Chapter Four · failure evidence

What Electrode & Electrolyte Design got wrong, from 92 dissertations

The records document various engineering and operational failures encountered during the synthesis, testing, and optimization of battery electrolytes and electrode materials. Researchers repeatedly found that modifications aimed at improving conductivity or stability often resulted in mechanical degradation, dendrite formation, poor rate capacity, or severe measurement instability. These records come from PhD theses at 27 institutions, 2021 to 2026. Each links to its thesis. They were extracted by language models reading the full text, so treat each as a lead to read, not a verdict.

Alternative electrode and electrolyte chemistries deliver lower capacity and catalytic performance than conventional baselines

16 theses · 10 institutions

Cell designs and modified electrolyte formulations repeatedly delivered lower discharge capacities, lower specific energies, and diminished power compared to established liquid baselines. Catalytic electrodes also showed higher overpotentials, increased degradation rates, and reduced product partial currents when compared against standard reference materials.

Lost to a baseline

GD25 slurry cathode (GD25-s) exhibited gravimetric charge storage far inferior to GD25 free-standing film electrodes.

Design of Organic Frameworks for Electrochemical Energy Storage Applications · Georgia Tech

Lost to a baseline

LiClO4-based EC electrolyte allowed only ~30 Li plating/stripping cycles before failure due to lack of fluorine-rich SEI formation.

SUPPRESSING PHYSICOCHEMICAL INSTABILITIES AT ELECTROCHEMICAL INTERFACES——TOWARDS SUSTAINABLE BATTERY ELECTRODES · Cornell

Lost to a baseline

NMC111 cathode half-cells infiltrated with Li2OHCl and using 3LiBH4-LiCl delivered an experimental capacity of ~100-120 mAh g^-1 (cycled between 3 and 4 V at 45 mA g^-1), underperforming the capacity realized in liquid electrolytes (~160 mAh g^-1).

Borohydride-based solid electrolytes and polymer composite separators for lithium-ion batteries · Georgia Tech

Lost to a baseline

Despite polysulfide shuttle suppression, SL/HFE low-concentration electrolytes showed faster long-term degradation and rising polarization over 200 cycles compared to standard cycling expectations due to thick, resistive SEI formation on the Li anode.

TUNING ELECTROLYTE COMPOSITION FOR ENHANCED PERFORMANCE OF LITHIUM-SULFUR BATTERIES · Georgia Tech

Lost to a baseline

Recycled [C4MIm][OTF] produced a lower energy density (~13 Wh kg-1) compared to neat/other electrolytes due to lower electrochemical stability.

Ionic liquid-assisted process: biomass-derived carbonaceous materials · Imperial

Lost to a baseline

Solid-state Co/Pd multilayer VCMA efficiency (858 Oe/V) was lower than liquid-electrolyte SmCo5 electrochemical cell systems (~10^4 Oe/V).

Reversible and Irreversible Effects of Magneto-Ionic Gating: Exchange, Anisotropy, and Magnetization · MIT

Tried and failed

potential-controlled electrode immersion applied to electrocatalytic reduction reactions. Outcome: worse than baseline. Reason: resulted in significantly lower partial current densities for hydrocarbon products compared to open-circuit immersion

Carbon dioxide reduction and related reactions on copper and carbon electrocatalysts · Imperial

Tried and failed

electrochemical reduction using unfunctionalized carbon electrodes applied to carbon dioxide reduction reaction. Outcome: worse than baseline. Reason: lacked catalytic active sites, favoring the competing hydrogen evolution reaction over CO2 conversion

ADVANCING ELECTROCHEMICAL PATHWAYS FOR UPCYCLING CARBON DIOXIDE EMISSIONS INTO SOLID CARBONATES AND SYNGAS · Cornell

Tried and failed

prolonged electrodeposition of metal oxide applied to porous carbon supercapacitor electrodes. Outcome: worse than baseline. Reason: excessive active material loading increased electrical resistance, reducing specific capacitance at high scan rates

Electrochemical studies of the applications of novel carbon-based materials · Oxford

Lost to a baseline

LSF electrodes decorated with bimetallic Ni0-Fe0 exsolutions exhibited lower electro-catalytic activity for H2 oxidation than electrodes decorated solely with pure Ni0.

Electrochemical switching of perovskite-type exsolution catalysts Elektrochemische Schaltung von perowskitartigen Exsolution Katalysatoren · DSpace-CRIS at TU Wien

Lost to a baseline

LPSC-based solid-state batteries with aluminum anodes achieved lower specific energy (293-307 Wh kg-1) than liquid-electrolyte aluminum batteries (311 Wh kg-1).

Probing Interfacial Dynamics in Solid-State Lithium Metal Batteries · Georgia Tech

Lost to a baseline

Mixed-metal and Fe-based catalysts (NiFe2O4, NiCoO2, Ni0.5Co0.5Fe2O4) had much higher overpotentials and degradation rates than baseline IrO2 (and Co3O4) in pure-water MEAs despite being superior in 3-electrode alkaline liquid cells

Advancing Anion-Exchange-Membrane Water Electrolyzer Devices: Catalyst Layer Interactions, Degradation Pathways, and Operational Development · Scholars' Bank

Considered and rejected

Considered and rejected: Rejected graphite electrodes due to 55-fold lower power density and negative net power compared to titanium MMO electrodes.

