Lynden Archer

Lynden Archer
Cornell University | CU · Department of Chemical and Biomolecular Engineering

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349
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Publications

Publications (349)
Article
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Solid‐state electrolytes (SSEs) formed inside an electrochemical cell by polymerization of a liquid precursor provide a promising strategy for overcoming problems with electrolyte wetting in solid‐state batteries. Hybrid solid‐state polymer electrolytes (HSPEs) created by in situ polymerization of a conventional liquid precursor containing electroc...
Article
The vast of majority of battery electrode materials of contemporary interest are of a crystalline nature. Crystals are, by definition, anisotropic from an atomic-structure perspective. The inherent structural anisotropy may give rise to favored mesoscale orientations and anisotropic properties whether the material is in a rest state or subjected to...
Article
Solid‐State Electrolytes In article number 2110333, Lynden A. Archer and co‐workers describe how polymerization of 1,3‐dioxolane, containing hairy nanoparticles of poly(ethylene glycol) chains densely grafted to SiO2 nanocores, inside an electrochemical cell, creates hybrid solid‐state electrolytes that offer enhanced wettability and additional deg...
Article
As a promising pathway toward low‐cost, long‐duration energy storage, rechargeable sodium batteries are of increasing interest. Batteries that incorporate metallic sodium as anode promise a high theoretical specific capacity of 1166 mAh g−1, and low reduction potential of −2.71 V. The high reactivity and poor electrochemical reversibility of sodium...
Article
Al-based batteries are considered an attractive alternative to Li metal batteries due to the use of Al metal as an anode with lower cost, lower reactivity and larger abundance compared to Li. Despite the aforementioned attributes, few electrolytes permit reversible electrodeposition of Al metal at room temperature. Thus, for the last 30 years, expe...
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Aqueous zinc batteries are attracting interest because of their potential for cost-effective and safe electricity storage. However, metallic zinc exhibits only moderate reversibility in aqueous electrolytes. To circumvent this issue, we study aqueous Zn batteries able to form nanometric interphases at the Zn metal/liquid electrolyte interface, comp...
Preprint
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How surface chemistry influences reactions occurring thereupon has been a long-standing question of broad scientific and technological interest for centuries. Recently, it has re-emerged as a critical question in a subdiscipline of chemistry - electrochemistry at heterointerphases, where the answers have implications for both how, and in what forms...
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We study the effects of interfacial kinetics on the electro-hydrodynamics of ion transport near an ion-selective surface using a combination of linear stability analysis and numerical simulation. The finite kinetics of the electrolyte–electrode interface affects the ion transfer and electroconvection in many ways. On a surface of fixed topography,...
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Control of crystallography of metal electrodeposit films has recently emerged as a key to achieving long operating lifetimes in next‐generation batteries. It is reported that the large crystallographic heterogeneity, e.g., broad orientational distribution, that appears characteristic of commercial metal foils, results in rough morphology upon plati...
Article
LiNO 3 is a widely used salt-additive that markedly improves the stability of ether-based electrolytes at a Li metal anode but is generally regarded as incompatible with alkyl carbonates. Here we find that contrary to common wisdom, cyclic carbonate solvents such as ethylene carbonate can dissolve up to 0.7 M LiNO 3 without any additives, largely i...
Article
LiNO 3 is a widely used salt-additive that markedly improves the stability of ether-based electrolytes at a Li metal anode but is generally regarded as incompatible with alkyl carbonates. Here we find that contrary to common wisdom, cyclic carbonate solvents such as ethylene carbonate can dissolve up to 0.7 M LiNO 3 without any additives, largely i...
Article
Secondary batteries based on earth-abundant, multivalent metals provide a promising path for high energy density and potentially low-cost electricity storage. Poor anodic reversibility caused by disordered metal crystallization during battery charging remains a fundamental, century-old challenge for the practical use of deep cycling metal batteries...
Article
Second life and recycling of retired automotive lithium-ion batteries (LIBs) have drawn growing attention, as large volumes of LIBs will retire in the coming decade. Here, we illustrate how battery chemistry, use, and recycling can influence the energy and environmental sustainability of LIBs. We find that LIBs with higher specific energy show bett...
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Lithium metal is a promising anode for energy-dense batteries but is hindered by poor reversibility caused by continuous chemical and electrochemical degradation. Here we find that by increasing the Li plating capacity to high values (e.g., 10–50 mAh cm⁻²), Li deposits undergo a morphological transition to produce dense structures, composed of larg...
