Porous metal–organic frameworks for methane storage and capture: status and challenges
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摘要: 在全球向可持续低碳经济转型的过程中，作为两大低碳能源技术，甲烷储存和甲烷捕集都面临着同样的挑战，即缺乏高效的吸附剂。MOFs（metal-organic frameworks）材料具有极高的比表面积、孔隙率和可调节的孔隙结构，在气体吸附储存领域拥有极大的潜在应用价值。本文首先介绍了MOFs的结构设计和合成方法，综述并强调了MOFs材料在CH4储存与捕集方面的研究进展及面临的问题。在CH4高压储存方面，从体积吸附量和质量吸附量两个目标出发，介绍了目前MOFs材料储存CH4的研究现状；在CH4常压捕集方面，重点强调了CH4/N2和CO2/CH4分离技术和CH4捕集技术。最后，对利用MOFs材料实现高效CH4储存和捕集存在的问题和挑战进行了分析和展望。Abstract: In the process of global transition to a sustainable low-carbon economy, the two major low-carbon energy technologies, namely, methane (CH4) storage and methane capture face the same challenge, that is, the lack of efficient adsorbents. Metal-organic framework (MOF) materials have potential value in the field of gas adsorption storage because of their high specific surface area, good porosity, and adjustable pore structure. In this study, the structural design and synthesis methods of MOFs are introduced, and the research progress and problems associated with MOF materials in methane storage and capture are reviewed. The current research status of methane storage at high pressure is introduced in terms of volumetric and gravimetric uptake. For methane capture at atmospheric pressure, emphasis is placed on CH4/N2 and CO2/CH4 separation and methane capture technologies. Finally, the problems and challenges of using MOF materials to achieve efficient methane storage and capture are analyzed and future prospects are presented.
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Key words:
- Metal-organic frameworks /
- Methane /
- Adsorption /
- Storage /
- Capture
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Figure 2. Bridging angles and girths in zeolites and IMs[16]. Reproduced with permission.
Figure 4. The three-dimensional coordination polymer, showing the pillaring of adjacent (6,3) Ni3(btc)2 sheets by 4,4’-bipy ligands[22]. Reproduced with permission.
Figure 5. ZIF series produced by solid-phase reaction method[26]. Reproduced with permission.
Figure 6. Clusters formed by NTA-Mg (a-Mg), NTA-Ca (Amurc) and CH4. The first adsorbed CH4 blocked the adsorption site of NTA-Mg, while the conical NTA-Ca could adsorb three CH4[73]. Reproduced with permission.
Figure 7. (a) Three types of cages in HKUST-1, and their diameters are 0.5 nm (dark green), 1.1 nm (orange) and 1.35 nm (blue); (b) The green, gray, red and light blue spheres of CD4 molecules adsorbed at the four holes of the octahedral cage represent Cu, C, O and D atoms, respectively[4]. Reproduced with permission.
Figure 8. Schematic diagram of excess adsorption, absolute adsorption and total adsorption (the left side of the red line is the adsorption area, the right side of the red line is the unadsorbed area, the green sphere represents the adsorbed molecules, and the blue sphere represents the unadsorbed molecules)[4]. Reproduced with permission.
Figure 9. Comparison of deliverable capacity at different storage temperatures (5−65 bar)[7]. Reproduced with permission.
Figure 10. (a) Relationship between gravimetric uptake and BET specific surface area at 270 K; (b) Relationship between volumetric uptake and pore volume at 298 K[7]. Reproduced with permission.
Figure 11. Schematic representation of monolithic and powder MOF synthesis[92]. Reproduced with permission.
Figure 12. (a) Crystal structure of NOTT-101, UTSA-76 and UTSA-110; (b) Comparison of USTA-110 methane gravimetric/volumetric uptake with other MOFs at 298 K and 65 bar[94]. Reproduced with permission.
Figure 13. Comparison of deliverable capacity between (a) rigid MOFs and (b) flexible MOFs; Total CH4 uptake of (c) Co (bdp) and (d) Fe (bdp) at 25 ℃[96]. Reproduced with permission.
Figure 14. The (a) primary (green), (b) secondary (black), and (c) ternary (orange) CH4 adsorption sites in MAF-38[97]. Reproduced with permission.
Figure 15. Comparison of gravimetric/volumetric absorption of MOFs at 270 K and 298 K[7]. Reproduced with permission.
Figure 16. Methane emissions from oil and gas, comparison of IEA and other estimates[118].
Figure 17. Oil and gas sector methane emissions 2000-2030 in the Sustainable Development Scenario[119].
Figure 18. (a,b) Comparison of CH4/N2 separation performance of some MOFs summarized by Liu[161]. Reproduced with permission.
Figure 19. The comparison of traditional methane adsorbent and nano-trap. The purple and green ellipsoids represent coordinatively unsaturated metal centers and alkyl groups, respectively[159]. Reproduced with permission.
Figure 20. Relationship between CH4 uptake and VSA/pore volume at 298 K, 1 bar and 65 bar.
Table 1. Examples of MOF materials for methane storage.
