Direct high-resolution mapping of electrocatalytic activity of semi-two-dimensional catalysts with single-edge sensitivity.

Abstract:

:The catalytic activity of low-dimensional electrocatalysts is highly dependent on their local atomic structures, particularly those less-coordinated sites found at edges and corners; therefore, a direct probe of the electrocatalytic current at specified local sites with true nanoscopic resolution has become critically important. Despite the growing availability of operando imaging tools, to date it has not been possible to measure the electrocatalytic activities from individual material edges and directly correlate those with the local structural defects. Herein, we show the possibility of using feedback and generation/collection modes of operation of the scanning electrochemical microscope (SECM) to independently image the topography and local electrocatalytic activity with 15-nm spatial resolution. We employed this operando microscopy technique to map out the oxygen evolution activity of a semi-2D nickel oxide nanosheet. The improved resolution and sensitivity enables us to distinguish the higher activities of the materials' edges from that of the fully coordinated surfaces in operando The combination of spatially resolved electrochemical information with state-of-the-art electron tomography, that unravels the 3D complexity of the edges, and ab initio calculations allows us to reveal the intricate coordination dependent activity along individual edges of the semi-2D material that is not achievable by other methods. The comparison of the simulated line scans to the experimental data suggests that the catalytic current density at the nanosheet edge is ∼200 times higher than that at the NiO basal plane.

authors

Sun T,Wang D,Mirkin MV,Cheng H,Zheng JC,Richards RM,Lin F,Xin HL

doi

10.1073/pnas.1821091116

subject

Has Abstract

pub_date

2019-06-11 00:00:00

pages

11618-11623

issue

24

eissn

0027-8424

issn

1091-6490

pii

1821091116

journal_volume

116

pub_type

杂志文章
  • Increased cell proliferation, but not reduced cell death, induces lymphocytosis in bovine leukemia virus-infected sheep.

    abstract::Lymphocyte homeostasis is the result of a critical balance between cell proliferation and death. Disruption of this subtle equilibrium can lead to the onset of leukemia, an increase in the number of lymphocytes being potentially due to both of these parameters. The relative importance of cell proliferation vs. apoptos...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.142100999

    authors: Debacq C,Asquith B,Kerkhofs P,Portetelle D,Burny A,Kettmann R,Willems L

    更新日期:2002-07-23 00:00:00

  • Cross-biome metagenomic analyses of soil microbial communities and their functional attributes.

    abstract::For centuries ecologists have studied how the diversity and functional traits of plant and animal communities vary across biomes. In contrast, we have only just begun exploring similar questions for soil microbial communities despite soil microbes being the dominant engines of biogeochemical cycles and a major pool of...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1215210110

    authors: Fierer N,Leff JW,Adams BJ,Nielsen UN,Bates ST,Lauber CL,Owens S,Gilbert JA,Wall DH,Caporaso JG

    更新日期:2012-12-26 00:00:00

  • On-demand high-capacity ride-sharing via dynamic trip-vehicle assignment.

    abstract::Ride-sharing services are transforming urban mobility by providing timely and convenient transportation to anybody, anywhere, and anytime. These services present enormous potential for positive societal impacts with respect to pollution, energy consumption, congestion, etc. Current mathematical models, however, do not...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1611675114

    authors: Alonso-Mora J,Samaranayake S,Wallar A,Frazzoli E,Rus D

    更新日期:2017-01-17 00:00:00

  • Purification of mouse interferon by affinity chromatography on a solid-phase immunoadsorbent.

    abstract::A solid-phase immunoadsorbent capable of binding mouse interferon has been prepared. Starting from crude tissue-culture material, interferon could be purified 1990 times in a single step of affinity chromatography. Overall recovery ranged from 55 to 103% with tissue culture and mouse-brain interferon; however, only 5%...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.70.4.1037

    authors: Sipe JD,de Maeyer-Guignard J,Fauconnier B,de Maeyer E

    更新日期:1973-04-01 00:00:00

  • Sir-two-homolog 2 (Sirt2) modulates peripheral myelination through polarity protein Par-3/atypical protein kinase C (aPKC) signaling.

    abstract::The formation of myelin by Schwann cells (SCs) occurs via a series of orchestrated molecular events. We previously used global expression profiling to examine peripheral nerve myelination and identified the NAD(+)-dependent deacetylase Sir-two-homolog 2 (Sirt2) as a protein likely to be involved in myelination. Here, ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1104969108

    authors: Beirowski B,Gustin J,Armour SM,Yamamoto H,Viader A,North BJ,Michán S,Baloh RH,Golden JP,Schmidt RE,Sinclair DA,Auwerx J,Milbrandt J