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Lithium metal electrodeposits in the form of irregular morphological features, loosely termed dendrites, on planar anode substrates. The deposits may lead to rapid battery failure and safety concerns. Due to the highly reducing nature of Li (−3.04 V versus standard hydrogen electrode [SHE]), a solid electrolyte interphase (SEI) inevitably forms at...
Article
Reversible electrodeposition of metals at liquid-solid interfaces is a requirement for long cycle life in rechargeable batteries that utilize metals as anodes. The process has been studied extensively from the perspective of the electrochemical transformations that impact reversibility, however, the fundamental challenges associated with maintainin...
Article
The solid electrolyte interphase (SEI) is a chemically distinct material phase formed by a combination of electrochemical reduction and chemical reactions at both the explicit and implicit interfaces in all electrochemical cells. The structure, chemistry, and thermodynamics of the materials that accumulate in such interfacial material phases have e...
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Although Li-based batteries have established a dominant role in the current energy-storage landscape, post-Li chemistries (for example, Al or Zn) are emerging as promising candidates for next-generation rechargeable batteries. Electrochemical cells using Al or Zn metal as the negative electrode are of interest for their potential low cost, intrinsi...
Article
Electroconvective (EC) instability and its influence on surface morphological perturbations (Morph) are important in many applications, including electrodialysis, batteries, and fuel cells. In this work, we study the effects of a two-dimensional channel flow on the EC and Morph instabilities using two approaches. In the bulk analysis, we derive the...
Article
Full-text available
Formation of rough, dendritic deposits is a critical problem in metal electrodeposition processes and could occur in next-generation, rechargeable batteries that use metallic electrodes. Electroconvection, which originates from the coupling of the imposed electric field and a charged fluid near an electrode surface, is believed to be responsible fo...
Article
Li-O2 batteries are considered the ultimate energy storage technology for their potential to store large amounts of electrical energy in a cost-effective and simple platform. Large overpotentials for the formation and oxidation of Li2O2 during discharging and charging have thus far confined this technology to a scientific curiosity. Herein, we cons...
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The physiochemical nature of reactive metal electrodeposits during the early stages of electrodeposition is rarely studied but known to play an important role in determining the electrochemical stability and reversibility of electrochemical cells that utilize reactive metals as anodes. We investigated the early-stage growth dynamics and reversibili...
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Scalable approaches for precisely manipulating the growth of crystals are of broad-based science and technological interest. New research interests have reemerged in a subgroup of these phenomena—electrochemical growth of metals in battery anodes. In this Review, the geometry of the building blocks and their mode of assembly are defined as key desc...
Article
When ion transport in a binary liquid electrolyte is driven at potentials above the thermal voltage, an extended space charge region forms at the electrolyte/electrode interface and triggers the hydrodynamic instability termed electroconvection. We experimentally show that this instability can be completely arrested in soft colloidal suspension ele...
Preprint
Electroconvection and its coupling with a morphological instability are important in many applications, including electrodialysis, batteries and fuel cells. In this work, we study the effects of a two-dimensional channel flow on the electroconvective and morphological instabilities using two approaches. In the bulk analysis, we consider the instabi...
Article
The propensity of lithium to form nonplanar, mossy, or dendritic electrodeposits at current densities below the diffusion limit is a well-known, fundamental barrier to commercialization of energy-dense storage in lithium metal batteries. It has been proposed that proliferation of Li dendrites can be eliminated by controlling the uniformity and size...
Preprint
Full-text available
Muscle stem cells (MuSCs) are an essential stem cell population for skeletal muscle homeostasis and regeneration throughout adulthood. MuSCs are an ideal candidate for cell therapies for chronic and acute muscle injuries and diseases given their inherent ability to self-renew and generate progenitor cells capable of myogenic commitment and fusion....
Article
Reactive metals are known to electrodeposit with irregular morphological features on planar substrates. A growing body of work suggest that multiple variables — composition, mechanics, structure, ion transport properties, reductive stability, and interfacial energy of interphases formed either spontaneously or by design on the metal electrode play...
Article
The propensity of metal anodes of contemporary interest (e.g., Li, Al, Na, and Zn) to form non-planar, dendritic morphologies during battery charging is a fundamental barrier to achievement of full reversibility. We experimentally investigate the origins of dendritic electrodeposition of Zn, Cu, and Li in a three-electrode electrochemical cell boun...
Article
Rational approaches for achieving fine control of the electrodeposition morphology of Li are required to create commercially-relevant rechargeable Li metal batteries.
