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5. Sol-gel processing of a covalent organic framework for the generation of hierarchically porous monolithic adsorbents

Author

Carrington, Mark E., Rampal, Nakul, Madden, David G., O’Nolan, Daniel, Casati, Nicola Pietro Maria, Divitini, Giorgio, Martín-Illán, Jesús Á., Tricarico, Michele, Cepitis, Ritums, Çamur, Ceren, Curtin, Teresa, Silvestre-Albero, Joaquin, Tan, Jin-Chong, Zamora, Felix, Taraskin, Sergei, Chapman, Karena W., and Fairen-Jimenez, David

Published
2022
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6. Self‐Shaping Monolithic Reticular Materials: Ingredients for Success.

Author

Albacete, Pablo, Asgari, Mehrdad, Yang, Yue, Al‐Shanks, Ali N., and Fairen‐Jimenez, David

Subjects
SCIENTIFIC literature, POROUS polymers, ADSORPTION capacity, ACTIVATED carbon, COORDINATION polymers
Abstract

Reticular materials are one of the more promising tools that humankind has developed to address the required energy transition. Despite their great potential showcased in the last decade, their use is so far mainly confined to the laboratory bench due to drawbacks derived from their powdery morphology. Unlike zeolites and activated carbons, the challenges in shaping and densification of reticular materials hamper their full implementation in the industry. Hence, strategies for shaping and integrating these materials need to be prioritized. Most of the existing strategies rely on applying mechanical pressure and adding chemical binders, but these approaches, although useful for shaping, diminish their final adsorption capacities and do not bring their theoretical, predicted performance. On the other hand, obtaining self‐shaped, dense bodies—so‐called monoliths—arises as a very promising and scalable alternative. Sol–gel monoliths are still scarce in the scientific literature despite their outstanding performance, particularly in terms of volumetric adsorption capacity. This review intends to help expand this scope by offering a rational guide on the self‐shaping of dense monoliths for reticular materials, as well as a complete revision of the state‐of‐the‐art in the field. [ABSTRACT FROM AUTHOR]

Published
2024
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8. An open-access database and analysis tool for perovskite solar cells based on the FAIR data principles

Author

Jacobsson, T. Jesper, Hultqvist, Adam, García-Fernández, Alberto, Anand, Aman, Al-Ashouri, Amran, Hagfeldt, Anders, Crovetto, Andrea, Abate, Antonio, Ricciardulli, Antonio Gaetano, Vijayan, Anuja, Kulkarni, Ashish, Anderson, Assaf Y., Darwich, Barbara Primera, Yang, Bowen, Coles, Brendan L., Perini, Carlo A. R., Rehermann, Carolin, Ramirez, Daniel, Fairen-Jimenez, David, Di Girolamo, Diego, Jia, Donglin, Avila, Elena, Juarez-Perez, Emilio J., Baumann, Fanny, Mathies, Florian, González, G. S. Anaya, Boschloo, Gerrit, Nasti, Giuseppe, Paramasivam, Gopinath, Martínez-Denegri, Guillermo, Näsström, Hampus, Michaels, Hannes, Köbler, Hans, Wu, Hua, Benesperi, Iacopo, Dar, M. Ibrahim, Bayrak Pehlivan, Ilknur, Gould, Isaac E., Vagott, Jacob N., Dagar, Janardan, Kettle, Jeff, Yang, Jie, Li, Jinzhao, Smith, Joel A., Pascual, Jorge, Jerónimo-Rendón, Jose J., Montoya, Juan Felipe, Correa-Baena, Juan-Pablo, Qiu, Junming, Wang, Junxin, Sveinbjörnsson, Kári, Hirselandt, Katrin, Dey, Krishanu, Frohna, Kyle, Mathies, Lena, Castriotta, Luigi A., Aldamasy, Mahmoud. H., Vasquez-Montoya, Manuel, Ruiz-Preciado, Marco A., Flatken, Marion A., Khenkin, Mark V., Grischek, Max, Kedia, Mayank, Saliba, Michael, Anaya, Miguel, Veldhoen, Misha, Arora, Neha, Shargaieva, Oleksandra, Maus, Oliver, Game, Onkar S., Yudilevich, Ori, Fassl, Paul, Zhou, Qisen, Betancur, Rafael, Munir, Rahim, Patidar, Rahul, Stranks, Samuel D., Alam, Shahidul, Kar, Shaoni, Unold, Thomas, Abzieher, Tobias, Edvinsson, Tomas, David, Tudur Wyn, Paetzold, Ulrich W., Zia, Waqas, Fu, Weifei, Zuo, Weiwei, Schröder, Vincent R. F., Tress, Wolfgang, Zhang, Xiaoliang, Chiang, Yu-Hsien, Iqbal, Zafar, Xie, Zhiqiang, and Unger, Eva

Published
2022
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9. Enhancing Drug Delivery Efficacy Through Bilayer Coating of Zirconium-Based Metal–Organic Frameworks: Sustained Release and Improved Chemical Stability and Cellular Uptake for Cancer Therapy

Author

Liu, Xiewen, primary, Obacz, Joanna, additional, Emanuelli, Giulia, additional, Chambers, Joseph E., additional, Abreu, Susana, additional, Chen, Xu, additional, Linnane, Emily, additional, Mehta, Joshua P., additional, Wheatley, Andrew E. H., additional, Marciniak, Stefan J., additional, and Fairen-Jimenez, David, additional

Published
2024
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10. Expanding the Reticular Chemistry Building Block Library toward Highly Connected Nets: Ultraporous MOFs Based on 18-Connected Ternary, Trigonal Prismatic Superpolyhedra

Author

Froudas, Konstantinos G., primary, Vassaki, Maria, additional, Papadopoulos, Konstantinos, additional, Tsangarakis, Constantinos, additional, Chen, Xu, additional, Shepard, William, additional, Fairen-Jimenez, David, additional, Tampaxis, Christos, additional, Charalambopoulou, Georgia, additional, Steriotis, Theodore A., additional, and Trikalitis, Pantelis N., additional

Published
2024
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14. Spin crossover {[Fe(atrz)3](OTs)2}n monolith: a green synthesis approach for Robust switchable materials.

