Abstract:
:The prominent size effect of metal nanoparticles shapes decisively nanocatalysis, but entanglement of the corresponding geometric and electronic effects prevents exploiting their distinct functionalities. In this work, we demonstrate that in palladium (Pd)-catalyzed aerobic oxidation of benzyl alcohol, the geometric and electronic effects interplay and compete so intensively that both activity and selectivity showed in volcano trends on the Pd particle size unprecedentedly. By developing a strategy of site-selective blocking via atomic layer deposition along with first principles calculations, we disentangle these two effects and unveil that the geometric effect dominates the right side of the volcano with larger-size Pd particles, whereas the electronic effect directs the left of the volcano with smaller-size Pd particles substantially. Selective blocking of the low-coordination sites prevents formation of the undesired by-product beyond the volcano relationship, achieving a remarkable benzaldehyde selectivity and activity at the same time for 4-nm Pd. Disentangling the geometric and electronic effects of metal nanoparticles opens a new dimension for rational design of catalysts.
journal_name
Sci Advjournal_title
Science advancesauthors
Wang H,Gu XK,Zheng X,Pan H,Zhu J,Chen S,Cao L,Li WX,Lu Jdoi
10.1126/sciadv.aat6413subject
Has Abstractpub_date
2019-01-18 00:00:00pages
eaat6413issue
1issn
2375-2548pii
aat6413journal_volume
5pub_type
杂志文章相关文献
Science Advances文献大全abstract::Association of peripheral proteins with lipid bilayers regulates membrane signaling and dynamics. Pleckstrin homology (PH) domains bind to phosphatidylinositol phosphate (PIP) molecules in membranes. The effects of local PIP enrichment on the interaction of PH domains with membranes is unclear. Molecular dynamics simu...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aay5736
更新日期:2020-02-19 00:00:00
abstract::Ammonia synthesis consumes 3 to 5% of the world's natural gas, making it a significant contributor to greenhouse gas emissions. Strategies for synthesizing ammonia that are not dependent on the energy-intensive and methane-based Haber-Bosch process are critically important for reducing global energy consumption and mi...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.1700336
更新日期:2018-04-27 00:00:00
abstract::Low seismic velocity regions in the mantle and crust are commonly attributed to the presence of silicate melts. Determining melt volume and geometric distribution is fundamental to understanding planetary dynamics. We present a new model for seismic velocity reductions that accounts for the anomalous compressibility o...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.1701312
更新日期:2017-12-13 00:00:00
abstract::Engineered surfaces with reversibly switching interfacial properties, such as wettability and liquid repellency, are highly desirable in diverse application fields but are rare. We have developed a general concept to prepare metallic porous surfaces with exceptionally powerful wettability switch capabilities and liqui...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aax0380
更新日期:2019-11-01 00:00:00
abstract::The progression in the hair follicle cycle from the telogen to the anagen phase is the key to regulating hair regrowth. Dermal papilla (DP) cells support hair growth and regulate the hair cycle. However, they gradually lose key inductive properties upon culture. DP cells can partially restore their capacity to promote...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aba1685
更新日期:2020-07-24 00:00:00
abstract::The geothermal heat flux is a critical thermal boundary condition that influences the melting, flow, and mass balance of ice sheets, but measurements of this parameter are difficult to make in ice-covered regions. We report the first direct measurement of geothermal heat flux into the base of the West Antarctic Ice Sh...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.1500093
更新日期:2015-07-10 00:00:00
abstract::Intrinsically disordered regions (IDRs) of proteins are implicated in key macromolecular interactions. However, the molecular forces underlying IDR function within multicomponent assemblies remain elusive. By combining thermodynamic and structural data, we have discovered an allostery-based mechanism regulating the so...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aax1836
更新日期:2019-11-27 00:00:00
abstract::Over millions of years, the oxidation of organic carbon contained within sedimentary rocks is one of the main sources of carbon dioxide to the atmosphere, yet the controls on this emission remain poorly constrained. We use rhenium to track the oxidation of rock-bound organic carbon in the mountain watersheds of New Ze...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.1701107
更新日期:2017-10-04 00:00:00
abstract::The inherent specificity and electrochemical reversibility of enzymes poise them as the biorecognition element of choice for a wide range of metabolites. To use enzymes efficiently in biosensors, the redox centers of the protein should have good electrical communication with the transducing electrode, which requires e...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aat0911
更新日期:2018-06-22 00:00:00
abstract::The high-lying vibrational states of the magnesium dimer (Mg2), which has been recognized as an important system in studies of ultracold and collisional phenomena, have eluded experimental characterization for half a century. Until now, only the first 14 vibrational states of Mg2 have been experimentally resolved, alt...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aay4058
更新日期:2020-04-03 00:00:00
abstract::Conjugated polymer-polyelectrolyte blends combine and couple electronic semiconductor functionality with selective ionic transport, making them attractive as the active material in organic biosensors and bioelectronics, electrochromic displays, neuromorphic computing, and energy conversion and storage. Although extens...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aao3659
更新日期:2017-12-15 00:00:00
abstract::At a time of heightened anxiety surrounding immigration, state governments have increasingly sought to manage immigrant and refugee flows. Yet the factors that influence where immigrants choose to settle after arrival remain unclear. We bring evidence to this question by analyzing population-level data for refugees re...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.abb0295
更新日期:2020-08-07 00:00:00
abstract::Cellular cross-talk between ubiquitination and other posttranslational modifications contributes to the regulation of numerous processes. One example is ADP-ribosylation of the carboxyl terminus of ubiquitin by the E3 DTX3L/ADP-ribosyltransferase PARP9 heterodimer, but the mechanism remains elusive. Here, we show that...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.abc0418
更新日期:2020-09-18 00:00:00