Article
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Solid‐state batteries enabled by solid‐state polymer electrolytes (SPEs) are under active consideration for their promise as cost‐effective platforms that simultaneously support high‐energy and safe electrochemical energy storage. The limited oxidative stability and poor interfacial charge transport in conventional polymer electrolytes are well kno...
Article
Strong polarization of the ion distribution in liquid electrolytes subjected to potential differences exceeding the thermal voltage, VT = kT/e, produces a hydrodynamic instability termed electroconvection at ion-selective interfaces. Electroconvection is desirable in some situations (e.g., electrodialysis) because it promotes mixing in a stagnant e...
Article
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Many modern energy devices rely on solid-liquid interfaces, highly reactive materials, or both, for their operation and performance. The difficulty of characterizing such materials means these devices often lack high-resolution characterization in an unaltered state. Room temperature FIB/SEM routinely enables nanoscale surface and cross-sectional i...
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Solid-state electrolytes (SSEs) have emerged as high-priority materials for safe, energy-dense and reversible storage of electrochemical energy in batteries. In this Review, we assess recent progress in the design, synthesis and analysis of SSEs, and identify key failure modes, performance limitations and design concepts for creating SSEs to meet r...
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The propensity of metals to form irregular and nonplanar electrodeposits at liquid-solid interfaces has emerged as a fundamental barrier to high-energy, rechargeable batteries that use metal anodes. We report an epitaxial mechanism to regulate nucleation, growth, and reversibility of metal anodes. The crystallographic, surface texturing, and electr...
Article
Understanding cation (H+, Li+, Na+, Al3+ etc.) intercalation/de‐intercalation chemistry in transition metal compounds is crucial for the design of cathode materials in aqueous electrochemical cells. Here we report that orthorhombic vanadium oxides (V2O5) supports highly reversible proton intercalation/de‐intercalation reactions in aqueous media, en...
Article
Understanding cation (H+, Li+, Na+, Al3+ etc.) intercalation/de‐intercalation chemistry in transition metal compounds is crucial for the design of cathode materials in aqueous electrochemical cells. Here we report that orthorhombic vanadium oxides (V2O5) supports highly reversible proton intercalation/de‐intercalation reactions in aqueous media, en...
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Rechargeable electrochemical cells with metallic anodes are of increasing scientific and technological interest. The complex composition, poorly defined morphology, heterogeneous chemistry, and unpredictable mechanics of interphases formed spontaneously on the anodes are often examined but rarely controlled. Here, we couple computational studies wi...
Article
The morphologies metal electrodeposits adopt during the earliest stages of electrodeposition are known to play a critical role in the recharge of electrochemical cells that use metals as anodes. Here we report results from a combined theoretical and experimental study of the early-stage nucleation and growth of electrodeposited lithium at liquid-so...
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Electrochemical cells based on alkali metal anodes are receiving intensive scientific interest as potentially transformative technology platforms for electrical energy storage. Chemical, morphological, mechanical and hydrodynamic instabilities at the metal anode produce uneven metal electrodeposition and poor anode reversibility, which, are among t...
Article
New electrolyte designs are necessary for overcoming multiple challenges posed by emerging lithium-metal battery chemistries. Task-specific viscoelastic electrolytes are specifically required that are capable of simultaneously sustaining reversible electrochemistry at the Li metal anode, maintaining high oxidative stability at the battery cathode,...
Article
Metallic sodium is receiving renewed interest as a battery anode material because the metal is earth‐abundant, inexpensive, and offers a high specific storage capacity (1166 mAh g−1 at −2.71 V vs the standard hydrogen potential). Unlike metallic lithium, the case for Na as the anode in rechargeable batteries has already been demonstrated on a comme...
Article
High-resolution Electron Imaging and Spectroscopy of Reactive Materials and Liquid-Solid Interfaces in Energy Storage Devices - Volume 25 Supplement - Michael J. Zachman, Zhengyuan Tu, Snehashis Choudhury, Taylor Moon, Qing Zhao, Lynden A. Archer, Lena F. Kourkoutis
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Electrochemical cells that utilize lithium and sodium anodes are under active study for their potential to enable high-energy batteries. Liquid and solid polymer electrolytes based on ether chemistry are among the most promising choices for rechargeable lithium and sodium batteries. However, uncontrolled anionic polymerization of these electrolytes...
