Bio‐Inspired Computational Design of Vascularized Electrodes for High‐Performance Fast‐Charging Batteries Optimized by Deep Learning

Abstract

Slow ionic transport and high voltage drop (IR drop) of homogeneous porous electrodes are the critical causes of severe performance degradation of lithium‐ion batteries at high charging rates. Herein, it is numerically demonstrated that a bio‐inspired vascularized porous electrode can simultaneously solve these two problems by introducing low tortuous channels and graded porosity, which can be verified by porous electrode theory. To optimize the vasculature structural parameters, artificial neural networks are employed to accelerate the computation of possible structures with high accuracy. Furthermore, an inverse‐design searching library is compiled to find the optimal vascular structures under different industrial fabrication and design criteria. The prototype delivers a customizable package containing optimal geometric parameters and their uncertainty and sensitivity analysis. Finally, the full‐vascularized cell shows a 66% improvement in charging capacity compared to the traditional homogeneous cell under 3.2 C current density in a numerical simulation. This computational research provides an innovative methodology to solve the fast‐charging problem in batteries and broaden the applicability of deep learning algorithms to different scientific or engineering areas.

Architected Low‐Tortuosity Electrodes with Tunable Porosity from Nonequilibrium Soft‐Matter Processing

“…[2,3,[12][13][14][15][16][17][18][19][20][21][22][23] To increase the energy density while maintaining a high power output, computational and experimental results suggest that the diameter of the low-tortuosity pores and the thickness of the solid matrix with the active charge-storing material should be in the range of 5-20 µm, smaller than what is obtained from many of the aforementioned fabrication methods. [3,[24][25][26] Critical in the design of these electrodes is the aspect ratio between the pore diameter (D p ) and overall thickness of the electrode (h e ), as well as the material-to-pore ratio given by the thickness of the solid matrix (t m ) and D p , which defines the electrode density Mass transport is performance-defining across energy storage devices, often causing limitations at high current rates. To optimize and balance the devicescale energy and power density for a given energy storage demand, tailored electrode architectures with precisely controllable phase dimensions are needed in combination with low-tortuosity channels that maximize the geometric component of diffusion and species flux.…”

“…Tailoring ratios between D p , t m and h e within low-tortuosity architectures to accommodate for the demanded in-plane supply of ions to the active material at a given current rate will allow for application-specific optimization between energy and power densities in this multidimensional parameter design space. [3,19,20,[24][25][26] Here we report the nonequilibrium soft matter processing technique of hybrid inorganic phase inversion (HIPI) that meets the challenge to fabricate free-standing and low-tortuosity composite electrode architectures. HIPI is a scalable manufacturing strategy that allows for individualized tuning of the most impactful structural features on relevant length scales.…”

“…[ 2,3,12–23 ] To increase the energy density while maintaining a high power output, computational and experimental results suggest that the diameter of the low‐tortuosity pores and the thickness of the solid matrix with the active charge‐storing material should be in the range of 5–20 µm, smaller than what is obtained from many of the aforementioned fabrication methods. [ 3,24–26 ] Critical in the design of these electrodes is the aspect ratio between the pore diameter ( D p ) and overall thickness of the electrode ( h e ), as well as the material‐to‐pore ratio given by the thickness of the solid matrix ( t m ) and D p , which defines the electrode density and porosity ( Figure A). Tailoring ratios between D p , t m and h e within low‐tortuosity architectures to accommodate for the demanded in‐plane supply of ions to the active material at a given current rate will allow for application‐specific optimization between energy and power densities in this multi‐dimensional parameter design space.…”

Unraveling the Effects of Hierarchical Bimodal Microscale Porosity on Thick Electrodes

“…Nature has already given plenty of examples for minimizing transport resistance in a certain system. 26 To adapt to external environments, a hierarchically porous network in natural systems could accomplish delivering nutrition with an extraordinary efficiency. 27,28 Systems with hierarchical pores that are interconnected in multiple length scales are often observed in plant peels, human bones, and vascular and respiratory systems.…”

“…Nature has already given plenty of examples for minimizing transport resistance in a certain system . To adapt to external environments, a hierarchically porous network in natural systems could accomplish delivering nutrition with an extraordinary efficiency. , Systems with hierarchical pores that are interconnected in multiple length scales are often observed in plant peels, human bones, and vascular and respiratory systems. , Considering this, we hypothesize that transport efficiency can be maximized, with porosity remaining constant while applying pore hierarchy in thick electrodes, as shown in the right part of Scheme a.…”