The synthesis of nanocrystals is in the limelight in modern nanotechnology. Biosynthesis of
nanoparticles by plant extracts is currently under exploitation. Not only could silver
nanoparticles ranging from 55 to 80 nm in size be fabricated, but also triangular or spherical
shaped gold nanoparticles could be easily modulated by reacting the novel sundried
biomass of Cinnamomum camphora leaf with aqueous silver or gold precursors at
ambient temperature. The marked difference of shape control between gold and
silver nanoparticles was attributed to the comparative advantage of protective
biomolecules and reductive biomolecules. The polyol components and the water-soluble
heterocyclic components were mainly responsible for the reduction of silver ions or
chloroaurate ions and the stabilization of the nanoparticles, respectively. The
sundried leaf in this work was very suitable for simple synthesis of nanoparticles.
Size effect has been regularly utilized to tune the catalytic activity and selectivity of metal nanoparticles (NPs). Yet, there is a lack of understanding of the size effect in the electrocatalytic reduction of CO2, an important reaction that couples with intermittent renewable energy storage and carbon cycle utilization. We report here a prominent size-dependent activity/selectivity in the electrocatalytic reduction of CO2 over differently sized Pd NPs, ranging from 2.4 to 10.3 nm. The Faradaic efficiency for CO production varies from 5.8% at -0.89 V (vs reversible hydrogen electrode) over 10.3 nm NPs to 91.2% over 3.7 nm NPs, along with an 18.4-fold increase in current density. Based on the Gibbs free energy diagrams from density functional theory calculations, the adsorption of CO2 and the formation of key reaction intermediate COOH* are much easier on edge and corner sites than on terrace sites of Pd NPs. In contrast, the formation of H* for competitive hydrogen evolution reaction is similar on all three sites. A volcano-like curve of the turnover frequency for CO production within the size range suggests that CO2 adsorption, COOH* formation, and CO* removal during CO2 reduction can be tuned by varying the size of Pd NPs due to the changing ratio of corner, edge, and terrace sites.
Coordinatively unsaturated Ni–N active sites facilitate CO2electroreduction and inhibit the competitive hydrogen evolution reaction, demonstrating selective and high-rate CO2electroreduction.
The development of oxygen evolution reaction (OER) electrocatalysts remains a major challenge that requires significant advances in both mechanistic understanding and material design. Recent studies show that oxygen from the perovskite oxide lattice could participate in the OER via a lattice oxygen-mediated mechanism, providing possibilities for the development of alternative electrocatalysts that could overcome the scaling relations-induced limitations found in conventional catalysts utilizing the adsorbate evolution mechanism. Here we distinguish the extent to which the participation of lattice oxygen can contribute to the OER through the rational design of a model system of silicon-incorporated strontium cobaltite perovskite electrocatalysts with similar surface transition metal properties yet different oxygen diffusion rates. The as-derived silicon-incorporated perovskite exhibits a 12.8-fold increase in oxygen diffusivity, which matches well with the 10-fold improvement of intrinsic OER activity, suggesting that the observed activity increase is dominantly a result of the enhanced lattice oxygen participation.
SUMMARY
Amplification of the MYCN oncogene in childhood neuroblastoma is often accompanied by mutational activation of ALK (anaplastic lymphoma kinase), suggesting their pathogenic cooperation. We generated a transgenic zebrafish model of neuroblastoma in which MYCN-induced tumors arise from a subpopulation of neuroblasts that migrate into the adrenal medulla analogue following organogenesis. Coexpression of activated ALK with MYCN in this model triples the disease penetrance and markedly accelerates tumor onset. MYCN overexpression induces adrenal sympathetic neuroblast hyperplasia, blocks chromaffin cell differentiation, and ultimately triggers a developmentally-timed apoptotic response in the hyperplastic sympathoadrenal cells. Coexpression of activated ALK with MYCN provides prosurvival signals that block this apoptotic response and allow continued expansion and oncogenic transformation of hyperplastic neuroblasts, thus promoting progression to neuroblastoma.
The electrochemical CO reduction reaction (CORR) typically uses transition metals as the catalysts. To improve the efficiency, tremendous efforts have been dedicated to tuning the morphology, size, and structure of metal catalysts and employing electrolytes that enhance the adsorption of CO. We report here a strategy to enhance CORR by constructing the metal-oxide interface. We demonstrate that Au-CeO shows much higher activity and Faradaic efficiency than Au or CeO alone for CORR. In situ scanning tunneling microscopy and synchrotron-radiation photoemission spectroscopy show that the Au-CeO interface is dominant in enhancing CO adsorption and activation, which can be further promoted by the presence of hydroxyl groups. Density functional theory calculations indicate that the Au-CeO interface is the active site for CO activation and the reduction to CO, where the synergy between Au and CeO promotes the stability of key carboxyl intermediate (*COOH) and thus facilitates CORR. Similar interface-enhanced CORR is further observed on Ag-CeO, demonstrating the generality of the strategy for enhancing CORR.
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