
Title |
Transport of hydrogen isotopes through interlayer spacing in van der Waals crystals |
Type |
A1 Journal article |
Year |
2018 |
Publication |
Nature nanotechnology |
Abbreviated Journal |
Nat Nanotechnol |
Volume |
13 |
Issue |
6 |
Pages |
468-+ |
Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
Abstract |
Atoms start behaving as waves rather than classical particles if confined in spaces commensurate with their de Broglie wavelength. At room temperature this length is only about one angstrom even for the lightest atom, hydrogen. This restricts quantum-confinement phenomena for atomic species to the realm of very low temperatures(1-5). Here, we show that van der Waals gaps between atomic planes of layered crystals provide angstrom-size channels that make quantum confinement of protons apparent even at room temperature. Our transport measurements show that thermal protons experience a notably higher barrier than deuterons when entering van der Waals gaps in hexagonal boron nitride and molybdenum disulfide. This is attributed to the difference in the de Broglie wavelengths of the isotopes. Once inside the crystals, transport of both isotopes can be described by classical diffusion, albeit with unexpectedly fast rates comparable to that of protons in water. The demonstrated angstrom-size channels can be exploited for further studies of atomistic quantum confinement and, if the technology can be scaled up, for sieving hydrogen isotopes. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000434715700015 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2018-04-04 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
1748-3387; 1748-3395 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
38.986 |
Times cited |
32 |
Open Access |
|
Notes |
; The authors acknowledge support from the Lloyd's Register Foundation, EPSRC – EP/N010345/1, the European Research Council ARTIMATTER project – ERC-2012-ADG and from Graphene Flagship. M.L.-H. acknowledges a Leverhulme Early Career Fellowship. ; |
Approved |
Most recent IF: 38.986 |
Call Number |
UA @ lucian @ c:irua:152014UA @ admin @ c:irua:152014 |
Serial |
5046 |
Permanent link to this record |
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Author |
Margui, E.; Hidalgo, M.; Queralt, I.; van Meel, K.; Fontas, C. |
Title |
Analytical capabilities of laboratory, benchtop and handheld X-ray fluorescence systems for detection of metals in aqueous samples pre-concentrated with solid-phase extraction disks |
Type |
A1 Journal article |
Year |
2012 |
Publication |
Spectrochimica acta: part B : atomic spectroscopy |
Abbreviated Journal |
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Volume |
67 |
Issue |
|
Pages |
17-23 |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
Abstract |
We aimed to achieve improved instrumental sensitivity and detection limits for the analysis of several elements (Cu, Ni, Zn, Pb and Cd) in aqueous samples with energy dispersive X-ray fluorescence spectrometry (EDXRF). The metals were pre-concentrated from aqueous solutions using commercially available organic-based solid-phase extraction (SPE) disks functionalized with iminodiacetate groups. These thin-layer organic materials provide an ideal support for XRF analysis. The elements were collected on the SPE extraction disks using a simple filtration procedure (starting with 1 L of aqueous sample) that allows direct XRF measurements to be performed in the field (in situ). We evaluated the analytical possibilities and drawbacks of using this pre-concentration procedure in combination with the following XRF configurations: a handheld unit, a benchtop EDXRF system and a high-energy polarized-beam EDXRF instrument (HE-P-EDXRF). Using the HE-P-EDXRF system, the detection limits for all metals were more than one order of magnitude lower than those attained using handheld and benchtop EDXRF instrumentation. For the detection of metal concentrations higher than similar to 20 mu g/L, however, handheld or benchtop systems remain a very good option due to their extreme simplicity of operation and low-cost, compact design. We demonstrate the application of these methodologies, using the three equipment systems, to the analysis of trace concentrations of metals in different types of aqueous samples, including tap water and waste water. (C) 2011 Elsevier B.V. All rights reserved. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000302757200003 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2011-12-19 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
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Edition |
|
ISSN |
0584-8547; 1873-3565 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
|
Times cited |
|
Open Access |
|
Notes |
|
Approved |
no |
Call Number |
UA @ admin @ c:irua:98338 |
Serial |
7454 |
Permanent link to this record |
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|
|
Author |
Marguí, E.; Van Grieken, R.; Fontàs, C.; Hidalgo, M.; Queralt, I. |
Title |
Preconcentration methods for the analysis of liquid samples by X-ray fluorescence techniques |
Type |
A1 Journal article |
Year |
2010 |
Publication |
Applied spectroscopy reviews |
Abbreviated Journal |
|
Volume |
45 |
Issue |
3 |
Pages |
179-205 |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
Abstract |
This article gives an overview of the state-of-the-art of multi-element and single-element preconcentration procedures prior to X-ray fluorescence (XRF) analysis of liquid samples. Many of these preconcentration methods were developed long ago and the purpose of this review is to present some new efficient variations of these methods and new techniques extending the possibilities of XRF for liquid solutions analysis. In addition, trends and future perspectives in this domain are also commented on and discussed in the last section of the review. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000277705800002 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2010-01-28 |
Series Editor |
|
Series Title |
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Abbreviated Series Title |
|
Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0066-5541 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
|
Times cited |
|
Open Access |
|
Notes |
|
Approved |
no |
Call Number |
UA @ admin @ c:irua:82557 |
Serial |
8400 |
Permanent link to this record |
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|
|
Author |
Marguí, E.; van Meel, K.; Van Grieken, R.; Buendía, A.; Fontás, C.; Hidalgo, M.; Queralt, I. |