Operation and configuration of reverse electrodialysis for thermal to electric conversion applications. · Cranfield

Considered and rejected

Considered and rejected: Rejected gold electrode substrates in favor of platinum electrode substrates due to gold's insufficient catalytic activity for low-temperature H2/CO sensing.

SMOX Gas Sensor Characterization of Classical Polycrystalline SnO2 Materials at Room Temperature and Spectroscopic Analysis of Their Time Dependent Performance Degradation · Publikationssystem UB Tuebingen

Lost to a baseline

At 25 °C, supercapacitors using piperidinium ether electrolyte 2 with 1.0 M LiTFSI exhibited an initial discharge capacitance of 16.1 F/g compared to 36.7 F/g for 1.0 M LiTFSI in propylene carbonate (PC).

Synthesis and characterization of ionic liquid electrolytes for use in electrical energy storage devices at elevated temperatures · OpenBU

Lost to a baseline

Supercapacitor with electrolyte 2 yielded 3.73 Wh/kg at 25 °C (1 A/g) vs 6.61 Wh/kg for standard propylene carbonate (PC) electrolyte.

Synthesis and characterization of ionic liquid electrolytes for use in electrical energy storage devices at elevated temperatures · OpenBU

Lost to a baseline

Supercapacitor initial capacitance at 25 °C was 16.1 F/g for electrolyte 2 vs 36.7 F/g for propylene carbonate.

Synthesis and characterization of ionic liquid electrolytes for use in electrical energy storage devices at elevated temperatures · OpenBU

Lost to a baseline

Initial specific discharge capacity of liquid electrolyte (LE) reference cells (1228-1258 mAh gS-1) was higher than pristine POSS (813 mAh gS-1) and TPTA (645 mAh gS-1) gel cells before cycling degradation.

ENGINEERING EFFICIENT ELECTROLYTES FOR HIGH-PERFORMANCE LITHIUM SULFUR BATTERIES · Cornell

Lost to a baseline

LPSC-based solid-state batteries with silicon anodes yielded lower specific energy (320–325 Wh kg-1) than liquid-electrolyte silicon batteries (345 Wh kg-1) due to higher solid electrolyte density.

Probing Interfacial Dynamics in Solid-State Lithium Metal Batteries · Georgia Tech

Lost to a baseline

Graphite anodes with 3LiBH4-LiCl delivered ~250 mAh g^-1 capacity (0.01-1 V), underperforming the conventional liquid electrolyte capacity (~372 mAh g^-1).

Borohydride-based solid electrolytes and polymer composite separators for lithium-ion batteries · Georgia Tech

Lost to a baseline

In thin/low-loading cathodes, 3M LiTFSI enabled higher raw discharge capacity than low-concentration electrolytes (though with higher polarization and viscosity).

TUNING ELECTROLYTE COMPOSITION FOR ENHANCED PERFORMANCE OF LITHIUM-SULFUR BATTERIES · Georgia Tech

Sensor and reference electrodes suffer from fabrication defects, surface sensitivity, and measurement instability

21 theses · 13 institutions

Microfabricated sensing electrodes and reference contacts frequently produced erratic open-circuit potentials, unrepeatable impedance spectra, or high charge-transfer resistance due to surface contamination and structural flaws. Thin-film pseudo-reference layers, nanoelectrode arrays, and modified sensor surfaces exhibited significant signal drift and poor batch-to-batch reproducibility across experimental setups.

Tried and failed

nanoscale electrolyte layer thickness scaling applied to solid-state electrochemical synaptic devices. Outcome: unstable. Reason: sub-200 nm electrolyte films caused severe electrical leakage and loss of conductance modulation

Protonic All-Solid-State Electrochemical Device as an Artificial Synapse for CMOS-Compatible Neuromorphic Computing · MIT

Lost to a baseline

Thin-film cysteamine pH electrode failed to achieve stable steady-state potentiometric readout compared to baseline rigid IrOx needle electrodes

Roll-to-Roll processable organic thin film transistor based circuits and their sensory application · Oxford

Tried and failed

metal electrodeposition and stripping calibration applied to electrochemical quartz crystal microbalance sensors. Outcome: unstable. Reason: residual deposited metal or substrate stripping degraded subsequent electrochemical measurement surfaces

Design and evaluation of mixed ionic/electronic conducting polymers for energy storage devices and organic electrochemical transistors · Imperial

Tried and failed

carbon nanotube intermediate layer in reference electrode applied to solid-state electrochemical reference electrodes. Outcome: unstable. Reason: caused unacceptable electrical instability and erratic, noisy sensor signals

A portable microfluidic electrochemical sensing platform for the real-time detection of clinical neurochemical markers · Imperial