abstract::Metal-organic frameworks (MOFs) have been attracting intensive attention because of their commendable potential in many applications. Postsynthetic modification for redesigning chemical characteristics and pore structures can greatly improve performance and expand functionality of MOF materials. Here, we develop a ver...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aax7270
更新日期:2020-05-01 00:00:00
abstract::We studied a bilayer system hosting two-dimensional electron systems (2DESs) in close proximity but isolated from one another by a thin barrier. One 2DES has low electron density and forms a Wigner solid (WS) at high magnetic fields. The other has much higher density and, in the same field, exhibits fractional quantum...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aao2848
更新日期:2019-03-15 00:00:00
abstract::Understanding the precise atomic structure of ice surfaces is critical for revealing the mechanisms of physical and chemical phenomena at the surfaces, such as ice growth, melting, and chemical reactions. Nevertheless, no conclusive structure has been established. In this study, noncontact atomic force microscopy was ...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.abb7986
更新日期:2020-09-11 00:00:00
abstract::Dysregulated physical stresses are generated during tumorigenesis that affect the surrounding compliant tissues including adipocytes. However, the effect of physical stressors on the behavior of adipocytes and their cross-talk with tumor cells remain elusive. Here, we demonstrate that compression of cells, resulting f...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aax5611
更新日期:2020-01-22 00:00:00
abstract::Plants produce a myriad of taxonomically restricted specialized metabolites. This diversity-and our ability to correlate genotype with phenotype-makes the evolution of these ecologically and medicinally important compounds interesting and experimentally tractable. Trichomes of tomato and other nightshade family plants...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aaw3754
更新日期:2019-04-24 00:00:00
abstract::Tropical forest fragmentation results in habitat and biodiversity loss and increased carbon emissions. Here, we link an increased likelihood of tropical forest loss to decreasing fragment size, particularly in primary forests. The relationship holds for protected areas, albeit with half the rate of loss compared with ...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aax8574
更新日期:2020-03-11 00:00:00
abstract::Recently, the complexity behind manipulations of reflected fields by metasurfaces has been addressed, showing that, even in the simplest scenarios, nonlocal response and excitation of auxiliary evanescent fields are required for perfect field control. In this work, we introduce purely local reflective metasurfaces for...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aau7288
更新日期:2019-02-15 00:00:00
abstract::The transcriptional repressors Polycomb repressive complex 1 (PRC1) and PRC2 are required to maintain cell fate during embryonic development. PRC1 and PRC2 catalyze distinct histone modifications, establishing repressive chromatin at shared targets. How PRC1, which consists of canonical PRC1 (cPRC1) and variant PRC1 (...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aax5692
更新日期:2020-04-01 00:00:00
abstract::Viscosity of fluids is strongly system dependent, varies across many orders of magnitude, and depends on molecular interactions and structure in a complex way not amenable to first-principles theories. Despite the variations and theoretical difficulties, we find a new quantity setting the minimal kinematic viscosity o...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aba3747
更新日期:2020-04-24 00:00:00
abstract::Passive radiative cooling functions by reflecting the solar spectrum and emitting infrared waves in broadband or selectively. However, cooling enclosed spaces that trap heat by greenhouse effect remains a challenge. We present a Janus emitter (JET) consisting of an Ag-polydimethylsiloxane layer on micropatterned quart...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.abb1906
更新日期:2020-09-04 00:00:00
abstract::Under rapid high-temperature, high-pressure loading, lattices exhibit complex elastic-inelastic responses. The dynamics of these responses are challenging to measure experimentally because of high sample density and extremely small relevant spatial and temporal scales. Here, we use an x-ray free-electron laser providi...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aau8044
更新日期:2019-03-08 00:00:00
abstract::Asymmetric interactions such as entropic (e.g., encoded by nonspherical shapes) or surface forces (e.g., encoded by patterned surface chemistry or DNA hybridization) provide access to functional states of colloidal matter, but versatile approaches for engineering asymmetric van der Waals interactions have the potentia...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.abb1327
更新日期:2020-06-19 00:00:00
abstract::The past few years have witnessed rapid advances in the synthesis of high-quality perovskite nanocrystals (PNCs). However, despite the impressive developments, the stability of PNCs remains a substantial challenge. The ability to reliably improve stability of PNCs while retaining their individual nanometer size repres...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.aax4424
更新日期:2019-11-29 00:00:00
abstract::The spin-polarized surface states of topological insulators (TIs) are attractive for applications in spintronics and quantum computing. A central challenge with these materials is to reliably tune the chemical potential of their electrons with respect to the Dirac point and the bulk bands. We demonstrate persistent, b...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.1500640
更新日期:2015-10-09 00:00:00
abstract::The cyclic GMP-AMP synthase (cGAS), a sensor of cytosolic DNA, is critical for the innate immune response. Here, we show that loss of cGAS in untransformed and cancer cells results in uncontrolled DNA replication, hyperproliferation, and genomic instability. While the majority of cGAS is cytoplasmic, a fraction of cGA...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.abb8941
更新日期:2020-10-14 00:00:00
abstract::Characterizing and understanding the emergence of multiple macroscopically ordered electronic phases through subtle tuning of temperature, pressure, and chemical doping has been a long-standing central issue for complex materials research. We report the first comprehensive studies of optical doping-induced emergence o...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.1400173
更新日期:2015-06-26 00:00:00
abstract::Photonic crystal nanocavities, which have modal volumes of the order of a cubic wavelength in the material, are of great interest as flexible platforms for manipulating photons. Recent developments in ultra-high quality factor nanocavities with long photon lifetimes have encouraged us to develop an ultra-compact and f...
journal_title:Science advances
pub_type: 杂志文章
doi:10.1126/sciadv.1501690
更新日期:2016-05-20 00:00:00