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DOE OSTI2024

An Advanced Cooling Device for Concentrated Photovoltaic Systems

Concentrated photovoltaics (CPV) have the potential to significantly enhance the energy conversion utilization of solar panels and reduce solar generation costs, making them a crucial area of advancement in solar power generation technology. However, the concentration of sunlight can lead to overheating of solar panels, resulting in a notable reduction in both the efficiency of solar power generation and the lifespan of the panels. This challenge remains the predominant technical hurdle that hinders the application of concentrated photovoltaic power generation technology. In this study, we propose a new cooling method for concentrated photovoltaic power generation systems via an integrated approach of incorporating Phase-Change Thermal Storage (PCTS) and Thermoelectric Generator (TEG) technology. This new method not only enhances the overall system's electricity generation efficiency but also effectively resolves the technical challenge of concentrated photovoltaic panel overheating issues, ensuring the continuity of concentrated photovoltaic power generation and extending the lifespan of solar panels and their components. In order to make full use of the wasted heat generated by photovoltaic power generation and effectively improve the power generation efficiency of the system, this work developed a phase change heat storage device based on a phase change material. This device uses the temperature difference between day and night to recover wasted heat from photovoltaic power generation. Through integration with the thermoelectric power generation system, thermal energy can be converted into electrical energy. In addition, the Peltier effect of thermoelectric materials is used to construct a photovoltaic panel overheating protection system, which significantly improves the reliability and service life of the system.

14 SOLAR ENERGY↗

DOE OSTI2020

Comparative study on the overall energy performance between photovoltaic and Low-E insulated glass units

In this report a novel semi-transparent building integrated photovoltaic (BIPV) laminate was developed and introduced in this paper. It was produced by cutting standard mono-crystalline silicon solar cells into small strips and then making electrical connections between each strip before laminating the cells between two layers of glass. The overall energy performance and energy saving potential of the BIPV insulated glass unit (IGU) under real world conditions were identified through a side by side comparative study. Compared to the reference IGU, the BIPV IGU had lower solar heat gain coefficient (SHGC) but much higher U-factor. The average HVAC electricity saving of the BIPV IGU was about 10% relative to the reference IGU. Daylighting measurement and analysis were carried out to evaluate the trade-offs associated with the BIPV IGU between daylight, glare, and lighting energy use. The results indicated that the BIPV IGU is better than the reference IGU in reducing discomfort glare. However, if the most conservative viewpoint near the window is used for the assessment, a lower transmittance BIPV IGU is required to bring the overall discomfort levels below the perceptible level. Lastly, the net energy saving potential associated with the novel BIPV IGU was identified based on the power, thermal and daylighting performance. On average, the BIPV IGU saved 16.8% of the total electricity use of the room. Further studies and improvement on the energy conversion efficiency of solar cells, the optimal transmittance as well as the thermal properties would make this technology more energy-efficient and affordable.

14 SOLAR ENERGY↗

DOE OSTI2024

Fundamental Science for Enhancing the Durability of Photoelectrodes for Solar Fuels Production

During the award period, we performed a series of investigations to address a key bottleneck in solar-driven fuel production, which is materials stability. Regardless of the activity of electrocatalysts or selectivity of products, or efficiency of the light absorbers, if the systems are not stable then there is no ultimate technological relevance for solar fuels production. Degradation of semiconductor photoelectrodes is a well-known, long-recognized impediment to implementation of practical stable solar fuels systems. Thus, we aimed to define the thermodynamics and kinetics of the (electro)chemical processes that underpin corrosion of semiconductor photoelectrodes. We also sought to develop protective coatings and kinetic control strategies to extend durability of semiconductor photoelectrodes.

14 SOLAR ENERGY↗

DOE OSTI2026

Development of Composite Photocatalyst Materials that are Highly Selective for Solar Hydrogen Production and their Evaluation in Z-Scheme Reactor Designs

The key technology gap preventing a vertically stacked dual-bed particle suspension reactor from achieving the DOE MYRD&D ultimate cost target for H 2 production remains the lack of materials in particle form factor that exhibit ≥10% solar-to-H 2 energy conversion (STH) efficiency as a suspension. Therefore, our project goals centered around strategies to increase the STH efficiency by enhancing photophysical properties of perovskite oxide particles including increased visible-light absorption, increased selectivity for electrocatalysis of the H 2 evolution reaction (HER) and the O 2 evolution reaction (OER) through development of ultrathin oxide coatings, correlating composition and structure to function, and improving understanding of multiscale transport and kinetic processes.

