The electrochemical generation of hydrogen is a key enabling technology for the production of sustainable fuels. Transition metal chalcogenides show considerable promise as catalysts for this reaction, but to date there are very few reports of tellurides in this context, and none of these transition metal telluride catalysts are especially active. Here, we show that the catalytic performance of metallic 1T′-MoTe2 is improved dramatically when the electrode is held at cathodic bias. As a result, the overpotential required to maintain a current density of 10 mA cm−2 decreases from 320 mV to just 178 mV. We show that this rapid and reversible activation process has its origins in adsorption of H onto Te sites on the surface of 1T′-MoTe2. This activation process highlights the importance of subtle changes in the electronic structure of an electrode material and how these can influence the subsequent electrocatalytic activity that is displayed.
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.
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