Table S1. Summary of data collections and structure refinements for crystals 1Rb-1h, 1Rb-2h, and 1Rb-4h.

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Supporting Information [NH 3 CH 3 ] [In SbS 9 SH]: A novel methylamine-directed indium thioantimonate with Rb + ion-exchange property Kai-Yao Wang a,b, Mei-Ling Feng a, Jian-Rong Li a and Xiao-Ying Huang *,a a State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, the Chinese, Academy of Sciences, Fuzhou, Fujian 350002, P.R. China b Graduate University of the Chinese Academy of Sciences, Beijing 10009, P. R. China Fax: +86 591 83793727; Tel: +86 591 83793727; E-mail: xyhuang@fjirsm.ac.cn Table S1. Summary of data collections and structure refinements for crystals 1Rb-1h, 1Rb-2h, and 1Rb-h. 1Rb 1h 1Rb 2h 1Rb h Empirical formula Formula weight Crystal system Space group T/K λ/å a/å b/å c/å α/º β/º γ/º V/Å 3 Z D c /Mg m -3 μ/mm -1 F(000) Measured refls. Independent refls. C 3.6 H 22.8 In N 3.6 O 0.1 Rb 0. S 10 Sb 105.07 13.8981() 13.8981() 13.8981() 268.52(13) 2.608 5.875 1969 2659 172 C 3.2 H 20.6 In N 3.2 O 0.2 Rb 0.8 S 10 Sb 1077.23 13.8535(8) 13.8535(8) 13.8535(8) 2658.8(3) 2.691 6.659 2002 2751 1781 C 2.75 H 18.12 In N 2.75 O 0.3125 Rb 1.25 S 10 Sb 1103.29 13.791(13) 13.791(13) 13.791(13) 2623.2() 2.79 7.577 2038 2652 1680 R int No. of parameters GOF Flack parameter a R 1, wr 2 [I > 2 (I)] R 1, wr 2 (all data) 0.022 9 1.027-0.15(11) 0.022, 0.1057 0.0616, 0.1198 0.0276 95 1.020 0.11(12) 0.0611, 0.152 0.099, 0.1639 0.0293 89 1.039 0.1(11) 0.0629, 0.1397 0.1239, 0.16 a R 1 = Fo - Fc / Fo, wr 2 = { w[(fo) 2 -(Fc) 2 ] 2 / w[(fo) 2 ] 2 } 1/2.

Table S2. Summary of data collections and structure refinements for crystals 1Rb-6h, 1Rb-12h 1Rb-8h and 1Cs-36h. 1Rb 6h 1Rb 12h 1Rb 8h 1Cs-36h Empirical formula C 2 H 1 In N 2 O 0.50 Rb 2 S 10 Sb C 1.3 H 10.15 In N 1.3 O 0.675 Rb 2.7 S 10 Sb C 0.7 H 6.85 In N 0.7 O 0.825 Rb 3.3 S 10 Sb C 3.71 H 23.25 In N 3.71 Cs 0.29 S 10 Sb Formula weight Crystal system Space group T/K λ/å a/å b/å c/å α/º β/º γ/º V/Å 3 Z D c /Mg m -3 μ/mm -1 F(000) Measured refls. Independent refls. Peak and hole/e Å -3 116.72 13.6686(13) 13.6686(13) 13.6686(13) 2553.7() 2.983 9.202 2100 2501 13 1.051/-1.003 1187.26 13.5292(3) 13.5292(3) 13.5292(3) 276.38(10) 3.18 10.85 2157 272 1333 1.603/-1.008 1222.00 13.957(2) 13.957(2) 13.957(2) 258.02(8) 3.302 12.11 2207 202 1322 1.188/-0.669 