Tried and failed

sputtered thin-film metallic pseudo-reference electrodes applied to potentiometric electrochemical sensing. Outcome: unstable. Reason: extreme sensitivity to surface conditions caused irreproducible open-circuit potential measurements

Circuits for Wireless Sensing · Cornell

Tried and failed

direct enzyme physical adsorption on noble metals applied to electrochemical biosensor electrodes. Outcome: worse than baseline. Reason: produced sensors with lower sensitivity compared to carbon screen-printed electrodes

Hardware and Software Interfaces Design for Multi-Panel Electrochemical Sensors · EPFL

Tried and failed

Non-faradaic impedance spectroscopy on microgap interdigitated electrodes applied to bacterial cell detection. Outcome: unstable. Reason: High microfabrication shorting defects and unrepeatable impedance spectra at small interelectrode spacings

The impact of mass transport and surface charging on the performance of field effect transistor biosensors · Georgia Tech

Tried and failed

manual dispensing and drop-casting of conductive inks applied to fabricating electrochemical sensors on flexible substrates. Outcome: unstable. Reason: produced uneven, non-reproducible electrode films with polymer ink bleeding into porous substrates

Plant-on-a-chip: monitoring chemical responses in living plants with printed sensors · Imperial

Tried and failed

incorporating ligand-stripped inorganic nanoparticles into polymer electrolytes applied to solid-state proton-conducting composite films. Outcome: unstable. Reason: proton conductivity was irreproducible across batches despite extensive variations in processing and annealing conditions

Surface chemistry and material integration of metal oxide nanocrystals · UT Austin

Tried and failed

electroless metal plating using published protocol applied to spectroscopic working electrode preparation. Outcome: did not generalise. Reason: failed to reproduce at a different institution despite identical nominal conditions

Probing lithium-mediated electrochemical nitrogen reduction using in situ infrared spectroscopy · Imperial

Tried and failed

feedback-controlled electrochemical deposition for nanogap fabrication applied to dual-barrel tunneling probe fabrication. Outcome: unstable. Reason: unstable current or lack of gap voltage decrease during electrodeposition

Quantum mechanical tunnelling probe for next-generation single molecule sensor · Imperial

Lost to a baseline

Charge-transfer resistance Rct of micro-/nano-optoelectrodes (190 kΩ) was higher than planar electrodes (81 kΩ) due to residual photoresist polymer residue.

Optical Nanoantennas Integrated with 3D Microelectrode Arrays: Hybrid Photonic-Electronic Modalities for Nano-Bio Interfacing · Virginia Tech

Lost to a baseline

Enzyme-based needle electrode (Yonemori et al. 2009) achieved a higher sensitivity (3.10 a.u./mg.dl⁻¹) than this work's glucose sensor (0.0354 a.u./mg.dl⁻¹).

Opto-chemical biosensor development, and analytics for point-of-care applications · Iowa State University Digital Repository

Lost to a baseline

Nanopore dual-electrode array exhibited a collection efficiency of 20% (for Fe2+/Fe3+), significantly below the maximum efficiencies of interdigitated electrodes.

Design and Characterization of Hybrid Biological-Inorganic Systems · Harvard

Lost to a baseline

Bare IrO2 electrodes exhibited higher impedance than PEDOT:PSS-coated TiN electrodes across large microelectrode diameters (D = 10, 50, 100 µm).

Multimodal And Multifunctional CMOS Cellular Sensing And Actuating Array With Enhanced Electronics-Biology Interface · Georgia Tech

Considered and rejected

Considered and rejected: Rejected roughened electrodes for bacterial SERS due to difficulties in maintaining consistent nanostructures and ensuring pathogen interaction

Raman spectroscopy for point of care urinary tract infection diagnosis · Imperial

Considered and rejected

Considered and rejected: Rejected using needle probe / electrode methods for thin-film flux detection due to large inaccuracies.

Development of a device for the determination of local magnetic properties of thin films on whole wafers Entwicklung eines Geräts zur Bestimmung lokaler magnetischer Eigenschaften von Dünnschichten auf ganzen Wafern · Leibniz Universität Hannover Repository

Considered and rejected

Considered and rejected: Polymer modification (e.g. Nafion, cellulose acetate) of electrodes was rejected as it overly complicated fabrication and lacked reproducibility for field screening.

Electrochemical method for the rapid in situ screening of heavy metals in soil and water samples · Cranfield

Considered and rejected

Considered and rejected: Rejected standard electrochemical reference electrodes as unreliable for isolating cathode impedances in these solid oxide cells.

Investigation and Improvement of SofC Composite Cathodes · Penn

Considered and rejected

Considered and rejected: Single-CNT bridging electrode architectures were rejected in favor of random CNT nanowire networks due to fabrication difficulties, fragility, low yield, and lack of reproducibility.

Complexing Carbon Nanomaterials and Reactive Metal Species for Selective Chemical Sensing and Tunable Catalysis · MIT

Considered and rejected

Considered and rejected: Microelectrode pH measurement of haemolymph in the microlitre range rejected due to inconsistent readings and technical instability.

