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DOE OSTI2025

Fundamental Research Aimed at Diverting Excess Reducing Power in Photosynthesis to Orthogonal Metabolic Pathways

Photosystems are incredible biological machines that use sunlight to drive the conversion of carbon dioxide to sugar. The amount of sunlight available for photosynthesis sometimes exceeds the amount of energy plants can use. This excess energy has to be safely dissipated through non-productive biological processes. The ultimate goal of this project is to understand whether we can utilize that otherwise unused excess energy. In our previous work, we showed that, in principle, it is possible to attach a catalyst to photosystem I and generate H2 using light. Our current strategy is to genetically fuse parts of the photosystem I complex with a recently discovered oxygen-tolerant [FeFe] hydrogenase. Our rationale is that such chimeric proteins may potentially result in the natural incorporation of the photosystem I-hydrogenase link using the inherent genetic machinery of the cell. In this project, we aim to verify that light-driven hydrogen production in this construction is possible. Throughout the project, we designed nanoconstructs that showcase the plausibility of this technology, at least in vitro. We take advantage of these constructs to investigate details of the coupling between photosystem I and a H2-producing enzyme called [FeFe] hydrogenase. This part of the project reveals details of the electron transfer between photosystem I and the attached hydrogenase, providing information that can lead to new strategies for improved biological photocatalysis. We also researched efficient and robust tethering of the [FeFe] hydrogenase to photosystem I in cyanobacteria. This work will highlight successful design strategies to guide the future development of photosynthetic biohybrids. Uncovering the principles governing the utilization of otherwise unusable energy significantly further our understanding of cyanobacterial photosynthesis. The work proposed establishes the feasibility of diverting excess energy under high light conditions to orthogonal enzymatic pathways and set design rules for efficient utilization of such a strategy for scientific and industrial applications in biosensing, renewable energy, and high-value chemicals production. The work addresses the DOE-BES Photosynthetic Systems program goal to develop a multidimensional understanding of photosystems that would provide specific metrics that instruct strategies for improving biological photosynthesis and for guiding the future development of bioreactors and biomimetic energy systems.

Photosynthetic systems, hydrogenase, cyanobacteria↗

DOE OSTI2022

Triggering cell death in cancers using self-illuminating nanocomposites

Bioinspired photocatalysis has resulted in efficient solutions for many areas of science and technology spanning from solar cells to medicine. Here we show a new bioinspired semiconductor nanocomposite (nanoTiO 2 DOPA-luciferase, TiDoL) capable of converting light energy within cancerous tissues into chemical species that are highly disruptive to cell metabolism and lead to cell death. This localized activity of semiconductor nanocomposites is triggered by cancer-generated activators. Adenosine triphosphate (ATP) is produced in excess in cancer tissues only and activates nearby immobilized TiDoL composites, thereby eliminating its off-target toxicity. The interaction of TiDoL with cancerous cells was probed in situand in real-time to establish a detailed mechanism of nanoparticle activation, triggering of the apoptotic signaling cascade, and finally, cancer cell death. Activation of TiDoL with non-cancerous cells did not result in cell toxicity. Exploring the activation of antibody-targeted semiconductor conjugates using ATP is a step toward a universal approach to single-cell-targeted medical therapies with more precision, efficacy, and potentially fewer side effects.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2020

Atmospheric Pressure Plasma Deposition of TiO2: A Review

Atmospheric pressure plasma (APP) deposition techniques are useful today because of their simplicity and their time and cost savings, particularly for growth of oxide films. Among the oxide materials, titanium dioxide (TiO2) has a wide range of applications in electronics, solar cells, and photocatalysis, which has made it an extremely popular research topic for decades. Here, we provide an overview of non-thermal APP deposition techniques for TiO2 thin film, some historical background, and some very recent findings and developments. First, we define non-thermal plasma, and then we describe the advantages of APP deposition. In addition, we explain the importance of TiO2 and then describe briefly the three deposition techniques used to date. We also compare the structural, electronic, and optical properties of TiO2 films deposited by different APP methods. Lastly, we examine the status of current research related to the effects of such deposition parameters as plasma power, feed gas, bias voltage, gas flow rate, and substrate temperature on the deposition rate, crystal phase, and other film properties. The examples given cover the most common APP deposition techniques for TiO2 growth to understand their advantages for specific applications. In addition, we discuss the important challenges that APP deposition is facing in this rapidly growing field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Fabrication of High Surface Area Microporous ZnO from ZnO/Carbon Sacrificial Composite Monolith Template

