About

Joseph DuChene is an Assistant Professor of Chemistry at the University of Massachusetts – Amherst. His research group focuses on designing and creating nanostructured catalysts that enable the sustainable synthesis of fuels and chemicals from readily abundant small molecules. Prior to his appointment at UMass Amherst, DuChene was a postdoctoral scholar in the group of Professor Harry Atwater at the California Institute of Technology. During his time at Caltech, he worked with the Joint Center for Artificial Photosynthesis, conducting fundamental studies on the energy distributions and ultrafast dynamics of plasmonic hot carriers in metal nanostructures. He also pioneered new plasmonic devices aimed at enhancing the selectivity of photoelectrochemical CO2 reduction. DuChene earned his Ph.D. in Physical Chemistry from the University of Florida in the group of Professor W. David Wei. His doctoral research involved developing in situ electrochemical and spectroscopic techniques to monitor charge-carrier dynamics in metal-semiconductor heterostructures and creating plasmonic photoelectrochemical cells for solar-to-fuel energy conversion.

Research topics

• Nanotechnology
• Materials science
• Chemistry
• Optics
• Photochemistry
• Optoelectronics
• Chemical physics
• Inorganic chemistry
• Computational chemistry
• Physics

Selected publications

• Mechanistic Insights into Electrochemical Nitrate Reduction with Cu Single Crystals

  ECS Meeting Abstracts · 2025-07-11

  article1st authorCorresponding

  Electrochemical reduction of nitrate (NO 3 ) to ammonia (NH 3 ) is a promising approach towards the sustainable synthesis of fertilizer while simultaneously remediating contaminated water. Despite several examples of Cu-based electrocatalysts producing ammonia at relatively high reaction rates, important details of the overall reaction mechanism on Cu surfaces remain unclear. In particular, the selectivity of low-index Cu surfaces for ammonia production across a range of solution pH is still poorly understood. Here, we report our studies of electrochemical nitrate reduction with Cu(100), Cu(110), and Cu(111) single-crystal electrodes. We quantified the product distribution and reaction rates across a range of applied potentials, which allowed for elucidating structure-function relationships with Cu electrodes. Our systematic study of electrocatalytic NO 3 reduction revealed that the Cu(100) surface exhibited superior NH 3 selectivity relative to the other two surfaces, demonstrating >95% Faradaic efficiency towards NH 3 over the broadest range of applied potentials. Overall, our study provides practical guidelines for improving the reaction selectivity for ammonia via electrochemical nitrate reduction with Cu-based electrodes.

  PublisherDOI

• Plasmon-Driven Synthesis of Cu Nanostructures

  Nano Letters · 2025-06-14 · 3 citations

  articleSenior authorCorresponding

  Plasmonic photochemistry holds great promise for optical control of materials growth at the nanoscale. To date, however, this unique approach to the synthesis of monometallic metal nanostructures remains restricted to just two elements: silver (Ag) and gold (Au). Here, we report the plasmon-driven synthesis of copper (Cu) nanostructures in aqueous solution via seed-mediated growth. The entire synthesis was conducted under an inert atmosphere, with precise control over solution pH and reaction temperature to prevent oxide formation. We found that the growth of triangular and hexagonal Cu nanoprisms was determined by the concentration of the surfactant polyvinylpyrrolidone in the growth solution. A series of photochemical experiments and control reactions were also performed to confirm that the growth of Cu nanostructures occurs via plasmonic photocatalysis. Our approach offers a unique route to the growth of Cu nanostructures and expands the domain of plasmon-driven synthesis to a new element in the periodic table.

  PublisherDOI

• <i>(Invited)</i> The Influence of Metal Band Structure on Plasmon-Driven Photocatalysis

  ECS Meeting Abstracts · 2025-11-24

  article1st authorCorresponding

  Plasmon-driven photocatalysis with metal nanoparticles holds great promise for photocatalysis, yet the complex interplay between metal band structure and incident photon energy on the resulting energy distribution of hot carriers is poorly understood. As such, the ability to design and synthesize metal nanostructures with desirable photocatalytic properties for a given reaction of interest remains out of reach. To address this challenge, we have developed procedures for the plasmon-driven synthesis of Cu, Ag, and Au nanostructures under identical experimental conditions. We found that the development of a plasmon-driven synthesis of Cu nanoparticles required the exclusion of molecular oxygen and strict control over solution pH to enable the plasmon-driven process to proceed. A series of control experiments confirmed that the growth of Cu nanoparticles occurs via plasmon excitation of the Cu seeds, in a manner similar to that previously discovered for both Ag and Au nanoparticles. Our approach provides a platform to systematically evaluate the role of metal band structure for all three plasmonic elements on the photocatalytic quantum yield of plasmon-driven photochemistry under conditions relevant to solar photocatalysis. We have studied the influence of sacrificial hole scavengers on hot-electron-driven reduction reactions, providing insight into the role of hot holes on plasmon-driven photocatalysis. We will also share our results involving the influence of nanoparticle defects on the plasmon-driven growth rate and compare the photocatalytic quantum yields of Cu, Ag, and Au nanoparticles. Overall, our approach offers a platform to understand the photocatalytic properties of hot carriers in plasmonic metals and elucidate the fundamental design principles for plasmonic photocatalysis with metal nanostructures.

