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Ἐπίκτητος Λιάπης
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1 Supporting Information Wiley-VCH Weinheim, Germany

2 Supplementary Figure 1. Synthetic results as detected by XRD (Cu-Kα). Simulation pattern of MCM-68 Relative Intensity / a.u. YNU-2P Conventional MCM theta / degree Relative Intensity / a.u. After direct calcination of YNU-2P at 4ºC for 3 h YNU-2P theta / degree YNU-2 (after calcination of silylated YNU-2P at 45ºC) Relative Intensity / a.u. YNU-2P-silylated theta / degree YNU-2P

3 Supplementary Figure 2. Structural drawing of (a)ynu-2p and (b)ynu-2 along [1] direction. In the Figure 2(a), pale yellow and pale red (pink) mean defective silicon and oxygen atoms, respectively. (a) TEBOP Na (b) H 2 O

4 Supplementary Figure 3. 1 H MAS NMR spectra of YNU-2. Blue and red curves were drawn with Y-offset of YNU-2P modified YNU-2P after post-synthetic silylation siliceous zeolite YNU-2 after calcination of modified YNU-2P 4 Arbitrary intensity 3 2 Š15.8ppm Chemical shift / ppm

5 Supplementary Figure 4. TG-DTA curves of YNU-2P Weight loss / wt% T / µv Temperature / C Time / min

6 Supplementary Figure 5. N 2 adsorption-desorption isotherms of YNU-2 and MCM adsorption Adsorped amount / cm 3 g -1 (STP) desorption YNU-2 S BET = 573 m 3 g -1 Pore volume (t-plot) =.29 cm 3 g Relative pressure (P/P ) 6 Adsorped amount / cm 3 g -1 (STP) adsorption desorption MCM-68 S BET = 628 m 3 g -1 Pore volume (t-plot) =.24 cm 3 g Relative pressure (P/P )

7 Title: A New Multi-Dimensional Microporous Silicate Isomorphous to Zeolite MCM-68 Supplementary Figure 6. SEM images of YNU-2P, YNU-2, and MCM-68. YNU-2P YNU-2 MCM-68

8 Supplementary Table 1. Structural parameters g, x, y, z and B of YNU-2P obtained by the Rietveld refinement. Estimated standard deviations (ESDs) are given as uncertainties in the last reported decimal digit. Site M g x y z B(Å 2 ) Si1 16k.844(5).1296(3).7492(3).1134(3) 2.17(4) Si2 16k (3).7515(3).273(3) = B(Si1) Si3 16k.92(5).34(3).2157(3).764(3) = B(Si1) Si4 16k (2).2569(3).1913(4) = B(Si1) Si5 16k (2).219(3).3139(3) = B(Si1) Si6 8j.395(8).593(7) = x.123(1) = B(Si1) Si7 8j.4(9).64(7) = x.2765(9) = B(Si1) Si8 16k (3).2537(3).4244(2) = B(Si1) O1 16k (3).741(3).1927(5) 2.97(6) O2 16k.873 I).464(5).752(5).817(4) = B(O1) O3 16k (5).6751(5).874(4) = B(O1) O4 16k (4).7563(4).323(5) = B(O1) O5 16k (4).6837(4).31(5) = B(O1) O6 16k (4).2542(5).1223(5) = B(O1) O7 16k.649 II).337(7).1324(9).947(6) = B(O1) O8 16k (4).2521(5).2551(5) = B(O1) O9 16k (3).1331(5).396(5) = B(O1) O1 16k (5).2487(5).3816(4) = B(O1) O11 4e = g(si6)..98(2) = B(O1) O12 4e = g(si7)..297(2) = B(O1) O13 8j (3) = x.1948(7) = B(O1) O14 8j.397 III).649(1) = x.199(2) = B(O1) O15 8j (4) = x.435(5) = B(O1) O16 8j = g(si1).172(6) = x.917(6) = B(O1) O17 8j (4) = x.2816(5) = B(O1) O18 8i = g(si3).689(6).226(6) = B(O1) O19 8i (5).2473(6) 1/2 = B(O1) N 4f = x 1/2 4.6(8) C1 8j.5.26 = x.56 = B(N1) C2 4g 1..5 = x 1/2 = B(N1) C3 16k = B(N1) C4 8i /2 = B(N1) C5 8j = x.557 = B(N1) C6 8j = x.615 = B(N1) C7 16k = B(N1) N1b 16k (8) C1b 16k = B(N1b) C2b 16k = B(N1b) C3b 16k = B(N1b) C4b 16k = B(N1b) C5b 16k = B(N1b) C6b 16k = B(N1b) C7b 16k = B(N1b) C8b 16k = B(N1b) C9b 16k = B(N1b) C1b 16k = B(N1b) C11b 16k = B(N1b) WO1 8i.714(5).7529(13).6113(8) 16.(6) WO2 8j =1-g(WO1).57(14) = x.44(2) = B(WO1) WO3 8i.46(2).941(2).477(2) = B(WO1) WO4 16k.341(11).964(2).565(2).83(2) = B(WO1) WO5 16k.468(12).9431(1).519(13).179(11) = B(WO1) Na1 8j.77(2).555(7) = x.7759(9) 21.4(2) Na2 4g.7(2).494(13) = x = B(Na1) Na3 16k.26(12).12(3).5(3).9(3) = B(Na1) Note: Scattering amplitude of carbons were modified in consideration of protons. All parameters of C and N sites were fixed except B parameters. WO1 and WO3 are OH, and WO3, WO4 and WO5 are water molecules in consideration of protons. Linear constrains were imposed for occupancies of oxygen sites as follows: I) g(o2) =.5 (g(si1) + g(si3)), II) g(o7) =.5 (g(si3) + g(si6)), III) g(o14) =.5 (g(si6) + g(si7)).