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Modern robots lack the multifunctional interconnected systems found in living organisms and are consequently unable to reproduce their efficiency and autonomy. Energy-storage systems are among the most crucial limitations to robot autonomy, but their size, weight, material and design constraints can be re-examined in the context of multifunctional,...
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Solid-state electrolytes with high room-temperature ionic conductivity and fast interfacial charge transport are a requirement for practical solid-state batteries. Here, we report that cationic aluminium species initiate ring-opening polymerization of molecular ethers inside an electrochemical cell to produce solid-state polymer electrolytes (SPEs)...
Article
Direct numerical simulations of a liquid electrolyte with polymer additives demonstrate that viscoelasticity promotes an earlier transition from steady to unsteady electroconvective flow. Viscoelasticity also decreases the overlimiting current resulting from convection by up to 40%. Both of these effects would reduce the time-averaged spatial varia...
Article
Conversion of low‐value, but thermodynamically stable chemical byproducts such as alkanes or CO2 to more valuable feedstocks is of broad‐based interest. These so‐called up‐conversion processes are expensive because they require energy‐intensive and catalytically‐driven processes to drive reaction against thermodynamic gradients. Here we show that t...
Article
Conversion of low‐value, but thermodynamically stable chemical byproducts such as alkanes or CO2 to more valuable feedstocks is of broad‐based interest. These so‐called up‐conversion processes are expensive because they require energy‐intensive and catalytically‐driven processes to drive reaction against thermodynamic gradients. Here we show that t...
Article
We report on the design of a battery electrode architecture in which ion and electronic transport pathways are continuous, and span the entire volume of a thick, non-planar electrode. It is shown that for a range of active materials conductivities, the length scale for electronic transport in such an architecture can be tuned by simple manipulation...
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Electrochemical cells based on aluminum (Al) are of long-standing interest because Al is earth abundant, low cost, and chemically inert. The trivalent Al ³⁺ ions also offer among the highest volume-specific charge storage capacities (8040 mAh cm ⁻³ ), approximately four times larger than achievable for Li metal anodes. Rapid and irreversible format...
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Practical lithium metal batteries require full and reversible utilization of thin metallic Li anodes. This introduces a fundamental challenge concerning how to create solid-electrolyte interphases (SEIs) that are able to regulate interfacial transport and protect the reactive metal, without adding appreciably to the cell mass. Here, we report on ph...
Article
Solid-state electrolytes are an attractive alternative to conventional liquid electrolytes in lithium batteries because of their intrinsic safety features and superior mechanical properties. Maintaining high bulk and interfacial ion fluxes in batteries that utilize solid-state electrolytes remains a significant challenge. We report on synthesis and...
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Probing the Native Structure and Chemistry of Dendrites and SEI Layers in Li-Metal Batteries by Cryo-FIB Lift-Out and Cryo-STEM - Volume 24 Supplement - Michael J. Zachman, Zhengyuan Tu, Lynden A. Archer, Lena F. Kourkoutis
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Full-text available
Solid-liquid interfaces are important in a range of chemical, physical and biological processes1-4, but are often not fully understood owing to the lack of high-resolution characterization methods that are compatible with both solid and liquid components5. For example, the related processes of dendritic deposition of lithium metal and the formation...
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Approaches for regulating electrochemical stability of liquid electrolytes in contact with solid-state electrodes are a requirement for efficient and reversible electrical energy storage in batteries. Such methods are particularly needed in electrochemical cells in which the working potentials of the electrodes lie well outside the thermodynamic st...
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Electrodeposition is a widely practiced method for creating metal, colloidal, and polymer coatings on conductive substrates. In the Newtonian liquid electrolytes typically used, the process is fundamentally unstable. The underlying instabilities have been linked to failure of microcircuits, dendrite formation on battery electrodes, and overlimiting...
Article
Lithium ion batteries (LIBs) are the dominant power source in portable device technology and are poised to play a similar, dominant role in electrified transportation systems. While significant strides have been made in recent years in evolving the cathode chemistry and electrolyte formulations to meet higher energy storage demands, almost all cont...
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Grenzschichten zwischen metallischer Elektrode und Elektrolyt (SEI) müssen elastisch sein und Volumenänderungen der Elektrode ausgleichen können. In ihrer Zuschrift (DOI: 10.1002/ange.201711598) beschreiben L. A. Archer et al. die Verwendung von SiCl4 als Vernetzungsreagens zur Abscheidung von Hybrid-Grenzschichten auf Li-Anoden. Die Hybrid-SEIs be...