08 HYDROGEN↗

DOE OSTI2021

Comprehensive energy balance analysis of photon-enhanced thermionic power generation considering concentrated solar absorption distribution

The present article reports a comprehensive energy balance analysis of a photon-enhanced thermionic emission (PETE) device when it is used for concentrated solar power (CSP) generation. To this end, we consider a realistic PETE device composed of a boron-doped silicon emitter on glass and a phosphorus-doped diamond collector on tungsten separated by the interelectrode vacuum gap. Here, depth-dependent spectral solar absorption and its photovoltaic and photothermal energy conversion processes are rigorously calculated to predict the PETE power output and energy conversion efficiency. Our calculation predicts that when optimized, the power output of the considered PETE device can reach 1.6 W/cm 2 with the energy conversion efficiency of ~ 18% for 100× solar concentration, which is substantially lower than those predicted in previous works under ideal conditions. In addition, the photon-enhancement ratio is lower than 10 and decreases with the increasing solar concentration due to the photothermal heating of the emitter assembly, suggesting that PETE should be more suitable for lowto- medium CSP below ~ 100× concentration. These observations signify the importance of a rigorous energy balance analysis based on spectral and spatial solar absorption distribution for the accurate prediction of PETE power generation.

14 SOLAR ENERGY↗

DOE OSTI2022

Solar reduction of carbon dioxide on copper-tin electrocatalysts with energy conversion efficiency near 20%

Abstract Copper catalysts modified with tin have been demonstrated to be selective for the electroreduction of carbon dioxide to carbon monoxide. However, such catalysts require the precise control of tin loading amount. Here, we develop a copper/tin-oxide catalyst with dominant tin oxide surface being formed via a spontaneous exchange reaction between sputtered tin and copper oxide. Even though the surface of this catalyst is tin-rich, it achieves an excellent performance towards carbon monoxide production in a flow cell. This contrasts with copper/tin-oxide prepared via atomic layer deposition since it yields selectivity towards carbon monoxide only on a copper-rich surface. Mechanism studies reveal that the tin sites on the tin-rich copper/tin-oxide surface achieve a suitable binding with adsorbed carbon monoxide under the presence of copper. Powered by a triple-junction solar cell, the copper/tin-oxide based electrolyzer sets a new benchmark solar-to-chemical energy conversion efficiency of 19.9 percent with a Faradaic efficiency of 98.9 percent towards carbon monoxide under simulated standard air mass 1.5 global illumination.

14 SOLAR ENERGY↗

DOE OSTI2023

Chapter 14: Surface plasmon resonance enhanced artificial photosynthesis of chemical fuels for energy storage