    更新日期:2011-10-25 00:00:00

  • Structural and biochemical studies of p21Ras S-nitrosylation and nitric oxide-mediated guanine nucleotide exchange.

    abstract::Ras is a guanine nucleotide-binding protein that cycles between inactive GDP-bound and active GTP-bound states to regulate a diverse array of cellular processes, including cell growth, apoptosis, and differentiation. The guanine nucleotide-bound state of Ras is tightly maintained by regulatory factors to promote regul...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1037299100

    authors: Williams JG,Pappu K,Campbell SL

    更新日期:2003-05-27 00:00:00

  • Reciprocity or near-reciprocity of highly coupled enzymatic processes at the multidimensional inflection point.

    abstract::It has recently been demonstrated that coupled enzymatic processes may possess, for a particular choice of the state variables, multidimensional inflection points in thermodynamic force-flow space. The conditions for reciprocity in the linear region near such a reference state, which may be far from equilibrium, are o...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.78.7.4314

    authors: Caplan SR

    更新日期:1981-07-01 00:00:00

  • Sequence information can be obtained from single DNA molecules.

    abstract::The completion of the human genome draft has taken several years and is only the beginning of a period in which large amounts of DNA and RNA sequence information will be required from many individuals and species. Conventional sequencing technology has limitations in cost, speed, and sensitivity, with the result that ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0230489100

    authors: Braslavsky I,Hebert B,Kartalov E,Quake SR

    更新日期:2003-04-01 00:00:00

  • Accumulation of newly synthesized mRNAs in response to human fibroblast (beta) interferon.

    abstract::Treatment of human fibroblast cells with human fibroblast (beta)interferon for up to 8 hr resulted in the accumulation of at least four mRNAs. The mRNAs were isolated from cellular polysomes and characterized by stimulation of translation in a wheat germ cell-free protein synthesis system. The mRNAs appear as early as...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.78.8.4763

    authors: Colonno RJ

    更新日期:1981-08-01 00:00:00

  • An unusual structural motif of antimicrobial peptides containing end-to-end macrocycle and cystine-knot disulfides.

    abstract::Four macrocyclic cystine-knot peptides of 29-31 residues, kalata, circulin A and B (CirA and CirB), and cyclopsychotride, have been isolated from coffee plants but have undetermined physiological functions. These macrocycles and 10 of their analogs prepared by chemical synthesis were tested against nine strains of mic...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.96.16.8913

    authors: Tam JP,Lu YA,Yang JL,Chiu KW

    更新日期:1999-08-03 00:00:00

  • Relationship between promoter structure and template specificities exhibited by the bacteriophage T3 and T7 RNA polymerases.

    abstract::To explore the basis for the template specificities of the bacteriophage T3 and T7 RNA polymerases (EC 2.7.7.6), we determined the nucleotide sequences of six promoters recognized by the T3 RNA polymerase and compared them with the previously determined promoter sequences recognized by the bacteriophage T7 RNA polymer...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.80.10.2814

    authors: Bailey JN,Klement JF,McAllister WT

    更新日期:1983-05-01 00:00:00

  • Estrogen receptor β regulates AKT activity through up-regulation of INPP4B and inhibits migration of prostate cancer cell line PC-3.

    abstract::Loss of the tumor suppressor, PTEN, is one of the most common findings in prostate cancer (PCa). This loss leads to overactive Akt signaling, which is correlated with increased metastasis and androgen independence. However, another tumor suppressor, inositol-polyphosphate 4-phosphatase type II (INPP4B), can partially ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.2007160117

    authors: Chaurasiya S,Wu W,Strom AM,Warner M,Gustafsson JÅ

    更新日期:2020-10-20 00:00:00

  • Direct and indirect punishment among strangers in the field.

    abstract::Many interactions in modern human societies are among strangers. Explaining cooperation in such interactions is challenging. The two most prominent explanations critically depend on individuals' willingness to punish defectors: In models of direct punishment, individuals punish antisocial behavior at a personal cost, ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1413170111

    authors: Balafoutas L,Nikiforakis N,Rockenbach B

    更新日期:2014-11-11 00:00:00

  • Binding site size limit of the 2:1 pyrrole-imidazole polyamide-DNA motif.