Acid-base balance in ageing and age-related disease · Imperial

Electrolyte formulations suffer from high viscosity, salt precipitation, and reduced ionic conductivity

18 theses · 11 institutions

Attempts to modify polymer and liquid electrolytes through excessive crosslinking, high salt concentrations, or weakly solvating solvents led to high viscosity and sluggish ion mobility. In other cases, exceeding solubility limits or introducing microscale particle fillers precipitated insulating phases and degraded bulk conductivity relative to unadulterated baselines.

Tried and failed

plasticiser addition to crosslinked polymer gel electrolytes applied to quasi-solid-state gel polymer electrolytes. Outcome: unstable. Reason: inherent matrix instability prevented significant ionic conductivity improvements over unplasticised crosslinked networks

ENGINEERING EFFICIENT ELECTROLYTES FOR HIGH-PERFORMANCE LITHIUM SULFUR BATTERIES · Cornell

Tried and failed

aliovalent cation doping to increase ionic conductivity applied to solid-state electrolyte crystalline lattices. Outcome: worse than baseline. Reason: exceeded the solid solution solubility limit, precipitating insulating impurity phases

Design and Development of High-Performance Solid Electrolyte for All-Solid-State Lithium Ion Batteries · Georgia Tech

Tried and failed

increasing ionic monomer content in polymer electrolytes applied to single-ion conducting solid polymer electrolytes. Reason: high ion content caused brittle crystallization, preventing sufficient electrode contact for electrochemical impedance measurements

Understanding ion transport in comb-branched polymer electrolytes to optimize electrochemical properties · UT Austin

Lost to a baseline

Room-temperature C/3 cycling of DMOHC cells caused lithium plating and failed compared to standard EC-based baseline electrolytes due to excessive viscosity.

Li-ion Cell Electrolytes For Enhanced Performance at High Temperatures · DalSpace

Lost to a baseline

CR05M20 crosslinked electrolyte suffered lower discharge capacity (0.32 mAh/cm2) and harsher capacity fading over 50 cycles than lower-crosslinked CR05M5 and CR1M10.

IN-SITU POLYMERIZED SOLID ELECTROLYTES FOR LITHIUM BATTERIES · Cornell

Lost to a baseline

PVA-NaOH gel electrolyte delivered orders of magnitude lower power density compared to standard PVA-KOH gel electrolyte due to lower ionic conductivity.

MEMS-Based Electrochemical Power Sources for Extended Operational Duration of Micro Unmanned Vehicles · Penn

Considered and rejected

Considered and rejected: Rejected using non-aqueous PEG electrolytes for pPFDA without hydrolysis activation because interfacial ion transport remained sluggish leading to open circuit.

UNDERSTANDING AND DESIGNING INTERPHASE IN ZINC AND LITHIUM ANODES · Cornell

Considered and rejected

Considered and rejected: High-concentrated 'solvent-in-salt' electrolytes (>3M) rejected due to poor wettability to separators and electrodes, increased viscosity, and decreased ionic conductivity

Hybrid Power-Energy Electrodes · IRIS - POLITO - prod

Considered and rejected

Considered and rejected: Oxygen substitution in sulfide solid electrolytes to improve moisture stability was noted as suboptimal because it degrades bulk ionic conductivity.

Development of high energy density Lithium-sulfur batteries · UT Austin

Considered and rejected

Considered and rejected: Rejected using 1,4-dioxane as weakly solvating solvent due to low salt solubility, high viscosity/melting point, and poor ionic conductivity with high-loading electrodes.

Designing Electrolytes for Durable and Fast-Charging Alkali-Ion Batteries · Virginia Tech

Tried and failed

increasing plasticizer concentration in crosslinked polymer gel applied to gel polymer electrolytes. Outcome: worse than baseline. Reason: excessive crosslinking increased storage modulus and reduced ionic conductivity

ENGINEERING EFFICIENT ELECTROLYTES FOR HIGH-PERFORMANCE LITHIUM SULFUR BATTERIES · Cornell

Tried and failed

swelling hydrogels in deionised water solvent applied to polyacrylamide hydrogel network. Outcome: worse than baseline. Reason: pure water has less favourable thermodynamic interaction with the polymer network than electrolyte solutions

Physics and Engineering of Moisture-Capturing Hydrogels for Water and Heat Harvesting · MIT

Tried and failed

direct macroscopic blending without in situ polymerization applied to plastic crystal embedded polymer electrolytes. Outcome: worse than baseline. Reason: lack of polymerization-induced phase separation degraded ionic conductivity and mechanical toughness

Designing 3D Structured Electrodes and Electrolytes for High-Performance Rechargeable Batteries · Georgia Tech

Tried and failed

fluorinated carboxylate electrolyte additives applied to low-temperature lithium-sulfur batteries. Outcome: worse than baseline. Reason: lower ionic conductivity without sufficient association energy benefits compared to standard salt

Overcoming the kinetic limitations of lithium-sulfur batteries · UT Austin

Tried and failed

solid polymer electrolyte solution casting applied to subzero temperature lithium metal batteries. Reason: electrolytes failed to cycle or operate at low temperature

Development of formable metal batteries (Mettery) · Imperial

Lost to a baseline

PEO:LiClO4 composite electrolytes with 1-5 µm SiO2 particles (10 wt.% and 30 wt.%) showed lower ionic conductivity across all measured temperatures compared to filler-free bulk PEO electrolyte.