Nanostructured noble metals such as Au, Ag, and Cu have interesting optical properties because of the oscillation motions of their surface electrons upon strong coupling with light under resonance conditions. This resonant oscillation motion of conduction electrons refers to surface plasmon resonance (SPR) and localized SPR (LSPR) when localized near the surface of a nanoparticle. The extinction spectrum of a solution of plasmonic nanoparticles has tunable wavelength responses from UV to NIR due to strong light scattering and absorption which are highly sensitive to the permittivity of the nanoparticles, their sizes and shapes, and chemical environment. Strong light scattering due to the LSPR of plasmonic nanoparticles creates a strong localized and far-field intensity capable of enhancing light absorption characteristics of a chromophore near a plasmonic surface. Engineering the chromophores’ radiative decay dynamics can be done by 1) increasing its radiative decay rate to increase its photoluminescence intensity and 2) increasing its nonradiative decay rates associated to direct charge transfer to the metal surface. Such interesting photophysical properties of a chromophore can be extended to other light-absorbing materials such as semiconductor thin films and nanostructures. This plasmonic effect on the photophysics of a light-absorbing material can be theoretically and experimentally validated. The phenomenon has also been applied to advanced optoelectronic devices such as organic light-emitting diodes (OLED)1 and organic photovoltaics (OPV).2-4 The local field created by the SPR can provide an intense EM field to enhance photoluminescence emission of an organic chromophore5-8 and Raman scattering of an organic molecule, and single-molecule Raman9-10 can be detected on specially designed LSPR substrate. (Figure 1 on SPR for energy) Recent studies suggest that LSPR can be incorporated in light-harvesting and conversion systems to increase energy conversion in a solar cell and photoelectrochemical cell and chemical transformations of CO2 to chemical fuels.11-12 Plasmonic active metals naturally exhibit catalytic activities for electrochemical fuel conversion that can be enhanced by engineering their structures to form unique catalytic structures such as symmetry-broken Au-Cu Janus nanocrystals.13 These studies are critical to addressing the global challenges of energy14-15 and CO2 emission from nonrenewable sources such as coal, petroleum, and natural gas.16-17 Electrochemical systems comprised of unique photonic structures and functions that enable efficient and affordable energy harvesting/conversion/storage are highly desired for providing safe and environment-friendly energy sources. This chapter reviews our recent work of LSPR enabled photoelectrochemical water splitting and recent advances in LSPR-enabled CO2 reduction and photochemical reactions reported in the literature. Scientific and technical challenges of applying LSPR to enhance these energy conversion and storage systems are discussed at the conclusion of this chapter.

Pan, Shanlin↗

DOE OSTI2022

De novo protein design of photochemical reaction centers

Abstract Natural photosynthetic protein complexes capture sunlight to power the energetic catalysis that supports life on Earth. Yet these natural protein structures carry an evolutionary legacy of complexity and fragility that encumbers protein reengineering efforts and obfuscates the underlying design rules for light-driven charge separation. De novo development of a simplified photosynthetic reaction center protein can clarify practical engineering principles needed to build new enzymes for efficient solar-to-fuel energy conversion. Here, we report the rational design, X-ray crystal structure, and electron transfer activity of a multi-cofactor protein that incorporates essential elements of photosynthetic reaction centers. This highly stable, modular artificial protein framework can be reconstituted in vitro with interchangeable redox centers for nanometer-scale photochemical charge separation. Transient absorption spectroscopy demonstrates Photosystem II-like tyrosine and metal cluster oxidation, and we measure charge separation lifetimes exceeding 100 ms, ideal for light-activated catalysis. This de novo-designed reaction center builds upon engineering guidelines established for charge separation in earlier synthetic photochemical triads and modified natural proteins, and it shows how synthetic biology may lead to a new generation of genetically encoded, light-powered catalysts for solar fuel production.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Plasma-Initiated Graft Polymerization of Acrylic Acid onto Fluorine-Doped Tin Oxide as a Platform for Immobilization of Water-Oxidation Catalysts

The discovery of new and versatile strategies for the immobilization of molecular water-oxidation catalysts (WOCs) is crucial for developing clean energy conversion devices [e.g., (photo)electrocatalytic cells for water splitting]. The traditional approach for surface attachment to transparent conductive oxides [e.g., fluorine doped tin oxide (FTO)] is via synthetic modification of the ligand architecture to incorporate functional groups such as carboxylic acids (-COOH) or phosphonates (-PO 3 H 2 ) prior to immobilization. However, challenges arising from desorption and the cumbersome derivatizations steps have limited the scope and applications of surface-bound WOCs. Herein, we report the successful immobilization of underivatized Ru(II)-based WOCs (Ru–Cat1 = [Ru(tpy) (bpy) (H 2 O)] 2+ (tpy = 2,2':6'2"–terpyridine and bpy = 2,2;-bipyridine) and Ru–Cat2 = [Ru(Mebimpy) (bpy) (H 2 O)] 2+ (Mebimpy = 2,6-bis(1-methylbenzimidazol-2-yl) pyridine)) and the Ru(II) polypyridyl chromophore Ru–C3 = [Ru(bpy) 3 ] 2+ onto a FTO plasma-grafted poly(acrylic acid) surface (PAA|FTO). Various characterization techniques such as attenuated total reflectance Fourier transform infrared spectroscopy, scanning electron microscopy, atomic force microscopy, and cyclic voltammetry measurements provide evidence for the plasma-induced grafted PAA|FTO film and immobilization. Surface stability and electrocatalytic properties of these new hybrid composite films upon cycling were investigated at different pH values. Immobilized Ru–Cat1 and Ru–Cat2 onto PAA|FTO displayed pH-dependent (RuIII/RuII) couples and onset potentials indicative of PCET (proton-coupled electron transfer) reactions. Based on cyclic voltammetry results and spectroscopic monitoring, the immobilized WOCs Ru–Cat1 and Ru–Cat2 exhibited a higher surface stability in neutral aqueous solutions relative to Ru–C3 upon electrochemical oxidation. Furthermore, we attribute the surface PCET and stability to the presence of a water ligand in the coordination sphere of immobilized Ru–Cat1 and Ru–Cat2 which can H-bond with negatively charged carboxylate groups of the cross-linked PAA brushes. Our findings demonstrate that the plasma-grafted polymeric network onto FTO offers a versatile platform to directly anchor unmodified homogeneous WOCs or chromophores for potential applications in solar-to-fuel energy conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Theory and Simulation of Metal–Insulator–Semiconductor (MIS) Photoelectrodes