Author

Martinez-Martinez, Ana, Albacete, Pablo, García-Hernández, Mar, Resines-Urien, Esther, Fairen-Jimenez, David, and Sánchez Costa, José

Subjects
SPIN crossover, SUSTAINABLE chemistry, NANOPARTICLE synthesis, LOW temperatures
Abstract

This work presents a straightforward, room-temperature synthesis of a robust {[Fe(atrz)3](OTs)2}n monolith. This approach offers a green alternative to traditional nanoparticle synthesis for manipulating spin crossover (SCO) behaviour. The monolith exhibits a more gradual SCO transition at lower temperatures compared to the bulk material, aligning with observations in smaller particle systems. Notably, the synthesis employs a solvent- and surfactant-free approach, simplifying the process and potentially reducing environmental impact, aligning with the principles of green chemistry. [ABSTRACT FROM AUTHOR]

Published
2024
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17. A Fluorinated BODIPY-Based Zirconium Metal–Organic Framework for In Vivo Enhanced Photodynamic Therapy

Author

Chen, Xu, primary, Mendes, Bárbara B., additional, Zhuang, Yunhui, additional, Conniot, João, additional, Mercado Argandona, Sergio, additional, Melle, Francesca, additional, Sousa, Diana P., additional, Perl, David, additional, Chivu, Alexandru, additional, Patra, Hirak K., additional, Shepard, William, additional, Conde, João, additional, and Fairen-Jimenez, David, additional

Published
2024
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18. Establishing ZIF‐8 as a reference material for hydrogen cryoadsorption: An interlaboratory study

Author

Villajos, Jose A., primary, Balderas-Xicohténcatl, Rafael, additional, Al Shakhs, Ali N., additional, Berenguer-Murcia, Ángel, additional, Buckley, Craig E., additional, Cazorla-Amoros, Diego, additional, Charalambopoulou, Georgia, additional, Couturas, Fabrice, additional, Cuevas, Fermin, additional, Fairen-Jimenez, David, additional, Heinselman, Karen N., additional, Humphries, Terry, additional, Kaskel, Stefan, additional, Kim, Hyunlim, additional, Marco-Lozar, Juan P., additional, Oh, Hyunchul, additional, Parilla, Philip A., additional, Paskevicius, Mark, additional, Senkovska, Irena, additional, Shulda, Sarah, additional, Silvestre-Albero, Joaquin, additional, Tampaxis, Christos, additional, Steriotis, Theodore, additional, Hirscher, Michael, additional, and Maiwald, Michael, additional

Published
2024
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26. Monolithic Zirconium‐Based Metal–Organic Frameworks for Energy‐Efficient Water Adsorption Applications

Author

Çamur, Ceren, primary, Babu, Robin, additional, Suárez del Pino, José A., additional, Rampal, Nakul, additional, Pérez‐Carvajal, Javier, additional, Hügenell, Philipp, additional, Ernst, Sebastian‐Johannes, additional, Silvestre‐Albero, Joaquin, additional, Imaz, Inhar, additional, Madden, David G., additional, Maspoch, Daniel, additional, and Fairen‐Jimenez, David, additional

Published
2023
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27. Feasibility of Coacervate-Like Nanostructure for Instant Drug Nanoformulation

Author

Zhu, Geyunjian H., primary, Azharuddin, Mohammad, additional, Pramanik, Bapan, additional, Roberg, Karin, additional, Biswas, Sujoy Kumar, additional, D’arcy, Padraig, additional, Lu, Meng, additional, Kaur, Apanpreet, additional, Chen, Alexander, additional, Dhara, Ashis Kumar, additional, Chivu, Alexandru, additional, Zhuang, Yunhui, additional, Baker, Andrew, additional, Liu, Xiewen, additional, Fairen-Jimenez, David, additional, Mazumder, Bismoy, additional, Chen, Rongjun, additional, Kaminski, Clemens F., additional, Kaminski Schierle, Gabriele S., additional, Hinkula, Jorma, additional, Slater, Nigel K. H., additional, and Patra, Hirak K., additional

Published
2023
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28. Monolithic Zirconium-Based Metal–Organic Frameworks for Energy-Efficient Water Adsorption Applications

Author

Universidad de Alicante. Departamento de Química Inorgánica, Çamur, Ceren, Babu, Robin, Suárez del Pino, Jose A., Rampal, Nakul, Pérez Carvajal, Javier, Hügenell, Philipp, Ernst, Sebastian-Johannes, Silvestre-Albero, Joaquín, Imaz, Inhar, Madden, David G., Maspoch, Daniel, Fairen-Jimenez, David, Universidad de Alicante. Departamento de Química Inorgánica, Çamur, Ceren, Babu, Robin, Suárez del Pino, Jose A., Rampal, Nakul, Pérez Carvajal, Javier, Hügenell, Philipp, Ernst, Sebastian-Johannes, Silvestre-Albero, Joaquín, Imaz, Inhar, Madden, David G., Maspoch, Daniel, and Fairen-Jimenez, David

Abstract

Space cooling and heating, ventilation, and air conditioning (HVAC) accounts for roughly 10% of global electricity use and are responsible for ca. 1.13 gigatonnes of CO2 emissions annually. Adsorbent-based HVAC technologies have long been touted as an energy-efficient alternative to traditional refrigeration systems. However, thus far, no suitable adsorbents have been developed which overcome the drawbacks associated with traditional sorbent materials such as silica gels and zeolites. Metal–organic frameworks (MOFs) offer order-of-magnitude improvements in water adsorption and regeneration energy requirements. However, the deployment of MOFs in HVAC applications has been hampered by issues related to MOF powder processing. Herein, three high-density, shaped, monolithic MOFs (UiO-66, UiO-66-NH2, and Zr-fumarate) with exceptional volumetric gas/vapor uptake are developed—solving previous issues in MOF-HVAC deployment. The monolithic structures across the mesoporous range are visualized using small-angle X-ray scattering and lattice-gas models, giving accurate predictions of adsorption characteristics of the monolithic materials. It is also demonstrated that a fragile MOF such as Zr-fumarate can be synthesized in monolithic form with a bulk density of 0.76 gcm−3 without losing any adsorption performance, having a coefficient of performance (COP) of 0.71 with a low regeneration temperature (≤ 100 °C).