Understanding Ion Conduction in Polymer-Ceramic Composite Electrolytes for Lithium Ion Batteries · MIT

Considered and rejected

Considered and rejected: Rejected neat MEEP and MEP as freestanding electrolytes because they formed viscous gels/liquids lacking dimensional stability under pressure.

Polyphosphazene- and Acrylate-Based Polymer Electrolytes for Lithium Batteries · Georgia Tech

Considered and rejected

Considered and rejected: Rejected room-temperature PEO solid polymer electrolytes due to excessive crystallinity below 65 °C, adopting PEGDME2000-based composite polymer electrolyte instead.

Cathodes Development and Cell Manufacturing for Innovative Li-ion and Na-ion Batteries · IRIS - UNICAM - prod

Considered and rejected

Considered and rejected: Sparingly solvating electrolyte / high-concentration salt approach was rejected due to large penalties to polysulfide solubility and Li+ mobility at room temperature

Overcoming the kinetic limitations of lithium-sulfur batteries · UT Austin

Considered and rejected

Considered and rejected: Tetrahydrofuran (THF) was rejected in favor of propylene carbonate (PC) for LiAsF6 electrolyte due to low dielectric constant limiting salt dissociation above 0.75 mol/dm3.

NOVEL ZINC AND LITHIUM NON-AQUEOUS BATTERIES FOR LOW RATE APPLICATIONS · De Montfort Open Research Archive (DORA)

Electrodes and current collectors experience mechanical fracture, chemical corrosion, and interfacial delamination

17 theses · 11 institutions

Active electrode layers and current-collecting foils frequently suffered severe mechanical cracking, swelling, or delamination under continuous electrochemical cycling and sonication. Furthermore, exposure to harsh chemical conditions or bias voltages triggered catastrophic oxidative corrosion, anodic dissolution, and rapid material degradation.

Tried and failed

acidic aqueous polymer gel electrolyte applied to solid-state supercapacitors. Outcome: unstable. Reason: The electrolyte dried out rapidly and the acid degraded the host polymer matrix.

Wet spun single-wall carbon nanotube fibres for structural energy storage devices · Imperial

Tried and failed

solid oxide electrolyte with molten metal anode applied to direct carbon fuel cells. Outcome: unstable. Reason: electrolytes suffered severe electrochemical thinning and degradation under current in the molten anode environment

Molten Metal Anodes for Direct Carbon-Solid Oxide Fuel Cells · Penn

Lost to a baseline

Liquid electrolyte coin cells destroyed 30 µm Al foil anodes in <70 cycles (swelling to >200 µm), performing far worse than SSB configurations

Aluminum-foil-based alloy anodes for solid-state batteries · Georgia Tech

Tried and failed

thermal annealing before hydrophobic coating deposition applied to porous gas-diffusion electrodes. Outcome: worse than baseline. Reason: pre-treatment heat application degraded the electrode structure and reduced overall electrochemical performance

Electrocatalyst performance at the gas/Electrolyte interface under high mass transport conditions · Imperial

Tried and failed

electrochemical dealloying of metal foil anodes applied to tin foil electrodes. Outcome: worse than baseline. Reason: reformed pure phase surface layer trapped unreacted core phases due to poor solid-state diffusivity

Investigating Reaction Mechanisms of Next-Generation Active Materials for Low-Temperature Lithium-Ion Batteries · Georgia Tech

Tried and failed

alloying active electrode with low-diffusivity metal applied to electrochemical metallization memristor devices. Outcome: unstable. Reason: low dopant diffusivity in the switching matrix failed to stabilize filament formation, showing poor switching uniformity and retention

Memristor-based AI Hardware for Reliable and Reconfigurable Neuromorphic Computing · MIT

Considered and rejected

Considered and rejected: Rejected metallic thin-film electrodes for high-strain DEAs due to elastic limits <5%, high Young's modulus, and susceptibility to cracking and conductivity loss

Reinforced Dielectric Elastomer Actuators: Anisotropic designs for the restoration of facial movements · EPFL

Considered and rejected

Considered and rejected: Rejected carbon paper and copper electrodes for alternating polarity due to severe electrode fracturing and catastrophic oxidative corrosion.