Title |
Method for the determination of Pd-catalyst residues in active pharmaceutical ingredients by means of high-energy polarized-beam energy dispersive X-ray fluorescence |
Type |
A1 Journal article |
Year |
2009 |
Publication |
Analytical chemistry |
Abbreviated Journal |
|
Volume |
81 |
Issue |
4 |
Pages |
1404-1410 |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
Abstract |
In medicinal chemistry, Pd is perhaps the most-widely utilized precious metal, as catalyst in reactions which represent key transformations toward the synthesis of new active pharmaceutical ingredients (APIs). The disadvantage of this metal-catalyzed chemistry is that expensive and toxic metal residues are invariably left bound to the desired product. Thus, stringent regulatory guidelines exist for the amount of residual Pd that a drug candidate is allowed to contain. In this work, a rapid and simple method for the determination of Pd in API samples by high-energy polarized-beam energy dispersive X-ray fluorescence spectrometry has been developed and validated according to the specification limits of current legislation (10 mg kg−1 Pd) and the International Conference on Harmonisation of Technical Requirements for Registration of Pharmaceuticals for Human Use (ICH guidelines). Sample and calibration standards preparation includes a first step of homogenization and then, in a second step, the pressing of the powdered material into pellets without any chemical treatment. The use of several synthetic calibration standards made of cellulose to simulate the API matrix appears to be an effective means to obtain reliable calibration curves with a good spread of data points over the working range. With the use of the best measuring conditions, the limit of detection (0.11 mg kg−1 Pd) as well as the limit of quantitation (0.37 mg kg−1 Pd) achieved meet rigorous requirements. The repeatability of the XRF measurement appeared to be less than 2%, while the precision of the whole method was around 7%. Trueness was evaluated by analyzing spiked API samples at the level of the specification limit and calculating the recovery factor, which was better than 95%. To study the applicability of the developed methodology for the intended purpose, three batches of the studied API were analyzed for their Pd content, and the attained results were comparable to those obtained by the daily routine method (acid digestion plus atomic spectroscopy) used in most pharmaceutical laboratories. |
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000263319000015 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2009-01-22 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
|
Series Issue |
|
Edition |
|
ISSN |
0003-2700; 5206-882x |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
|
Times cited |
|
Open Access |
|
Notes |
|
Approved |
no |
Call Number |
UA @ admin @ c:irua:74340 |
Serial |
8220 |
Permanent link to this record |
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|
|
Author |
van Meel, K.; Fontàs, C.; Van Grieken, R.; Queralt, I.; Hidalgo, M.; Marguí, E. |
Title |
Application of high-energy polarised beam energy dispersive X-ray fluorescence spectrometry to cadmium determination in saline solutions |
Type |
A1 Journal article |
Year |
2008 |
Publication |
Journal of analytical atomic spectrometry |
Abbreviated Journal |
|
Volume |
23 |
Issue |
7 |
Pages |
1034-1037 |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
Abstract |
|
Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000257146000017 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2008-04-22 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0267-9477 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
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Times cited |
|
Open Access |
|
Notes |
|
Approved |
no |
Call Number |
UA @ admin @ c:irua:69424 |
Serial |
7476 |
Permanent link to this record |
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|
|
Author |
Marguí, E.; Fontàs, C.; van Meel, K.; Van Grieken, R.; Queralt, I.; Hidalgo, M. |
Title |
High-energy polarized-beam energy-dispersive X-ray fluorescence analysis combined with activated thin layers for cadmium determination at trace levels in complex environmental liquid samples |
Type |
A1 Journal article |
Year |
2008 |
Publication |
Analytical chemistry |
Abbreviated Journal |
|
Volume |
80 |
Issue |
7 |
Pages |
2357-2364 |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
Abstract |
|
Address |
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Corporate Author |
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Thesis |
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Publisher |
|
Place of Publication |
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Editor |
|
Language |
|
Wos |
000254593500015 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2008-03-08 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
0003-2700; 5206-882x |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
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Times cited |
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Open Access |
|
Notes |
|
Approved |
no |
Call Number |
UA @ admin @ c:irua:68425 |
Serial |
8032 |
Permanent link to this record |
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|
|
Author |
Marguí, E.; Padilla, R.; Hidalgo, M.; Queralt, I.; Van Grieken, R. |
Title |
High-energy polarized-beam EDXRF for trace metal analysis of vegetation samples in environmental studies |
Type |
A1 Journal article |
Year |
2006 |
Publication |
X-ray spectrometry |
Abbreviated Journal |
|
Volume |
35 |
Issue |
3 |
Pages |
169-177 |
Keywords |
A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
Abstract |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
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Editor |
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Language |
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Wos |
000237818300005 |
Publication Date ![sorted by Publication Date field, descending order (down)](img/sort_desc.gif) |
2006-03-23 |
Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
|
ISSN |
0049-8246 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
Impact Factor |
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Times cited |
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Open Access |
|
Notes |
|
Approved |
no |
Call Number |
UA @ admin @ c:irua:57751 |
Serial |
8031 |
Permanent link to this record |