Published
2023

29. Feasibility of Coacervate-Like Nanostructure for Instant Drug Nanoformulation

Author

Zhu, Geyunjian H., Azharuddin, Mohammad, Pramanik, Bapan, Roberg, Karin, Biswas, Sujoy Kumar, D´arcy, Padraig, Lu, Meng, Kaur, Apanpreet, Chen, Alexander, Dhara, Ashis Kumar, Chivu, Alexandru, Zhuang, Yunhui, Baker, Andrew, Liu, Xiewen, Fairen-Jimenez, David, Mazumder, Bismoy, Chen, Rongjun, Kaminski, Clemens F., Schierle, Gabriele S. Kaminski, Hinkula, Jorma, Slater, Nigel K. H., Patra, Hirak K., Zhu, Geyunjian H., Azharuddin, Mohammad, Pramanik, Bapan, Roberg, Karin, Biswas, Sujoy Kumar, D´arcy, Padraig, Lu, Meng, Kaur, Apanpreet, Chen, Alexander, Dhara, Ashis Kumar, Chivu, Alexandru, Zhuang, Yunhui, Baker, Andrew, Liu, Xiewen, Fairen-Jimenez, David, Mazumder, Bismoy, Chen, Rongjun, Kaminski, Clemens F., Schierle, Gabriele S. Kaminski, Hinkula, Jorma, Slater, Nigel K. H., and Patra, Hirak K.

Abstract

Despite the enormous advancements in nanomedicine research, a limited number of nanoformulations are available on the market, and few have been translated to clinics. An easily scalable, sustainable, and cost-effective manufacturing strategy and long-term stability for storage are crucial for successful translation. Here, we report a system and method to instantly formulate NF achieved with a nanoscale polyelectrolyte coacervate-like system, consisting of anionic pseudopeptide poly(L-lysine isophthalamide) derivatives, polyethylenimine, and doxorubicin (Dox) via simple "mix-and-go" addition of precursor solutions in seconds. The coacervate-like nanosystem shows enhanced intracellular delivery of Dox to patient-derived multidrug-resistant (MDR) cells in 3D tumor spheroids. The results demonstrate the feasibility of an instant drug formulation using a coacervate-like nanosystem. We envisage that this technique can be widely utilized in the nanomedicine field to bypass the special requirement of large-scale production and elongated shelf life of nanomaterials., Funding Agencies|EU [706694]; MIIC International Postdoc grant (Linkoping University); British Council; UKIERI; Engineering and Physical Sciences Research Council; MRC [MR/T030968/1]; SPARC [P325]

Published
2023
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30. A Fluorinated BODIPY-Based Zirconium Metal–Organic Framework for In VivoEnhanced Photodynamic Therapy

Author

Chen, Xu, Mendes, Bárbara B., Zhuang, Yunhui, Conniot, João, Mercado Argandona, Sergio, Melle, Francesca, Sousa, Diana P., Perl, David, Chivu, Alexandru, Patra, Hirak K., Shepard, William, Conde, João, and Fairen-Jimenez, David

Abstract

Photodynamic therapy (PDT), an emergent noninvasive cancer treatment, is largely dependent on the presence of efficient photosensitizers (PSs) and a sufficient oxygen supply. However, the therapeutic efficacy of PSs is greatly compromised by poor solubility, aggregation tendency, and oxygen depletion within solid tumors during PDT in hypoxic microenvironments. Despite the potential of PS-based metal–organic frameworks (MOFs), addressing hypoxia remains challenging. Boron dipyrromethene (BODIPY) chromophores, with excellent photostability, have exhibited great potential in PDT and bioimaging. However, their practical application suffers from limited chemical stability under harsh MOF synthesis conditions. Herein, we report the synthesis of the first example of a Zr-based MOF, namely, 69-L2, exclusively constructed from the BODIPY-derived ligands via a single-crystal to single-crystal post-synthetic exchange, where a direct solvothermal method is not applicable. To increase the PDT performance in hypoxia, we modify 69-L2with fluorinated phosphate-functionalized methoxy poly(ethylene glycol). The resulting 69-L2@F is an oxygen carrier, enabling tumor oxygenation and simultaneously acting as a PS for reactive oxygen species (ROS) generation under LED irradiation. We demonstrate that 69-L2@F has an enhanced PDT effect in triple-negative breast cancer MDA-MB-231 cells under both normoxia and hypoxia. Following positive results, we evaluated the in vivoactivity of 69-L2@F with a hydrogel, enabling local therapy in a triple-negative breast cancer mice model and achieving exceptional antitumor efficacy in only 2 days. We envision BODIPY-based Zr-MOFs to provide a solution for hypoxia relief and maximize efficacy during in vivoPDT, offering new insights into the design of promising MOF-based PSs for hypoxic tumors.

Published
2024
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37. Monolithic Zirconium-based Metal-Organic Frameworks for Energy-Efficient Water Sorption Applications

Author

Çamur, Ceren, Babu, Robin, Suárez del Pino, José A., Rampal, Nakul, Pérez-Carvajal, Javier, Hügenell, Philipp, Ernst, Sebastian-Johannes, Silvestre-Albero, Joaquin, Imaz, Inhar, Madden, David G., Maspoch, Daniel, Fairen-Jimenez, David, and Publica

Abstract

Space cooling and heating, ventilation, and air conditioning (HVAC) accountsfor roughly 10% of global electricity use and are responsible for ca. 1.13gigatonnes of CO2emissions annually. Adsorbent-based HVAC technologieshave long been touted as an energy-efficient alternative to traditionalrefrigeration systems. However, thus far, no suitable adsorbents have beendeveloped which overcome the drawbacks associated with traditional sorbentmaterials such as silica gels and zeolites. Metal-organic frameworks (MOFs)offer order-of-magnitude improvements in water adsorption and regenerationenergy requirements. However, the deployment of MOFs in HVACapplications has been hampered by issues related to MOF powderprocessing. Herein, three high-density, shaped, monolithic MOFs (UiO-66,UiO-66-NH2, and Zr-fumarate) with exceptional volumetric gas/vapor uptakeare developed - solving previous issues in MOF-HVAC deployment. Themonolithic structures across the mesoporous range are visualized usingsmall-angle X-ray scattering and lattice-gas models, giving accuratepredictions of adsorption characteristics of the monolithic materials. It is alsodemonstrated that a fragile MOF such as Zr-fumarate can be synthesized inmonolithic form with a bulk density of 0.76 gcm-3without losing anyadsorption performance, having a coefficient of performance (COP) of 0.71with a low regeneration temperature (≤100°C).