Towards Sacrificial Anode-Free Alkyne Electrocarboxylation · Queens University Institutional Repository

Tried and failed

defect-engineered compressed graphene film electrodes applied to lithium-ion battery anodes. Outcome: worse than baseline. Reason: multilayer solid electrolyte interphase formation blocked interlayer ion transport pathways, causing low initial coulombic efficiency

Design of Organic Frameworks for Electrochemical Energy Storage Applications · Georgia Tech

Tried and failed

direct covalent polymer grafting via esterification applied to metal oxide nanoparticle electrode slurries. Outcome: worse than baseline. Reason: caused severe capacity fade, poor rate capability, and high charge transfer resistance

Understanding interfacial phenomena for the creation of next-generation high-capacity battery electrodes · Georgia Tech

Tried and failed

block copolymer electrospun porous carbon fibers applied to flexible supercapacitor electrodes. Outcome: unstable. Reason: severe mechanical deformation caused structural degradation and contact loss in gel electrolyte

Block Copolymer Derived Porous Carbon Fiber for Energy and Environmental Science · Virginia Tech

Tried and failed

protective interface coating designed for solid-state mechanics applied to liquid electrolyte battery cathode. Outcome: worse than baseline. Reason: absence of mechanical constriction in liquid electrolyte caused worse cycling than bare cathode

Dynamic Electrochemical Processes at Solid-solid Interfaces in Alkaline Ion Batteries · Harvard

Tried and failed

Electron beam deposited chromium gold electrodes applied to electrochemical microfluidic sensing. Outcome: unstable. Reason: chromium adhesion layer oxidised under negative pre-deposition potential causing electrode corrosion and detachment

Design and Fabrication of Microfluidic Electrochemical Sensor for Lead Detection in Drinking Water · YorkSpace

Tried and failed

electrophoretic deposition on metal nanowires applied to graphene oxide coating on silver nanowires. Outcome: unstable. Reason: applied positive bias caused the metal nanowires on the electrode to undergo anodic dissolution

Development of Solution-Processed Stable Silver Nanowire Networks for Transparent Electrodes · MIT

Lost to a baseline

Electrodeposited granular gold nanostructures underperformed oxygen-plasma-functionalized ITO, delaminating 100% of PEDOT pads after 60 s probe sonication compared to 180 s survival on bare ITO.

Electrogenetics: Genetically Encoded Electrophysiology · DukeSpace

Considered and rejected

Considered and rejected: Rejected drawing crystalline metals (e.g., BiSn, Sn) for stimulation electrodes due to severe electrode surface degradation and electrochemical instability under electrical pulsing

Ultimate Feature Sizes in Thermally Drawn Fibers: from Fundamental Analysis to Novel Functional Fibers · EPFL

Considered and rejected

Considered and rejected: Rejected thin (<5 nm) tunneling insulator MIS photoelectrodes due to rapid chemical corrosion and lack of long-term stability in alkaline solutions.

Si-based photovoltaic and photoelectrochemical cells for high-efficiency solar energy harvesting · UT Austin

Electrode processing methods suffer from low porosity, film defects, and mass transport limitations

13 theses · 10 institutions

Fabricating thick slurry electrodes or incorporating high polymer contents created dense structures that impeded liquid convection and caused severe electrolyte depletion. Alternative manufacturing techniques like photopolymerization or drying methods failed to yield freestanding coatings, introduced high surface roughness, or trapped residual species that increased resistance.

Considered and rejected

Considered and rejected: Rejected pure GEL-NB formulations because they failed to form freestanding structural hydrogels suitable as electrode coatings.

An engineered biosynthetic hydrogel for 3D neural tissue interfaces · Imperial

Considered and rejected

Considered and rejected: Rejected creating dense particle-based slurry cathodes thicker than 110 µm because added theoretical capacity is inaccessible due to electrolyte depletion.

Transport Modeling and Design of Electrode Architectures for High Energy Density Batteries · ScholarlyCommons at Penn

Considered and rejected

Considered and rejected: Decided against using high polymer solids (>16 wt%) for gradient electrodes because resulting low porosities could not sustain forced liquid convection.

Designer Porous Carbon Electrodes for Redox Flow Batteries · MIT

Considered and rejected

Considered and rejected: LiCoO2 cathode rejected because it suffers from cycling instability and is very difficult to electrodeposit.

Utilization Of Mems Techniques For The Fabrication Of Scalable Energy Storage Devices · Penn

Considered and rejected

Considered and rejected: Graphite anode rejected due to difficulty in electrodepositing into scalable 3-D scaffold structures.

Utilization Of Mems Techniques For The Fabrication Of Scalable Energy Storage Devices · Penn

Considered and rejected

Considered and rejected: Rejected nanomaterial stretchable electrodes (carbon nanotubes, silver nanowires, graphene) due to inherently high surface roughness and low conductivity compared to conventional metals.

