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Article: H-Bond-Mediated Selectivity Control of Formate versus CO during CO₂ Photoreduction with Two Cooperative Cu/X Sites

Zhuo, Tian-Ci / Song, Yang / Zhuang, Gui-Lin / Chang, Lu-Ping / Yao, Shuang / Zhang, Wei / Wang, Ye / Wang, Ping / Lin, Wenbin / Lu, Tong-Bu / Zhang, Zhi-Ming

Journal of the American Chemical Society. 2021 Apr. 19, v. 143, no. 16

2021

Abstract: ... μmol g–¹ in 10 h by hierarchical integration of photosensitizers and monometallic [bpy-Cu/ClX] (X = Cl ... or adenine) catalysts into a stable Eu-bpy metal–organic framework. However, replacing X ... with pyridine in [bpy-CuCl/X] significantly reduced formate production while increasing the CO yield to 960 μmol ...

Abstract	It is highly desirable to achieve solar-driven conversion of CO₂ to valuable fuels with controlled selectivity. The existing catalysts are mainly explored for CO production but rarely for formate generation. Herein, highly selective photoreduction of CO₂ to formate (99.7%) was achieved with a high yield of 3040 μmol g–¹ in 10 h by hierarchical integration of photosensitizers and monometallic [bpy-Cu/ClX] (X = Cl or adenine) catalysts into a stable Eu-bpy metal–organic framework. However, replacing X with pyridine in [bpy-CuCl/X] significantly reduced formate production while increasing the CO yield to 960 μmol g–¹. Systematic investigations revealed that the catalytic process is mediated by the H-bond synergy between Cu-bound X and CO₂-derived species, and the selectivity of HCOO– can be controlled by simply replacing the coordination ligands. This work provides a molecularly precise structural model to provide mechanistic insights for selectivity control of CO₂ photoreduction.
Keywords	adenine ; carbon dioxide ; catalytic activity ; coordination polymers ; formates ; ligands ; models ; photoreduction ; pyridines
Language	English
Dates of publication	2021-0419
Size	p. 6114-6122.
Publishing place	American Chemical Society
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.0c13048
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: NAD(P)H: Quinone oxidoreductase 1 overexpression in hepatocellular carcinoma potentiates apoptosis evasion through regulating stabilization of X-linked inhibitor of apoptosis protein.

Cancer letters

2019 Volume 451, Page(s) 156–167

Abstract: NAD(P)H: quinone oxidoreductase 1 (NQO1) is an antioxidant enzyme which is associated with poor ... cells enhanced protein stability of X-linked inhibitor of apoptosis protein (XIAP) by increasing ...

Abstract	NAD(P)H: quinone oxidoreductase 1 (NQO1) is an antioxidant enzyme which is associated with poor prognosis in human breast, colon, lung and liver cancers. However, the molecular mechanisms underlying the pro-tumorigenic function of NQO1 remains unclear. This study investigated the function of NQO1 in the context of hepatocellular carcinoma (HCC) development. We found that NQO1 was frequently up-regulated in human liver cancer, and its high expression level was correlated with the tumor stage and low survival rate of HCC patients. Loss-of-function of NQO1 inhibited growth in HCC cells with increased apoptosis in vitro, and suppressed orthotopic tumorigenicity in vivo. Mechanistically, high level of NQO1 in HCC cells enhanced protein stability of X-linked inhibitor of apoptosis protein (XIAP) by increasing its phosphorylation at Ser 87. Reintroduction of wile type XIAP and the phospho-mimic mutants XIAP
MeSH term(s)	Animals ; Apoptosis ; Carcinoma, Hepatocellular/enzymology ; Carcinoma, Hepatocellular/pathology ; Cell Line, Transformed ; Humans ; Liver Neoplasms/enzymology ; Liver Neoplasms/pathology ; Male ; Mice ; Mice, Inbred BALB C ; NAD(P)H Dehydrogenase (Quinone)/genetics ; NAD(P)H Dehydrogenase (Quinone)/metabolism ; Phosphorylation ; X-Linked Inhibitor of Apoptosis Protein/metabolism
Chemical Substances	X-Linked Inhibitor of Apoptosis Protein ; XIAP protein, human ; NAD(P)H Dehydrogenase (Quinone) (EC 1.6.5.2) ; NQO1 protein, human (EC 1.6.5.2)
Language	English
Publishing date	2019-03-10
Publishing country	Ireland
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	195674-7
ISSN	1872-7980 ; 0304-3835
ISSN (online)	1872-7980
ISSN	0304-3835
DOI	10.1016/j.canlet.2019.02.053
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Book ; Online: Hole-Doped Room-Temperature Superconductivity in H$_{3}$S$_{1-x}$Z$_x$ (Z=C, Si)