  PublisherDOI

• (Invited) Plasmon-Driven Photochemistry for the Synthesis of Metal Nanostructures

  ECS Meeting Abstracts · 2024-08-09

  article1st authorCorresponding

  Plasmon-driven photocatalysis with metal nanoparticles holds great promise for initiating and controlling chemical reactions at the nanoscale. One interesting application of plasmonic photochemistry involves the synthesis of metal nanostructures from cationic precursors. Despite more than twenty years of study however, this unique approach to material synthesis remains restricted to just two elements: silver (Ag) and gold (Au). To date, this process is yet to be observed with any other metals. Here, we report the plasmon-driven synthesis of copper (Cu) nanoparticles in aqueous solution via a seed-mediated growth strategy. The plasmonic synthesis is amenable to various Cu precursors, but is highly sensitive to the type of hole scavenger used in the reaction. We also found that the exclusion of oxygen from the system, both in the initial synthesis of Cu seeds and in their subsequent growth into larger nanoparticles, was essential for enabling the plasmon-driven process to proceed. A series of control experiments, supported by photoelectrochemical measurements, were performed to confirm that the growth of Cu nanoparticles occurs via plasmon excitation of the Cu seeds. Overall, our approach offers a unique route to the synthesis of Cu nanoparticles and expands the domain of plasmon-driven photochemistry to a new element.

  PublisherDOI

• Electrochemical Growth and Restructuring of Cu Surfaces for Steering the Selectivity of Electrocatalytic CO₂ Reduction

  ECS Meeting Abstracts · 2023-08-28

  article1st authorCorresponding

  The electrocatalytic reduction of CO 2 into value-added chemicals is commonly performed with catalysts composed of Cu due to its unique ability to create carbon-carbon bonds. Numerous studies have shown that the surface facets of the Cu catalyst play an important role on the observed distributions of both C 1 products (i.e. carbon monoxide vs. methane) and C 2 products (i.e. ethanol vs. ethylene). Here, we discuss our efforts towards controlling the surface facets of Cu electrocatalysts via electrochemical treatments for steering the selectivity of CO 2 reduction in aqueous media. Using both planar Cu films and Cu nanoparticles, we will show how the applied potential and chemical composition of the growth solution can be manipulated to tailor the surface facets of Cu electrocatalysts. Finally, we will present the results of electrocatalytic CO 2 reduction with these Cu catalysts and highlight opportunities for using simple electrochemical techniques to manipulate and control the surface facets of electrocatalysts for the production of chemical fuels.

  PublisherDOI

• Probing the Catalytically Active Region in a Nanoporous Gold Gas Diffusion Electrode for Highly Selective Carbon Dioxide Reduction

  ACS Energy Letters · 2022-01-27 · 32 citations

  articleOpen access

  We report the use of a nanoporous gold (np-Au) catalyst for CO2 reduction in a gas diffusion electrode (GDE) and characterize the role of wetting in electrochemical performance. The np-Au catalyst has pores on the order of 20 nm and is cross-sectionally isotropic, enabling Faradaic efficiencies for CO of greater than 95% across a wide range of potentials and a maximum partial current density for CO of 168 mA/cm2. Secondary ion mass spectroscopy and in situ copper underpotential deposition were employed to provide insights into catalyst wetting. At a typical CO2 flow rate of 50 SCCM, approximately half of the catalyst is in contact with the electrolyte during operation, and the dry region exists in the bottom half of the nanoporous catalyst. We discuss implications of the nanoporous GDE wetting characteristics for catalyst performance and the design of improved GDE architectures that can maximize the catalytically active area.

  PublisherOA PDFDOI

• Unassisted Highly Selective Gas-Phase CO₂ Reduction with a Plasmonic Au/p-GaN Photocatalyst Using H₂O as an Electron Donor

  ACS Energy Letters · 2021-04-20 · 89 citations

  article

  Surface plasmon resonances in metal nanostructures enable the generation of nonequilibrium hot electron–hole pairs, which has received wide interest as a means to drive chemical reactions at the nanoscale. However, harvesting hot holes in plasmonic heterostructures to drive oxidation reactions to balance the photocatalytic CO2 reduction reaction has been challenging. Further, details of the balanced redox reaction pathways for gas-phase photocatalysis have been difficult to identify. Here, we report an Au/p-GaN plasmonic heterostructure photocatalyst in which unassisted, self-sustaining, highly selective photocatalytic CO2 reduction to CO is directly balanced by water oxidation, operating under solar illumination. We find remarkable enhancements in CO yield for heterostructures that employ a metal/insulator/semiconductor configuration with an ultrathin aluminum oxide layer between composite Au/Cu nanoparticles and p-GaN. Our work underscores the potential for plasmonic heterostructure photocatalysts to perform selective and unassisted gas-phase photocatalytic CO2 reduction to convert solar energy into chemical fuels.

