battery design logic

=chemistry =batteries =energy

 

 

Why do I like the battery chemistries I do?

 

 

background

 

A battery is a chemical reaction separated by a barrier that only allows ions and inert molecules to pass. This couples the reaction to transfer of electric charge. Most batteries use a liquid electrolyte that dissolves ions but not reactants. For example, an alkaline battery uses zinc metal and manganese oxides, and neither dissolves in alkaline water, but zinc ions do.

If there's leakage, even at 1/1000th the maximum discharge rate, that's a big problem. The reactants must have negligible solubility in the electrolyte, and usually that's only the case for solids, because low solubility implies strong self-interaction which usually implies high melting points, so electrodes are generally solid. The reactants must also have some electrical conductivity, even if they're small particles embedded in a conductive matrix.

Lithion-ion batteries typically use a polypropylene mesh as separator, and the battery layers are so thin that even that mesh is a nontrivial fraction of the battery cost. It's possible to make polymer membranes that are selective for positive or negative ions. This involves a complex internal microstructure. Such membranes are obviously much more expensive than a mesh and liquid electrolyte - too expensive for batteries for electric cars. For grid energy storage, the charge/discharge rates are much lower, so membranes are closer to economic viability, but still too expensive and/or not durable enough. (Also, electricity is worth more in an electric car than as grid power.) Ion-selective polymer membranes also tend to have some leakage, which can permanently reduce battery capacity for some chemistries. Cost also depends on voltage: higher voltage is better. Form Energy has a low cell voltage, and the membranes are too expensive. So, ion-selective polymer membranes are rejected.

A ceramic electrolyte is obviously much more expensive than a flexible polymer membrane, which is already too expensive. It's hard to make lots of thin ceramic without cracks that stuff can leak through or metal dendrites can form through. Ceramic electrolytes can work at high temperatures and make things like sodium-sulfur batteries work, but they're too expensive. So, ceramic electrolytes are rejected.

Dendritic deposition is a big problem for batteries. Alkaline batteries can't be recharged mainly because the zinc metal forms needles because a shorter path has less resistance. Lithium metal does the same thing, which is why lithium complexed with graphite is used despite being more expensive and having less capacity. The electrolyte needs to reach everywhere in the graphite, but it also has to all be connected to be conductive. That requires somewhat expensive processing.

There are rechargeable zinc flow batteries. If electrolyte flows over the zinc surface fast enough, it prevents dendritic deposition. However, doing this is more expensive.

There are now many startups pursuing lithium-metal batteries with ceramic electrolytes to block dendrites. Thin ceramic electrolytes without cracks are too expensive for this, so those startups will fail. Another problem is getting good contact, which usually requires high pressure (which can cause ceramics to crack) or a liquid on the lithium-metal side. Having a liquid there leads to another problem: resistance. In lithium-ion batteries, a solid-electrolyte interphase (SEI) forms on the particles of lithium x graphite, from decomposition of the electrolyte. This SEI increases resistance and thickens over time, reducing capacity, but it protects the Li x graphite from further reaction. With a lithium-metal battery, the SEI forms on a flat sheet, so the surface area is lower, so the resistance is higher.

 

 

sodium-ion

 

Lithium is somewhat expensive. How about a lithium-ion battery, but with sodium instead? Sodium gives only 0.3v lower voltages than lithium, which is good. The extra mass of Na vs Li isn't a big problem, and neither is diffusion rate through electrolyte. The problem is with the electrodes.

Na doesn't complex with graphite as well as Li does. You need a lot more graphite to do the same thing. So, the negative electrodes for Na-ion batteries are a problem.

Li is a smaller ion than Na, which means it fits into crystals better. For example, the structure of LiFePO4 is more similar to FePO4 than NaFePO4 is. That means Na gives higher resistance and faster degradation of positive electrodes. So, the negative electrodes for Na-ion batteries are also a problem. There are some organic molecules that work with sodium, but they're too expensive, degrade over time, and have poor specific energy.


magnesium

 

Magnesium is cheap, has good theoretical capacity, and gives the same voltage as sodium. The main problem is that it has a much higher charge density than lithium, so it has stronger interactions with everything, which increases the energy barrier of it moving between things. This is especially a problem in the SEI.