Published
2023
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38. Size-tuneable and immunocompatible polymer nanocarriers for drug delivery in pancreatic cancer

Author

Popov, Andrea Bistrović, Melle, Francesca, Linnane, Emily, González-López, Cristina, Ahmed, Ishtiaq, Parshad, Badri, Franck, Christoph O, Rahmoune, Hassan, Richards, Frances M, Muñoz-Espín, Daniel, Jodrell, Duncan I, Fairen-Jimenez, David, Fruk, Ljiljana, Richards, Frances M [0000-0001-7947-7853], Fairen-Jimenez, David [0000-0002-5013-1194], and Apollo - University of Cambridge Repository

Subjects
Pancreatic Neoplasms, Drug Carriers, Drug Delivery Systems, Polymers, Histocompatibility, Tumor Microenvironment, Humans, Nanoparticles, General Materials Science
Abstract

Nanocarriers have emerged as one of the most promising approaches for drug delivery. Although several nanomaterials have been approved for clinical use, the translation from lab to clinic remains challenging. However, by implementing rational design strategies and using relevant models for their validation, these challenges are being addressed. This work describes the design of novel immunocompatible polymer nanocarriers made of melanin-mimetic polydopamine and Pluronic F127 units. The nanocarrier preparation was conducted under mild conditions, using a highly reproducible method that was tuned to provide a range of particle sizes (

Published
2022

39. From computational high-throughput screenings to the lab: taking metal-organic frameworks out of the computer

Author

Li, Aurelia, Bueno-Perez, Rocio, Madden, David, Fairen-Jimenez, David, Apollo-University Of Cambridge Repository, Li, Aurelia [0000-0001-8298-3992], Bueno-Perez, Rocio [0000-0002-1472-6852], Madden, David [0000-0003-3875-9146], Fairen-Jimenez, David [0000-0002-5013-1194], and Apollo - University of Cambridge Repository

Subjects
3403 Macromolecular and Materials Chemistry, 34 Chemical Sciences, General Chemistry
Abstract

Metal-organic frameworks (MOFs) are one of the most researched designer materials today, as their high tunability offers scientists a wide space to imagine all kinds of possible structures. Their uniquely flexible customisability spurred the creation of hypothetical datasets and the syntheses of more than 100 000 MOFs officially reported in the Cambridge Structural Database. To scan such large numbers of MOFs, computational high-throughput screenings (HTS) have become the customary method to identify the most promising structure for a given application, and/or to spot useful structure-property relationships. However, despite all these data-mining efforts, only a fraction of HTS studies have identified synthesisable top-performing MOFs that were then further investigated in the lab. In this perspective, we review these specific cases and suggest possible steps to push future HTS more systematically towards synthesisable structures.

Published
2022

40. Densified HKUST-1 Monoliths as a Route to High Volumetric and Gravimetric Hydrogen Storage Capacity

Author

Madden, David Gerard, Rampal, Nakul, Babu, Robin, Al Shakhs, Ali N., Zhang, Shi Yuan, Rance, Graham A., Perez, Javier, Maria Casati, Nicola Pietro, Cuadrado-Collados, Carlos, Rice, Nicholas P., Gennett, Thomas, Parilla, Philip, Shulda, Sarah, Hurst, Katherine E., Stavila, Vitalie, Allendorf, Mark D., Silvestre-Albero, Joaquin, Forse, Alexander C., Champness, Neil R., Chapman, Karena W., and Fairen-Jimenez, David

Subjects
Colloid and Surface Chemistry, Biochemistry, General Chemistry, Catalysis
Abstract

We are currently witnessing the dawn of hydrogen (H2) economy, where H2 will soon become a primary fuel for heating, transportation, and long-distance and long-term energy storage. Among diverse possibilities, H2 can be stored as a pressurized gas, a cryogenic liquid, or a solid fuel via adsorption onto porous materials. Metal-organic frameworks (MOFs) have emerged as adsorbent materials with the highest theoretical H2 storage densities on both a volumetric and gravimetric basis. However, a critical bottleneck for the use of H2 as a transportation fuel has been the lack of densification methods capable of shaping MOFs into practical formulations while maintaining their adsorptive performance. Here, we report a high-throughput screening and deep analysis of a database of MOFs to find optimal materials, followed by the synthesis, characterization, and performance evaluation of an optimal monolithic MOF (monoMOF) for H2 storage. After densification, this monoMOF stores 46 g L-1 H2 at 50 bar and 77 K and delivers 41 and 42 g L-1 H2 at operating pressures of 25 and 50 bar, respectively, when deployed in a combined temperature-pressure (25-50 bar/77 K ? 5 bar/160 K) swing gas delivery system. This performance represents up to an 80% reduction in the operating pressure requirements for delivering H2 gas when compared with benchmark materials and an 83% reduction compared to compressed H2 gas. Our findings represent a substantial step forward in the application of high-density materials for volumetric H2 storage applications.

Published
2022

42. The development of a comprehensive toolbox based on multi-level, high-throughput screening of MOFs for CO/N2 separations

Author

Rampal, Nakul, Ajenifuja, Abdulmalik, Tao, Andi, Balzer, Christopher, Cummings, Matthew S, Evans, Arwyn, Bueno-Perez, Rocio, Law, David J, Bolton, Leslie W, Petit, Camille, Siperstein, Flor, Attfield, Martin P, Jobson, Megan, Moghadam, Peyman Z, Fairen-Jimenez, David, Rampal, Nakul [0000-0002-6187-5631], Ajenifuja, Abdulmalik [0000-0003-0836-2260], Balzer, Christopher [0000-0002-9767-8437], Cummings, Matthew S [0000-0003-2837-1228], Evans, Arwyn [0000-0001-8383-8594], Bueno-Perez, Rocio [0000-0002-1472-6852], Petit, Camille [0000-0002-3722-7984], Siperstein, Flor [0000-0003-3464-2100], Attfield, Martin P [0000-0001-6508-1751], Jobson, Megan [0000-0001-9626-5879], Moghadam, Peyman Z [0000-0002-1592-0139], Fairen-Jimenez, David [0000-0002-5013-1194], and Apollo - University of Cambridge Repository

Subjects
3403 Macromolecular and Materials Chemistry, 34 Chemical Sciences
Abstract

The separation of CO/N2 mixtures is a challenging problem in the petrochemical sector due to the very similar physical properties of these two molecules, such as size, molecular weight and boiling point. To solve this and other challenging gas separations, one requires a holistic approach. The complexity of a screening exercise for adsorption-based separations arises from the multitude of existing porous materials, including metal-organic frameworks. Besides, the multivariate nature of the performance criteria that needs to be considered when designing an optimal adsorbent and a separation process - i.e. an optimal material requires fulfillment of several criteria simultaneously - makes the screening challenging. To address this, we have developed a multi-scale approach combining high-throughput molecular simulation screening, data mining and advanced visualization, as well as process system modelling, backed up by experimental validation. We have applied our recent advances in the engineering of porous materials' morphology to develop advanced monolithic structures. These conformed, shaped monoliths can be used readily in industrial applications, bringing a valuable strategy for the development of advanced materials. This toolbox is flexible enough to be applied to multiple adsorption-based gas separation applications.

