Noble metals or oxide catalysts have traditionally been loaded or doped to enhance the gas sensing properties of oxide semiconductor chemiresistors. However, the selective detection of various chemicals for a wide range of new applications remains a challenging problem. In this paper, we propose a novel bilayer design with an oxide chemiresistor sensing layer and nanoscale catalytic Au overlayer to provide high controllability for gas sensing characteristics. The Au nanocluster overlayer significantly enhances the methylbenzene response of a SnO thick film sensor by reforming gases into more reactive species and suppresses the responses to reactive interference gases through oxidative filtering, leading to excellent selectivity to methylbenzene. Gas sensing characteristics can be tuned by controlling the morphology, amount, and number density of Au nanoclusters through the variation in the Au coating thickness (0.5-3 nm) and thermal annealing conditions (0.5-4 h at 550 °C). Furthermore, the general validity of the proposed Au-coated bilayer sensor design was confirmed through the enhancement of response and selectivity toward methylbenzenes by coating Au nanoclusters onto ZnO and CoO sensors. The sensing mechanism, advantages, and potential applications of bilayer sensors are discussed from the perspective of the separation of sensing and catalytic reactions, as well as the reforming and oxidation of analyte gases in association with the configuration of the sensing layer and Au catalytic overlayer.
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http://dx.doi.org/10.1021/acsami.9b11079 | DOI Listing |
Adv Mater
January 2025
School of Pharmaceutical and Chemical Engineering, Taizhou University, Jiaojiang, 318000, P. R. China.
Efficient charge separation at the semiconductor/cocatalyst interface is crucial for high-performance photoelectrodes, as it directly influences the availability of surface charges for solar water oxidation. However, establishing strong molecular-level connections between these interfaces to achieve superior interfacial quality presents significant challenges. This study introduces an innovative electrochemical etching method that generates a high concentration of oxygen vacancy sites on BiVO surfaces (Ov-BiVO), enabling interactions with the oxygen-rich ligands of MIL-101.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford Street, Cambridge, Massachusetts 02138, United States.
A conventional performance metric for electrocatalysts that promote the oxygen evolution reaction (OER) is the current density at a given overpotential. However, the assumption that increased current density at lower overpotentials indicates superior catalyst design is precarious for OER catalysts in the working environment, as the crystalline lattice is prone to deconstruction and amorphization, thus greatly increasing the concentration of catalytic active sites. We show this to be the case for La incorporation into CoO.
View Article and Find Full Text PDFACS Sens
December 2024
State Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, China.
Constructing a bilayer structure has not been reported as a method to mitigate the adverse effect of water poisoning on oxide chemiresistors while simultaneously enhancing gas selectivity and sensitivity. To address this challenge, pyrochlore-BiSnO has been first utilized as an overlayer on a ZnO sensing layer for constructing a bilayer acetone chemiresistor, leading to remarkable improvement in the performance for trace-level (500 p-p-b) acetone detection under high humidity (80% relative humidity). In addition, owing to the catalytic predecompositions of ethanol across the overlayer, an outstanding acetone gas selectivity (/ = 2.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
Boron-based catalysts have exhibited excellent olefin selectivity in the oxidative dehydrogenation of propane (ODHP) reaction. The substrate material should be a potential platform for performance modulation of boron catalysts in this reaction since the introduction of subsurface Ni promoters significantly improves the activity. In this study, we deciphered the substrate effect and identified a performance descriptor to comprehend the roles of subsurface materials in BO/metal/BN ODHP catalysts by evaluating different metal promoters.
View Article and Find Full Text PDFAdv Mater
November 2024
State Key Laboratory of Pulp and Paper Engineering, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China.
Benzene, toluene, and p-xylene (BTpX) are among the most important commodity chemicals, but their productions still heavily rely on fossil resources and thus pose serious environmental burdens and energy crisis. Herein, the tandem upgrading of bio-furans is reported to high-yield BTpX by rationally constructing a versatile PtSn intermetallic coupling ordered-mesoporous SnO (OM-SnO) catalyst. It is shown that with increasing reduction temperature from 200 to 350°C, Pt nanoparticles (NPs) are first formed on OM-SnO, then converted to PtSn intermetallic nanoparticles (iNPs), and finally to PtSn iNPs with a gradually-thickened SnO overlayer.
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