1060.15 13.56(1) 13.56(1) 13.56(1) 2688.87(3) 2.616 5.533 197 22567 1927 1.166/-0.912 R int No. of parameters GOF Flack parameter a R 1, wr 2 [I > 2 (I)] R 1, wr 2 (all data) 0.0359 92 1.0 0.09(9) 0.065, 0.136 0.1122, 0.1667 0.030 62 1.020 0.05(5) 0.0570, 0.1177 0.0892, 0.1308 0.021 62 1.006 0.00(2) 0.0319, 0.085 0.0361, 0.0887 0.0510 79 1.08 0.0(9) 0.009, 0.1227 0.056, 0.1275 a R 1 = Fo - Fc / Fo, wr 2 = { w[(fo) 2 -(Fc) 2 ] 2 / w[(fo) 2 ] 2 } 1/2. Table S3. Selected bond lengths (Å) and angles ( ) for compounds 1 and 1Rb-2h. 1 1Rb-2h In(1)-S(2)#1 2.62(19) In(1)-S(2)#1 2.28(3) In(1)-S(2) 2.62(19) In(1)-S(2) 2.28(3) In(1)-S(2)#2 2.62(19) In(1)-S(2)#2 2.28(3) In(1)-S(1) 2.76() In(1)-S(1) 2.27(7) In(2)-S() 2.35(19) In(2)-S() 2.25(3) In(2)-S(2) 2.52(19) In(2)-S(2) 2.3(3) In(2)-S()#1 2.673(18) In(2)-S()#1 2.0(3) In(2)-S(3) 2.75(17) In(2)-S(3) 2.71(3)

Sb(1)-S(3) 2.35(18) Sb(1)-S(3) 2.31(3) Sb(1)-S(3)#3 2.35(18) Sb(1)-S(3)# 2.31(3) Sb(1)-S(3)# 2.35(18) Sb(1)-S(3)#5 2.31(3) S()-In(2)#2 2.673(18) S()-In(2)#2 2.0(3) S(2)#1-In(1)-S(2) 112.07() S(2)#1-In(1)-S(2) 112.01(7) S(2)#1-In(1)-S(2)#2 112.07() S(2)#1-In(1)-S(2)#2 112.01(7) S(2)-In(1)-S(2)#2 112.07() S(2)-In(1)-S(2)#2 112.01(7) S(2)#1-In(1)-S(1) 106.73(5) S(1)-In(1)-S(2)#1 106.80(7) S(2)-In(1)-S(1) 106.73(5) S(1)-In(1)-S(2) 106.80(7) S(2)#2-In(1)-S(1) 106.73(5) S(1)-In(1)-S(2)#2 106.80(7) S()-In(2)-S(2) 116.3(7) S()-In(2)-S(2) 11.20(10) S()-In(2)-S()#1 112.60(9) S()-In(2)-S()#1 111.95(1) S(2)-In(2)-S()#1 108.63(7) S()#1-In(2)-S(2) 111.88(11) S()-In(2)-S(3) 105.21(7) S()-In(2)-S(3) 107.23(10) S(2)-In(2)-S(3) 106.7(7) S(2)-In(2)-S(3) 10.13(10) S()#1-In(2)-S(3) 106.97(6) S()#1-In(2)-S(3) 106.75(9) S(3)-Sb(1)-S(3)#3 95.9(6) S(3)-Sb(1)-S(3)# 95.82(9) S(3)-Sb(1)-S(3)# 95.9(6) S(3)-Sb(1)-S(3)#5 95.82(9) S(3)#3-Sb(1)-S(3)# 95.9(6) S(3)#-Sb(1)-S(3)#5 95.82(9) In(1)-S(2)-In(2) 103.50(7) In(1)-S(2)-In(2) 103.58(11) Sb(1)-S(3)-In(2) 99.18(6) Sb(1)-S(3)-In(2) 95.9(9) In(2)-S()-In(2)#2 102.59(7) In(2)-S()-In(2)#2 102.3(10) Symmetry transformations used to generate equivalent atoms for 1: #1 y+1/2, -z+1/2, -x+1; #2 -z+1, x-1/2, -y+1/2; #3 z+1/2, -x+3/2, -y+1; # -y+3/2, -z+1, x-1/2; for 1Rb-2h: #1 z, x, y; #2 y, z, x; #3 z+1/2, -x+3/2, -y+1; # -z+1, x+1/2, -y+3/2; #5 y-1/2, -z+3/2, -x+1. Table S. N%, C%, H% analyses and ICP-OES results of the pristine compound 1 and the ion-exchanged products. Exchanged Cations N, C, H