A metal–insulator–semiconductor (MIS) structure is an attractive photoelectrode-catalyst architecture for promoting photoelectrochemical reactions, such as the formation of H 2 by proton reduction. The metal catalyzes the generation of H 2 using electrons generated by photon absorption and charge separation in the semiconductor. The insulator layer between the metal and the semiconductor protects the latter element from photo-corrosion and, also, significantly impacts the photovoltage at the metal surface. Understanding how the insulator layer determines the photovoltage and what properties lead to high photovoltages is critical to the development of MIS structures for solar-to-chemical energy conversion. Herein, we present a continuum model for charge-carrier transport from the semiconductor to the metal with an emphasis on mechanisms of charge transport across the insulator. The polarization curves and photovoltages predicted by this model for a Pt/HfO 2 /p-Si MIS structure at different HfO 2 thicknesses agree well with experimentally measured data. The simulations reveal how insulator properties (i.e., thickness and band structure) affect band bending near the semiconductor/insulator interface and how tuning them can lead to operation closer to the maximally attainable photovoltage, the flat-band potential. This phenomenon is understood by considering the change in tunneling resistance with insulator properties. The model shows that the best MIS performance is attained with highly symmetric semiconductor/insulator band offsets (e.g., BeO, MgO, SiO 2 , HfO 2 , or ZrO 2 deposited on Si) and a low to moderate insulator thickness (e.g., between 0.8 and 1.5 nm). Beyond 1.5 nm, the density of filled interfacial trap sites is high and significantly limits the photovoltage and the solar-to-chemical conversion rate. These conclusions are true for photocathodes and photoanodes. This understanding provides critical insight into the phenomena enhancing and limiting photoelectrode performance and how this phenomenon is influenced by insulator properties. The study gives guidance toward the development of next-generation insulators for MIS structures that achieve high performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

An Advanced Cooling Device for Concentrated Photovoltaic Systems

Gou, Yimeng↗

DOE OSTI2022

Rational design of photosynthetic reaction center protein maquettes

New technologies for efficient solar-to-fuel energy conversion will help facilitate a global shift from dependence on fossil fuels to renewable energy. Nature uses photosynthetic reaction centers to convert photon energy into a cascade of electron-transfer reactions that eventually produce chemical fuel. The design of new reaction centers de novo deepens our understanding of photosynthetic charge separation and may one day allow production of biofuels with higher thermodynamic efficiency than natural photosystems. Recently, we described the multi-step electron-transfer activity of a designed reaction center maquette protein (the RC maquette), which can assemble metal ions, tyrosine, a Zn tetrapyrrole, and heme into an electron-transport chain. Here, we detail our modular strategy for rational protein design and show that the intended RC maquette design agrees with crystal structures in various states of assembly. A flexible, dynamic apo-state collapses by design into a more ordered holo-state upon cofactor binding. Crystal structures illustrate the structural transitions upon binding of different cofactors. Spectroscopic assays demonstrate that the RC maquette binds various electron donors, pigments, and electron acceptors with high affinity. We close with a critique of the present RC maquette design and use electron-tunneling theory to envision a path toward a designed RC with a substantially higher thermodynamic efficiency than natural photosystems.

