Publications by authors named "Samuel Dull"

Platinum is an important material with applications in oxygen and hydrogen electrocatalysis. To better understand how its activity can be modulated through electrolyte effects in the double layer microenvironment, herein we investigate the effects of different acid anions on platinum for the oxygen reduction/evolution reaction (ORR/OER) and hydrogen evolution/oxidation reaction (HER/HOR) in pH 1 electrolytes. Experimentally, we see the ORR activity trend of HClO > HNO > HSO, and the OER activity trend of HClO [Formula: see text] HNO ∼ HSO.

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Although nanoporous carbons are ubiquitous materials that are used in many clean energy and environmental applications, most are in powder form, thus requiring binders to hold particles together. This results in uncontrolled and complex pathways between particles, potentially exacerbating mass transport issues. To overcome these problems, we have developed an unprecedented binderless, self-supported, nanoporous carbon scaffold (NCS) with tunable and monodisperse pores (5-100+ nm), high surface area ( 200-575 m g), and 3-dimensional scalability (1-150+ cm, 1-1000 μm thickness).

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Understanding the differences between reactions driven by elevated temperature or electric potential remains challenging, largely due to materials incompatibilities between thermal catalytic and electrocatalytic environments. We show that Ni, N-doped carbon (NiPACN), an electrocatalyst for the reduction of CO to CO (CO R), can also selectively catalyze thermal CO to CO via the reverse water gas shift (RWGS) representing a direct analogy between catalytic phenomena across the two reaction environments. Advanced characterization techniques reveal that NiPACN likely facilitates RWGS on dispersed Ni sites in agreement with CO R active site studies.

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Ni,N-doped carbon catalysts have shown promising catalytic performance for CO electroreduction (CO R) to CO; this activity has often been attributed to the presence of nitrogen-coordinated, single Ni atom active sites. However, experimentally confirming Ni-N bonding and correlating CO reduction (CO R) activity to these species has remained a fundamental challenge. We synthesized polyacrylonitrile-derived Ni,N-doped carbon electrocatalysts (Ni-PACN) with a range of pyrolysis temperatures and Ni loadings and correlated their electrochemical activity with extensive physiochemical characterization to rigorously address the origin of activity in these materials.

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It is frequently desired to synthesize supported metal catalysts that consist of very small clusters or single atoms. In this work, we combine strong electrostatic adsorption (SEA) of HPtCl and engineered oxide supports to ultimately produce very small Pt clusters, including a large fraction of single Pt atoms. The supports are synthesized by depositing controlled amounts of SiO onto AlO (SiO@AlO) that has been previously grafted with bulky organic templates.

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