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Zhang, for their continuous support and care. My love and deep appreciation to Zhihao Chen for always being at my side. His motivation and continuous care help me recover from the sadness of homesick and overcome the challenging in my life and study. All these would not happen without them.
Table of Contents Table of Contents ................................................................................................................................................. I Abbreviations ....................................................................................................................................................... V 1 Motivation .................................................................................................................................................... 1 2 General introduction ............................................................................................................................... 3 2.1 Origin of MOFs - Coordination polymers ............................................................................... 3 2.2 Definition, Chemistry and features of MOFs ........................................................................ 7 2.2.1 Definition and nomenclature of MOFs ................................................................ 7 2.2.2 MOF features .................................................................................................................. 8 2.3 Synthetic approaches, modification and applications of MOFs ................................ 14 2.3.1 Traditional synthesis approaches ...................................................................... 14 2.3.2 Reticular synthesis ................................................................................................... 15 2.3.3 Way to the modification of MOFs ....................................................................... 16 2.3.4 Application of MOFs ................................................................................................. 23 3 Controlled secondary building unit approach to the formation of the isostructural Ru II,II and Ru II,III analogs of [M3(BTC)2]n ........................................................... 26 3.1 Preparation and investigation of the Ru II,III -analogs of [M3(BTC)2]n ...................... 28 3.1.1 The family of [M3(BTC)2]n...................................................................................... 28 3.1.2 Background and the state-of-the-art in research on Ru-analogs of [M3(BTC)2]n.................................................................................................................. 29 3.1.3 [Ru3(BTC)2Yy]n·G g obtained by CSA using [Ru2(OOCR)4X] and [Ru2(OOCCH3)4]A: synthesis and characterization ..................................... 31 3.1.4 Pre-activation by solvent exchange ................................................................... 37 3.1.5 Study of [Ru3(BTC)2Yy]n·G g after solvent exchange .................................... 38 3.1.6 Summary ....................................................................................................................... 48 3.2 Elaboration of Ru II,II analog of [M3(BTC)2]n........................................................................ 50
Page 1: Controlled Modification of Metal-Or
Page 5: This thesis is based on the work pe
Page 8 and 9: Bochum) for the study of XPS and UH
Page 12 and 13: II 3.2.1 Synthesis and characteriza
Page 14 and 15: IV 7.3.4 Synthesis of Cu-DEMOF samp
Page 16 and 17: VI DMSO dobdc e.g. EA EDX EtOH EXAF
Page 18 and 19: VIII TOF UHV UiO UMCM vs WCA XANES
Page 20 and 21: 2 Chapter 1 limitations of the (non
Page 22 and 23: 4 Chapter 2 For the synthesis of CP
Page 24 and 25: 6 Chapter 2 cavities is able to rev
Page 26 and 27: 8 Chapter 2 2.2.2 MOF features Adva
Page 28 and 29: 10 Chapter 2 Figure 2.5. A series o
Page 30 and 31: 12 Chapter 2 the material is retain
Page 32 and 33: 14 Chapter 2 2.3 Synthetic approach
Page 34 and 35: 16 Chapter 2 Expansion of this stru
Page 36 and 37: 18 Chapter 2 (H2BPDC) [75] or other
Page 38 and 39: 20 Chapter 2 Cr III CUSs of MIL-101
Page 40 and 41: 22 Chapter 2 Figure 2.14. Schematic
Page 42 and 43: 24 Chapter 2 adsorbate-surface inte
Page 44 and 45: 3 Controlled secondary building uni
Page 46 and 47: 28 Chapter 3 3.1 Preparation and in
Page 48 and 49: 30 Chapter 3 formula of [Ru3 II,III
Page 50 and 51: Intensity, a. u. 32 Chapter 3 quali
Page 52 and 53: 34 Chapter 3 After activating the R
Page 54 and 55: 36 Chapter 3 presence of the residu
