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At least 937 records · Page 52
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Multifunctional Films Deposited by Atomic Layer Deposition for Tailored Interfaces of Electrochemical Systems

A new strategy for electrochemical interfaces that utilizes multilayer films deposited by atomic layer deposition (ALD) is introduced. Manganese-rich and nickel-rich cathode oxides were coated with a novel bilayer film of metal fluorides. Subsequent exposure to prolonged, high-voltage electrochemical cycling vs graphite electrodes revealed that the bilayer film can greatly enhance the high-voltage stability of cathode oxides. In particular, in manganese-rich cells, capacity fade due to manganese dissolution was substantially reduced and impedance rise was virtually eliminated. Furthermore, in nickel-rich NMC-811 cells, impedance rise was reduced by ~80%, compared to the NMC-811 baseline, after ~300 h of high-voltage exposure during cycling. Here, the multilayer film strategy presents an exciting opportunity for tailoring designs and materials for electrochemical interfaces in advanced lithium-ion batteries and beyond.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Investigating the Catalytic Requirements of Perovskite Fuel Electrodes Using Ultra-Low Metal Loadings

Solid Oxide Fuel Cells (SOFC) with La 0.3 Sr 0.7 TiO 3 (LST)–yttria-stabilized ZrO 2 (YSZ) anodes were prepared by impregnation of LST into porous YSZ scaffolds and then modified by Atomic Layer Deposition (ALD) of Ni, Pt, Pd, Fe, Co. and CeO 2 . Weight loadings as low as 0.01% of Pt, Ni, and Pd were sufficient to decrease anode impedances by orders of magnitude for operation in humidified H 2 at 973 K. The effects of CeO 2 , Co, and Fe were less but still significant. Sintering at higher temperatures was important. Furthermore, possible ways of stabilizing the metal particles and implications for developing ceramic anodes are discussed.

25 ENERGY STORAGE↗
DOE OSTI2018

Efficient Capacitive Deionization Using Thin Film Sodium Manganese Oxide

Capacitive deionization (CDI) is an emerging electrochemical desalination technology, which could outperform other desalination technologies if new electrode materials are developed with high electrochemical salt sorption capacities. Recent work has demonstrated improved desalination efficiency using redox-active materials in hybrid CDI (hCDI) electrodes. Here, we report new charge-storage behavior in thin-film sodium manganese oxide (NMO) which promises to enable new levels of desalination efficiency. We deposit thin-film MnO via atomic layer deposition (ALD), and electrochemically convert it to NMO in NaCl(aq). NMO coated electrodes exhibit increases in charge storage capacity up to 170 times higher than uncoated electrodes. Electrochemical quartz crystal microbalance (EQCM) measurements reveal that thin-film NMO leads to the electrochemical removal of 2.3 Na+ ions per electron. This super-stoichiometric removal of Na+ is corroborated by ab initio modeling that predicts a new electrochemical phenomenon at the NMO surface, which we term electron-decoupled ion transfer, or “EDIT.” We also describe a new custom low-volume and low-mass-loading hCDI cell which enables the study of the desalination performance of the EDIT mechanism. An hCDI cell comprised of NMO-coated carbon nanotube (CNT) cathode and Ag nanoparticle-decorated CNT anode yields a ~20-fold improvement in charge storage over bare CNT electrodes. The hCDI cell has a reversible charging efficiency (mol NaCl (mol e-)-1) of 123 ± 5% and a coulombic efficiency of 93%, corroborating our EQCM results and the EDIT mechanism. The EDIT mechanism, as well as the hCDI cell design that enabled its study, promise to hasten the development of hCDI devices with unprecendented performance

ab initio modeling↗
DOE OSTI2024

aldsim

SF-24-041 aldsim is a Python module that provides a set of ALD models that allow the user to explore the behavior of self-limited chemistries inside common reactor configurations.