analyses Experiment (%) (Calc.) compound 1 5.32,.88, 2.1 (5.3,.66, 2.) Rb + exchange for 1h.73,.27, 2.22 (.78,.10, 2.18) Rb + exchange for 2h.03, 3.71, 2.01 (.16, 3.57, 1.93) Rb + exchange for h 3.37, 3.12, 1.7 (3.9, 2.99, 1.66) ICP-OES results Estimated formulae Exchange Rb 0.5 In.00 Rb 0.77 In.00 Rb 1.22 In.00 / / Rb 0. (NH 3 CH 3 ) 3.6 In SbS 9 SH 0.1H 2 O Rb 0.8 (NH 3 CH 3 ) 3.2 In SbS 9 SH 0.2H 2 O Rb 1.25 (NH 3 CH 3 ) 2.75 In SbS 9 SH 0.3125H 2 O yield (%) 10 20 31.3

Rb + exchange for 6h 2.25, 2.21, 1.22 Rb 1.71 In.00 Rb 2 (NH 3 CH 3 ) 2 In SbS 9 SH 50 (2., 2.09, 1.23) 0.5H 2 O Rb + exchange for 12h 1.36, 1.38, 0.88 Rb 2.2 In.00 Rb 2.7 (NH 3 CH 3 ) 1.3 In SbS 9 SH 67.5 (1.53, 1.32, 0.86) 0.675H 2 O Rb + exchange for 2h 0.76, 0.87, 0.3 Rb 3.35 In.00 Rb 3.3 (NH 3 CH 3 ) 0.7 In SbS 9 SH 82.5 (0.80, 0.69, 0.57) 0.825H 2 O Rb + exchange for 36h 0.75, 0.95, 0.57 Rb 3.22 In.00 Rb 3.22 (NH 3 CH 3 ) 0.78 In SbS 9 SH 80.5 (0., 0.77, 0.61) 0.825H 2 O Rb + exchange for 8h 0.7, 0., 0.57 Rb 3.18 In.00 Rb 3.18 (NH 3 CH 3 ) 0.82 In SbS 9 SH 79.5 (0.9, 0.81, 0.63) 0.825H 2 O Na + exchange for 2h 5.0,.55, 1.98 Na 0.20 In.00 Na 0.18 (NH 3 CH 3 ) 3.82 In SbS 9 SH.5 (5.17,.3, 2.0) 0.H 2 O Na + exchange for 36h.,.56, 2.3 Na 0.33 In.00 Na 0.19 (NH 3 CH 3 ) 3.81 In SbS 9 SH.8 (5.11,.38, 2.6) 0.8H 2 O Na + exchange for 8h.76,.37, 2.3 Na 0.32 In.00 Na 0.2 (NH 3 CH 3 ) 3.8 In SbS 9 SH 5.0 (5.10,.37, 2.5) 0.8H 2 O K + exchange for 2h 3.72, 3.50, 1.55 K 1.3 In.00 K 0.95 (NH 3 CH 3 ) 3.05 In SbS 9 SH 23.8 (.07, 3.9, 1.97) 0.6H 2 O K + exchange for 36h 3.68,3.9, 2.03 K 1.31 In.00 K 1.09 (NH 3 CH 3 ) 2.91 In SbS 9 SH 27.3 (3.87, 3.32, 1.92) 0.8H 2 O K + exchange for 8h 3.63, 3.38, 1.99 K 1.23 In.00 K 1.06 (NH 3 CH 3 ) 2.9 In SbS 9 SH 26.5 (3.92, 3.36, 1.92) 0.7H 2 O Cs + exchange for 2h.5,.17, 1.9 weak emission Cs 0.35 (NH 3 CH 3 ) 3.65 In SbS 9 SH 8.8 (.77,.09, 2.21) 0.3H 2 O Cs + exchange for 36h.87,.59, 2.15 weak emission Cs 0.29 (NH 3 CH 3 ) 3.71 In SbS 9 SH 7.3 (.89,.20, 2.23) 0.1H 2 O Cs + exchange for 8h.75,.39, 2.10 weak emission Cs 0.3 (NH 3 CH 3 ) 3.7 In SbS 9 SH 7.5 (.87,.17, 2.23) 0.2H 2 O Rb + + Na + 0.70, 0.72, 0.61 Na 0.18 Rb 2.61 In.00 Rb 3.11 Na 0.21 (NH 3 CH 3 ) 0.68 In SbS 9 SH Rb + : 77.8 exchange for 2h (0.79, 0.67, 0.56) 0.83H 2 O Na + : 5.2 Rb + + K + 0.73, 0.73, 0.55 K 0.1 Rb 2.18 In.00 Rb 2.82 K 0.53 (NH 3 CH 3 ) 0.65 In SbS 9 SH Rb + : 70.5 exchange