Li-metal is considered as the most promising anode material to advance the development of next-generation energy storage devices owing to its unparalleled theoretical specific capacity and extremely low redox electrochemical potential. However, safety concerns and poor cycling retention of Li-metal batteries (LMBs) caused by uncontrolled Li dendrite growth still limit their broad application.
Herein, liquid polydimethylsiloxane (PDMS) terminated by -OCH 3 groups is proposed as a graftable additive to reinforce the anode dendrite suppression for LMBs. Such a grafting triggers the formation of a conformal hybrid solid electrolyte interphase (SEI) with increased fractions of LiF and Li-Si-O-based moieties, which serve as a rigid barrier and ionic conductor for uniform Li-ion flow and Li-mass deposition. The grafting protected anode endows Li/Li symmetric cells with a long lifetime over 1800 h with a much smaller voltage gap (≈25 mV) betweenLi plating and stripping, than the naked anode. The coulombic efficiency values for Li/Cu asymmetric cells in carbonate electrolyte can reach up to 97% even at a high current density of 3 mA cm −2 or high capacity up to 4 mAh cm −2 . The liquid PDMS additive shows advantage over solid siloxane additives with poor grafting ability in terms of Li surface compaction and SEI stabilization.
Garnet based solid-state batteries have the advantages of wide electrochemical window and good chemical stability. However, at Li-garnet interface, the poor interfacial wettability due to Li
2
CO
3
passivation usually causes large resistance and unstable contact. Here, a Li
2
CO
3
-affiliative mechanism is proposed for air-accessible interface engineering of garnet electrolyte via facile liquid metal (LM) painting. The natural LM oxide skin enables a superior wettability of LM interlayer towards ceramic electrolyte and Li anode. Therein the removal of Li
2
CO
3
passivation network is not necessary, in view of its delamination and fragmentation by LM penetration. This dissipation effect allows the lithiated LM nanodomains to serve as alternative Li-ion flux carriers at Li-garnet interface. This mechanism leads to an interfacial resistance as small as 5 Ω cm
2
even after exposing garnet in air for several days. The ultrastable Li plating and stripping across LM painted garnet can last for 9930 h with a small overpotential.
Due to their intrinsic physical properties potentially useful for imaging and therapy as well as their highly engineerable surface, biocompatible inorganic nanoparticles offer novel platforms to develop advanced diagnostic and therapeutic agents for improved detection and more efficacious treatment of major diseases. The in vivo application of inorganic nanoparticles was demonstrated more than two decades ago, however it turns out to be very complicated as nanomaterials exhibit much more sophisticated pharmacokinetic properties than conventional drugs. In this review, we first discuss the in vivo behavior of inorganic nanoparticles after systematic administration, including the basic requirements for nanoparticles to be used in vivo, the impact of the particles' physicochemical properties on their pharmacokinetics, and the effects of the protein corona formed across the nano-bio interface. Next, we summarize the state-of-the-art of the preparation of biocompatible inorganic nanoparticles and bioconjugation strategies for obtaining target-specific nanoprobes. Then, the advancements in sensitive tumor imaging towards diagnosis and visualization of the abnormal signatures in the tumor microenvironment, together with recent studies on atherosclerosis imaging are highlighted. Finally, the future challenges and the potential for inorganic nanoparticles to be translated into clinical applications are discussed.
Titanium and zirconium oxide cluster anions with dimensions up to nanosize are prepared by laser ablation and reacted with carbon monoxide in a fast low reactor. The cluster reactions are characterized by time-of-flight mass spectrometry and density functional theory calculations. The oxygen atom transfers from (TiO(2))(n)O(-) (n = 3-25) to CO and formations of (TiO(2))(n)(-) are observed, whereas the reactions of (ZrO(2))(n)O(-) (n = 3-25) with CO generate the CO addition products (ZrO(2))(n)OCO(-), which lose CO(2) upon the collisions (studied for n = 3-9) with a crossed helium beam. The computational study indicates that the (MO(2))(n)O(-) (M = Ti, Zr; n = 3-8) clusters are atomic radical anion (O(-)) bonded systems, and the energetics for CO oxidation by the O(-) radicals to form CO(2) is strongly dependent on the metals as well as the cluster size for the titanium system. Atomic oxygen radical anions are important reactive intermediates, while it is difficult to capture and characterize them for condensed phase systems. The reactivity pattern of the O(-)-bonded (TiO(2))(n)O(-) and (ZrO(2))(n)O(-) correlates very well with different behaviors of titania and zirconia supports in the low-temperature catalytic CO oxidation.
The chitinase 3-like 1 gene (CHI3L1) is abnormally expressed in the hippocampus of subjects with schizophrenia and may be involved in the cellular response to various environmental events that are reported to increase the risk of schizophrenia. Here, we provide evidence that the functional variants at the CHI3L1 locus influence the genetic risk of schizophrenia. First, using case-control and transmission/disequilibrium-test (TDT) methodologies, we detected a significant association between schizophrenia and haplotypes within the promoter region of CHI3L1 in two independent cohorts of Chinese individuals. Second, the at-risk CCC haplotype (P=.00058 and .0018 in case-control and TDT studies, respectively) revealed lower transcriptional activity (P=2.2 x 10(-7)) and was associated with lower expression (P=3.1 x 10(-5)) compared with neutral and protective haplotypes. Third, we found that an allele of SNP4 (rs4950928), the tagging SNP of CCC, impaired the MYC/MAX-regulated transcriptional activation of CHI3L1 by altering the transcriptional-factor consensus sequences, and this may be responsible for the decreased expression of the CCC haplotype. In contrast, the protective TTG haplotype was associated with a high level of CHI3L1 expression. Our findings identify CHI3L1 as a potential schizophrenia-susceptibility gene and suggest that the genes involved in the biological response to adverse environmental conditions are likely to play roles in the predisposition to schizophrenia.
Laser-ablation-generated AuCeO2(+) and CeO2(+) oxide clusters were mass-selected using a quadrupole mass filter and reacted with H2 in an ion trap reactor at ambient conditions. The reactions were characterized by mass spectrometry and density functional theory calculations. The gold-cerium bimetallic oxide cluster AuCeO2(+) is more reactive in H2 activation than the pure cerium oxide cluster CeO2(+). The gold atom is the active adsorption site and facilitates the heterolytic cleavage of H2 in collaboration with the separated O(2-) ion of the CeO2 support. To the best of our knowledge, this is the first example of thermal H2 activation by a closed-shell atomic cluster, which provides molecular-level insights into the single gold atom catalysis over metal oxide supports.
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