Materials BET(m2 g−1) Vp(cm3 g−1) CH4 total uptake CH4 excess uptake(mg g−1) Delivery(cm3 cm−3) mg g−1 cm3 cm−3 T(K) P(bar) mg g−1 cm3 cm−3 T(K) P(bar) Al-soc-MOF-1[83] 5590 2.30 410 197 298 65 - - - - 201(5–80 bar) Co(bdp)[96] 2911(Langmuir) - - 203 298 65 - - - - 197 HKUST-1[100-101] 1850 0.78 216 267 298 65 178 220 298 65 190 monoHKUST-1[92] 1193 0.52 177 267 298 69 151 227 298 69 172 LIFM-82[102] 1624 0.71 210 271 298 80 - - - - 217(5–80 bar) MAF-38[97] 2022 - 247 263 298 65 - - - - 187 MFM-115a[103] 3394 1.38 278 238 298 65 - - - - 191 MIL-53(Al)[104] 1100 0.59 ≥96 155 304 35 - - - - MIL-53(Cr)[104] 1100 0.56 ≥96 165 304 35 - - - - - MIL-10[p0(Cr)[105] 1900 1.10 152 150 303 60 - - - - - MIL-101(Cr)[105-106] 4230 2.15 217.6 135 303 60 - - - - - MOF-5[107] 3800 1.55 - 132 298 35 ~160[108] - 300 60 - MOF-177[95] 4700 1.83 - 208 298 80 - - - - 185(5–80 bar) MOF-200[80] 4530 3.59 - - - - 234 - 298 80 - MOF-210[80] 6240 3.6 - - - - 264 - 298 80 157(5–80 bar) MOF-519[84] 2400 0.928 190 259 298 65 - - - - 230(5–80 bar) MOF-905[95] 3490 1.34 270 206 298 65 - - - - 203(5–80 bar) MOF-905-Naph[95] 3640 1.39 - 211 298 80 - - - - 184(5–80 bar) MOF-905-Me2[95] 3310 1.25 - 217 298 80 - - - - 188(5–80 bar) MOF-905-NO2[95] 3380 1.29 - 203 298 80 - - - - 177(5–80 bar) MOF-950[95] 3440 1.30 - 209 398 80 - - - - 174(5–80 bar) Ni-MOF-74[91, 100] 1350 0.51 148 251 298 65 125 210 298 65 129 NJU-Bai43[109] 3090 1.22 283 254 298 65 - - - - 198 NOTT-101a[81, 94] 2805 1.08 247 237 298 65 - - - - 181 NU-111[91, 98] 4930 2.09 360 205 298 65 262 150 298 65 179 NU-125[91] 3120 1.29 287 232 298 65 223 181 298 65 183 NU-135[110] 2600 1.02 219 230 298 65 - - - - 170 NU-1500-Al[99] 3560 1.46 290 200 296 65 - - - - 181(5–80 bar) NU-1501-Al[99] 7310 2.91 410 163 296 65 - - - - 174(5–80 bar) NU-1501-Fe[99] 7140 2.90 400 168 296 65 - - - - 176(5–80 bar) PCN-14[91, 112] 2000 0.85 197 230 298 65 157 183 298 65 157 PCN-66[114] 4000 1.63 - 187 398 65 177.6 110 298 35 152 PCN-68 [115] 5109 2.13 - 187 298 65 185.6 99 298 35 157 UTSA-20[91] 1620 0.66 181 230 298 65 150 191 298 65 170 UTSA-76[82, 113] 2820 1.09 263 257 298 65 - - - - 197 UTSA-110a[94] 3241 1.263 288 241 298 65 - - - - 190 ZIF-8[108] - - ~85 - 300 36 70 - 300 36 - ZJU-70 [114] 1791 0.676 - 211 298 65 - - - - - 
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Table 2. Examples of CH4 adsorption and separation from CH4/N2 (100 kPa).
Materials CH4 total uptake (mmol g−1) CH4/N2 selectivities Temperature (K) Al-CDC[161] 1.44 13.1 298 ATC-Cu[159] 2.90 9.7 298 CAU-8-BPDC[152] 0.85 4.9 298 CAU-21-BPDC[152] 0.99 11.9 298 [Co3(C4O4)2(OH)2][153] 0.41 12.5 298 Co-MA-BPY[151] 0.92 7.2 298 Co-MOF-74[154] 1.91 3.2 298 Cu-MOF[160] 0.64 10.8 298 Mg-MOF-74[154] 1.66 1.5 298 MIL-100(Cr)[154] 0.60 3.0 298 MOF-5[155] 0.13 1.13 298 MOF-177[155] 0.56 4.0 298 Ni-MA-BPY[151] 1.01 7.4 298 [Ni3(HCOO)6][156] 0.82 6.2 298 PCN-222[157] 0.35 4.8 298 V2Cl2.8(btdd)[158] 1.00 27* 298 *represents N2/CH4 selectivity
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Table 3. Typical examples of CO2/CH4 separation.
Materials CO2 total uptake (mol kg−1) CO2/CH4 selectivities Pressure (kPa) Temperature(K) IITKGP-6[164] 1.67 5.1 100 295 Cu-MOF[165] - 6 100 303 MIL-53(Al)[166] 4.3(3.5bar) 4.10 100–3500 303 UTSA-16[167] 4.2 29.8 200 296 Mg-MOF-74[168] 8.56 105.1 200 296 CuBTC[169] 5.27 7.4 200 296 MIL-101[169] 2.16 9.6 200 296 SIFSIX-2-Cu[170] 1.85 5.3 100 298 SIFSIX-2-Cu-i[170] 5.41 33 100 298 SIFSIX-3-Zn[170] 2.55 231 100 298
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