YANGUAS-GIL, ANGEL↗
DOE OSTI2023

Integrating collapsible plasmonic gaps on near-field probes for polarization-resolved mapping of plasmon-enhanced emission in 2D material

Scanning near-field optical microscopy (SNOM) is an important technique used to study the optical properties of material systems at the nanoscale. In previous work, we reported on the use of nanoimprinting to improve the reproducibility and throughput of near-field probes including complicated optical antenna structures such as the ‘campanile’ probe. However, precise control over the plasmonic gap size, which determines the near-field enhancement and spatial resolution, remains a challenge. Here, we present a novel approach to fabricating a sub-20 nm plasmonic gap in a near-field plasmonic probe through the controlled collapse of imprinted nanostructures using atomic layer deposition (ALD) coatings to define the gap width. The resulting ultranarrow gap at the apex of the probe provides a strong polarization-sensitive near-field optical response, which results in an enhancement of the optical transmission in a broad wavelength range from 620 to 820 nm, enabling tip-enhanced photoluminescence (TEPL) mapping of 2-dimensional (2D) materials. We demonstrate the potential of this near-field probe by mapping a 2D exciton coupled to a linearly polarized plasmonic resonance with below 30 nm spatial resolution. This work proposes a novel approach for integrating a plasmonic antenna at the apex of the near-field probe, paving the way for the fundamental study of light-matter interactions at the nanoscale.

Zhou, Junze (ORCID:000000020682767X)↗
DOE OSTI2024

X-ray nano-holotomography reconstruction with simultaneous probe retrieval

In conventional tomographic reconstruction, the pre-processing step includes flat-field correction, where each sample projection on the detector is divided by a reference image taken without the sample. When using coherent X-rays as a probe, this approach overlooks the phase component of the illumination field (probe), leading to artifacts in phase-retrieved projection images, which are then propagated to the reconstructed 3D sample representation. The problem intensifies in nano-holotomography with focusing optics, which, due to various imperfections creates high-frequency components in the probe function. Here, we present a new iterative reconstruction scheme for holotomography, simultaneously retrieving the complex-valued probe function. Implemented on GPUs, this algorithm results in 3D reconstruction resolving twice thinner layers in a 3D ALD standard sample measured using nano-holotomography.

Nikitin, Viktor↗
DOE OSTI2013

Final Report: DE- FC36-05GO15063, Fundamental Studies of Advanced High-Capacity, Reversible Metal Hydrides

The project was component of the US DOE, Metal Hydride Center of Excellence (MHCoE). The Sandia National Laboratory led center was established to conduct highly collaborative and multi-disciplinary applied R&D to develop new reversible hydrogen storage materials that meet or exceed DOE/FreedomCAR 2010 and 2015 system targets for hydrogen storage materials. Our approach entailed a wide variety of activities ranging from synthesis, characterization, and evaluation of new candidate hydrogen storage materials; screening of catalysts for high capacity materials requiring kinetics enhancement; development of low temperature methods for nano-confinement of hydrides and determining its effects on the kinetics and thermodynamics of hydrides; and development of novel processes for the direct re-hydrogenation of materials. These efforts have resulted in several advancements the development of hydrogen storage materials. We have greatly extended the fundamental knowledge about the highly promising hydrogen storage carrier, alane (AlH 3 ), by carrying out the first crystal structure determinations and the first determination of the heats of dehydrogenation of β–AlH 3 and γ-AlD 3 . A low-temperature homogenous organometallic approach to incorporation of Al and Mg based hydrides into carbon aerogels has been developed that that allows high loadings without degradation of the nano-porous scaffold. Nano-confinement was found to significantly improve the dehydrogenation kinetics but not effect the enthalpy of dehydrogenation. We conceived, characterized, and synthesized a novel class of potential hydrogen storage materials, bimetallic borohydrides. These novel compounds were found to have many favorable properties including release of significant amounts of hydrogen at moderate temperatures (75-190 º C). However, in situ IR studies in tandem with thermal gravimetric analysis have shown that about 0.5 equivalents of diborane are released during the dehydrogenation making re-hydrogenation effectively impossible and precluding these compounds from further consideration as hydrogen storage materials. The hydrogen cycling of >11 wt % between MgB 2 to Mg(BH 4 ) 2 was achieved but required very forcing conditions. Under moderate conditions (dehydrogenation 200°C; re-hydrogenation 250°C, 120 atm H 2 ), Mg(BH 4 ) 2 undergoes reversible dehydrogenation to Mg(B 3 H 8 ) 2 . Although the 2.5 wt% cycling capacity does not meet current on-board storage targets, this result provides first example of direct hydrogen cycling of a borohydride under moderate conditions and demonstrates the plausibility of finding mild, PEM fuel cell relevant conditions for the high capacity, reversible dehydrogenation of borohydrides. A method was developed for the room temperature, direct hydrogenation of Ti-doped LiH/Al in liquefied dimethyl ether under 100 atm of H 2 . The process has been optimized such that Ti-doped LiAlH 4 is obtained in >95% yield. The WTT energy efficiency our direct synthesis process has been estimated to approach the 60% U.S. DOE target. Thus our simplification of the hydrogenation half-cycle may provide the key to harnessing the long-recognized potential of this lightweight, high capacity material as a practical hydrogen carrier. Finally, we have gained insight into the fundamental basis of the enhanced hydrogen cycling kinetics of Ti-doped NaAlH 4 through studies by solid state 1 H NMR, anelastic spectroscopy; muon spin rotation; and positron annihilation.