9 Supplementary Table 2: Bond lengths, l, and bond angles, φ, in YNU-2P calculated from refined lattice and structural parameters. l (Å) φ ( º) φ ( º) Si1 O (1) O1 Si1 O (5) O8 Si5 O (5) Si1 O (1) O1 Si1 O (5) O8 Si5 O (5) Si1 O (1) O1 Si1 O (6) O8 Si5 O (5) Si1 O (8) O2 Si1 O (6) O1 Si5 O (6) Si2 O (8) O2 Si1 O (7) O1 Si5 O (6) Si2 O (9) O3 Si1 O (6) O4 Si5 O (5) Si2 O (5) O5 Si2 O (5) O7 Si6 O7 114 (2) Si2 O (8) O5 Si2 O (5) O7 Si6 O (11) Si3 O (1) O5 Si2 O4 11. (5) O7 Si6 O (13) Si3 O (14) O1 Si2 O (5) O7 Si6 O (11) Si3 O (1) O1 Si2 O (5) O7 Si6 O (13) Si3 O (6) O17 Si2 O (6) O14 Si6 O (2) Si4 O (7) O6 Si3 O (7) O9 Si7 O (12) Si4 O (11) O6 Si3 O (6) O9 Si7 O (1) Si4 O (5) O6 Si3 O (6) O9 Si7 O (13) Si4 O (1) O7 Si3 O (8) O9 Si7 O (1) Si5 O1 1.56(1) O7 Si3 O (7) O9 Si7 O (13) Si5 O4 1.57(7) O2 Si3 O (6) O14 Si7 O12 19 (2) Si5 O (8) O5 Si4 O (6) O3 Si8 O (6) Si5 O (9) O5 Si4 O (4) O3 Si8 O (6) Si6 O7(x2) 1.53(14) O5 Si4 O (6) O3 Si8 O (6) Si6 O (11) O6 Si4 O (7) O1 Si8 O (6) Si6 O (14) O6 Si4 O (4) O1 Si8 O (6) Si7 O9(x2) 1.539(11) O13 Si4 O (7) O19 Si8 O (6) Si7 O (16) Si7 O (16) Average φ 19.5 Si8 O (1) Si8 O (9) Si8 O (5) Si8 O (6) Average l(si O) 1.59 Na1 O12 2.5(4) Na1 O14(x2) 2.26(2) Na2 O11(x2) 2.34(4) Na3 O2 2.37(5) Na3 O7 1.56(5)