09 BIOMASS FUELS↗

DOE OSTI2022

Protonic Ceramics for Energy Storage & Electricity Generation with Ammonia (Final Report)

The commercial product resulting from this R&D project will enable cost-effective synthesis of the Carbon Neutral Liquid Fuel (CNLF) ammonia, a common chemical, at a small scale for energy and industrial applications using only intermittent renewable energy, water, and air as feedstocks. These products are also capable of producing electrical energy from the CNLF in a fuel cell mode of operation. Thus, the eventual commercial product enables both single direction production of either CLNF or electricity, or alternatively functions as a fully reversible, self-contained energy storage device. The renewed interest in developing electrolysis systems is driven, in part, by the burgeoning renewable, solar, and wind industries and the need for an energy conversion and storage technology that can convert intermittent solar and wind energy into the production of hydrogen. Electrolysis systems integrated into both distributed and central renewable power plants would utilize solar and wind energy as their primary power source to produce renewably generated hydrogen for local energy storage or chemical feedstock purposes. Ammonia is an excellent surrogate for hydrogen transportation. NH3 presents an attractive alternative to hydrogen as a working fluid in reversible devices towards a sustainable green energy-oriented future. Ammonia can be easily liquefied at room temperature at about 8 bar or at -33°C at ambient pressure. In contrast, the liquefaction temperature of hydrogen is -253°C at ambient pressure. NH3 has a significantly higher volumetric energy density (12.7 MJ/L) than compressed hydrogen (4.5 MJ/L at ~70 MPa) or liquefied hydrogen (8.5 MJ/L). Additionally, ammonia is a widely used raw material for agriculture fertilizer and thus has well-established storage, transport, and handling processes (about 180 million tons of ammonia are produced annually). Techno-economic analysis suggests ammonia is the least expensive fuel among hydrogen, gasoline, natural gas, liquefied petroleum gas, and methanol.

08 HYDROGEN↗

DOE OSTI2025

Sequential Infiltration Synthesis of Cadmium Sulfide Discrete Atom Clusters

Abstract Exposure of soft material templates to alternating volatile chemical precursors can produce inorganic deposition within the permeable template (e.g. a polymer thin film) in a process akin to atomic layer deposition (ALD). While such sequential infiltration synthesis (SIS) processes have now been demonstrated for many metal oxides, we report an SIS process for a transition metal sulfide – CdS. Gas phase dimethyl cadmium and hydrogen sulfide precursors infiltrated into poly(4‐vinylpyridine) thin films result in the 3D‐nucleation of clusters consistent with a cubane‐type Cd 4 S 4 core that are variably terminated with methyl, thiol and hydroxy capping ligands. First principles models and simulation of few‐atom Cd‐based clusters are consistent with electronic and vibrational spectroscopy and grazing‐incidence total X‐ray scattering measurements of 3D‐cluster‐arrays synthesized at 80 °C. The direct synthesis of few‐atom transition metal sulfide clusters within polymer thin films will provide a versatile new route to precision architectures for light‐absorbing materials including solar energy harvesting and conversion applications.

Jayaweera, Nuwanthaka P. [Material Science Divisio↗

DOE OSTI2025

Sequential Infiltration Synthesis of Cadmium Sulfide Discrete Atom Clusters

Exposure of soft material templates to alternating volatile chemical precursors can produce inorganic deposition within the permeable template (e.g. a polymer thin film) in a process akin to atomic layer deposition (ALD). While such sequential infiltration synthesis (SIS) processes have now been demonstrated for many metal oxides, we report an SIS process for a transition metal sulfide – CdS. Gas phase dimethyl cadmium and hydrogen sulfide precursors infiltrated into poly(4-vinylpyridine) thin films result in the 3D-nucleation of clusters consistent with a cubane-type Cd 4 S 4 core that are variably terminated with methyl, thiol and hydroxy capping ligands. First principles models and simulation of few-atom Cd-based clusters are consistent with electronic and vibrational spectroscopy and grazing-incidence total X-ray scattering measurements of 3D-cluster-arrays synthesized at 80 °C. The direct synthesis of few-atom transition metal sulfide clusters within polymer thin films will provide a versatile new route to precision architectures for light-absorbing materials including solar energy harvesting and conversion applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Effects of Anionic Polymer Modification of Dye‐Sensitized Niobate Photocatalysts on Solar‐Driven Z‐Scheme Overall Water Splitting