08 HYDROGEN↗
DOE OSTI2017

Development of Charge Drain Coatings: Final CRADA Report

The primary goal of this CRADA project was to develop and optimize tunable resistive coatings prepared by atomic layer deposition (ALD) for use as charge-drain coatings on the KLA-Tencor digital pattern generators (DPGs).

36 MATERIALS SCIENCE↗
DOE OSTI2017

Catalytic and Transport Behaviors of Model and Porous and Composite Nanostructures

As stressed in the Basic Energy Sciences Advisory Committee (BESAC) Report “New Science for a Secure and Sustainable Energy Future” (December 2008), solving our Nation’s energy challenges will entail more than incremental changes in present materials-related technologies; new, advanced routes to nanostructured materials with transformational properties will be required. Herein we describe the design and fabrication of a hybrid biotic/abiotic membrane reactor that, mimicking natural systems, employs the metalloenzyme, carbonic anhydrase, to separate CO 2 from N 2 with unprecedented purity and rate. The membrane design, synthesis, and operation are based on multiple biomimetic and nanoscale fabrication strategies, nanoscale dimensional features, and nanoscale physical phenomena, for example: 1) Bottom-up self-assembly of a membrane comprising a periodic, aligned, cylindrical nanopore array with 8 nm diameter pores designed to accommodate carbonic anhydrase (CA) enzymes 2) Top-down Atomic Layer Deposition (ALD) and plasma processing of the nanopore array to create 18nm deep (by 8nm in diameter) superhydrophilic pores bounded by hydrophobic/superhydrophobic interfaces 3) Formation of a continuous, defect free, ultra-thin (~18-nm thick) but strong water membrane by capillary condensation within the uniformly-sized, superhydrophilic nanopore array 4) Accommodation of CA within the water filled nanopore array (~2 CAs per hydrophilic pore channel) to achieve an effective CA concentration within the 18-nm thick water membrane over 10X greater than achievable in solution Exposed to a mixture of CO 2 and N 2 this biomimetic membrane rapidly and selectively dissolves CO 2 within the CA filled water nano-channels on the ‘upstream side’ and regenerates CO 2 at the superhydrophobic interface on the ‘downstream’ side. In combination, the high CA concentration and exceptionally short diffusion distances enable rapid and highly selective CO 2 separation from N 2 and H 2 . Our membrane has a combined CO 2 flux and selectivity that exceed by orders of magnitude all existing CO 2 membranes and for the first time meet the US Department of Energy guidelines for CO 2 sequestration technologies. (The performance of our membrane was recognized by an R&D100 Award and the first R&D100 Green Technology Award in 2015 and an issued US Patent in 2017). We believe this membrane could be employed in combination with sequestration to help reduce greenhouse gas emissions and provide a viable, economically feasible pathway to achieve the goals of the 2016 Paris Accord, which aims to maintain a global temperature rise this century less than 2°C above pre-industrial levels. Further this membrane concept could be adapted to other enzymes to accomplish other separations of interest, e.g. H 2 . We also have established processing-structure-property relationships of ultrathin membrane-like monolayer materials that are intrinsically catalytic. Establishing processing-structure-property relationships for monolayer materials is crucial for a vast range of applications spanning optics, catalysis, electronics, and energy. Presently, for MoS 2 , a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Using high-resolution transmission electron microscopy supported by density functional theory, we unambiguously solved the structure of MoS 2 monolayers and showed lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T’ (clustered Mo). These changes alter the energetics of MoS 2 interactions with hydrogen ((GH), and, with respect to catalysis, the 1T’ transformation renders the normally inert basal plane amenable towards hydrogen adsorption and H 2 evolution achieving Hydrogen Evolution Reaction (HER) catalytic activity comparable to 2H MoS 2 edges on Au(111), one of the most active HER catalysts known.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2017