Published
2021
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43. How Reproducible are Surface Areas Calculated from the BET Equation? (Adv. Mater. 27/2022)

Author

Osterrieth, Johannes W. M., primary, Rampersad, James, additional, Madden, David, additional, Rampal, Nakul, additional, Skoric, Luka, additional, Connolly, Bethany, additional, Allendorf, Mark D., additional, Stavila, Vitalie, additional, Snider, Jonathan L., additional, Ameloot, Rob, additional, Marreiros, João, additional, Ania, Conchi, additional, Azevedo, Diana, additional, Vilarrasa‐Garcia, Enrique, additional, Santos, Bianca F., additional, Bu, Xian‐He, additional, Chang, Ze, additional, Bunzen, Hana, additional, Champness, Neil R., additional, Griffin, Sarah L., additional, Chen, Banglin, additional, Lin, Rui‐Biao, additional, Coasne, Benoit, additional, Cohen, Seth, additional, Moreton, Jessica C., additional, Colón, Yamil J., additional, Chen, Linjiang, additional, Clowes, Rob, additional, Coudert, François‐Xavier, additional, Cui, Yong, additional, Hou, Bang, additional, D'Alessandro, Deanna M., additional, Doheny, Patrick W., additional, Dincă, Mircea, additional, Sun, Chenyue, additional, Doonan, Christian, additional, Huxley, Michael Thomas, additional, Evans, Jack D., additional, Falcaro, Paolo, additional, Ricco, Raffaele, additional, Farha, Omar, additional, Idrees, Karam B., additional, Islamoglu, Timur, additional, Feng, Pingyun, additional, Yang, Huajun, additional, Forgan, Ross S., additional, Bara, Dominic, additional, Furukawa, Shuhei, additional, Sanchez, Eli, additional, Gascon, Jorge, additional, Telalović, Selvedin, additional, Ghosh, Sujit K., additional, Mukherjee, Soumya, additional, Hill, Matthew R., additional, Sadiq, Muhammed Munir, additional, Horcajada, Patricia, additional, Salcedo‐Abraira, Pablo, additional, Kaneko, Katsumi, additional, Kukobat, Radovan, additional, Kenvin, Jeff, additional, Keskin, Seda, additional, Kitagawa, Susumu, additional, Otake, Ken‐ichi, additional, Lively, Ryan P., additional, DeWitt, Stephen J. A., additional, Llewellyn, Phillip, additional, Lotsch, Bettina V., additional, Emmerling, Sebastian T., additional, Pütz, Alexander M., additional, Martí‐Gastaldo, Carlos, additional, Padial, Natalia M., additional, García‐Martínez, Javier, additional, Linares, Noemi, additional, Maspoch, Daniel, additional, Suárez del Pino, Jose A., additional, Moghadam, Peyman, additional, Oktavian, Rama, additional, Morris, Russel E., additional, Wheatley, Paul S., additional, Navarro, Jorge, additional, Petit, Camille, additional, Danaci, David, additional, Rosseinsky, Matthew J., additional, Katsoulidis, Alexandros P., additional, Schröder, Martin, additional, Han, Xue, additional, Yang, Sihai, additional, Serre, Christian, additional, Mouchaham, Georges, additional, Sholl, David S., additional, Thyagarajan, Raghuram, additional, Siderius, Daniel, additional, Snurr, Randall Q., additional, Goncalves, Rebecca B., additional, Telfer, Shane, additional, Lee, Seok J., additional, Ting, Valeska P., additional, Rowlandson, Jemma L., additional, Uemura, Takashi, additional, Iiyuka, Tomoya, additional, van der Veen, Monique A., additional, Rega, Davide, additional, Van Speybroeck, Veronique, additional, Rogge, Sven M. J., additional, Lamaire, Aran, additional, Walton, Krista S., additional, Bingel, Lukas W., additional, Wuttke, Stefan, additional, Andreo, Jacopo, additional, Yaghi, Omar, additional, Zhang, Bing, additional, Yavuz, Cafer T., additional, Nguyen, Thien S., additional, Zamora, Felix, additional, Montoro, Carmen, additional, Zhou, Hongcai, additional, Kirchon, Angelo, additional, and Fairen‐Jimenez, David, additional

Published
2022
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44. Turning Molecular Springs into Nano-Shock Absorbers: The Effect of Macroscopic Morphology and Crystal Size on the Dynamic Hysteresis of Water Intrusion–Extrusion into-from Hydrophobic Nanopores

Author

Zajdel, Paweł, primary, Madden, David G., additional, Babu, Robin, additional, Tortora, Marco, additional, Mirani, Diego, additional, Tsyrin, Nikolay Nikolaevich, additional, Bartolomé, Luis, additional, Amayuelas, Eder, additional, Fairen-Jimenez, David, additional, Lowe, Alexander Rowland, additional, Chorążewski, Mirosław, additional, Leao, Juscelino B., additional, Brown, Craig M., additional, Bleuel, Markus, additional, Stoudenets, Victor, additional, Casciola, Carlo Massimo, additional, Echeverría, María, additional, Bonilla, Francisco, additional, Grancini, Giulia, additional, Meloni, Simone, additional, and Grosu, Yaroslav, additional

Published
2022
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46. Insights into the electric double-layer capacitance of two-dimensional electrically conductive metal-organic frameworks

Author

Gittins, Jamie W, Balhatchet, Chloe J, Chen, Yuan, Liu, Cheng, Madden, David G, Britto, Sylvia, Golomb, Matthias J, Walsh, Aron, Fairen-Jimenez, David, Dutton, Siân E, Forse, Alexander C, Gittins, Jamie W [0000-0002-9106-8910], Balhatchet, Chloe J [0000-0001-9159-1384], Chen, Yuan [0000-0002-8744-4557], Liu, Cheng [0000-0002-3509-951X], Madden, David G [0000-0003-3875-9146], Britto, Sylvia [0000-0003-1515-307X], Golomb, Matthias J [0000-0001-6749-0129], Walsh, Aron [0000-0001-5460-7033], Fairen-Jimenez, David [0000-0002-5013-1194], Dutton, Siân E [0000-0003-0984-5504], Forse, Alexander C [0000-0001-9592-9821], and Apollo - University of Cambridge Repository