Ge, Yanfeng / Zhang, Fan / Dias, Ranga P. / Hemley, Russell J. / Yao, Yugui

2020

Abstract: ... compressed C-S-H system [Nature 586, 373-377 (2020)]. Our work opens a new avenue for substantially raising ... on the superconductivity of H$_3$S with the $Im\bar{3}m$ structure at megabar pressure. The hole doping can fine-tune ... This can boost the critical temperature from the original 203 K to 289 K and 283 K, respectively, for H$_3$S$_{0 ...

Abstract	We examine the effects of the low-level substitution of S atoms by C and Si atoms on the superconductivity of H$_3$S with the $Im\bar{3}m$ structure at megabar pressure. The hole doping can fine-tune the Fermi energy to reach the electronic density-of-states peak maximizing the electron-phonon coupling. This can boost the critical temperature from the original 203 K to 289 K and 283 K, respectively, for H$_3$S$_{0.962}$C$_{0.038}$ at 260 GPa and H$_3$S$_{0.960}$Si$_{0.040}$ at 230 GPa. The former may provide an explanation for the recent experimental observation of room-temperature superconductivity in a highly compressed C-S-H system [Nature 586, 373-377 (2020)]. Our work opens a new avenue for substantially raising the critical temperatures of hydrogen-rich materials. Comment: 5 pages, 2 figures
Keywords	Condensed Matter - Superconductivity ; Condensed Matter - Materials Science
Publishing date	2020-11-25
Publishing country	us
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article ; Online: Theoretical study on the reaction CX3 + SiH(CH3)3 (X = H, F).

Zhang, Hui / Yang, Liu / Liu, Jing-Yao / Li, Ze-Sheng

Journal of computational chemistry

2012 Volume 33, Issue 2, Page(s) 203–210

Abstract: Theoretical investigations are carried out on the multiple-channel reactions, CH(3) + SiH(CH(3))(3) → products and CF(3) + SiH(CH(3))(3) → products. The minimum energy paths (MEP) are calculated at the MP2/6-311 + G(d,p) level, and energetic information ... ...

Abstract	Theoretical investigations are carried out on the multiple-channel reactions, CH(3) + SiH(CH(3))(3) → products and CF(3) + SiH(CH(3))(3) → products. The minimum energy paths (MEP) are calculated at the MP2/6-311 + G(d,p) level, and energetic information is further refined by the MC-QCISD (single point) method. The rate constants for major reaction channels are calculated by the canonical variational transition state theory (CVT) with small-curvature tunneling (SCT) correction over the temperature range 200-1500 K. The theoretical rate constants are in good agreement with the available experimental data and are found to be k(1a)(T) = 1.93 × 10(-24) T(3.15) exp(-1214.59/T) and k(2a)(T) = 1.33 × 10(-25) T(4.13) exp(-397.94/T) (in unit of cm(3) molecule(-1) s(-1)). Our calculations indicate that hydrogen abstraction channel from SiH group is the major channel due to the smaller barrier height among five channels considered.
MeSH term(s)	Hydrocarbons/chemistry ; Kinetics ; Methane ; Models, Chemical ; Quantum Theory ; Silanes/chemistry ; Thermodynamics
Chemical Substances	Hydrocarbons ; Silanes ; Methane (OP0UW79H66)
Language	English
Publishing date	2012-01-15
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	1479181-x
ISSN	1096-987X ; 0192-8651
ISSN (online)	1096-987X
ISSN	0192-8651
DOI	10.1002/jcc.21964
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Article ; Online: X- and H-shape two dimensional conjugated oligomers with anthracene as the node.

Cui, Weibin / Fu, Yingying / Qu, Yao / Tian, Hongkun / Zhang, Jingping / Xie, Zhiyuan / Geng, Yanhou / Wang, Fosong

Chemistry, an Asian journal

2010 Volume 5, Issue 4, Page(s) 932–940

Abstract: X- and H-shape two-dimensional (2D) conjugated oligomers (X- and H-mers) and relevant model ... compounds, the X- and H-mers are featured with broader absorption spectra and narrower energy bandgaps ... orbital (LUMO) also indicate that these X- and H-mers are 2D conjugated. Solution processed bulk ...