Laser Materials Processing Final Report CRADA No. TC-1526-98

This CRADA project was a joint effort between Lawrence Livermore National Laboratory (LLNL) and United Technologies Corporation (UTC)/Pratt & Whitney (P&W) to demonstrate process capability for drilling holes in turbine airfoils using LLNL-developed femtosecond laser machining technology. The basis for this development was the ability of femtosecond lasers to drill precision holes in variety of materials with little or no collateral damage. The ultimate objective was to develop a laser machine tool consisting of an extremely advanced femtosecond laser subsystem to be developed by LLNL on a best-effort basis and a drilling station for turbine blades and vanes to be developed by P&W. In addition, P&W was responsible for commercializing the system. The goal of the so called Advanced Laser Drilling (ALD) system was to drill specified complex hole-shapes in turbine blades and vanes with a high degree precision and repeatability and simultaneously capable of very high speed processing.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Research three-dimensional hierarchical graphite architectures for anodes for fast charging

With current lithium ion batteries optimized for performance under relatively low charge rate conditions, implementation of XFC has been hindered by drawbacks including Li plating, kinetic polarization, and heat dissipation. This project will utilize model-informed design of 3-D hierarchical electrodes to tune key XFC related variables like 1) bulk porosity/tortuosity 2) vertical pore diameter, spacing, and lattice 3) crystallographic orientation of graphite particles relative to exposed surfaces 4) interfacial chemistry of the graphite surfaces through "artificial sEr formation using ALD 5) current collector surface roughness (aspect ratio, roughness factor, etc.). A key aspect of implementing novel electrodes is characterizing them in relevant settings. For this project, ultimately led out of University of Michigan by Neil Dasgupta, that includes both coin cell and 2+ Ah pouch cell testing, as well as comparison testing against baselines. Sandia National Labs will be conducting detailed cell characterization on iterative versions/improvements of the model-based hierarchical electrodes, as well as COTS cells for baseline comparisons. Key metrics include performance under fast charge conditions, as well as the absence or degree of lithium plating. Sandia will use their unique high precision cycling and rapid EIS capabilities to accurately characterize performance and any lithium plating during 6C charging and beyond, coupling electrochemical observations with cell teardown. Sandia will also design custom fixturing to cool cells during rapid charge, to decouple any kinetic effects brought about by cell heating and allow comparisons between different cells and charge rates. Using these techniques, Sandia will assess HOH electrodes from the University of Michigan, as well as aiding in iterative model and electrode design.