Fabrication of porous materials from the standard sacrificial template method allows metal oxide nanostructures to be produced and have several applications in energy, filtration and constructing sensing devices. However, the low surface area of these nanostructures is a significant drawback for most applications. Here, we report the synthesis of ZnO/carbon composite monoliths in which carbon is used as a sacrificial template to produce zinc oxide (ZnO) porous nanostructures with a high specific surface area. The synthesized porous oxides of ZnO with a specific surface area of 78 m2/g are at least one order of magnitude higher than that of the ZnO nanotubes reported in the literature. The crucial point to achieving this remarkable result was the usage of a novel ZnO/carbon template where the carbon template was removed by simple heating in the air. As a high surface area porous nanostructured ZnO, these synthesized materials can be useful in various applications including catalysis, photocatalysis, separation, sensing, solar energy harvest and Zn-ion battery and as supercapacitors for energy storage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1977

Mars - Photodesorption from mineral surfaces and its effects on atmospheric stability

Kinetic constraints are employed to identify the reactive chemisorbed complexes, to describe the mechanism of UV-accelerated desorption from Fe (+2) on mineral surfaces, and to estimate the photodesorption rate on Mars. In particular, it is proposed that gases such as O2, CO2, CO, H2O and N2 undergo an adsorption-desorption process at octahedrally coordinated Fe (+2) surface sites to produce seven-coordinate transition-state complexes. The ligand field stabilization energy acquired by these complexes lies between 16 and 18 kcal per mole. Published photocatalysis data are used to assess the role of photodesorption in Martian atmospheric chemistry and stability.

Huguenin, R. L.↗

NASA NTRS1979

Future production of hydrogen from solar energy and water - A summary and assessment of U.S. developments

The paper examines technologies of hydrogen production. Its delivery, distribution, and end-use systems are reviewed, and a classification of solar energy and hydrogen production methods is suggested. The operation of photoelectric processes, biophotolysis, photocatalysis, photoelectrolysis, and of photovoltaic systems are reviewed, with comments on their possible hydrogen production potential. It is concluded that solar hydrogen derived from wind energy, photovoltaic technology, solar thermal electric technology, and hydropower could supply some of the hydrogen for air transport by the middle of the next century.

Hanson, J. A.↗

NASA NTRS1982

A study of the photocatalytic effects of aqueous suspensions of platinized semiconductor materials on the reaction rates of candidate redox reactions

The effectiveness of powdered semiconductor materials in photocatalyzing candidate redox reactions was investigated. The rate of the photocatalyzed oxidation of cyanide at platinized TiO2 was studied. The extent of the cyanide reaction was followed directly using an electroanalytical method (i.e. differential pulse polarography). Experiments were performed in natural or artificial light. A comparison was made of kinetic data obtained for photocatalysis at platinized powders with rate data for nonplatinized powders.

Miles, A. M.↗

NASA NTRS1992

Heterogeneous photocatalytic oxidation of atmospheric trace contaminants

A two year study to examine the feasibility of using heterogeneous photocatalysis for spacecraft air purification was begun at North Carolina State University on November 1, 1990. The original grant proposal included examination of the rates of destruction of anticipated spacecraft-generated air contaminants, including alcohols, aldehydes, chlorinated compounds, as well as trace levels of volatile compounds containing nitrogen, sulfur, and silicon. The progress made in the second six month period of 5/1/91-11/1/91 is discussed.