Abstract	X- and H-shape two-dimensional (2D) conjugated oligomers (X- and H-mers) and relevant model compounds have been synthesized through the introduction of different conjugated segments at the 9,10 and 2,6-positions of anthracene, and their properties were studied in detail. Comparing with the model compounds, the X- and H-mers are featured with broader absorption spectra and narrower energy bandgaps. Computational studies on the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) also indicate that these X- and H-mers are 2D conjugated. Solution processed bulk heterojunction (BHJ) solar cells with [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) as the acceptor material exhibited the power conversion efficiency (PCE) up to 0.53 %.
Language	English
Publishing date	2010-04-01
Publishing country	Germany
Document type	Journal Article
ISSN	1861-471X
ISSN (online)	1861-471X
DOI	10.1002/asia.200900591
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Article ; Online: Theoretical study of X⁻ · 1 · YF (1 = triazine, X = Cl, Br and I, Y = H, Cl, Br, I, PH₂ and AsH₂): noncovalently electron-withdrawing effects on anion-arene interactions.

Chen, Yishan / Yao, Lifeng

Journal of molecular modeling

2014 Volume 20, Issue 1, Page(s) 2076

Abstract: The ternary complexes X(-) · 1 · YF (1 = triazine, X = Cl, Br and I, Y = H, Cl, Br, I, PH2 and AsH2 ... on anion-arene interactions. The results indicate that in binary complexes (1 · X(-)), both weak σ-type and ...

Abstract	The ternary complexes X(-) · 1 · YF (1 = triazine, X = Cl, Br and I, Y = H, Cl, Br, I, PH2 and AsH2) have been investigated by MP2 calculations to understand the noncovalently electron-withdrawing effects on anion-arene interactions. The results indicate that in binary complexes (1 · X(-)), both weak σ-type and anion-π complexes can be formed for Cl(-) and Br(-), but only anion-π complex can be formed for I(-). Moreover, the hydrogen-bonding complex is the global minimum for all three halides in binary complexes. However, in ternary complexes, anion-π complex become unstable and only σ complex can retain in many cases for Cl(-) and Br(-). Anion-π complex keeps stable only when YF = HF. In contrast with binary complexes, σ complex become the global minimum for Cl(-) and Br(-) in ternary complexes. These changes in binding mode and strength are consistent with the results of covalently electron-withdrawing effects. However, in contrast with the covalently electron-withdrawing substituents, Cl(-) and Br(-) can attack the aromatic carbon atom to form a strong σ complex when the noncovalently electron-withdrawing effect is induced by halogen bonding. The binding behavior for I(-) is different from that for Cl(-) and Br(-) in two aspects. First, the anion-π complex for I(-) can also keep stable when the noncovalent interaction is halogen bonding. Second, the anion-π complex for I(-) is the global minimum when it can retain as a stable structure.
Language	English
Publishing date	2014-01-25
Publishing country	Germany
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	1284729-X
ISSN	0948-5023 ; 1610-2940
ISSN (online)	0948-5023
ISSN	1610-2940
DOI	10.1007/s00894-014-2076-0
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Book ; Online: Realising square and diamond lattice $S=1/2$ Heisenberg antiferromagnet models in the $\alpha$ and $\beta$ phases of the coordination framework, KTi(C$_2$O$_4$)$_2\cdot$\textit{x}H$_2$O

Abdeldaim, Aly H. / Li, Teng / Farrar, Lewis / Tsirlin, Alexander A. / Yao, Wenjiao / Gibbs, Alexandra S. / Manuel, Pascal / Lightfoot, Philip / Nilsen, Gøran J. / Clark, Lucy

2020

Abstract: ... Ti$^{3+}$ coordination framework, KTi(C$_2$O$_4$)$_2\cdot$xH$_2$O. Single-crystal X-ray and powder ...

