Reid

Electrolyte Immersion Increases Photoconductivity in a Model Polymer Photocathode

Daniel Morton — Mon, 28 Jul 2025 19:41:39 +0000

Electrolyte Immersion Increases Photoconductivity in a Model Polymer Photocathode Daniel Morton Mon, 07/28/2025 - 13:41

ACS ENERGY LETTERS, 2025, 10, 4019-4026

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Finding the On switch for more efficient light-driven chemistry

Daniel Morton — Mon, 07 Jul 2025 16:34:22 +0000

Finding the On switch for more efficient light-driven chemistry Daniel Morton Mon, 07/07/2025 - 10:34

Daniel Morton

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Collaboration led by RASEI members Obadiah Reid and Garry Rumbles solves a long-standing puzzle in important organic chemical transformation.

In the world of organic chemistry, making new molecules, the building blocks for everything from advanced electronic materials to pharmaceuticals, is a bit like being a chef. Chemists are always looking to improve the recipe, to make it faster, cheaper, more efficient, and produce less waste. In recent years one of the most exciting new ‘cooking techniques’ is nickel photocatalysis, which uses abundant, low-cost nickel and the power of light to enable chemists to build complex molecules under mild conditions.

This technique has emerged as something of a game-changer in building molecules, but it comes with a significant puzzle. The nickel catalyst, as it is normally added to a reaction, is in a dormant state (called a ‘pre-catalyst’). To get the reaction moving, the catalyst needs to be ‘woken up’. For years, scientists were not sure what the wake-up call was. The activation from pre-catalyst to the functioning catalyst was something of a black box, with numerous theories for what was happening. This led to the assumption that each reaction was unique, and each reaction required its own individual and complicated startup sequence. This has often required a lot of work to find the right ‘On switch’.

This collaborative study, led by RASEI researchers Obadiah Reid and Garry Rumbles at the National Renewable Energy Laboratory (NREL), brings together expertise from the SLAC National Accelerator Laboratory, Brookhaven National Laboratory, Argonne National Laboratory and Northeastern University. Together, the scientists have identified key features of the transformation from pre-catalyst to active catalyst. In the report, just published in Nature Communications, the team shows that there is a universal ‘On switch’ to start these powerful reactions, and the key to this transformation is light.

Imagine a high-tech machine delivered in a locked crate. You know that once you get it out and get it running, it can do amazing things, but you don’t have the key. For years, chemists were essentially trying to pick the lock in different ways every time they wanted to use it. This study describes a universal key for getting the crate open.

It was found that light, either directly, or transferred from another light-absorbing molecule, provide a jolt of energy that breaks a bond in the nickel pre-catalyst structure. This process, which is called photolysis, activates the nickel complex, getting it ready to do the chemistry. This initial step is something that has previously been proposed but never fully proven.

The team brought together a sophisticated array of tools to effectively investigate this mechanism, including incredibly fast laser systems that can watch chemical changes happen in fractions of a second. This allowed them to witness the ‘unlocking’ process in real-time and identify the exact sequence of events. They observed that after the initial light-induced bond breaking, the catalyst can then interact with molecules in the surrounding solvent, forming a temporary ‘reservoir’ that holds the catalyst in a state ready for the main reaction.

Building this body of evidence and developing these findings required a significant team effort, bringing together scientists from across the country, from multiple national labs and universities. RASEI Scientists at CU Boulder and NREL used advanced spectroscopy to track the catalyst’s behavior, while researchers at SLAC used high-powered X-rays to confirm changes in the structure of the nickel complex. This combination of knowledge and experience with cutting-edge instrumentation was essential in providing a complete understanding of these reactions begin.

Development of a unified explanation for how one of the most important tools in an organic chemist’s toolbox is initiated has important implications. Understanding this fundamental activation step allows chemists to move from guessing to designing. Not only does this support improvement in the activation of existing reactions, it also provides opportunities to design new transformations, all of which will streamline the manufacture of chemical commodities, such as pharmaceuticals and materials.

JULY 2025

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Photolytic activation of Ni(II)X2L explains how Ni-mediated cross coupling begins

Daniel Morton — Tue, 01 Jul 2025 17:11:39 +0000

Photolytic activation of Ni(II)X2L explains how Ni-mediated cross coupling begins Daniel Morton Tue, 07/01/2025 - 11:11

NATURE COMMUNICATIONS, 2025, 16, 5530

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Polymer nanoparticle photocatalysts realized in non-aqueous solvents

Daniel Morton — Thu, 22 May 2025 21:57:02 +0000

Polymer nanoparticle photocatalysts realized in non-aqueous solvents Daniel Morton Thu, 05/22/2025 - 15:57

SUSTAINABLE ENERGY & FUELS, 2025, 9, 14, 3796-3807

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Scientists move microscopic solar chemical factories out of water to unlock new transformations

Daniel Morton — Wed, 07 May 2025 16:42:05 +0000

Scientists move microscopic solar chemical factories out of water to unlock new transformations Daniel Morton Wed, 05/07/2025 - 10:42

Daniel Morton

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Four RASEI Fellows work together to expand the potential applications of nanoparticle photocatalysts

We all understand the power of the sun. We feel it on a hot summer’s day, we see it harnessed in solar panels that power our homes and cities. Chemical photocatalysis develops approaches to shrink that ability to harness this energy down to a molecular scale, and uses this energy to power chemical reaction, to power the building of important organic molecules, the foundations of pharmaceuticals, materials, and clean fuels.