    abstract::Polyamides containing N-methylimidazole (Im) and N-methylpyrrole (Py) amino acids can be combined in antiparallel side-by-side dimeric complexes for sequence-specific recognition in the minor groove of DNA. Six polyamides containing three to eight rings bind DNA sites 5-10 bp in length, respectively. Quantitative DNas...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.93.14.6981

    authors: Kelly JJ,Baird EE,Dervan PB

    更新日期:1996-07-09 00:00:00

  • IL-38 inhibits microglial inflammatory mediators and is decreased in amygdala of children with autism spectrum disorder.

    abstract::Autism spectrum disorder (ASD) is characterized by impaired social interactions and communication. The pathogenesis of ASD is not known, but it involves activation of microglia. We had shown that the peptide neurotensin (NT) is increased in the serum of children with ASD and stimulates cultured adult human microglia t...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.2004666117

    authors: Tsilioni I,Pantazopoulos H,Conti P,Leeman SE,Theoharides TC

    更新日期:2020-07-14 00:00:00

  • Indirect reciprocity with private, noisy, and incomplete information.

    abstract::Indirect reciprocity is a mechanism for cooperation based on shared moral systems and individual reputations. It assumes that members of a community routinely observe and assess each other and that they use this information to decide who is good or bad, and who deserves cooperation. When information is transmitted pub...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1810565115

    authors: Hilbe C,Schmid L,Tkadlec J,Chatterjee K,Nowak MA

    更新日期:2018-11-27 00:00:00

  • Reduced vacuolar β-1,3-glucan synthesis affects carbohydrate metabolism as well as plastid homeostasis and structure in Phaeodactylum tricornutum.

    abstract::The β-1,3-glucan chrysolaminarin is the main storage polysaccharide of diatoms. In contrast to plants and green algae, diatoms and most other algal groups do not accumulate storage polysaccharides in their plastids. The diatom Phaeodactylum tricornutum possesses only a single gene encoding a putative β-1,3-glucan synt...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1719274115

    authors: Huang W,Haferkamp I,Lepetit B,Molchanova M,Hou S,Jeblick W,Río Bártulos C,Kroth PG

    更新日期:2018-05-01 00:00:00

  • Ultrashort antibacterial and antifungal lipopeptides.

    abstract::Host-defense cationic antimicrobial peptides ( approximately 12-50 aa long) play an essential protective role in the innate immune system of all organisms. Lipopeptides, however, are produced only in bacteria and fungi during cultivation, and they are composed of specific lipophilic moieties attached to anionic peptid...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0606129103

    authors: Makovitzki A,Avrahami D,Shai Y

    更新日期:2006-10-24 00:00:00

  • A complex history of rearrangement in an orthologous region of the maize, sorghum, and rice genomes.

    abstract::The sequences of large insert clones containing genomic DNA that is orthologous to the maize adh1 region were obtained for sorghum, rice, and the adh1-homoeologous region of maize, a remnant of the tetraploid history of the Zea lineage. By using all four genomes, it was possible to describe the nature, timing, and lin...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1434476100

    authors: Ilic K,SanMiguel PJ,Bennetzen JL

    更新日期:2003-10-14 00:00:00

  • Oxytocin, the peptide that bonds the sexes also divides them.

    abstract::Facilitation of social attraction and bonding by the evolutionarily conserved neuropeptide oxytocin is well-established in female mammals. However, accumulating behavioral evidence suggests that oxytocin may have evolved sex-specific functional roles in the domain of human social cognition. A critical question is how ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1602620113

    authors: Gao S,Becker B,Luo L,Geng Y,Zhao W,Yin Y,Hu J,Gao Z,Gong Q,Hurlemann R,Yao D,Kendrick KM

    更新日期:2016-07-05 00:00:00

  • Consequences of seafood mislabeling for marine populations and fisheries management.

    abstract::Over the past decade, seafood mislabeling has been increasingly documented, raising public concern over the identity, safety, and sustainability of seafood. Negative outcomes from seafood mislabeling are suspected to be substantial and pervasive as seafood is the world's most highly traded food commodity. Here we prov...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.2003741117

    authors: Kroetz K,Luque GM,Gephart JA,Jardine SL,Lee P,Chicojay Moore K,Cole C,Steinkruger A,Donlan CJ

    更新日期:2020-12-01 00:00:00

  • Slab melting versus slab dehydration in subduction-zone magmatism.

    abstract::The second critical endpoint in the basalt-H(2)O system was directly determined by a high-pressure and high-temperature X-ray radiography technique. We found that the second critical endpoint occurs at around 3.4 GPa and 770 °C (corresponding to a depth of approximately 100 km in a subducting slab), which is much shal...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1010968108

    authors: Mibe K,Kawamoto T,Matsukage KN,Fei Y,Ono S

    更新日期:2011-05-17 00:00:00

  • Transcriptional profiling of a mouse model for Rett syndrome reveals subtle transcriptional changes in the brain.