Abstract	We report the crystal structures and magnetic properties of two psuedo-polymorphs of the $S=1/2$ Ti$^{3+}$ coordination framework, KTi(C$_2$O$_4$)$_2\cdot$xH$_2$O. Single-crystal X-ray and powder neutron diffraction measurements on $\alpha$-KTi(C$_2$O$_4$)$_2\cdot$xH$_2$O confirm its structure in the tetragonal $I4/mcm$ space group with a square planar arrangement of Ti$^{3+}$ ions. Magnetometry and specific heat measurements reveal weak antiferromagnetic interactions, with $J_1\approx7$ K and $J_2/J_1=0.11$ indicating a slight frustration of nearest- and next-nearest-neighbor interactions. Below $1.8$ K, $\alpha$ undergoes a transition to G-type antiferromagnetic order with magnetic moments aligned along the $c$ axis of the tetragonal structure. The estimated ordered moment of Ti$^{3+}$ in $\alpha$ is suppressed from its spin-only value to $0.62(3)~\mu_B$, thus verifying the two-dimensional nature of the magnetic interactions within the system. $\beta$-KTi(C$_2$O$_4$)$_2\cdot$2H$_2$O, on the other hand, realises a three-dimensional diamond-like magnetic network of Ti$^{3+}$ moments within a hexagonal $P6_222$ structure. An antiferromagnetic exchange coupling of $J\approx54$ K -- an order of magnitude larger than in $\alpha$ -- is extracted from magnetometry and specific heat data. $\beta$ undergoes N\'eel ordering at $T_N=28$ K, with the magnetic moments aligned within the $ab$ plane and a slightly reduced ordered moment of $0.79~\mu_B$ per Ti$^{3+}$. Through density-functional theory calculations, we address the origin of the large difference in the exchange parameters between the $\alpha$ and $\beta$ psuedo-polymorphs. Given their observed magnetic behaviors, we propose $\alpha$-KTi(C$_2$O$_4$)$_2\cdot$xH$_2$O and $\beta$-KTi(C$_2$O$_4$)$_2\cdot$2H$_2$O as close to ideal model $S=1/2$ Heisenberg square and diamond lattice antiferromagnets, respectively. Comment: 12 pages, 7 figures
Keywords	Condensed Matter - Strongly Correlated Electrons ; Condensed Matter - Materials Science
Subject code	530 ; 519
Publishing date	2020-09-07
Publishing country	us
Document type	Book ; Online
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Article: New coordination motifs of melamine directed by N-H---X (X = Cl or Br) hydrogen bonds.

Zhang, Lei / Zhang, Jian / Li, Zhao-Ji / Cheng, Jian-Kai / Yin, Pei-Xiu / Yao, Yuan-Gen

Inorganic chemistry

2007 Volume 46, Issue 15, Page(s) 5838–5840

Abstract: Unusual mu(2)- and mu(3)-coordination modes of melamine are found in two organic-inorganic hybrid copper halides, [Cu(2)Br(2)(MA)](n) (1) and [Cu(3)Cl(3)(MA)](n) (2) (MA = melamine), in which the MA ligand affords two N-heterocycle N atoms to link (Cu(2) ... ...

Abstract	Unusual mu(2)- and mu(3)-coordination modes of melamine are found in two organic-inorganic hybrid copper halides, [Cu(2)Br(2)(MA)](n) (1) and [Cu(3)Cl(3)(MA)](n) (2) (MA = melamine), in which the MA ligand affords two N-heterocycle N atoms to link (Cu(2)Br(2))infinity stairs and serves as a novel mu(3) bridge to give a 3D framework, respectively.
Language	English
Publishing date	2007-07-23
Publishing country	United States
Document type	Journal Article
ZDB-ID	1484438-2
ISSN	1520-510X ; 0020-1669
ISSN (online)	1520-510X
ISSN	0020-1669
DOI	10.1021/ic7005138
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Article ; Online: Temperature-controlled syntheses of substituted 1,2,4-triazolelead(II) complexes: active lone pair and N-H...X (X = Cl, Br, I) hydrogen bonds.

Cheng, Jian-Kai / Zhang, Jian / Yin, Pei-Xiu / Lin, Qi-Pu / Li, Zhao-Ji / Yao, Yuan-Gen

Inorganic chemistry

2009 Volume 48, Issue 21, Page(s) 9992–9994

Abstract: ... environment around the center metal is distinctly influenced by the stereochemical 6s(2) lone pair and N-H...X ... Three isomorphous lead(II) complexes with a new {N(3)SX}-coordinated (X = Cl, Br, I) mode have been ... synthesized and characterized by X-ray diffraction. The structural analyses reveal that the coordination ...

