asset_index	element_type	label	page	caption_source	suppress_in_index	duplicate_of	duplicate_reason	region_rescue_reason	visual_group_id	parent_visual_label	parent_visual_type	confidence	bbox	section	caption_preview	caption
1	figure	Docling Figure 1	1	missing_caption	False							0.55	[314.57, 410.37, 242.33, 104.54]	* S Supporting Information		
2	figure	Fig. 1	3	direct_caption_ref	False							0.82	[161.38, 66.05, 301.22, 412.29]	* S Supporting Information	Figure 1. (a) low magni fi cation and (b) high resolution STEM-HAADF images of the PNS layer in a pristine particle. White arrows in (b) indicate ordered features along (20 -2) planes. Red arrows in (b) indicated Li-sla…	Figure 1. (a) low magni fi cation and (b) high resolution STEM-HAADF images of the PNS layer in a pristine particle. White arrows in (b) indicate ordered features along (20 -2) planes. Red arrows in (b) indicated Li-slabs being inserted heavy TM cations in the PNS layer. A [010] direction C 2/ m crystal structure is shown as inset map in (b). Green: Li; Blue: Ni; Purple: Mn; Red: O. (c) STEM-HAADF image of EDS mapping area. The particle was tilted to [010] zone and its surface facets were determined. (d) Corresponding Ni elemental mapping. (e) Line scan signal counts across the PNS layer, whose location is shown in the STEM-HAADF image; (f) Quantitative Ni/Mn atomic ratios along the line scan. The Ni/Mn ratios are around 0.35 in bulk region, which is close to the designed value 0.33.
3	figure	Fig. 2	4	direct_caption_ref	False							0.82	[160.9, 64.69, 301.7, 350.7]	* S Supporting Information	Figure 2. (a-d) Low magni fi cation STEM-HAADF images to show cycling induced corrosion. Cracks and pits are highlighted by red arrows. (002) surface planes show strong resistance to corrosion. e-h) [010] zone axis SAED…	Figure 2. (a-d) Low magni fi cation STEM-HAADF images to show cycling induced corrosion. Cracks and pits are highlighted by red arrows. (002) surface planes show strong resistance to corrosion. e-h) [010] zone axis SAED patterns. Extra di ff raction spots appeared in cycled samples, which are highlighted by red and blue circles. Red circles indicated the formation of ordered structure. (10 -1) ordered plane is clearly seen after cycling. Blue circles come from double di ff raction. (i -l) High resolution STEM-HAADF images to show the cycling induced structure change on particle surfaces. Pristine samples (i) shows homogeneous structure from surface to bulk. Dashed lines in (j, k) highlight the thickness of the SRL. In (l), the whole areas were transformed. (m) [101] zone axis STEM-HAADF image and its fast Fourier transformation image. Blue arrows indicate the ordered features of (20 -2) planes and extra di ff raction spots. (n) [010] zone axis STEM-HAADF image to show spinel structure and I41 structure in a 45 cycled sample.
4	figure	Fig. 3	5	direct_caption_ref	False							0.82	[104.5, 67.51, 412.09, 458.65]	* S Supporting Information	Figure 3. (a-d) EDS mapping results from a 45 cycled LMR particle. The particle was tilted to the [010] zone axis and three surface facets were determined in (b). (e) Quantitative Ni/Mn ratios from surface and bulk posi…	Figure 3. (a-d) EDS mapping results from a 45 cycled LMR particle. The particle was tilted to the [010] zone axis and three surface facets were determined in (b). (e) Quantitative Ni/Mn ratios from surface and bulk positions as marked in (a); (f) line scan signal counts; (g) Quantitative Ni/ Mn atomic ratios along the line scan. The Ni/Mn ratios are around 0.26 in bulk region. (h)Low loss EELS spectra and (i) high low EELS spectra from di ff erent samples. 4.7 V bulk: spectrum collected from 4.7 V overcharged sample ' s bulk region; 100S: spectra collected from the surface of 100 cycled sample; 45S: spectra collected from the surface of 45 cycled sample; PNS: spectra collected from the Ni-rich surface of pristine sample; PS: spectra collected from pristine sample surface without Ni-rich layer; Li2O: spectrum collected from Li2O sample; Bulk: spectrum collected from pristine sample ' s bulk region. The degree of Li -K edge depression is 4.7 V bulk >100S > 45S ≈ PNS > PS. The order of Mn L3/L2 ratio is 100S > 45S > PNS ≈ PS ≈ Bulk.
5	figure	Fig. 4	7	direct_caption_ref	False							0.82	[99.49, 65.21, 426.88, 349.49]	* S Supporting Information	Figure 4. Comparison between experimental results and simulation results of di ff erent crystal models for the SRL from the [010] zone axis. I41 structure matches best in the four crystal models.	Figure 4. Comparison between experimental results and simulation results of di ff erent crystal models for the SRL from the [010] zone axis. I41 structure matches best in the four crystal models.
6	figure	Fig. 5	7	direct_caption_ref	False							0.82	[142.46, 454.0, 339.52, 205.34]	* S Supporting Information	Figure 5. Schematic diagram to show cycling induced surface layer evolution. At left side, the pristine particle has a C 2/ m structure and PNS layers are located at (20 -2) surface planes. After cycling, due to Ni 2+ m…	Figure 5. Schematic diagram to show cycling induced surface layer evolution. At left side, the pristine particle has a C 2/ m structure and PNS layers are located at (20 -2) surface planes. After cycling, due to Ni 2+ migration from bulk to surface, Mn 2+ surface aggregation and Li + depletion in surface layer, SRL is developed on particle surface except the PNS. The structure of surface layer transforms from original C 2/ m into I41 and fi nally developed spinel structure due to progressive TM enrichment and Li depletion. I41 structure is the main phase in the SRL.