  PublisherDOI

• <i>Operando</i> Local pH Measurement within Gas Diffusion Electrodes Performing Electrochemical Carbon Dioxide Reduction

  The Journal of Physical Chemistry C · 2021-09-17 · 63 citations

  articleOpen access

  The local pH near the surface of a CO2 reduction electrocatalyst strongly impacts catalytic selectivity and activity. Here, confocal fluorescence microscopy was used to map the electrolyte pH near a copper gas diffusion electrode during CO2 reduction with micron spatial resolution in three dimensions. We observed that the local pH increased from pH 6.8 to greater than pH 10 as the current density was increased from 0 to 28 mA/cm2 in a 100 mM KHCO3 electrolyte. Variations in the pH across the surface indicate areas of locally increased activity. Within deep trenches of the active layer, the local pH increases as trench width decreases. Computational models confirm these experimental results and also showed that the catalyst found within narrow trenches is more active than that found at the surface of the electrode. This study suggests that the overpotential required to perform selective CO2 reduction can be reduced by increasing the density of narrow trench regions in the microporous layer.

  PublisherOA PDFDOI

• Bicarbonate or Carbonate Processes for Coupling Carbon Dioxide Capture and Electrochemical Conversion

  ACS Energy Letters · 2020-03-03 · 134 citations

  article

  Designing a scalable system to capture CO₂ from the air and convert it into valuable chemicals, fuels, and materials could be transformational for mitigating climate change. Climate models predict that negative greenhouse gas emissions will be required by the year 2050 in order to stay below a 2 °C change in global temperature. The processes of CO₂ capture, CO₂ conversion, and finally product separation all require significant energy inputs; devising a system that simultaneously minimizes the energy required for all steps is an important challenge. To date, a variety of prototype or pilot-level CO₂ capture and/or conversion systems have been designed and built targeting the individual objectives of either capture or conversion. One approach has focused on CO₂ removal from the atmosphere and storage of pure pressurized CO₂. Other efforts have concentrated on CO₂ conversion processes, such as electrochemical reduction or fermentation. Only a few concepts or analyses have been developed for complete end-to-end processes that perform both CO₂ capture and transformation.

  PublisherDOI

• Band Edge Tailoring in Few-Layer Two-Dimensional Molybdenum Sulfide/Selenide Alloys

  The Journal of Physical Chemistry · 2020-01-01

  article

  Chemical alloying is a powerful approach to tune the electronic structure of semiconductors and has led to the synthesis of ternary and quaternary two-dimensional (2D) dichalcogenide semiconductor alloys (e.g., MoSSe₂, WSSe₂, etc.). To date, most of the studies have been focused on determining the chemical composition by evaluating the optical properties, primarily via photoluminescence and reflection spectroscopy of these materials in the 2D monolayer limit. However, a comprehensive study of alloying in multilayer films with direct measurement of electronic structure, combined with first-principles theory, is required for a complete understanding of this promising class of semiconductors. We have combined first-principles density functional theory calculations with experimental characterization of MoS₂₍₁₋ₓ₎Se₂ₓ (where x ranges from 0 to 1) alloys using X-ray photoelectron spectroscopy to evaluate the valence and conduction band edge positions in each alloy. Moreover, our observations reveal that the valence band edge energies for molybdenum sulfide/selenide alloys increase as a function of increasing selenium concentration. These experimental results agree well with the results of density functional theory calculations showing a similar trend in calculated valence band edges. Our studies suggest that alloying is an effective technique for tuning the band edges of transition-metal dichalcogenides, with implications for applications such as solar cells and photoelectrochemical devices.

  Publisher

Frequent coauthors

• Harry A. Atwater

  California Institute of Technology

  49 shared

• Giulia Tagliabue

  29 shared

• Wen‐Hui Cheng

  National Cheng Kung University

  26 shared

• Alex J. Welch

  California Institute of Technology

  25 shared

• Wei David Wei

  University of Florida

  15 shared

• Rengui Li

  Dalian National Laboratory for Clean Energy

  15 shared

• Jeffrey B. Neaton

  University of California, Berkeley

  15 shared

• Elizabeth A. Peterson

  Los Alamos National Laboratory

  13 shared

Labs

• DuChene LabPI

  Designs and creates nanostructured catalysts capable of sustainably synthesizing fuels and chemicals from readily abundant small molecules.