Ollis, David F.↗

NASA NTRS2009

Measuring the Photocatalytic Breakdown of Crystal Violet Dye using a Light Emitting Diode Approach

A simple method to estimate the photocatalytic reactivity performance of spray-on titanium dioxide coatings for transmissive glass surfaces was developed. This novel technique provides a standardized method to evaluate the efficiency of photocatalytic material systems over a variety of illumination levels. To date, photocatalysis assessments have generally been conducted using mercury black light lamps. Illumination levels for these types of lamps are difficult to vary, consequently limiting their use for assessing material performance under a diverse range of simulated environmental conditions. This new technique uses an ultraviolet (UV) gallium nitride (GaN) light emitting diode (LED) array instead of a traditional black light to initiate and sustain photocatalytic breakdown. This method was tested with a UV-resistant dye (crystal violet) applied to a titanium dioxide coated glass slide. Experimental control is accomplished by applying crystal violet to both titanium dioxide coated slides and uncoated control slides. A slide is illuminated by the UV LED array, at various light levels representative of outdoor and indoor conditions, from the dye side of the slide. To monitor degradation of the dye over time, a temperature-stabilized white light LED, whose emission spectrum overlaps with the dye absorption spectrum, is used to illuminate the opposite side of the slide. Using a spectrometer, the amount of light from the white light LED transmitted through the slide as the dye degrades is monitored as a function of wavelength and time and is subsequently analyzed. In this way, the rate of degradation for photocatalytically coated versus uncoated slide surfaces can be compared. Results demonstrate that the dye absorption decreased much more rapidly on the photocatalytically coated slides than on the control uncoated slides, and that dye degradation is dependent on illumination level. For photocatalytic activity assessment purposes, this experimental configuration and methodology minimizes many external variable effects and enables small changes in absorption to be measured. This research also compares the advantages of this innovative LED light source design over traditional mercury black light systems and non- LED lamp approaches. This novel technology begins to address the growing need for a standard method that can assess the performance of photocatalytic materials before deployment for large scale, real world use.

Ryan, Robert E.↗

NASA NTRS2009

An LED Approach for Measuring the Photocatalytic Breakdown of Crystal Violet Dye

A simple technique to assess the reactivity of photocatalytic coatings sprayed onto transmissive glass surfaces was developed. This new method uses ultraviolet (UV) gallium nitride (GaN) light-emitting diodes (LEDs) to drive a photocatalytic reaction (the photocatalytic breakdown of a UV-resistant dye applied to a surface coated with the semiconductor titanium dioxide); and then a combination of a stabilized white light LED and a spectrometer to track the dye degradation as a function of time. Simple, standardized evaluation techniques that assess photocatalytic materials over a variety of environmental conditions, including illumination level, are not generally available and are greatly needed prior to in situ application of photocatalytic technologies. To date, much research pertaining to this aspect of photocatalysis has been limited and has focused primarily on laboratory experiments using mercury lamps. Mercury lamp illumination levels are difficult to control over large ranges and are temporally modulated by line power, limiting their use in helping to understand and predict how photocatalytic materials will behave in natural environmental settings and conditions. The methodology described here, using steady-state LEDs and time series spectroradiometric techniques, is a novel approach to explore the effect of UV light on the photocatalytic degradation of a UV resistant dye (crystal violet). GaN UV LED arrays, centered around 365 nm with an adjustable DC power supply, are used to create a small, spatially uniform light field where the steady state light level can be varied over three to four orders of magnitude. For this study, a set of glass microscope slides was custom coated with a thinly sprayed layer of photocatalytic titanium dioxide. Crystal violet was then applied to these titanium-dioxide coated slides and to uncoated control slides. The slides were then illuminated at various light levels from the dye side of the slide by the UV LED array. To monitor dye degradation on the slides over time, a temperature-stabilized white light LED was used to illuminate the opposite side of the slides. As the dye degraded, the amount of light from the white light LED transmitted through the slide was monitored with a spectrometer and subsequently analyzed to determine and compare the rate of dye degradation for photocatalytically coated versus uncoated slide surfaces. The long-term stability of the spectrometer/white light LED combination, which required only a single reference spectra to be taken for a time series sequence of several hours, enabled accurate measurements of transmitted light over time. Time series transmission curves were generated and results demonstrated that over time the transmission increased much more rapidly on the coated slides than on the control slides. This experimental configuration and methodology for photocatalytic activity measurement minimizes many external variable effects and allows low light level studies to be performed. This study also compares the advantages of this novel LED light source design to traditional mercury lamp systems and non-LED lamp approaches that have conventionally been used. The methodology and experimental design research summarized in this abstract is partly funded by the Department of Homeland Security, Science and Technology Directorate, and by the NASA Stennis Space Center Innovative Partnerships Program.