10 Supplementary Table 3. Structural parameters g, x, y, z and B of YNU-2 obtained by the Rietveld refinement. Estimated standard deviations (ESDs) are given as uncertainties in the last reported decimal digit. Site M g x y z B(Å 2 ) Si1 16k (4).7489(4).118(4) 1.7(5) Si2 16k (4).7544(4).2741(3) = B(Si1) Si3 16k (4).2187(4).741(3) = B(Si1) Si4 16k (3).2576(3).1893(4) = B(Si1) Si5 16k (3).2213(4).3112(4) = B(Si1) Si6 8j.97(9).594(4) = x.1178(6) = B(Si1) Si7 8j.98(8).587(3) = x.2783(5) = B(Si1) Si8 16k (4).2573(4).4232(3) = B(Si1) O1 16k (4).7414(4).1953(6) 1.98(8) O2 16k (6).752(6).884(5) = B(O1) O3 16k (6).6774(5).916(5) = B(O1) O4 16k (5).7568(5).388(7) = B(O1) O5 16k (5).6863(5).347(8) = B(O1) O6 16k 1..85(5).2658(5).122(5) = B(O1) O7 16k (5).1347(7).883(5) = B(O1) O8 16k (6).256(7).2516(7) = B(O1) O9 16k (4).1353(5).349(7) = B(O1) O1 16k (6).2483(7).3798(5) = B(O1) O11 4e 1..98(1) = B(O1) O12 4e (1) = B(O1) O13 8j (4) = x.1861(8) = B(O1) O14 8j (4) = x.198(1) = B(O1) O15 8j (4) = x.471(6) = B(O1) O16 8j (6) = x.986(7) = B(O1) O17 8j (5) = x.291(8) = B(O1) O18 8i (8).2315(8) = B(O1) O19 8i (7).25 1/2 = B(O1) WO1 16k.64(1).488(1).747(9).14(1) 22.6(3) WO2 8j.4(1).19(3).745(3) 1/2 = B(WO1) WO3 8i.34(1).54(4).22(3) = B(WO1) WO4 8i.367(8).2(3).69(4) 1/2 = B(WO1) WO5 16k.23(1).7(3).625(4).83(4) = B(WO1) All WO are water molecules in consideration of scattering amplitude of protons.

11 Supplementary Table 4: Bond lengths, l, and bond angles, φ, in YNU-2 calculated from refined lattice and structural parameters. l (Å) φ ( º) φ ( º) Si1 O (11) O2 Si1 O (7) O4 Si5 O (8) Si1 O (11) O2 Si1 O (7) O4 Si5 O (6) Si1 O (12) O2 Si1 O (8) O4 Si5 O (8) Si1 O (7) O3 Si1 O (7) O1 Si5 O (8) Si2 O (8) O3 Si1 O (7) O1 Si5 O (6) Si2 O (11) O1 Si1 O (8) O9 Si5 O (8) Si2 O (12) O17 Si2 O (8) O7 Si6 O7 11. (11) Si2 O (1) O17 Si2 O (8) O7 Si6 O (8) Si3 O (8) O17 Si2 O (8) O7 Si6 O (7) Si3 O (12) O5 Si2 O (7) O7 Si6 O (8) Si3 O (1) O5 Si2 O (7) O7 Si6 O (7) Si3 O (1) O1 Si2 O (7) O11 Si6 O (11) Si4 O (12) O18 Si3 O (8) O12 Si7 O (8) Si4 O (9) O18 Si3 O (9) O12 Si7 O (8) Si4 O (12) O18 Si3 O (7) O12 Si7 O (13) Si4 O (6) O7 Si3 O (7) O9 Si7 O (1) Si5 O (9) O7 Si3 O (7) O9 Si7 O (7) Si5 O (12) O2 Si3 O (7) O9 Si7 O (7) Si5 O (9) O8 Si4 O (8) O15 Si8 O (7) Si5 O (13) O8 Si4 O (6) O15 Si8 O (8) Si6 O7(x2) (12) O8 Si4 O (9) O15 Si8 O (8) Si6 O (12) O5 Si4 O (8) O3 Si8 O (6) Si6 O (13) O5 Si4 O (5) O3 Si8 O (8) Si7 O (17) O6 Si4 O (8) O19 Si8 O (7) Si7 O9(x2) (11) Si7 O (1) Average φ 19.5 Si8 O (1) Si8 O (2) Si8 O (7) Si8 O (11) Average l 1.59

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