25 ENERGY STORAGE↗
DOE OSTI2020

Research three-dimensional hierarchical graphite architectures for anodes for fast charging

With current lithium ion batteries optimized for performance under relatively low charge rate conditions, implementation of XFC has been hindered by drawbacks including Li plating, kinetic polarization, and heat dissipation. This project will utilize model-informed design of 3-D hierarchical electrodes to tune key XFCrelated variables like 1) bulk porosity/tortuosity 2) vertical pore diameter, spacing, and lattice 3) crystallographic orientation of graphite particles relative to exposed surfaces 4) interfacial chemistry of the graphite surfaces through "artificial sEr' formation using ALD 5) current collector surface roughness (aspect ratio, roughness factor, etc.). A key aspect of implementing novel electrodes is characterizing them in relevant settings. For this project, ultimately led out of University of Michigan by Neil Dasgupta, that includes both coin cell and 2+ Ah pouch cell testing, as well as comparison testing against baselines. Sandia National Labs will be conducting detailed cell characterization on iterative versions/improvements of the model-based hierarchical electrodes, as well as COTS cells for baseline comparisons. Key metrics include performance under fast charge conditions, as well as the absence or degree of lithium plating. Sandia will use their unique high precision cycling and rapid EIS capabilities to accurately characterize performance and any lithium plating during 6C charging and beyond, coupling electrochemical observations with cell teardown. Sandia will also design custom fixturing to cool cells during rapid charge, to decouple any kinetic effects brought about by cell heating and allow comparisons between different cells and charge rates. Using these techniques, Sandia will assess HOH electrodes from the University of Michigan, as well as aiding in iterative model and electrode design.

25 ENERGY STORAGE↗
DOE OSTI2019

Magnetic Field Tolerant Large Area Picosecond Photon Detectors for Particle Identification (Phase I Final Report)

Incom is reporting on success in its DOE SBIR Phase I feasibility demonstration of our ability to optimize and characterize the magnetic field insensitivity of Large Area Picosecond Photon Detectors (LAPPDs) which we manufacture, this was accomplished principally by decreasing MCP pore sizes. LAPPDs are cost-effective ultra-high time precision imaging quantum photodetectors that incorporate Incom’s unique large-area ALD- (Atomic Layer Deposition) GCA- (Glass Capillary Array) MCPs (Microchannel Plates). Several applications of LAPPDs, including for potential upgrades to existing DoE NP detectors or as part of proposed designs for future DoE NP experiments (including at the future EIC Electron Ion Collider) will require LAPPD operation in strong magnetic fields. We are improving and verifying the performance of LAPPDs in strong magnetic fields both by modifying their internal construction and most importantly by modifying their constituents by using smaller-pore MCPs; we and others have shown that this improves magnetic field insensitivity in MCP-PMTs like our LAPPD. We have begun a series of magnetic field tests at Argonne National Laboratory on 6 x 6cm MCP-PMTs constructed at ANL using Incom MCPs, and on 20 x 20cm LAPPDs constructed at Incom again using Incom MCPs, each in a series of devices containing MCPs of ever smaller pore diameters, from 20μ to 10μ to 5μ; in addition to improving magnetic field insensitivity, smaller pores will improve LAPPD timing and thus benefit physics performance in future DoE NP detectors, including at the EIC.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Safe, Low-Cost, High Energy-Density, Solid-State Li-Ion Batteries

