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Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A. This journal is The Royal Society of Chemistry 2017 Supporting Information Ultrathin Petal-like NiAl Layered Double oxide/sulfide Composites as Advanced Electrode for High-performance Asymmetric Supercapacitor Lei Li a, Kwan San Hui b*, Kwun Nam Hui c*, and Young-Rae Cho a* a School of Materials Science and Engineering, Pusan National University, San 30 Jangjeondong, Geumjeong-gu, Busan 609-735, Republic of Korea b School of Mathematics, University of East Anglia, Norwich, NR4 7TJ, United Kingdom c Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Macau, China *Corresponding author: E-mail: k.hui@uea.ac.uk (Kwan San Hui) E-mail: bizhui@umac.mo (Kwun Nam Hui) E-mail: yescho@pusan.ac.kr (Young Rae Cho) 1

Table S1. Elements composition (at%) of the NiAl LDO/LDS composites analyzed by XPS Sample Element Ni Al O S C NiAl LDO/LDS 31.65 8.76 35.71 5.06 18.82 2

Fig. S1. (a) XRD pattern of NiAl LDO/LDS composites at different sulfidation temperature, and the corresponding SEM images of (b) 400 C,(c) 600 C and (d) 700 C. 3

Fig. S2. XPS pattern of the oxygen element in the NiAl LDO/LDS composites. 4

Fig. S3. (a) TEM image, (b) AFM image, and (c) height profile of the NiAl LDO/LDS composites. 5

Fig. S4. Cycling performance and Coulombic efficiency of the NiAl LDH and NiAl LDO/LDS composites at a current density of 5 A g 1. 6

Table S2. EIS fitting parameters of NiAl LDH and NiAl LDO/LDS electrodes Sample R s (Ω) C dl (F) R ct (Ω) W (Ω) C F (F) NiAl LDH 0.665 0.0024 12.53 2.452 1.94 NiAl LDO/LDS 0.499 0.0058 0.308 2.612 3.52 7

Table S3. Comparison of the electrochemical performance of the NiAl LDO/LDS composites with the reported materials in literature Materials Current density Specific capacitance Ref. (A g -1 ) (F g -1 ) CoNi 0.5 LDH 1 1938 [1] Ni 1-x Co x Al-LDH 1 1902 [2] CNTs/NiAl-LDH 1 694 [3] MXene/NiAl LDH 1 1061 [4] NiCo 2 O 4 @NiCoAl- 1 1814.24 [5] LDH Co 3 O 4 @NiCoAl- 1 1104 [6] LDH Ni 3 S 2 1 1670 [7] Ni 3 S 2 @Ni(OH) 2 /G 5.1 1037.5 [8] NiO/Ni 3 S 2 1 2153 [9] MnCo 2 S 4 1 2067 [10] NiS 2 1 1020.2 [11] NiS 2 /ZnS 1 1198 [12] Nickel sulfides/mos 2 0.5 757 [13] Ni 3 S 2 /NiS 2 1158 [14] 8

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