Pt‐intercalated calcium niobate nanosheets (Pt/HCa 2 Nb 3 O 10 ) sensitized by a Ru(II) complex dye are good photocatalysts for producing H 2 from aqueous solutions containing I − as a reversible electron donor. These materials are applicable to Z‐scheme overall water splitting in combination with a WO 3 ‐based O 2 ‐evolving photocatalyst under simulated sunlight. In this work, the effects of anionic polymer modification of the dye‐sensitized nanosheets are examined by adsorbing sodium poly(styrenesulfonate) (PSS), sodium polyacrylate, sodium polymethacrylate (PMA), or sodium poly(4‐styrenesulfonic‐ co ‐maleic acid) onto the dye‐sensitized nanosheet surface. For half‐cell H 2 ‐evolution reaction in the presence of NaI, all of the polymers have a positive impact on the activity under visible light at lower light intensity, whereas only PMA is effective under high light‐intensity condition. For Z‐scheme overall water splitting with PtO x /H‐Cs‐WO 3 , PSS and PMA give almost the same solar‐to‐hydrogen energy conversion efficiencies (0.12% ± 0.01%) under optimized conditions. However, PMA operates better than PSS at relatively low and high NaI concentrations, which are in general disadvantageous for the H 2 ‐ and O 2 ‐evolving components of the Z‐scheme, respectively.

Energy & Fuels↗

DOE OSTI2023

Effects of Anionic Polymer Modification of Dye‐Sensitized Niobate Photocatalysts on Solar‐Driven Z‐Scheme Overall Water Splitting

In article number 2300629, Mallouk, Maeda and co-workers report that a surface modification of a dye-sensitized calcium niobate nanosheet photocatalyst with anionic polymers such as sodium polymethacrylate improves the activity for solar water splitting, giving a maximum solar-to-hydrogen energy conversion efficiency of 0.12±0.01% and an apparent quantum yield of 5.1% at 420 nm.

Yamamoto, Haruka↗

DOE OSTI2023

Ferroelectric Polarization in BaTiO 3 Nanocrystals Controls Photoelectrochemical Water Oxidation and Photocatalytic Hydrogen Evolution

Ferroelectric (FE) semiconductors such as BaTiO 3 support a remnant polarization after the application of an electric field that can promote the separation of photogenerated charge carriers. Here, we demonstrate FE-enhanced photocatalytic hydrogen evolution and photoelectrochemical water oxidation with barium titanate nanocrystals for the first time. Nanocrystals of the ferroelectric tetragonal structure type were obtained by a hydrothermal synthesis from TiO 2 and barium hydroxide in 63% yield. BaTiO 3 nanocrystal films on tantalum substrates exhibit water oxidation photocurrents of 0.141 mA cm –2 at 1.23 V RHE under UV light (60 mW cm –2 ) illumination. Electric polarization at 52.8 kV cm –1 normal to the film plane increases the photocurrent by a factor of 2 or decreases it by a factor of 3.5, depending on the field polarity. It also shifts the onset potential by –0.15 or +0.09 V and it modifies the surface photovoltage signal. Lastly, exposure to an electric field increases the H 2 evolution rate of Pt/BaTiO 3 by a factor of ~1.5, and it raises the selectivity of photodeposition of silver onto the (001) facets of the nanocrystal. All FE enhancements can be removed by heating samples above the Curie temperature of BaTiO 3 . Furthermore, these findings can be explained by FE dipole-induced changes to the potential drop across the space charge layer of the material. The ability to use the ferroelectric effect to enhance hydrogen evolution and water oxidation is of potential interest for the development of improved solar energy for fuel conversion systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