We developed intrinsically safe, robust, low-cost, high-energy-density solid-state Li-ion batteries, by integrating high conductivity garnet-type solid Li ion electrolytes and several different cathodes in tailored microstructures, fabricated by low-cost supported thin-film ceramic techniques, to overcome the primary technological barriers to next generation battery technology. In this ARPA-E project we employed Li-garnet solid-state electrolytes pioneered by one of the co-investigators (Thangadurai) which has room temperature (RT) conductivity of ~10 -3 S cm -1 . The highly stable garnet SSE allowed the use of S, NMC, and other cathodes with Li metal anodes without stability or flammability concerns. We studied the garnet’s stability when exposed to CO 2 and humidity (with or without an ALD coating) and showed that the material can be processed in ambient air for most steps prior to battery assembly, significantly reducing production costs. We extensively studied and scaled up the synthesis of the powder and explored external suppliers of garnet to determine the best pathway for commercial success. We used low-cost and scalable tapecasting fabrication methods to create porous-dense-porous “trilayer” solid electrolyte microstructures with a ~20 μm separating dense layer, and >70% porosity porous layers to host the electrodes. These scalable multilayer ceramic fabrication techniques, without need for dry rooms or vacuum equipment, also provide for dramatically reduced manufacturing costs. The tailored microstructured electrode supports (scaffold) increased interfacial area ~50x, overcoming the high impedance typical of planar geometry SSLiBs, resulting in record-setting 10 mA/cm 2 lithium cycling in a symmetric cell. We expanded our tapecasting ability and showed tapes >25m in length by the end of the project. We demonstrated the ability to sinter garnet without the use of a garnet powderbed, which could have been a major obstacle and waste of material at scale. At the same time, we expanded the size of our trilayers from coin cells (0.7 cm 2 ) to the full format design (30 cm 2 ). To develop full cells, we demonstrated 250 Wh/kg at room temperature with commercial NMC electrode films in a bilayer configuration. Similarly, we demonstrated 280 Wh/kg trilayer Li-S cells at room temperature with >90% capacity retention over 300 cycles. At 90°C we demonstrated 350 Wh/kg with a Li-S trilayer. The high thermal stability of the garnet electrolyte also enabled extended cycling (400 cycles) of a Li-TiS 2 cell at 150 °C, showcasing the exceptional safety and nonflammability of the solid-state trilayer batteries. Ion Storage Systems has taken this technology and knowledge to produce trilayer garnet electrolytes and is building out facilities to commercialize high performance solid state batteries. ISS has hired a strong staff, identified and communicated with a large number of potential partners, and successfully secured follow-on funding.

25 ENERGY STORAGE↗
DOE OSTI2020

Integrated Harsh Environment Gas / Temperature Wireless Microwave Acoustic Sensor System for Fossil Energy Applications

There is a significant need for sensors capable of detecting gases, such as H 2 , O 2 , NO x , SO x within harsh environments encountered in power plants, industrial manufacturing, oil and gas exploration, and aerospace applications. This project successfully demonstrated the use of wireless microwave acoustic sensor technology for the detection of gases (H 2 or O 2 ) from ambient temperatures up to 650°C. The work focused on langasite (LGS) based surface acoustic wave resonator (SAWR) sensors as the harsh-environment sensor platform and explored multiple combinations of high-temperature thin films and device structures which were used to increase the sensor platform stability and detection capability at temperatures in the operational range of 150°C to 700°C. Specific material configurations that were investigated include: yttria-stabilized-zirconia (YSZ) decorated with Pt nanoparticles, atomic layer deposited (ALD) Al 2 O 3 , palladium, and Pt/Al 2 O 3 co-deposited electrode alloys. Through the deposition of YSZ at temperatures as high as 850°C and the use of graded alloy concentrations of Pt in the fabrication of the Pt/Al 2 O 3 electrode structures, film stress problems were mitigated, and sensor operation and stability achieved. To test and evaluate SAWR sensor performance for the detection of H 2 and O 2 under the influence of temperature variations, a comprehensive gas sensor control system and test apparatus was created to operate within a laboratory box furnace-controlled environment. In addition to the advancement in thin film materials through the deposition and fabrication techniques mentioned above, the work characterized the performance of sensors containing these films in the presence of oxidizing and reducing gases between 25°C and 700°C. In particular, the work revealed that the exposure of the SAWR sensor surfaces to oxidizing environments significantly improve the sensor response to H 2 , whereas the exposure of the sensor to reducing environments at high temperatures (≈ 500°C) renders the sensor irresponsive to H 2 , requiring sensor surface treatment at high temperatures (above 500°C) to recover the responsiveness to H 2 . The SAWR sensors have been also tested for wireless operation and array operation using multiple orientations to resolve the detection of gases under temperature variations. The work developed at the University of Maine was aided by a collaboration with the NETL Research and Innovation Center, Pittsburgh, PA, where thin film materials and device structures fabricated at UMaine were tested and characterized using NETL gas reactors and surface analysis techniques. SAWR sensors fabricated at UMaine were exposed multiple times to temperatures up to 700°C and H 2 concentrations up to 100% in the NETL facilities to measure the sensor performance. Environetix Technologies Corporation, a UMaine harsh-environment sensor spin-off company, also provided support and assistance in sensor system testing and implementation. The sensor small size and configuration allows flexible sensor placement and embedding of multiple sensor arrays into a variety of components within power systems and other aerospace or industrial settings that need to be interrogated wirelessly. The SAW platform is an attractive option for high-temperature harsh-environment gas sensing applications due to its inherent features, namely small size, capability of battery-free and wireless operation, and cost effective scale production using well-established production techniques from the semiconductor industry. The research findings achieved in this work, particularly advances regarding the fabrication and performance of the SAWR gas sensor platform, can be adapted and transferred to industrial power plants and other harsh environments.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2020