Abstract	Three isomorphous lead(II) complexes with a new {N(3)SX}-coordinated (X = Cl, Br, I) mode have been synthesized and characterized by X-ray diffraction. The structural analyses reveal that the coordination environment around the center metal is distinctly influenced by the stereochemical 6s(2) lone pair and N-H...X hydrogen bonds. Additionally, doubly deprotonated trzS(2-) (HtrzSH = 1,2,4-triazole-3-thiol) generated in situ via deamination and dehydrazination of ahtrzS(-) (ahtrzSH = 4-amino-3-hydrazino-5-mercapto-1,2,4-triazole) was first observed in a semiconducting three-dimensional coordination network at higher reaction temperature.
Language	English
Publishing date	2009-11-02
Publishing country	United States
Document type	Journal Article
ZDB-ID	1484438-2
ISSN	1520-510X ; 0020-1669
ISSN (online)	1520-510X
ISSN	0020-1669
DOI	10.1021/ic901653y
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Article ; Online: Persistent H. pylori colonization in early acquisition age of mice related with higher gastric sialylated Lewis x, IL-10, but lower interferon-γ expressions.

Yang, Yao-Jong / Yang, Hsiao-Bai / Wu, Jiunn-Jong / Sheu, Bor-Shyang

Journal of biomedical science

2008 Volume 16, Page(s) 34

Abstract: ... week, the young mice with a persistence of H. pylori colonization had higher sialyl-Le(x), higher IL-10 ... sialyl-Le(x )and IL-10, but a lower IFN-γ correlates to the consequent persistence of H. pylori ... Background: H. pylori infection is less prevalent in childhood. This study validated ...

Abstract	Background: H. pylori infection is less prevalent in childhood. This study validated whether the rates of H. pylori colonization depend on different acquisition ages, and correlate with the different gastric Lewis antigens or cytokine expressions after H. pylori acquisition. Methods: We applied a young (7-day-old) C57BL/6 mice group (n = 50) and adult (6-week-old) C57BL/6 mice group (n = 50). In each group, 30 mice were challenged with H. pylori and 20 mice served as naïve control. The success of H. pylori colonization was assessed on the 2(nd )week and the 8(th )week, respectively. The intensity of the Lewis x, sialylated Lewis x(sialyl-Le(x)), and cytokine expressions, including TNF-α, IFN-γ, IL-6, IL-10, and IL-1β, were immunochemically stained and graded. Results: On the 2(nd )week after H. pylori challenge, the colonization rates of H. pylori were similar between the young mice group and the adult mice group (89% vs. 100%, P > 0.05). However, on the 8(th )week, the H. pylori colonization rate was significantly lower in the young mice group than in the adult mice group (53% vs. 95%, P = 0.003). On the 8(th )week, the young mice with a persistence of H. pylori colonization had higher sialyl-Le(x), higher IL-10, and lower IFN-γ than those of the mice that lost colonization during the 2(nd )to the 8(th )week (P < 0.05). Conclusion: The persistence of H. pylori colonization could be an acquisition-age determinant process. After H. pylori exposure at an early acquisition age, the host response with a higher sialyl-Le(x )and IL-10, but a lower IFN-γ correlates to the consequent persistence of H. pylori colonization.
MeSH term(s)	Age Factors ; Animals ; Gene Expression Regulation/immunology ; Helicobacter Infections/immunology ; Helicobacter Infections/metabolism ; Helicobacter pylori/immunology ; Helicobacter pylori/metabolism ; Interferon-gamma/biosynthesis ; Interferon-gamma/immunology ; Interleukin-10/biosynthesis ; Interleukin-10/immunology ; Lewis Blood Group Antigens ; Mice ; Oligosaccharides/biosynthesis ; Oligosaccharides/immunology
Chemical Substances	IL10 protein, mouse ; Lewis Blood Group Antigens ; Lewis a oligosaccharide ; Oligosaccharides ; Interleukin-10 (130068-27-8) ; Interferon-gamma (82115-62-6)
Language	English
Publishing date	2008-12-27
Publishing country	England
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	1193378-1
ISSN	1423-0127 ; 1021-7770
ISSN (online)	1423-0127
ISSN	1021-7770
DOI	10.1186/1423-0127-16-34
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