for 2h (0.76, 0.65, 0.55) 0.8H 2 O K + : 13.3 Rb + + Cs +.83,.12, 2.07 Rb 0.11 In.00 Rb 0.11 Cs 0.23 (NH 3 CH 3 ) 3.66 In SbS 9 SH Rb + : 2.8 exchange for 2h (.83,.1, 2.20) 0.09H 2 O Cs + : 5.8 Rb + + Na + + K + 0.50, 0.7, 0.59 Na 0.01 K 0. Rb 2.68 In.00 Rb 3.03 Na 0.01 K 0.50 (NH 3 CH 3 ) 0.6 In SbS 9 SH Rb + : 75.8 exchange for 2h (0.53,0.6,0.6) 0.885H 2 O Na + : 0.25 K + : 12.5 Rb + + Na + + K + + Cs +.60,.12, 2.1 Na 0.03 K 0.8 Rb 0.10 In.00 Rb 0.06 Na 0.02 K 0.32 Cs 0.13 (NH 3 CH 3 ) 3.7 In SbS 9 SH Rb + : 1.5 exchange for 2h (.62, 3.96, 2.12) 0.13H 2 O Na + : 0.5 K + : 8.0 Cs + : 3.3

Figure S1. Thermogravimetric curves for (a) 1 and the 2h Na + -, K + -, Rb + -, Cs + -exchanged products and (b) 1 and the time-dependent Rb + -exchanged products. Figure S2. Thermogravimetric curves for 1 and the time-dependent Rb + -exchanged products in the low-temperature region. Table S5. Thermogravimetric analyses of 1 and the Na + -, K + -, Rb + -, Cs + -exchanged products in 2h. Exchanged cation Estimated formula Experimental weight loss at ~20 3 C (%) Calculated weight loss (%) Pristine \ 20.16 20.31 (2.50 H 2 S+ CH 3 NH 2 ) Na + Na 0.18 (NH 3 CH 3 ) 3.82 In SbS 9 SH 0.H 2 O 18.16 0.62 K + K 0.95 (NH 3 CH 3 ) 3.05 In SbS 9 SH 0.6H 2 O 1.35 Rb + Rb 3.3 (NH 3 CH 3 ) 0.7 In SbS 9 SH 0.825H 2 O 3.9 1.01 1.5 17.72 (1.91 H 2 S+3.82 CH 3 NH 2 ) 0.61 (H 2 O) 13.98 (1.53 H 2 S+3.05 CH 3 NH 2 ) 1.03 (H 2 O).15 (0.85 H 2 S+0.7 CH 3 NH 2 ) 1.22 (H 2 O)

Cs + Cs 0.35 (NH 3 CH 3 ) 3.65 In SbS 9 SH 0.3H 2 O 16.91 0.5 16.37 (1.825 H 2 S+3.65 CH 3 NH 2 ) 0.50 (H 2 O) Table S6. Thermogravimetric analyses of 1 and the time-dependent Rb + -exchanged products. Reaction Estimated formula Experimental Calculated weight losses (%) time weight losses at ~20 3 C (%) 1h Rb 0. (NH 3 CH 3 ) 3.6 In SbS 9 SH 0.1H 2 O 17.51 0.2 2h Rb 0.8 (NH 3 CH 3 ) 3.2 In SbS 9 SH 0.2H 2 O 15.72 0.2 h Rb 1.25 (NH 3 CH 3 ) 2.75 In SbS 9 SH 0.3125H 2 O 12.99 0.75 6h Rb 2 (NH 3 CH 3 ) 2 In SbS 9 SH 0.5H 2 O 9.79 1.0 12h Rb 2.7 (NH 3 CH 3 ) 1.3 In SbS 9 SH 0.675H 2 O 6.31 1.8 2h Rb 3.3 (NH 3 CH 3 ) 0.7 In SbS 9 SH 0.825H 2 O 3.9 1.5 18.02 (2.3 H 2 S+3.6 CH 3 NH 2 ) 0.17 (H 2 O) 15.85 (2.1 H 2 S+3.2 CH 3 NH 2 ) 0.33 (H 2 O) 13.52(1.875 H 2 S+2.75 CH 3 NH 2 ) 0.51 (H 2 O) 9.87 (1.5 H 2 S+2 CH 3 NH 2 ) 0.78 (H 2 O) 6.81 (1.15 H 2 S+1.3 CH 3 NH 2 ) 1.02 (H 2 O).15 (0.85 H 2 S+0.7 CH 3 NH 2 ) 1.22 (H 2 O)