Subjects
34 Chemical Sciences, 7 Affordable and Clean Energy, 4016 Materials Engineering, 40 Engineering
Abstract

Two-dimensional electrically conductive metal-organic frameworks (MOFs) have emerged as promising model electrodes for use in electric double-layer capacitors (EDLCs). However, a number of fundamental questions about the behaviour of this class of materials in EDLCs remain unanswered, including the effect of the identity of the metal node and organic linker molecule on capacitive performance and the limitations of current conductive MOFs in these devices relative to traditional activated carbon electrode materials. Herein, we address both these questions via a detailed study of the capacitive performance of the framework Cu3(HHTP)2 (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) with an acetonitrile-based electrolyte, finding a specific capacitance of 110 – 114 F g−1 at current densities of 0.04 – 0.05 A g−1 and a modest rate capability. By, directly comparing its performance with the previously reported analogue, Ni3(HITP)2 (HITP = 2,3,6,7,10,11-hexaiminotriphenylene), we illustrate that capacitive performance is largely independent of the identity of the metal node and organic linker molecule in these nearly isostructural MOFs. Importantly, this result suggests that EDLC performance in general is uniquely defined by the 3D structure of the electrodes and the electrolyte, a significant finding not demonstrated using traditional electrode materials. Finally, we probe the limitations of Cu3(HHTP)2 in EDLCs, finding a limited cell voltage window of 1.3 V and only a modest capacitance retention of 81 % over 30,000 cycles, both significantly lower than state-of-the-art porous carbons. These important insights will aid the design of future conductive MOFs with greater EDLC performances.

Published
2021

47. How Reproducible are Surface Areas Calculated from the BET Equation?

Author

Universidad de Alicante. Departamento de Química Inorgánica, Osterrieth, Johannes W. M., Rampersad, James, Madden, David G., Rampal, Nakul, Skoric, Luka, Connolly, Bethany M., Allendorf, Mark D., Stavila, Vitalie, Snider, Jonathan L., Ameloot, Rob, Marreiros, João, Coudert, François-Xavier, Cui, Yong, Hou, Bang, D'Alessandro, Deanna M., Doheny, Patrick W., Dincă, Mircea, Sun, Chenyue, Doonan, Christian, Huxley, Michael Thomas, Evans, Jack D., Bara, Dominic, Falcaro, Paolo, Ricco, Raffaele, Farha, Omar, Idrees, Karam B., Islamoglu, Timur, Feng, Pingyun, Yang, Huajun, Forgan, Ross S., Furukawa, Shuhei, Sanchez, Eli, Gascon, Jorge, Telalović, Selvedin, Ghosh, Sujit K., Mukherjee, Soumya, Hill, Matthew R., Sadiq, Muhammed Munir, Horcajada, Patricia, DeWitt, Stephen J. A., Salcedo-Abraira, Pablo, Kaneko, Katsumi, Kukobat, Radovan, Kenvin, Jeff, Keskin, Seda, Kitagawa, Susumu, Otake, Ken-ichi, Lively, Ryan P., Llewellyn, Phillip L., Lotsch, Bettina V., Emmerling, Sebastian T., Pütz, Alexander M., Martí-Gastaldo, Carlos, Padial, Natalia M., Garcia-Martinez, Javier, Linares, Noemi, Maspoch, Daniel, Rosseinsky, Matthew J., Suárez del Pino, Jose A., Moghadam, Peyman Z., Oktavian, Rama, Morris, Russel E., Wheatley, Paul S., Navarro, Jorge, Petit, Camille, Danaci, David, Katsoulidis, Alexandros P., Schröder, Martin, Han, Xue, Yang, Sihai, Serre, Christian, Mouchaham, Georges, Sholl, David S., Thyagarajan, Raghuram, Siderius, Daniel, van der Veen, Monique A., Snurr, Randall Q., Goncalves, Rebecca B., Telfer, Shane, Lee, Seok J., Ting, Valeska P., Rowlandson, Jemma L., Uemura, Takashi, Iiyuka, Tomoya, Rega, Davide, Van Speybroeck, Veronique, Rogge, Sven M.J., Lamaire, Aran, Walton, Krista S., Bingel, Lukas W., Wuttke, Stefan, Andreo, Jacopo, Yaghi, Omar, Ania, Conchi O., Zhang, Bing, Yavuz, Cafer T., Nguyen, Thien S., Zamora, Félix, Montoro, Carmen, Zhou, Hongcai, Kirchon, Angelo, Fairen-Jimenez, David, Azevedo, Diana, Vilarrasa-García, Enrique, Santos, Bianca F., Bu, Xian-He, Chang, Ze, Bunzen, Hana, Champness, Neil R., Griffin, Sarah L., Chen, Banglin, Lin, Rui-Biao, Coasne, Benoit, Cohen, Seth, Moreton, Jessica C., Colón, Yamil J., Chen, Linjiang, Clowes, Rob, Universidad de Alicante. Departamento de Química Inorgánica, Osterrieth, Johannes W. M., Rampersad, James, Madden, David G., Rampal, Nakul, Skoric, Luka, Connolly, Bethany M., Allendorf, Mark D., Stavila, Vitalie, Snider, Jonathan L., Ameloot, Rob, Marreiros, João, Coudert, François-Xavier, Cui, Yong, Hou, Bang, D'Alessandro, Deanna M., Doheny, Patrick W., Dincă, Mircea, Sun, Chenyue, Doonan, Christian, Huxley, Michael Thomas, Evans, Jack D., Bara, Dominic, Falcaro, Paolo, Ricco, Raffaele, Farha, Omar, Idrees, Karam B., Islamoglu, Timur, Feng, Pingyun, Yang, Huajun, Forgan, Ross S., Furukawa, Shuhei, Sanchez, Eli, Gascon, Jorge, Telalović, Selvedin, Ghosh, Sujit K., Mukherjee, Soumya, Hill, Matthew R., Sadiq, Muhammed Munir, Horcajada, Patricia, DeWitt, Stephen J. A., Salcedo-Abraira, Pablo, Kaneko, Katsumi, Kukobat, Radovan, Kenvin, Jeff, Keskin, Seda, Kitagawa, Susumu, Otake, Ken-ichi, Lively, Ryan P., Llewellyn, Phillip L., Lotsch, Bettina V., Emmerling, Sebastian T., Pütz, Alexander M., Martí-Gastaldo, Carlos, Padial, Natalia M., Garcia-Martinez, Javier, Linares, Noemi, Maspoch, Daniel, Rosseinsky, Matthew J., Suárez del Pino, Jose A., Moghadam, Peyman Z., Oktavian, Rama, Morris, Russel E., Wheatley, Paul S., Navarro, Jorge, Petit, Camille, Danaci, David, Katsoulidis, Alexandros P., Schröder, Martin, Han, Xue, Yang, Sihai, Serre, Christian, Mouchaham, Georges, Sholl, David S., Thyagarajan, Raghuram, Siderius, Daniel, van der Veen, Monique A., Snurr, Randall Q., Goncalves, Rebecca B., Telfer, Shane, Lee, Seok J., Ting, Valeska P., Rowlandson, Jemma L., Uemura, Takashi, Iiyuka, Tomoya, Rega, Davide, Van Speybroeck, Veronique, Rogge, Sven M.J., Lamaire, Aran, Walton, Krista S., Bingel, Lukas W., Wuttke, Stefan, Andreo, Jacopo, Yaghi, Omar, Ania, Conchi O., Zhang, Bing, Yavuz, Cafer T., Nguyen, Thien S., Zamora, Félix, Montoro, Carmen, Zhou, Hongcai, Kirchon, Angelo, Fairen-Jimenez, David, Azevedo, Diana, Vilarrasa-García, Enrique, Santos, Bianca F., Bu, Xian-He, Chang, Ze, Bunzen, Hana, Champness, Neil R., Griffin, Sarah L., Chen, Banglin, Lin, Rui-Biao, Coasne, Benoit, Cohen, Seth, Moreton, Jessica C., Colón, Yamil J., Chen, Linjiang, and Clowes, Rob