Page 56 and 57: Intensity, a. u. 38 Chapter 3 the a
Page 58 and 59: 40 Chapter 3 extent than acetic aci
Page 60 and 61:
42 Chapter 3 Ru-nodes. Therefore, r
Page 62 and 63:
44 Chapter 3 decomposition of [BF4]
Page 64 and 65:
deriv. normalized E) 46 Chapter 3 F
Page 66 and 67:
48 Chapter 3 3.1.6 Summary Applying
Page 68 and 69:
50 Chapter 3 3.2 Elaboration of Ru
Page 70 and 71:
52 Chapter 3 with that of the Ru II
Page 72 and 73:
54 Chapter 3 Figure 3.20. (a) XANES
Page 74 and 75:
4 Linker-based MOF solid solutions:
Page 76 and 77:
58 Chapter 4 4.1 Introduction 4.1.1
Page 78 and 79:
60 Chapter 4 framework [Cu2(ndc)2(d
Page 80 and 81:
62 Chapter 4 partial replacing of B
Page 82 and 83:
64 Chapter 4 in the case of ip intr
Page 84 and 85:
66 Chapter 4 4.2.1.1 Crystallinity
Page 86 and 87:
68 Chapter 4 suggesting the absence
Page 88 and 89:
70 Chapter 4 Table 4.1. The molar f
Page 90 and 91:
72 Chapter 4 Figure 4.11. IR spectr
Page 92 and 93:
74 Chapter 4 taking into account th
Page 94 and 95:
76 Chapter 4 As quantitative digest
Page 96 and 97:
78 Chapter 4 (Figure 4.16). Notably
Page 98 and 99:
80 Chapter 4 framework Ru-species (
Page 100 and 101:
82 Chapter 4 Figure 4.20. XANES spe
Page 102 and 103:
84 Chapter 4 It is important to not
Page 104 and 105:
86 Chapter 4 Ru δ+ have been obser
Page 106 and 107:
88 Chapter 4 Figure 4.25. UHV-IR sp
Page 108 and 109:
90 Chapter 4 Table 4.5. Possible de
Page 110 and 111:
CO 2 adsorbed, mmol/g 92 Chapter 4
Page 112 and 113:
H 2 adsorbed, mmol/g 94 Chapter 4 F
Page 114 and 115:
CO 2 adsorbed, mmol/g 96 Chapter 4
Page 116 and 117:
H 2 adsorbed, mmol/g 98 Chapter 4 8
Page 118 and 119:
H 2 adsorbed, mmol/g 100 Chapter 4
Page 120 and 121:
102 Chapter 4 presence of H2. [236]
Page 122 and 123:
104 Chapter 4 reactive metal center
Page 124 and 125:
106 Chapter 4 4.2.6 Conclusions App
Page 126 and 127:
108 Chapter 4 4.3 Defects Engineeri
Page 128 and 129:
Intensity, a. u. 110 Chapter 4 as-s
Page 130 and 131:
weight loss, % 112 Chapter 4 100 Cu
Page 132 and 133:
weight loss, % 114 Chapter 4 record
Page 134 and 135:
116 Chapter 4 4.3.2 Composition and
Page 136 and 137:
V, cm 3 /g 118 Chapter 4 500 400 30
Page 138 and 139:
120 Chapter 4 Figure 4.50. From lef
Page 140 and 141:
5 Simultaneous introduction of vari
Page 142 and 143:
124 Chapter 5 preferred like Cu 2+
Page 144 and 145:
126 Chapter 5 5.2 Preparation and S
Page 146 and 147:
128 Chapter 5 Figure 5.5. Pawley Fi
Page 148 and 149:
130 Chapter 5 5.3 Compositional cha
Page 150 and 151:
132 Chapter 5 Table 5.3. The assign
Page 152 and 153:
134 Chapter 5 framework are dominan
Page 154 and 155:
136 Chapter 5 5.4 Synthesis, compos
Page 156 and 157:
138 Chapter 5 obtained Pd-doped sol
Page 158 and 159:
140 Chapter 5 Figure 5.18. Deconvol
Page 160 and 161:
V, cm 3 /g 142 Chapter 5 sorption i
Page 162 and 163:
144 Chapter 5 time as well as the i
Page 164 and 165:
146 Chapter 5 5.6 Conclusions In su
Page 166 and 167:
148 Chapter 6 coordinating anion),
Page 168 and 169:
7 Experimental Section In this Chap
Page 170 and 171:
152 Chapter 7 as water and hydroxyl
Page 172 and 173:
154 Chapter 7 internal standards an
Page 174 and 175:
156 Chapter 7 Uppermost layer is in
Page 176 and 177:
158 Chapter 7 to the more tightly b
Page 178 and 179:
160 Chapter 7 7.2 Experimental data
Page 180 and 181:
162 Chapter 7 [Ru2(OOCC(CH3)3)4(H2O
Page 182 and 183:
164 Chapter 7 Figure 7.7. The PXRD
Page 184 and 185:
166 Chapter 7 [Ru2(OOCCH3)4(H2O)2]B
Page 186 and 187:
168 Chapter 7 [Ru2(OOCCH3)4](THF)2
Page 188 and 189:
170 Chapter 7 [Ru3(BTC)2(OH)1.5]n·
Page 190 and 191:
172 Chapter 7 [Ru3(BTC)2]n∙(AcOH)
Page 192 and 193:
174 Chapter 7 Table 7.3. Feeding mo
Page 194 and 195:
176 Chapter 7 For comparison of the
Page 196 and 197:
178 Chapter 7 7.3.4 Synthesis of Cu
Page 198 and 199:
180 Chapter 7 D3 The mixture of H3B
Page 200 and 201:
182 Chapter 7 D5 This sample was re
Page 202 and 203:
184 Chapter 7 The synthesis of D7 a
Page 204 and 205:
186 Chapter 7 7.4 Experimental data
Page 206 and 207:
188 Chapter 7 Figure 7.26. PXRD pat
Page 208 and 209:
190 Chapter 7 7.4.2 Hydrogenation o
Page 210 and 211:
192 Chapter 7 7.5 Supplementary det
Page 212 and 213:
8 Bibliography [1] A. J. Ihde, The
Page 214 and 215:
196 Bibliography [61] S. Ma, D. Sun
Page 216 and 217:
198 Bibliography [121] T. K. Prasad
Page 218 and 219:
200 Bibliography [180] Y. Kobayashi
Page 220 and 221:
202 Bibliography [239] A. L. Harreu
Page 222 and 223:
204 Bibliography [297] A. P. Hammer
Page 224 and 225:
206 Appendix List of Presentations
Page 226:
208 Appendix 05. 2015 Grant from th
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