One of the technologies used to harness light on the molecular level are a class of particles called organic nanoparticles (oNPs). Think of them as tiny, solar-powered factories, expertly designed to capture light and use its energy to drive chemical reactions. The oNPs are made from readily available earth-abundant materials, offering a cheap, clean, and sustainable alternative to a range of more traditional chemical reactions, which can often rely on rare, expensive metals that are hard to get hold of and can produce significant waste.

However, the oNPs, for all their potential as chemical factories, do have one significant limitation, they can only be built and operated in water. This is a fundamental roadblock. While water is essential for life, it is often a very poor environment for performing chemical reactions and can be very detrimental for the complex and delicate sequence of chemical transformations required for producing valuable products. The full power of these nano-factories was, quite literally, stuck in the water.

To understand this challenge, imagine that you have designed the world’s most efficient and powerful engine. It is a true engineering breakthrough, but it comes with a major catch, it can only run while completely submerged in the ocean. This is fine if you want to get around in a submarine, or a boat, but you can’t put it into a car, or a plane, or a generator on land, where you need it most. The potential of this new innovation is trapped, unable to be used for countless valuable applications.

That is similar to the situation faced by the researchers, led by RASEI Fellows Stephen Barlow, Seth Marder, Obadiah Reid and Garry Rumbles. The oNPs were confined to water-based reaction media, in order to realize their full potential the team needed to find a way to move these delicate ‘nano-factories’ from water to the ‘dry-land’ of other chemical environments, known as non-aqueous solvents, without the oNPs collapsing or breaking down.

This study describes a solution that the team developed. They devised a multi-step process to gently coax the oNPs out of their native water environment and prepare them to operate in different chemical solvents.

The process they developed is analogous to making salad dressing in the kitchen. It begins by mixing the water containing the nanoparticles with an oily substance (in this study oleic acid) and shaking it. This creates an emulsion, where tiny droplets of water are suspended in the oil, much like a vinaigrette. During this process the oNPs leave the water and move into the oil, which wraps around them like a protective coating. Finally the water is gently remove, leaving the oNPs safely suspended in their new oily environment. The protective layer formed around them allows them to be seamlessly transferred to a range of new non-aqueous solvents, ready to get to work.

A key part of this study was demonstrating that the oNP ‘factories’ were still functional after their transfer to new solvent systems. Using a suite of tools the team were able to confirm that the transferred oNPs could still absorb light and perform the chemical reactions.

With these findings the potential of the oNPs can be explored and expanded. It reveals new opportunities, not only in putting together organic molecules, but also in the synthesis of clean fuels, such as hydrogen.

MAY 2025

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Electrostatic Work Causes Unexpected Reactivity in Ionic Photoredox Catalysts in Low Dielectric Constant Solvents

Daniel Morton — Thu, 03 Apr 2025 20:25:22 +0000

Electrostatic Work Causes Unexpected Reactivity in Ionic Photoredox Catalysts in Low Dielectric Constant Solvents Daniel Morton Thu, 04/03/2025 - 14:25

THE JOURNAL OF PHYSICAL CHEMISTRY B, 2025, 129, 15, 3895-3901

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Synthesis and Characterization of Zintl-Phase BaCd2P2 Quantum Dots for Optoelectronic Applications

Daniel Morton — Mon, 24 Mar 2025 20:17:21 +0000

Synthesis and Characterization of Zintl-Phase BaCd2P2 Quantum Dots for Optoelectronic Applications Daniel Morton Mon, 03/24/2025 - 14:17

ACS NANO, 2025, 19, 12, 12345-12353

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(NH3(CH2)7NH3)2Sn3I10, a Vacancy-Ordered Three-Dimensional Tin(II) Perovskite-Derived Semiconductor

Daniel Morton — Wed, 19 Feb 2025 22:45:21 +0000

(NH3(CH2)7NH3)2Sn3I10, a Vacancy-Ordered Three-Dimensional Tin(II) Perovskite-Derived Semiconductor Daniel Morton Wed, 02/19/2025 - 15:45

CHEMISTRY OF MATERIALS, 2025, ASAP

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SPECS 2025 Annual Meeting

Daniel Morton — Wed, 12 Feb 2025 23:49:33 +0000

SPECS 2025 Annual Meeting Daniel Morton Wed, 02/12/2025 - 16:49

Daniel Morton

SPECS EFRC

In February of 2025 RASEI hosted the 2025 SPECS Annual Meeting, bringing together researchers from across the nation to discuss recent updates and plan future research.

The Center for Soft PhotoElectroChemical Systems, or SPECS, is a US Department of Energy funded Energy Frontiers Research Center. The focus of SPECS is to understand and develop organic polymers, so called soft materials, that can be used in transporting electrons, for applications in batteries, electronics, solar energy harvesting, and thermoelectrics.

Each year members of the Center, which include researchers from seven institutions across the United States, come together to discuss recent research discoveries and brainstorm new ideas to drive the field forward. Participants at this years meeting included representatives from CU Boulder, NREL, The University of Arizona, Emory University, University of Kentucky, Georgia Institute of Technology, and Stanford University.

The two day meeting was a great opportunity for the community to build relationships across the different institutes, present their research, and develop new ideas for future directions.

02/11/2025

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Free-Charge Carrier Generation in Homojunction Non-Polymeric Organic Semiconductor Films – The Role of the Optical Frequency Dielectric Constant

Daniel Morton — Thu, 21 Nov 2024 20:31:22 +0000

Free-Charge Carrier Generation in Homojunction Non-Polymeric Organic Semiconductor Films – The Role of the Optical Frequency Dielectric Constant Daniel Morton Thu, 11/21/2024 - 13:31

ADVANCED OPTICAL MATERIALS, 2025, 12, 36, 2401825

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