Abstract

Porosity and surface area analysis play a prominent role in modern materials science. At the heart of this sits the Brunauer–Emmett–Teller (BET) theory, which has been a remarkably successful contribution to the field of materials science. The BET method was developed in the 1930s for open surfaces but is now the most widely used metric for the estimation of surface areas of micro- and mesoporous materials. Despite its widespread use, the calculation of BET surface areas causes a spread in reported areas, resulting in reproducibility problems in both academia and industry. To prove this, for this analysis, 18 already-measured raw adsorption isotherms were provided to sixty-one labs, who were asked to calculate the corresponding BET areas. This round-robin exercise resulted in a wide range of values. Here, the reproducibility of BET area determination from identical isotherms is demonstrated to be a largely ignored issue, raising critical concerns over the reliability of reported BET areas. To solve this major issue, a new computational approach to accurately and systematically determine the BET area of nanoporous materials is developed. The software, called “BET surface identification” (BETSI), expands on the well-known Rouquerol criteria and makes an unambiguous BET area assignment possible.

Published
2022

48. An open-access database and analysis tool for perovskite solar cells based on the FAIR data principles

Author

Jacobsson, Jesper, Hultqvist, Adam, Garcia-Fernandez, Alberto, Anand, Aman, Al-Ashouri, Amran, Hagfeldt, Anders, Crovetto, Andrea, Abate, Antonio, Ricciardulli, Antonio Gaetano, Vijayan, Anuja, Kulkarni, Ashish, Anderson, Assaf Y., Darwich, Barbara Primera, Yang, Bowen, Coles, Brendan L., Perini, Carlo A. R., Rehermann, Carolin, Ramirez, Daniel, Fairen-Jimenez, David, Di Girolamo, Diego, Jia, Donglin, Avila, Elena, Juarez-Perez, Emilio J., Baumann, Fanny, Mathies, Florian, Gonzalez, G. S. Anaya, Boschloo, Gerrit, Nasti, Giuseppe, Paramasivam, Gopinath, Martinez-Denegri, Guillermo, Nasstrom, Hampus, Michaels, Hannes, Kobler, Hans, Wu, Hua, Benesperi, Iacopo, Dar, M. Ibrahim, Bayrak Pehlivan, Ilknur, Gould, Isaac E., Vagott, Jacob N., Dagar, Janardan, Kettle, Jeff, Yang, Jie, Li, Jinzhao, Smith, Joel A., Pascual, Jorge, Jeronimo-Rendon, Jose J., Montoya, Juan Felipe, Correa-Baena, Juan-Pablo, Qiu, Junming, Wang, JunXin, Sveinbjornsson, Kari, Hirselandt, Katrin, Dey, Krishanu, Frohna, Kyle, Mathies, Lena, Castriotta, Luigi A., Aldamasy, Mahmoud H., Vasquez-Montoya, Manuel, Ruiz-Preciado, Marco A., Flatken, Marion A., Khenkin, Mark, V, Grischek, Max, Kedia, Mayank, Saliba, Michael, Anaya, Miguel, Veldhoen, Misha, Arora, Neha, Shargaieva, Oleksandra, Maus, Oliver, Game, Onkar S., Yudilevich, Ori, Fassl, Paul, Zhou, Qisen, Betancur, Rafael, Munir, Rahim, Patidar, Rahul, Stranks, Samuel D., Alam, Shahidul, Kar, Shaoni, Unold, Thomas, Abzieher, Tobias, Edvinsson, Tomas, David, Tudur Wyn, Paetzold, Ulrich W., Zia, Waqas, Fu, Weifei, Zuo, Weiwei, Schroeder, Vincent R. F., Tress, Wolfgang, Zhang, Xiaoliang, Chiang, Yu-Hsien, Iqbal, Zafar, Xie, Zhiqiang, Unger, Eva, Jacobsson, Jesper, Hultqvist, Adam, Garcia-Fernandez, Alberto, Anand, Aman, Al-Ashouri, Amran, Hagfeldt, Anders, Crovetto, Andrea, Abate, Antonio, Ricciardulli, Antonio Gaetano, Vijayan, Anuja, Kulkarni, Ashish, Anderson, Assaf Y., Darwich, Barbara Primera, Yang, Bowen, Coles, Brendan L., Perini, Carlo A. R., Rehermann, Carolin, Ramirez, Daniel, Fairen-Jimenez, David, Di Girolamo, Diego, Jia, Donglin, Avila, Elena, Juarez-Perez, Emilio J., Baumann, Fanny, Mathies, Florian, Gonzalez, G. S. Anaya, Boschloo, Gerrit, Nasti, Giuseppe, Paramasivam, Gopinath, Martinez-Denegri, Guillermo, Nasstrom, Hampus, Michaels, Hannes, Kobler, Hans, Wu, Hua, Benesperi, Iacopo, Dar, M. Ibrahim, Bayrak Pehlivan, Ilknur, Gould, Isaac E., Vagott, Jacob N., Dagar, Janardan, Kettle, Jeff, Yang, Jie, Li, Jinzhao, Smith, Joel A., Pascual, Jorge, Jeronimo-Rendon, Jose J., Montoya, Juan Felipe, Correa-Baena, Juan-Pablo, Qiu, Junming, Wang, JunXin, Sveinbjornsson, Kari, Hirselandt, Katrin, Dey, Krishanu, Frohna, Kyle, Mathies, Lena, Castriotta, Luigi A., Aldamasy, Mahmoud H., Vasquez-Montoya, Manuel, Ruiz-Preciado, Marco A., Flatken, Marion A., Khenkin, Mark, V, Grischek, Max, Kedia, Mayank, Saliba, Michael, Anaya, Miguel, Veldhoen, Misha, Arora, Neha, Shargaieva, Oleksandra, Maus, Oliver, Game, Onkar S., Yudilevich, Ori, Fassl, Paul, Zhou, Qisen, Betancur, Rafael, Munir, Rahim, Patidar, Rahul, Stranks, Samuel D., Alam, Shahidul, Kar, Shaoni, Unold, Thomas, Abzieher, Tobias, Edvinsson, Tomas, David, Tudur Wyn, Paetzold, Ulrich W., Zia, Waqas, Fu, Weifei, Zuo, Weiwei, Schroeder, Vincent R. F., Tress, Wolfgang, Zhang, Xiaoliang, Chiang, Yu-Hsien, Iqbal, Zafar, Xie, Zhiqiang, and Unger, Eva

