Carbon capture and utilization involve multiple energy- and cost-intensive steps. Dual-function materials (DFMs) can reduce these demands by coupling CO adsorption and conversion into a single material with two functionalities: a sorbent phase and a metal for catalytic CO conversion. The role of metal catalysts in the conversion process seems salient from previous work, but the underlying mechanisms remain elusive and deserve deeper investigation to achieve maximum utilization of the two phases.
View Article and Find Full Text PDFAdv Mater
December 2024
Encapsulation of metal nanoparticles within oxide materials has been shown as an effective strategy to improve activity, selectivity, and stability in several catalytic applications. Several approaches have been proposed to encapsulate nanoparticles, such as forming core-shell structures, growing ordered structures (zeolites or metal-organic frameworks) on nanoparticles, or directly depositing support materials on nanoparticles. Here, a general nanocasting method is demonstrated that can produce diverse encapsulated metal@oxide structures with different compositions (Pt, Pd, Rh) and multiple types of oxides (AlO, AlO-CeO, ZrO, ZnZrO, InO, MnO, TiO) while controlling the size and dispersion of nanoparticles and the porous structure of the oxide.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Multicomponent catalysts can be designed to synergistically combine reaction intermediates at interfacial active sites, but restructuring makes systematic control and understanding of such dynamics challenging. We here unveil how reducibility and mobility of indium oxide species in Ru-based catalysts crucially control the direct, selective conversion of CO to ethanol. When uncontrolled, reduced indium oxide species occupy the Ru surface, leading to deactivation.
View Article and Find Full Text PDFBimetallic alloys made from immiscible elements are characterized by their tendency to segregate on the macroscopic scale, but their behavior is known to change at the nanoscale. Here, we demonstrate that in the Ru-In system, In atoms preferentially decorate the surface of 6 nm Ru nanoparticles, forming Ru-In superficial immiscible alloys. This surface decoration dramatically affects the catalytic performance of the system, even at small atomic fractions of In added to Ru.
View Article and Find Full Text PDFConspectusMethane complete oxidation is an important reaction that is part of the general scheme used for removing pollutants contained in emissions from internal combustion engines and, more generally, combustion processes. It has also recently attracted interest as an option for the removal of atmospheric methane in the context of negative emission technologies. Methane, a powerful greenhouse gas, can be converted to carbon dioxide and water via its complete oxidation.
View Article and Find Full Text PDFNanoscale
February 2022
The dehydration of alcohols is an important class of reactions for the development of fossil-free fuel and chemical industries. Acid catalysts are well known to enhance the reactivity of alcohols following two main pathways of either dehydration to olefins or dehydrogenation to ketones/aldehydes. TiO surfaces have been well documented for primary and secondary alcohol dehydration with selectivity ranging from 1-100% towards dehydration products based on process conditions and catalyst structure.
View Article and Find Full Text PDFDefects may display high reactivity because the specific arrangement of atoms differs from crystalline surfaces. We demonstrate that high-temperature steam pretreatment of palladium catalysts provides a 12-fold increase in the mass-specific reaction rate for carbon-hydrogen (C–H) activation in methane oxidation compared with conventional pretreatments. Through a combination of experimental and theoretical methods, we demonstrate that an increase in the grain boundary density through crystal twinning is achieved during the steam pretreatment and oxidation and is responsible for the increased reactivity.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2020
The demand for display technology is expected to increase with the continuous spread of portable electronics and with the expected emergence of flexible, wearable, and transparent display devices. A touch screen is a critical component in display technology that enables user interface operations, and the future generation of touch screens, the so-called 3D touch screens, is expected to be able to detect multiple levels of pressure. To enable 3D touch screens, transparent pressure sensors with high linearity over a working range that encompasses the pressure range of human touch (10-100 kPa) are required.
View Article and Find Full Text PDFSensor-to-sensor variability and high hysteresis of composite-based piezoresistive pressure sensors are two critical issues that need to be solved to enable their practical applicability. In this work, a piezoresistive pressure sensor composed of an elastomer template with uniformly sized and arranged pores, and a chemically grafted conductive polymer film on the surface of the pores is presented. Compared to sensors composed of randomly sized pores, which had a coefficient of variation (CV) in relative resistance change of 69.
View Article and Find Full Text PDFACS Appl Mater Interfaces
May 2019
An ultrahigh sensitive capacitive pressure sensor based on a porous pyramid dielectric layer (PPDL) is reported. Compared to that of the conventional pyramid dielectric layer, the sensitivity was drastically increased to 44.5 kPa in the pressure range <100 Pa, an unprecedented sensitivity for capacitive pressure sensors.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2019
Electronic skin are devices that mimic the functionalities of human skin, which require high sensitivity, large dynamic range, high spatial uniformity, low-cost and large-area processability, and the capacity to differentiate various external inputs. We herein introduce a versatile droplet-based microfluidic-assisted emulsion self-assembly process to generate three-dimensional microstructure-based high-performance capacitive and piezoresistive pressure sensors for electronic skin applications. Our technique can generate uniformly sized micropores that are self-assembled in an orderly close-packed manner over a large area, which results in high spatial uniformity.
View Article and Find Full Text PDFTactile sensors that can mechanically decouple, and therefore differentiate, various tactile inputs are highly important to properly mimic the sensing capabilities of human skin. Herein, we present an all-solution processable pressure insensitive strain sensor that utilizes the difference in structural change upon the application of pressure and tensile strain. Under the application of strain, microcracks occur within the multiwalled carbon nanotube (MWCNT) network, inducing a large change in resistance with gauge factor of ∼56 at 70% strain.
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