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VIII TOF UHV UiO UMCM vs WCA XANES XAS XPS ZIF turnover frequency ultra high vacuum Universitetet i Oslo University of Michigan Crystalline Material versus weakly coordinating anion X-ray absorption near edge structure X-ray absorption sepctroscopy X-ray photoelectron spectroscopy zeolitic imidazolate framework
1 Motivation Looking through the essential fields in nature and in our daily life, one can find that porous materials play an important role. For example, porous rocks can store water, petroleum and natural gas. Activated carbon as a prominent example of porous materials have been widely used in various applications involving purification of gas, gold and water, as well as filters in gas masks and respirators, etc. Another famous example is zeolites, which are broadly used as ion-exchange beds in domestic and commercial water purification and softening, catalysts in oil tracking, etc. As zeolite-like architectures, metal-organic frameworks (MOFs) represent a young class of hybrid inorganic-organic crystalline porous materials, formed from organic linkers and inorganic build blocks (metal nodes). Ability to tune the inorganic building blocks as well as the diverse characteristics of the organic moieties featured in MOFs ensures its great advantage in comparison with the conventional porous materials (e.g. zeolites and activated carbons), which attracted huge attentions over last decades. Nowadays, MOFs are also extensively investigated as porous materials promising for gas storage/separation, sensing, drug delivery and catalysis, etc. Various synthetic approaches applied to MOFs afford to achieve their rich diversity, high level of complexity and functionality. For example, reticular synthesis (versatile design of functionalized organic linkers), design of mixed-component MOFs via post-synthetic modification (including metal and linker exchange), or mixed-linker/metal copolymerization has attracted huge attention with this regard. To note, the coordinatively unsaturated metal sites (CUS) in MOFs play a key role in many applications, especially in enhanced catalytic activity and effective gas sorption/separation. Hence, increased complexity by means of mixed-component MOFs can be combined with the generation of defects around the metal centers, which could lead to more open metal sites, or in the case of clustering of the point defects, mesoporous MOFs can be obtained. Thus, it comes to the “so-called” defect-engineering MOFs (DEMOFs). This manner of advanced modification of MOFs holds enormous potential to optimize the materials properties beyond the
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 10 and 11: Zhang, for their continuous support
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 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
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64 Chapter 4 in the case of ip intr
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66 Chapter 4 4.2.1.1 Crystallinity
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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
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80 Chapter 4 framework Ru-species (
Page 100 and 101:
82 Chapter 4 Figure 4.20. XANES spe
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84 Chapter 4 It is important to not
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86 Chapter 4 Ru δ+ have been obser
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88 Chapter 4 Figure 4.25. UHV-IR sp
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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]
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104 Chapter 4 reactive metal center
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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
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weight loss, % 112 Chapter 4 100 Cu
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weight loss, % 114 Chapter 4 record
Page 134 and 135:
116 Chapter 4 4.3.2 Composition and
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V, cm 3 /g 118 Chapter 4 500 400 30
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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
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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),
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7 Experimental Section In this Chap
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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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