    abstract::The Mecp2 gene has been shown to be mutated in most cases of human Rett syndrome, and mouse models deleted for the ortholog have been generated. Lineage-specific deletion of the gene indicated that the Rett-like phenotype is caused by Mecp2 deficiency in neurons. Biochemical evidence suggests that Mecp2 acts as a glob...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.242566899

    authors: Tudor M,Akbarian S,Chen RZ,Jaenisch R

    更新日期:2002-11-26 00:00:00

  • Hypersensitive site 6 of the Th2 locus control region is essential for Th2 cytokine expression.

    abstract::The T helper type 2 (Th2) cytokine genes Il4, Il5, and Il13 are contained within a 140-kb region of mouse chromosome 11 and their expression is controlled by a locus control region (LCR) embedded within this locus. The LCR is composed of a number of DNase I-hypersensitive sites (HSs), which are believed to encompass t...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1304720110

    authors: Williams A,Lee GR,Spilianakis CG,Hwang SS,Eisenbarth SC,Flavell RA

    更新日期:2013-04-23 00:00:00

  • Optofluidic wavelength division multiplexing for single-virus detection.

    abstract::Optical waveguides simultaneously transport light at different colors, forming the basis of fiber-optic telecommunication networks that shuttle data in dozens of spectrally separated channels. Here, we reimagine this wavelength division multiplexing (WDM) paradigm in a novel context--the differentiated detection and i...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1511921112

    authors: Ozcelik D,Parks JW,Wall TA,Stott MA,Cai H,Parks JW,Hawkins AR,Schmidt H

    更新日期:2015-10-20 00:00:00

  • Multimodular biosensors reveal a novel platform for activation of G proteins by growth factor receptors.

    abstract::Environmental cues are transmitted to the interior of the cell via a complex network of signaling hubs. Receptor tyrosine kinases (RTKs) and trimeric G proteins are two such major signaling hubs in eukaryotes. Conventionally, canonical signal transduction via trimeric G proteins is thought to be triggered exclusively ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.1420140112

    authors: Midde KK,Aznar N,Laederich MB,Ma GS,Kunkel MT,Newton AC,Ghosh P

    更新日期:2015-03-03 00:00:00

  • Local instrumental variables and latent variable models for identifying and bounding treatment effects.

    abstract::This paper examines the relationship between various treatment parameters within a latent variable model when the effects of treatment depend on the recipient's observed and unobserved characteristics. We show how this relationship can be used to identify the treatment parameters when they are identified and to bound ...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.96.8.4730

    authors: Heckman JJ,Vytlacil EJ

    更新日期:1999-04-13 00:00:00

  • Lifting cusp forms to Maass forms with an application to partitions.

    abstract::For 2 < k [abstract: see text] we define lifts of cuspidal Poincaré series in S(k)(Gamma(0)(N)) to weight 2 - k harmonic weak Maass forms. This construction answers a question of Dyson by providing the general framework "explaining" Ramanujan's mock theta functions. As an application, we show that the number of partit...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0611414104

    authors: Bringmann K,Ono K

    更新日期:2007-03-06 00:00:00

  • Phasic excitation of dopamine neurons in ventral VTA by noxious stimuli.

    abstract::Midbrain dopamine neurons play central roles in reward processing. It is widely assumed that all dopamine neurons encode the same information. Some evidence, however, suggests functional differences between subgroups of dopamine neurons, particularly with respect to processing nonrewarding, aversive stimuli. To direct...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.0811507106

    authors: Brischoux F,Chakraborty S,Brierley DI,Ungless MA

    更新日期:2009-03-24 00:00:00

  • Autologous and allogeneic typing of human leukemia cells: definition of surface antigens restricted to lymphocytic leukemia cells.

    abstract::Serum from a patient (CO) with acute lymphoblastic leukemia was reactive in immunoadherence assays with autologous leukemia cells but not with autologous blood lymphocytes or bone marrow cells during complete remission. Extensive absorption tests with an array of leukemia cells and normal cells were performed in order...

    journal_title:Proceedings of the National Academy of Sciences of the United States of America

    pub_type: 杂志文章

    doi:10.1073/pnas.80.8.2341

    authors: Naito K,Yamaguchi H,Horibe K,Shiku H,Takahashi T,Suzuki S,Yamada K

    更新日期:1983-04-01 00:00:00