Identifying Reactive Trends in Glycerol Electro-Oxidation Using an Automated Screening Approach: 28 Ways to Electrodeposit an Au Electrocatalyst

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Raghuram Gaddam, Zirui Wang, Yichen Li, Lauren C. Harris, Michael A. Pence, Efren R. Guerrero, Paul J. A. Kenis, Andrew A. Gewirth, Joaquín Rodríguez-López
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引用次数: 0

Abstract

Automated, rapid electrocatalyst discovery techniques that comprehensively address the exploration of chemical spaces, characterization of catalyst robustness, reproducibility, and translation of results to (flow) electrolysis operation are needed. Responding to the growing interest in biomass valorization, we studied the glycerol electro-oxidation reaction (GEOR) on gold in alkaline media as a model reaction to demonstrate the efficacy of such methodology introduced here. Our platform combines individually addressable electrode arrays with HardPotato, a Python application programming interface for potentiostat control, to automate electrochemical experiments and data analysis operations. We systematically investigated the effects of reduction potential (El) and pulse width (PW) on GEOR activity during the electrodeposition (Edep) of gold, evaluating 28 different conditions in triplicate measurements with great versatility. Our findings reveal a direct correlation between El and GEOR activity. Upon CV cycling, we recorded a 52% increase in peak current density and a −0.25 V shift in peak potential as El varied from −0.2 to −1.4 V. We also identified an optimal PW of ∼1.0 s, yielding maximum catalytic performance. The swift analysis enabled by our methodology allowed us to correlate performance enhancements with increased electrochemical surface area and preferential deposition of Au(110) and Au(111) sites, even in disparate Edep conditions. We validate our methodology by scaling the Edep process to larger electrodes and correlating intrinsic activity with product speciation via flow electrolysis measurements. Our platform highlights opportunities in automation for electrocatalyst discovery to address pressing needs toward industrial decarbonization, such as biomass valorization.

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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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