Low-noise Stretchable Organic Photodiodes Using an Elastomeric Bulk Heterojunction · Georgia Tech

Considered and rejected

Considered and rejected: Rejected non-aged or as-purchased mirror-polished nickel electrodes due to lack of stable in-situ electrocatalytic NiOOH layer

Insights into the Electrochemical Behavior of Coronavirus · Texas Tech

Tried and failed

direct in situ photopolymerization of hydrogel electrolytes applied to conducting polymer electrochemical transistors. Outcome: worse than baseline. Reason: in situ polymerization hindered channel dedoping capacity under electrical bias

Organic electrochemical transistors with PVA hydrogels/PEDOT:PSS channel · Imperial

Tried and failed

nanoparticle suspension additives in liquid monomer applied to in-situ polymerized battery electrolytes. Outcome: worse than baseline. Reason: particle addition degraded Coulombic efficiency and failed to provide intended ion compensation

IN-SITU POLYMERIZED SOLID ELECTROLYTES FOR LITHIUM BATTERIES · Cornell

Considered and rejected

Considered and rejected: Rejected incorporating PP1o1-TFSI directly into the bulk RTIL electrolyte for supercapacitors, choosing instead to infuse it into the carbon electrode (55 wt% AC, 30 wt% PP1o1-TFSI, 11 wt% AB, 7 wt% PVDF) to prevent competition with bulk ions and preserve bulk electrochemical stability.

Synthesis and characterization of ionic liquid electrolytes for use in electrical energy storage devices at elevated temperatures · OpenBU

Considered and rejected

Considered and rejected: Slurry-based electrode processing in favor of a solvent-free dry electrode process for flexible battery configuration

Development of niobium-based oxide anodes with the Wadsley-Roth shear structure for fast-charging and durable lithium-ion batteries · Georgia Tech

Considered and rejected

Considered and rejected: Rejected freeze-drying and supercritical drying for electrode preparation because capillary and restacking forces lower effective surface area; solvent exchange was selected instead.

Ionic Liquids as Electrolytes for Reduced Graphene Oxide Based Supercapacitors · Queens University Institutional Repository

Considered and rejected

Considered and rejected: Rejected heat-assisted evaporation of droplet solution because it permanently degraded electrode-nanotube baseline resistance

MINIATURIZED NEUTRON RADIATION DETECTOR USING BORON-NITRIDE AND MULTI-WALLED CARBON NANOTUBES · Calhoun

Considered and rejected

Considered and rejected: Decided against further exploration of NHS-graphene electrodes due to inability to control competing non-specific adsorption versus covalent trans-esterification.

Development of electrochemical sensors for nucleic acid biomarkers · Imperial

Solid electrolytes and metal anodes fail by dendrite penetration and catastrophic short circuiting

8 theses · 4 institutions

Inhomogeneous solid electrolyte interphases and poor mechanical toughness allow metal dendrites to penetrate through electrolyte cracks and microvoids during electrodeposition. Operating solid-state configurations at elevated currents or temperatures accelerated interphase decomposition and shorted the cells.

Tried and failed

solution casting composite electrolyte without polymer crosslinker applied to solid state lithium battery electrolyte. Outcome: unstable. Reason: phase separation and low mechanical strength led to early short circuit from dendrite penetration

Development of formable metal batteries (Mettery) · Imperial

Tried and failed

electrodeposition in pure carbonate solvent electrolytes applied to lithium metal anodes. Outcome: unstable. Reason: inhomogeneous solid electrolyte interphase causes dendritic morphology and low Coulombic efficiency

Electrodeposition and reversibility of Lithium metal in liquid electrolytes · Cornell

Tried and failed

single-layer solid electrolyte configuration applied to solid-state lithium metal batteries. Outcome: unstable. Reason: dendrite penetration through cracks causing short-circuits without multilayer mechanical protection

Electrochemical and Mechano-Electrochemical Stabilities in Solid-State Lithium Metal Batteries · Harvard

Tried and failed

slow initial nucleation current during electrodeposition applied to anode-free solid-state battery cycling. Outcome: no signal. Reason: did not improve cycling lifetime or prevent dendrite-induced short-circuiting during subsequent cycles

Probing Interfacial Dynamics in Solid-State Lithium Metal Batteries · Georgia Tech

Tried and failed

increasing plasticizing additive concentration applied to solid polymer electrolytes. Outcome: unstable. Reason: excess liquid additive degraded mechanical strength, causing premature dendrite penetration and short-circuiting

Development of formable metal batteries (Mettery) · Imperial

Tried and failed

direct melt-infiltrated solid electrolyte on metal anodes applied to all-solid-state lithium metal batteries. Outcome: unstable. Reason: interfacial chemical decomposition and rapid dendrite growth causing short-circuiting above low current densities

Low melting point solid electrolytes for scalable manufacturing of all-solid-state li-ion batteries · Georgia Tech

Tried and failed

single-layer unconstrained solid electrolyte baseline applied to high-current-density solid-state battery cycling. Outcome: unstable. Reason: unconstrained lithium dendrite penetration caused rapid capacity decay at high current density

Dynamic Electrochemical Processes at Solid-solid Interfaces in Alkaline Ion Batteries · Harvard

Considered and rejected

Considered and rejected: Rejected the Monroe-Newman stability model / criterion (shear modulus of electrolyte > 2x that of electrode to prevent dendrites) as oversimplified because it assumes perfect interfacial adherence and zero local concentration changes, contradicting experimental evidence that dendrites still penetrate high-modulus ceramic electrolytes.