Functional Photoresists for Energy Applications. Final Report

Monolithic ultralow-density porous bulk materials have recently attracted much interest due to many emerging applications in the areas of catalysis, energy storage and conversion, and thermal insulation. They are also important components of high energy density (HED) and inertial confinement fusion (ICF) targets. However, despite tremendous progress that has been made in the synthesis of porous materials, deterministic and independent control over microscopic architecture, density and composition remain key issues, and their integration in high precision devices requires cost and time-intensive mechanical machining that not only reduces reproducibility by generating debris but also limits the complexity of the 3D shapes that can be realized. In this project, we overcame these limitations by developing a universal templating capability that provides deterministic and independent control over density, composition, architecture, and macroscopic sample shape. This was achieved by developing the technology to 1) 3D print ultrahigh resolution, ultra-high precision polymeric micro-lattice templates, 2) coat these templates with the desired materials, and 3) removing the template (Fig. 1a). Atomic layer deposition (ALD) provides the atomic scale coating thickness accuracy required for precisely controlling density. While this templating approach had been demonstrated in prior work, limitations in suitable photoresists, 3D print technologies, print design, and template removal techniques did not allow the fabrication of millimeter-sized high-precision parts with sub-micron resolution. To enable this technology, we developed 1) two-photon polymerization (TPP) print designs that enable the fabrication of millimeter-sized, mechanically robust polymeric templates with sub-micron resolution and 2) a continuum level TPP printing simulation capability for additional print design guidance; 3) atomistic models to study photoresist polymerization kinetics and network topography, 4) refractive index matched polymeric and preceramic TPP photoresists, and 5) functional TPP photoresists including porous voxel structures and self-immolative polymer photoresist chemistries; and 6) damage free template removal techniques that enable the fabrication of defect-free high-precision low-density foam components. We also developed a templating approach for pure carbon microlattices with a unique tube-in-tube ligament morphology. As a test platform, we pursued the fabrication of foam liners that promise to further increase the neutron yield in indirect drive ICF experiments by improving implosion symmetry control and coupling between the laser and the deuterium-tritium fuel. This application requires fabrication and integration of a ultra-high precision, millimeter-sized, thin-walled (200-400 micrometer thick), low-density (10-30 mg/cc), high atomic number (high Z) cylindrical foam tube into the gold hohlraum of an indirect drive ICF target (Fig. 1b). While our hohlraum liner test case will mainly find application in HED and ICF experiments, the underlying science will also directly apply to previously developed nanoparticle and additive manufacturing technologies and will advance those techniques as well.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Pushing the efficiency limit of low-cost, industrially relevant Si solar cells to > 22.5% by advancing cell structures and technology innovations (Final Report)