Li-ion batteries use electrolytes like LiPF6, LiBF4, and LiClO4. These form SEIs that have low but adequate Li+ ion conductivity. If you try to make a Mg-ion battery with the corresponding Mg salts, you get a SEI of MgO or MgF2, and those aren't conductive at all.

 

 

what's the goal?

 

Suppose you replace the Li of a Li-ion battery with Na or Mg and get the same performance. This is good because it reduces material costs, but the cost of Li is only a fraction of the battery cost, so the improvement is limited. If the positive electrode gets more expensive, or performance is worse, then it's probably not worth it.

The positive electrode of Li-ion batteries is expensive because:

- it might contain cobalt and/or nickel
- it has to be porous with electrolyte contacting small particles
- it needs to be continuously connected with conductive material

 

These complex requirements require somewhat expensive processing, and that's part of what I wanted to avoid.

 

 

sulfur

 

What if you used sulfur <-> sulfide as a reaction? Solid sulfur isn't electrically conductive, but polysulfides are soluble in, for example, water and molten sulfur. Sulfur particles can be reduced at their surface, dissolving as polysulfides that are reduced to sulfides.

Of course, you then have a liquid containing polysulfides, which would react with the negative electrode. The polysulfides must be kept separate from it to avoid permanent degradation, which is hard. This requires a ceramic membrane or a very high-performance polymer membrane, which is too expensive.

There are startups working on lithium-sulfur batteries, but they have no solution for this problem, so they will fail. Sodium-sulfur batteries work, but again, the ceramic electrolyte is too expensive.

 

 

bromine

 

Zinc-bromine batteries have been made. Bromine, conveniently, can be stored as a liquid at room temperature, and it's easy to convert between Br- and Br2 so electrode overpotential is low.

A membrane is obviously needed to prevent Br2 from just reacting with zinc directly. You might note that Br2 is not charged, which means ion-selective membranes can't reject it very effectively. How, then, do zinc-bromine batteries prevent Br2 from crossing over? The answer is, they don't. Lifetimes are short and continuous electrolyte regeneration to put the bromine back was too expensive. You also still need a cation-exchange membrane because bromine forms Br3- ions, and again, that's somewhat expensive.

Anyway, the specific energy of zinc-bromine batteries is too low for good electric cars.

 

 

what options remain?

 

Suppose we want to make a low-cost battery with abundant materials that's suitable for electric cars.

- Lithium, cobalt, nickel, vanadium are rejected because they're expensive and limited.
- Palladium, platinum, and rhodium are too expensive and rare to use even as catalysts.
- Ceramic electrolytes are too expensive. Polymer membranes are too expensive.
- Current lithium-ion anode and cathode materials are rejected for being too expensive.
- Because lithium is rejected, current lithium-ion cathode materials that don't work well for other ions are rejected.
- Chemistries with specific energy too low for electric cars are rejected.

 

What is left?

The anode must be solid metal. That means the SEI must have lower resistance than current ones. It also means a method to prevent dendritic deposition is needed.

The only cathode options left are:

- things that are too expensive
- manganese oxide
- things that aren't conductive

 

While it's not a problem for non-rechargeable alkaline batteries, manganese oxide cathodes tend to have relatively poor cycle life. When used with Mg, there's a tendency to form non-conductive MgO layers.

If the active material at the cathode isn't conductive, then it must react and dissolve at the surface, and it must be inside a conductive liquid.

If the cathode has a conductive liquid (CL), then there must be a separate electrolyte layer to prevent self-discharge. Membranes are too expensive, so that must be another electrolyte liquid (EL). For it to be a separate layer, CL and EL must be immiscible. To prevent battery degradation, the active material must have negligible solubility in EL. For acceptable conductivity and self-discharge, the conductive material must have much higher solubility in CL than EL, >1000x higher.

For all this to be the case, CL and EL must be maximally different types of liquid, but both must conduct ions.

The biggest difference between CL and EL you can get while conducting ions through both is low-polarity ethers vs something high-polarity. High-polarity stuff tends to react with a metal anode, so EL must be low-polarity, and CL must then be high-polarity.

High polarity means strong interactions, but CL also needs to be liquid and have low viscosity, which are conflicting requirements.

 

 

So, those are the requirements I tried to meet:

- nonpolar EL
- very polar CL
- very polar cathode active material
- solid metal anode
- low-resistance SEI
- no dendritic deposition

 

The result worked as far as I was able to test it, but that required several new elements, which seems to make designs hard to understand.

 




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