1

Supporting Information

Probing Enhanced Lithium-Ion Transport Kinetics in 2D

Holey Nanoarchitectured Electrodes

Xiao Zhang 1,7

, Andrea M. Bruck 2,7

, Yue Zhu 1, Lele Peng

1, Jing Li

2, Eric Stach

3, Yimei Zhu

4,

Kenneth J.

Takeuchi 2,5

, Esther S. Takeuchi 2,5,6

, Amy C. Marschilok2,5,8

and Guihua Yu 1,8

1Materials Science and Engineering Program and Department of Mechanical Engineering, The University

of Texas at Austin, Austin, Texas 78712, United States

2Department of Materials Science and Chemical Engineering, SUNY-Stony Brook University, Stony

Brook, New York 11790, United States

3Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia,

Pennsylvania 19104, USA

4Condensed Matter Physics and Materials Science, Brookhaven National Laboratory, Upton, New York

11973, United States

5Department of Chemistry, SUNY-Stony Brook University, Stony Brook, New York 11794, United States

6Energy Sciences Directorate, Brookhaven National Laboratory, Interdisciplinary Sciences Building,

Upton, New York 11973, United States

7These authors contributed equally to this work.

8Authors to whom any correspondence should be addressed.

*E-mail: ghyu@austin.utexas.edu and amy.marschilok@stonybrook.edu

2

Supporting Figures

Figure S1. (a) (b) STEM images of the as-synthesized ZFO HNS exhibiting 2D holey nanosheet architecture.

3

Figure S2. Pore size histograms of as-synthesized ZFO HNS. (Size information was obtained

directly from TEM images.)

4

Figure S3. (a) Specific capacities of ZFO NP and ZFO HNS under different current densities

(0.4, 0.8, 1.6, 3.2 and 5.0 A g-1). (Data is plotted based on rate performance results of 4 samples.)

5

Figure S4. Charge-discharge profiles of (a) ZFO NP and (b) ZFO HNS.

6

Figure S5. Cycling tests of ZFO NP and ZFO HNS under current density of 0.4 A g-1.

7

Figure S6. Variation of cell voltage of (a) ZFO NP and (b) ZFO HNS versus square root of

titration time in a single titration step satisfying linear relationship of GITT calculation

supposition.

8

Figure S7. CV curves of ZFO NP and ZFO HNS under scan rate of 0.02 mV s-1.

9

Figure S8. (a) Original data of in situ XRD showing phase evolution and (b) corresponding

discharge profile of ZFO NP.

10

Figure S9. Galvanostatic discharge curves of ZFO NP and ZFO HNS during the first discharge

in the pouch cell.

11

Figure S10. (a) Cyclic voltammetry under different scan rates and (b) b-value evaluation using

the relationship between peak current and scan rate of ZFO NP and the same set (c-d) of ZFO

HNS.

12

Figure S11. Simulated equivalent circuit of the Nyquist plots.

This equivalent circuit model includes a series resistance (Rs), SEI resistance (RSEI) and

capacitance (RSEI), electron transfer resistance (Re) and capacitance (Ce), charge transfer

resistance (Rct), double-layer capacitance (Cdl) and Warburg impedance (W), respectively.

13

Table S1. Summarized average values of particle size and pore size of ZFO HNS and ZFO NP samples.

Samples Average particle size / nm Average pore size / nm

ZFO HNS 7.7 6.8

ZFO NP 6.1

14

Table S2. Simulated charge transfer impedance (Rct) in ZFO HNS and ZFO NP under various electron

equivalents.

Electron equivalents ZFO HNS ZFO NP

0 ee 63.1 Ω 963.5 Ω

2.1 ee 86.2 Ω 1565.0 Ω

5.0 ee 26.8 Ω 1187.0 Ω

7.9 ee 21.6 Ω 535.7 Ω

Fully discharged 20.5 Ω 501.0 Ω

15

Table S3. Simulated SEI impedance (RSEI) in ZFO HNS and ZFO NP under various electron

equivalents.

Electron equivalents ZFO HNS ZFO NP

0 ee 23.4 Ω 25.4 Ω

2.1 ee 31.5 Ω 37.4 Ω

5.0 ee 3.6 Ω 11.7 Ω

7.9 ee 3.9 Ω 14.8 Ω

Fully discharged 3.3 Ω 11.5 Ω