Phase field-based electro-chemo-mechanical models for predicting interface degradation in solid-state batteries · Imperial

Considered and rejected

Considered and rejected: Rejected operating solid-state XPE electrolytes at elevated temperatures (>70 °C) without liquid swelling, as the exchange current density outpaced limiting transport, causing rapid cell shorting.

ENABLING STABLE LITHIUM NUCLEATION AND GROWTH VIA CROSSLINKED POLYMER ELECTROLYTES AND ELECTRODE/ELECTROLYTE INTERPHASES · Cornell

Considered and rejected

Considered and rejected: Rejected the LGPS (Li10GeP2S12 and Li10SnP2S12) family of solid-state electrolytes for practical lithium-metal batteries due to severe continuous mixed ionic-electronic interphase growth and absence of lithium plating.

Probing Interfacial Dynamics in Solid-State Lithium Metal Batteries · Georgia Tech

Considered and rejected

Considered and rejected: Using undoped Li5.5PS4.5Cl1.5 as the central electrolyte layer in multilayer all-solid-state batteries was rejected due to an excessively low decomposition energy (Ehull) that fails to promptly heal microcracks and prevent Li dendrite propagation.

Dynamic Electrochemical Processes at Solid-solid Interfaces in Alkaline Ion Batteries · Harvard

Left open by the authors

Problems the authors named and did not get to.

Left open

Improve cycling stability of DRXPS cathodes to over 500-1000 cycles using surface coatings, lattice doping, concentration gradients, and advanced electrolyte additives. Blocker: Requires a wet lab for battery material synthesis, coating application, and physical electrochemical cycle testing.

Polyanionizing rocksalt cathodes for lithium-ion batteries · MIT

Left open

Examine molecular interactions during battery cycling under varied SOC restrictions and electrolyte compositions to clarify negative kq mechanisms. Blocker: Requires wet lab electrochemistry equipment and static cell cycling experiments with specific chemical electrolytes.

Characterization of Electrodes and Electrolytes for Aqueous Organic Redox Flow Batteries Using Static Cells · Harvard

Left open

Develop electrolytes and interphases that lower the bulk-to-surface diffusivity ratio to prevent ion piling-up at the electrolyte/electrode interface. Blocker: Requires wet lab chemical synthesis and electrochemical characterization apparatus

Electrodeposition and reversibility of Lithium metal in liquid electrolytes · Cornell

Left open

Formulate and test an electrolyte stable against electrochemical decomposition and compatible with zinc battery electrode chemistries. Blocker: Requires a wet chemistry laboratory, physical chemical synthesis, and electrochemical testing apparatus.

SUPPRESSING PHYSICOCHEMICAL INSTABILITIES AT ELECTROCHEMICAL INTERFACES——TOWARDS SUSTAINABLE BATTERY ELECTRODES · Cornell

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Investigate FeF3-based solid-state sodium-ion batteries using solid electrolytes to reduce cathode dissolution. Blocker: Requires a wet/materials chemistry laboratory and experimental apparatus for synthesizing solid electrolytes and assembling solid-state battery cells

IMPROVING ELECTROCHEMICAL PERFROMANCE OF IRON TRIFLUORIDE (FeF3) IN SODIUM-ION BATTERIES · Georgia Tech

Left open

Fabricate and design large-scale inorganic-polymer composite solid-state electrolytes to prevent dendrite growth in sodium-based batteries. Blocker: Requires a wet lab and specialized physical materials synthesis and electrochemical testing equipment.

Nature-inspired carbon materials for emerging sodium-based energy storage technologies · Imperial

Left open

Formulate and test electrolytes that improve Li-ion mobility and desolvation kinetics while maintaining conductivity and charge transfer. Blocker: Requires a wet-lab chemistry setup to synthesize electrolytes and conduct electrochemical nitrogen reduction experiments.

The consequences of electrolyte engineering in electrochemical nitrogen reduction to ammonia · Imperial

Left open

Prepare aqueous polysulfide electrolytes with thiosulfate additives and evaluate their impact on thiosulfate formation and cell decay rates. Blocker: Requires a wet chemistry lab and battery testing hardware to synthesize electrolytes and measure electrochemical degradation

Aqueous Polysulfide Electrodes for Low-Cost Grid-Scale Energy Storage · MIT

Left open

Develop and optimize tailored electrolyte formulations and additives to reduce low-temperature charge transfer resistance on alloy anodes. Blocker: Requires a wet chemistry laboratory and electrochemical testing apparatus to synthesize and evaluate electrolyte formulations.

Investigating Reaction Mechanisms of Next-Generation Active Materials for Low-Temperature Lithium-Ion Batteries · Georgia Tech

Left open

Evaluate long-term cycling stability and optimize supercapacitor cells assembled using recycled ionic liquid electrolytes. Blocker: Requires wet lab facilities, electrochemical testing hardware, and physical synthesis of materials and recycled ionic liquids.

Ionic liquid-assisted process: biomass-derived carbonaceous materials · Imperial

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