Supplementary Information Mesoscale Origin of the Enhanced Cycling-Stability of the SiConductive Polymer Anode for Li-ion Batteries Meng Gu1, Xingcheng Xiao2, Gao Liu,3* Suntharampillai Thevuthasan1, Donald R. Baer1, Ji-Guang Zhang4, Jun Liu4, Nigel D. Browning5, and Chongmin Wang1* 1 Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA 99352, USA 2 General Motors Global Research & Development Center, 30500 Mound Road, Warren MI 48090, USA 3 Lawrence Berkeley National Laboratory, 1 Cyclotron Rd Berkeley, CA 94720, USA 4 Energy and Environmental Directorate, Pacific Northwest National Laboratoy, Richland, WA 99352, USA, 5 Fundamental and Computational Science Directorate, Pacific Northwest National Laboratory, Richland, WA 99352, USA *Authors to whom all correspondence should be addressed: gliu@lbl.gov; Chongmin.wang@pnnl.gov The supporting information includes the following content 1) Supporting on-line movie showing the concordant deformation of silicon nanoparticle-conductive polymer composite upon lithiation/delithiation and the lithium insertion process in the materials prepared by conventional method. 2) Additional figures Fig S1 (a) overall view TEM image of the classic composite anode (b) schematic drawing of the classic composite approach Fig S2 The experimental (a) and schematic drawing of the set-up for in-situ electrochemical dilatometer measurement 1 Fig S3. Plotted area changes of the functional composite, single np #1, #2 during in-situ lithiation observation. Fig S4 Experimental in-situ TEM observation showing that part of the Si NPs remains unlithiated during the lithiation process; Note that the unlithiated region shows dark crystalline diffraction contrast in the TEM image. 2 Fig S1 (a) overall view TEM image of the classic composite anode (b) schematic drawing of the classic composite approach 3 Fig S2 The experimental (a) and schematic drawing of the set-up for in-situ electrochemical dilatometer measurement 4 Area change (times) 3.0 functional composite single np 1 single np 2 2.5 2.0 1.5 1.0 0.0 0.5 1.0 Lithiation state Fig S3. Plotted area changes of the functional composite, single np #1, #2 during in-situ lithiation observation. 5 Fig S4 Experimental in-situ TEM observation showing that part of the Si NPs remains unlithiated during the lithiation process; Note that the unlithiated region shows dark crystalline diffraction contrast in the TEM image. 6