The overall objective of this program is to achieve ~23% bifacial n-type cell efficiencies by developing and implementing optimized homogeneous or selective boron (B) emitter on front and tunnel oxide passivated contact (TOPCon) on rear side, in combination with advanced fine-line screen-printing metallization with floating busbars. During this research project, first we developed a technology roadmap to drive the 21% n-PERT cell efficiency from 21% to 23% by transforming the cell design to n-TOPCon and establishing the requirements for each layer, including B emitter, rear n-TOPCon, n-base Si and screen-printed contacts. Next, consistent with our roadmap, we developed advanced homogeneous implanted B emitter (150-180 Ω/⌫) passivated with ALD Al 2 O 3 layer capped with PECVD SiN x /SiO x double-layer antireflection coating This gave a very low recombination current density of 10-15 fA/cm 2 prior to metallization. In addition, we demonstrated metallized recombination current density of ~31 fA/cm 2 for this advanced homogeneous B emitter with industrial screen-printed, fire-through contacts with 40 μm wide grid lines, floating busbars and implementation of an advanced Ag-Al paste which resulted in local or reduced area metal-Si contact under the grid lines with virtually no emitter surface etching. This paste reduced the full area metallized J oe,metal from >1100 fA/cm 2 to ~700 fA/cm 2 . We also developed novel processes for the formation of p + /p ++ selective B emitter by a) single B diffusion with selective etch back and b) two-steps diffusion with implanted B in field region and APCVD B diffusion under the metal grid. We achieved very low un-metallized recombination current density (J 0 ) of ~18 fA/cm 2 for the selective p ++ p + emitters (30/150 Ω/⌫) and metallized J 0 of ~28 fA/cm 2 with ~3% screen-printed metal contact to p ++ regions. Next, we developed the technology for n-TOPCon by growing phosphorus-doped LPCVD and PECVD poly-Si on top of ~ 15Å chemically grown (NAO) tunnel oxide. After an optimized anneal at 875 °C for 30 min, passivated n-TOPCon have unmetallized J 0 of ~ 5 fA/cm 2 which went down further to ~ 1 fA/cm 2 after a 700 Å SiN x capping layer and simulated contact firing cycle at 770 °C. After screen-printed fire-through metallization on this n-TOPCon with ~13% metal coverage, metallized J 0 value increased to only ~5 fA/cm 2 which is among the lowest reported value to the best of our knowledge for screen-printed metallization. Finally, we integrated all the above technology innovations and enhancements and demonstrated low-cost manufacturable screen-printed n-TOPCon bifacial Si solar cell with ~23% efficiencies. Based on the experimental and theoretical understanding developed in this project, we have developed a new technology roadmap that shows that implementation of busbarless contacts, 10-20 ms bulk lifetime Si, and selective B emitter or selective TOPCon on the front can drive ~23% efficient cells achieved in this research to ~25% at low-cost.

14 SOLAR ENERGY↗
DOE OSTI2023

HydroGEN Seedling: Monolithically Integrated Thin Film/Silicon Tandem Photoelectrodes for High-Efficiency and Stable Photoelectrochemical Water Splitting

In this project, we propose to develop monolithically integrated Si-based tandem photoelectrodes to achieve both high solar-to-hydrogen (STH) efficiency (>15%) and long-term stability (>1,000 hours) in spontaneous water splitting systems. The proposed tandem devices consist of a Ta 3 N 5 , BCTSSe, or In 0.5 Ga 0.5 N top junction, which has a bandgap of ~1.7-2.0 eV and can split the solar spectrum with the Si bottom junction. Ta 3 N 5 , BCTSSe, and InGaN will be grown/deposited on a low-resistivity nanowire tunnel junction on Si substrates using atomic layer deposition (ALD), sputtering, and molecular beam epitaxy (MBE), respectively. Both n and p-type Si solar wafers will be utilized, which can serve as the photoanode or photocathode, respectively. We will use N-rich GaN ultrathin passivation layers to protect photoelectrodes from corrosion and oxidation.

08 HYDROGEN↗