Investigating the impact of dynamic structural changes of Au/rutile catalysts on the catalytic activity of CO oxidation

The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on reducible oxides,dynamic surface reconstruction phenomena,including strong metal–support interaction(SMSI)and oxygen vacancy formation,complicate the determination of the structural–functional relationship at the active sites.Here,we performed a systematic investigation of the dynamic behavior of Au nanocatalysts supported on flame‐synthesized TiO_(2),which takes predominantly a rutile phase,using CO oxidation above room temperature as a probe reaction.Our analysis conclusively elucidated a negative correlation between the catalytic activity of Au/TiO_(2) and the oxygen vacancy at the Au/TiO_(2) interface.Although the reversible formation and retracting of SMSI overlayers have been ubiquitously observed on Au/TiO_(2) samples,the catalytic consequence of SMSI remains inconclusive.Density functional theory suggests that the electron transfer from TiO_(2) to Au is correlated to the presence of the interfacial oxygen vacancies,retarding the catalytic activation of CO oxidation.

Changes in intracellular and extracellular proteins after ERGIC3 knockdown in lung cancer:Proteins interacting with ERGIC3,HORN,and FLNA

Objective:Endoplasmic reticulum-Golgi intermediate compartment 3(ERGIC3)promotes cell proliferation and metastasis in lung cancer,but its molecular mechanism is unclear.Methods:The GLC-82 cells were randomly divided into the ERGIC3i group and the negative control group.The cells were transfected with ERGIC3 siRNA or control siRNA in the groups,respectively.The ERGIC3-interacting proteins expressed in cells or extracellularly were isolated by the immunoprecipitation method and detected by isobaric tags for relative and absolute quantitation and liquid chromatography-tandem mass spectrometry.The differentially expressed proteins were determined by bioinformatic methods.Results:After ERGIC3 knockdown,88 extracellular differentially expressed proteins,41 upregulated and 47 down-regulated,were detected in the supernatant of cultured cells.Among 52 intracellular differentially expressed proteins,33 were up-regulated and 19 down-regulated.Cluster analysis showed that the extracellular differential proteins are mainly involved in Ca2+binding and transport and I-kappa B kinase/NF-kappa B signal transduction.The upregulated proteins are mainly involved in the biological process of H3-K27 and H3-K4 methylation in cells.Co-immunoprecipitation assay showed that proteins interacting with ERGIC3 were rich in cytoskeleton construction and RHO GTPases activated p21-activated kinases.The intersection of these two research methods shows that ERGIC3 interacts with HORN and filamin A(FLNA).Conclusion:Proteomic analyses reveal that ERGIC3 acts as a vesicle transmembrane protein on the distribution of various extracellular and intracellular proteins and regulates the extracellular and intracellular biological processes by specifically binding hornin(HORN)and FLNA proteins.These findings maybe provide new methods and ideas for ERGIC3 as a therapeutic target for lung cancer.

Universal,predominant exciton transfer in perovskite nanocrystal solids

Perovskite nanocrystal(PNC)solids are promising materials for optoelectronic applications.Recent studies have shown that exciton diffusion in PNC solids occurs via alternate exciton hopping(EH)and photon recycling(PR).The energy disorder induced by the size distribution is a common factor in PNC solids,and the impact of this energy disorder on the exciton diffusion remains unclear.Here,we investigated the exciton diffusion in CsPbBr3 NC solids with a Gaussian size distribution of 11.2±6.8 nm via steady and time-resolved photoluminescence(PL)spectroscopy with multiple detection bands in transmission mode.Our results indicated that exciton diffusion was controlled by a downhill transfer among the different energy sites through the disordered energy landscape,as confirmed by the accompanying low-temperature PL analysis.A detailed examination revealed that the acceptor distribution in tandem with the reabsorption coefficient determined the contribution of EH and PR to exciton transfer between different energy sites.Consequently,the exciton diffusion mechanism varied in PNC solids of different thicknesses:in a thin solid with a thickness of several hundred nanometers,the exciton transfer was dominated by efficient EH and PR from the high-energy sites to the lower-energy sites;in a few-micrometer-thick solid,transfer from the medium-energy sites toward the lower-energy sites also became prominent and occurred mainly through PR.These findings enhance the understanding of the vital role that the acceptor distribution plays in the exciton diffusion process in PNC solids,providing important insights for optoelectronic applications based on PNC solids.Our work also exploits the use of commonly available tools for in-depth exciton diffusion studies,which reveals the interior diffusion information that is usually hidden in surface sensitive PL imaging methods.

Valorizing carbon dioxide via electrochemical reduction on gas-diffusion electrodes

The electrochemical carbon dioxide(CO_(2))reduction provides a means to upgrade CO_(2)into value-added chemicals.When powered by renewable electric-ity,CO_(2)electroreduction holds the promise of chemical manufacturing with carbon neutrality.A commercially relevant CO_(2)electroreduction process should be highly selective and productive toward desired products,energetically efficient for power conversion,and stable for long-term operation.To achieve these goals,designing gas-diffusion catalytic electrodes and prototyping reactors built upon in-depth understandings of the reaction mechanisms are of para-mount importance.In this review,the fundamentals of gas-diffusion electrodes are briefly presented.Then,the most recent advances in developing high-performance CO_(2)reduction using gas-diffusion electrodes are overviewed.Reactor engineering aiming at enhancing productivity,energy efficiency,CO_(2)single-pass utilization,and operating lifetime is further discussed.Challenges in developing CO_(2)electroreduction systems are included.The prospects for advancing CO_(2)electroreduction toward practical applications are also narrated.

N,S-Doped Carbon Dots as Additive for Suppression of Zinc Dendrites in Alkaline Electrolyte

The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc-based batteries.It is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the electrolyte.In this study,N,S-doped carbon dots(TU-CQDs)were synthesized and used as additives to regulate zinc deposition in a typical KOH electrolyte.The experimental and three-dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the electrolyte.Therefore,TU-CQDs can not only inhibit the hydrogen evolution reaction,but also achieve uniform zinc deposition.The in-situ synchrotron radiation X-ray imaging elucidated that TU-CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping process.This work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte.

Electron-beam-induced degradation of halide-perovskite-related semiconductor nanomaterials

The instability of lead halide perovskites in various application-related conditions is a key challenge to be resolved. We investigated the formation of metal nanoparticles during transmission electron microscopy(TEM) imaging of perovskite-related metal halide compounds. The metal nanoparticle formation on these materials originates from stimulated desorption of halogen under electron beams and subsequent aggregation of metal atoms. Based on shared mechanisms,the TEM-based degradation test can help to evaluate the material stability against light irradiation.