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Achieving flexible large-scale reactivity tuning by controlling the phase, thickness and support of two-dimensional ZnO.

ABSTRACT: Tuning surface reactivity of catalysts is an effective strategy to enhance catalytic activity towards a chemical reaction. Traditional reactivity tuning usually relies on a change of the catalyst composition, especially when large-scale tuning is desired. Here, based on density functional theory calculations, we provide a strategy for flexible large-scale tuning of surface reactivity, i.e. from a few tenths of electronvolts (eV) to multiple eV, merely through manipulating the phase, thickness, and support of two-dimensional (2D) ZnO films. 2D ZnO films have three typical phases, i.e. graphene, wurtzite, and body-centered-tetragonal structures, whose intrinsic stability strongly depends on the thickness and/or the chemical nature of the support. We show that the adsorption energy of hydrogen differs by up to 3 eV on these three phases. For the same phase, varying the film thickness and/or support can lead to a few tenths of eV to 2 eV tuning of surface reactivity. We further demonstrate that flexible large-scale tuning of surface reactivity has a profound impact on the reaction kinetics, including breaking the Brønsted-Evans-Polanyi relationship.

SUBMITTER: Lin L

PROVIDER: S-EPMC8635171 | biostudies-literature | 2021 Dec

REPOSITORIES: biostudies-literature

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Achieving flexible large-scale reactivity tuning by controlling the phase, thickness and support of two-dimensional ZnO.

Lin Le L Zeng Zhenhua Z Fu Qiang Q Bao Xinhe X

Chemical science 20211104 46

Tuning surface reactivity of catalysts is an effective strategy to enhance catalytic activity towards a chemical reaction. Traditional reactivity tuning usually relies on a change of the catalyst composition, especially when large-scale tuning is desired. Here, based on density functional theory calculations, we provide a strategy for flexible large-scale tuning of surface reactivity, <i>i.e.</i> from a few tenths of electronvolts (eV) to multiple eV, merely through manipulating the phase, thick ...[more]

PMID: 34976348

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Project description:Nanomaterials for highly selective and sensitive sensors toward specific gas molecules of volatile organic compounds (VOCs) are most important in developing new-generation of detector devices, for example, for biomarkers of diseases as well as for continuous air quality monitoring. Here, we present an innovative preparation approach for engineering sensors, which allow for full control of the dopant concentrations and the nanoparticles functionalization of columnar material surfaces. The main outcome of this powerful design concept lies in fine-tuning the reactivity of the sensor surfaces toward the VOCs of interest. First, nanocolumnar and well-distributed Ag-doped zinc oxide (ZnO:Ag) thin films are synthesized from chemical solution, and, at a second stage, noble nanoparticles of the required size are deposited using a gas aggregation source, ensuring that no percolating paths are formed between them. Typical samples that were investigated are Ag-doped and Ag nanoparticle-functionalized ZnO:Ag nanocolumnar films. The highest responses to VOCs, in particular to (CH3)2CHOH, were obtained at a low operating temperature (250 °C) for the samples synergistically enhanced with dopants and nanoparticles simultaneously. In addition, the response times, particularly the recovery times, are greatly reduced for the fully modified nanocolumnar thin films for a wide range of operating temperatures. The adsorption of propanol, acetone, methane, and hydrogen at various surface sites of the Ag-doped Ag8/ZnO(0001) surface has been examined with the density functional theory (DFT) calculations to understand the preference for organic compounds and to confirm experimental results. The response of the synergistically enhanced sensors to gas molecules containing certain functional groups is in excellent agreement with density functional theory calculations performed in this work too. This new fabrication strategy can underpin the next generation of advanced materials for gas sensing applications and prevent VOC levels that are hazardous to human health and can cause environmental damages.

Dataset Information

Achieving flexible large-scale reactivity tuning by controlling the phase, thickness and support of two-dimensional ZnO.

Publications

Achieving flexible large-scale reactivity tuning by controlling the phase, thickness and support of two-dimensional ZnO.

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