Ryan, Robert E.↗

NASA NTRS2007

Photocatalytic/Magnetic Composite Particles

Photocatalytic/magnetic composite particles have been invented as improved means of exploiting established methods of photocatalysis for removal of chemical and biological pollutants from air and water. The photocatalytic components of the composite particles are formulated for high levels of photocatalytic activity, while the magnetic components make it possible to control the movements of the particles through the application of magnetic fields. The combination of photocatalytic and magnetic properties can be exploited in designing improved air- and water treatment reactors.

Wu, Chang-Yu↗

NASA NTRS2011

Radiation-Resistant Hybrid Lotus Effect for Achieving Photoelectrocatalytic Self-Cleaning Anticontamination Coatings

An experiment involving radiation-resistant hydrophobic coatings is planned for space exposure and experimental testing on the International Space Station (ISS) in 2011. The Lotus biocide coatings are designed for supporting space exploration missions. This innovation is an antibacterial, anti-contamination, and self-cleaning coating that uses nano-sized semiconductor semimetal oxides to neutralize biological pathogens and toxic chemicals, as well as to mitigate dust accumulation (see figure). The Lotus biocide coating is thin (approximately microns thick), lightweight, and the biocide properties will not degrade with time or exposure to biological or chemical agents. The biocide is stimulated chemically (stoichiometric reaction) through exposure to light (photocatalysis), or by an applied electric field (electrocatalysis). The hydrophobic coating samples underwent preliminary high-energy proton and alpha-ray (helium ion) irradiations at the Lawrence Berkeley National Laboratory 88" cyclotron and demonstrated excellent radiation resistance for a portion of the Galactic Cosmic Ray (GRC) and Solar Proton spectrum. The samples will undergo additional post-flight studies when returned to Earth to affirm further the radiation resistance properties of the space exposed coatings.

Taylor, Edward W.↗

NASA NTRS2012

Visible Light Responsive Catalysts Using Quantum Dot-Modified Ti02 for Air and Water Purification

The method of photocatalysis utilizing titanium dioxide, TiO2, as the catalyst has been widely studied for trace contaminant control for both air and water applications because of its low energy consumption and use of a regenerable catalyst. Titanium dioxide requires ultraviolet light for activation due to its band gap energy of 3.2 eV. Traditionally, Hg-vapor fluorescent light sources are used in PCO reactors and are a setback for the technology for space application due to the possibility of Hg contamination. The development of a visible light responsive (VLR) TiO2-based catalyst could lead to the use of solar energy in the visible region (approx.45% of the solar spectrum lies in the visible region; > 400 nm) or highly efficient LEDs (with wavelengths > 400 nm) to make PCO approaches more efficient, economical, and safe. Though VLR catalyst development has been an active area of research for the past two decades, there are few commercially available VLR catalysts; those that are available still have poor activity in the visible region compared to that in the UV region. Thus, this study was aimed at the further development of VLR catalysts by a new method - coupling of quantum dots (QD) of a narrow band gap semiconductor (e.g., CdS, CdSe, PbS, ZnSe, etc.) to the TiO2 by two preparation methods: 1) photodeposition and 2) mechanical alloying using a high-speed ball mill. A library of catalysts was developed and screened for gas and aqueous phase applications, using ethanol and 4-chlorophenol as the target contaminants, respectively. Both target compounds are well studied in photocatalytic systems serve as model contaminants for this research. Synthesized catalysts were compared in terms of preparation method, type of quantum dots, and dosage of quantum dots.

Coutts, Janelle L.↗

NASA NTRS2013

Studying the Use of Photocatalytic Coatings to Increase Building/Structure Sustainability and Cleanliness at NASA Stennis Space Center

TiO2 coated surfaces demonstrated both visually through photographic representation, and quantitatively, through reflectance measurements that they improved upon the current state of cleanliness upon the surfaces that they were applied to. TiO2 has the potential to both maintain and increase building s sustainability and the overall appearance of cleanliness TiO2 coated slides degraded soot under UV light compared to soot samples on plain uncoated slides under the same conditions Degradation of soot by photocatalysis was far more apparent than degradation of soot by UV light alone This demonstration provides the foundation for a laboratory model that could be used to simulate real world applications for photocatalytic materials Additional research is required to better understand the full potential of TiO2

Underwood, Lauren↗

NASA NTRS2014

Visible-Light-Responsive Catalysts Using Quantum Dot-Modified TiO2 for Air and Water Purification

Photocatalysis, the oxidation or reduction of contaminants by light-activated catalysts, utilizing titanium dioxide (TiO2) as the catalytic substrate has been widely studied for trace contaminant control in both air and water applications. The interest in this process is due primarily to its low energy consumption and capacity for catalyst regeneration. Titanium dioxide requires ultraviolet light for activation due to its relatively large band gap energy of 3.2 eV. Traditionally, Hg-vapor fluorescent light sources are used in PCO reactors; however, the use of mercury precludes the use of this PCO technology in a spaceflight environment due to concerns over crew Hg exposure. The development of a visible-light responsive (VLR) TiO2-based catalyst would eliminate the concerns over mercury contamination. Further, VLR development would allow for the use of ambient visible solar radiation or highly efficient LEDs, both of which would make PCO approaches more efficient, flexible, economical, and safe. Though VLR catalyst development has been an active area of research for the past two decades, there are few commercially available VLR catalysts. Those VLR catalysts that are commercially available do not have adequate catalytic activity, in the visible region, to make them competitive with those operating under UV irradiation. This study was initiated to develop more effective VLR catalysts through a novel method in which quantum dots (QD) consisting of narrow band gap semiconductors (e.g., CdS, CdSe, PbS, ZnSe, etc.) are coupled to TiO2 via two preparation methods: 1) photodeposition and 2) mechanical alloying using a high-speed ball mill. A library of catalysts was developed and screened for gas and aqueous phase applications using ethanol and 4-chlorophenol as the target contaminants, respectively. Both target compounds are well studied in photocatalytic systems and served as model contaminants for this research. Synthesized catalysts were compared in terms of preparation method, nature of the quantum dots, and dosage of quantum dots.

visible light↗

NASA NTRS2014

Visible-Light Responsive Catalysts Using Quantum Dot-Modified TiO2 for Air and Water Purification

visible light↗

NASA NTRS2015

Visible-Light-Responsive Catalyst Development for Volatile Organic Carbon Remediation Project

Photocatalysis is a process in which light energy is used to 'activate' oxidation/reduction reactions. Unmodified titanium dioxide (TiO2), a common photocatalyst, requires high-energy UV light for activation due to its large band gap (3.2 eV). Modification of TiO2 can reduce this band gap, leading to visible-light-responsive (VLR) photocatalysts. These catalysts can utilize solar and/or visible wavelength LED lamps as an activation source, replacing mercury-containing UV lamps, to create a "greener," more energy-efficient means for air and water revitalization. Recently, KSC developed several VLR catalysts that, on preliminary evaluation, possessed high catalytic activity within the visible spectrum; these samples out-performed existing commercial VLR catalysts.

Technology Portfolio System↗

NASA NTRS2016

Photocatalytic Conversion of CO2 on Mars

Light on Mars shows potential for providing the energy means necessary for enhanced In-Situ Resource Utilization (ISRU). Through photocatalysis, the energy barrier required to convert CO2 is lowered and CH4 production is favorable.

Photoreactor↗