Abstract

Making large datasets findable, accessible, interoperable and reusable could accelerate technology development. Now, Jacobsson et al. present an approach to build an open-access database and analysis tool for perovskite solar cells. Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences.

Published
2022
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49. Sol-gel processing of a covalent organic framework for the generation of hierarchically porous monolithic adsorbents

Author

Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Carrington, Mark E., Rampal, Nakul, Madden, David G., O’Nolan, Daniel, Casati, Nicola Pietro Maria, Divitini, Giorgio, Martín-Illán, Jesús Á., Tricarico, Michele, Cepitis, Ritums, Çamur, Ceren, Curtin, Teresa, Silvestre-Albero, Joaquín, Tan, Jin-Chong, Zamora, Félix, Taraskin, Sergei, Chapman, Karena W., Fairen-Jimenez, David, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Carrington, Mark E., Rampal, Nakul, Madden, David G., O’Nolan, Daniel, Casati, Nicola Pietro Maria, Divitini, Giorgio, Martín-Illán, Jesús Á., Tricarico, Michele, Cepitis, Ritums, Çamur, Ceren, Curtin, Teresa, Silvestre-Albero, Joaquín, Tan, Jin-Chong, Zamora, Félix, Taraskin, Sergei, Chapman, Karena W., and Fairen-Jimenez, David

Abstract

Covalent organic frameworks (COFs) have emerged as a versatile material platform for such applications as chemical separations, chemical reaction engineering, and energy storage. Their inherently low mechanical stability, however, frequently renders existing methods of pelletization ineffective, contributing to pore collapse, pore blockage, or insufficient densification of crystallites. Here, we present a process for the shaping and densifying of COFs into robust centimeter-scale porous monoliths without the need for templates, additives, or binders. This process minimizes mechanical damage from shear-induced plastic deformation and further provides a network of interparticle mesopores that we exploit in accessing analyte capacities above those achievable from the intrinsic COF structure. Using a lattice-gas model, we accurately capture the monolithic structure across the mesoporous range and tie pore architecture to performance in both gas-storage and -separation applications. Collectively, these results represent a substantial step in the practical applicability of COFs and other mechanically weak porous materials.

Published
2022

50. Densified HKUST-1 Monoliths as a Route to High Volumetric and Gravimetric Hydrogen Storage Capacity

Author

Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Madden, David G., O’Nolan, Daniel, Rampal, Nakul, Babu, Robin, Çamur, Ceren, Al Shakhs, Ali N., Zhang, Shi-Yuan, Rance, Graham A., Perez, Javier, Casati, Nicola Pietro Maria, Cuadrado-Collados, Carlos, O’Sullivan, Denis, Rice, Nicholas P., Gennett, Thomas, Parilla, Philip, Shulda, Sarah, Hurst, Katherine E., Stavila, Vitalie, Allendorf, Mark D., Silvestre-Albero, Joaquín, Forse, Alexander C., Champness, Neil R., Chapman, Karena W., Fairen-Jimenez, David, Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Madden, David G., O’Nolan, Daniel, Rampal, Nakul, Babu, Robin, Çamur, Ceren, Al Shakhs, Ali N., Zhang, Shi-Yuan, Rance, Graham A., Perez, Javier, Casati, Nicola Pietro Maria, Cuadrado-Collados, Carlos, O’Sullivan, Denis, Rice, Nicholas P., Gennett, Thomas, Parilla, Philip, Shulda, Sarah, Hurst, Katherine E., Stavila, Vitalie, Allendorf, Mark D., Silvestre-Albero, Joaquín, Forse, Alexander C., Champness, Neil R., Chapman, Karena W., and Fairen-Jimenez, David

Abstract

We are currently witnessing the dawn of hydrogen (H2) economy, where H2 will soon become a primary fuel for heating, transportation, and long-distance and long-term energy storage. Among diverse possibilities, H2 can be stored as a pressurized gas, a cryogenic liquid, or a solid fuel via adsorption onto porous materials. Metal–organic frameworks (MOFs) have emerged as adsorbent materials with the highest theoretical H2 storage densities on both a volumetric and gravimetric basis. However, a critical bottleneck for the use of H2 as a transportation fuel has been the lack of densification methods capable of shaping MOFs into practical formulations while maintaining their adsorptive performance. Here, we report a high-throughput screening and deep analysis of a database of MOFs to find optimal materials, followed by the synthesis, characterization, and performance evaluation of an optimal monolithic MOF (monoMOF) for H2 storage. After densification, this monoMOF stores 46 g L–1 H2 at 50 bar and 77 K and delivers 41 and 42 g L–1 H2 at operating pressures of 25 and 50 bar, respectively, when deployed in a combined temperature–pressure (25–50 bar/77 K → 5 bar/160 K) swing gas delivery system. This performance represents up to an 80% reduction in the operating pressure requirements for delivering H2 gas when compared with benchmark materials and an 83% reduction compared to compressed H2 gas. Our findings represent a substantial step forward in the application of high-density materials for volumetric H2 storage applications.

Published
2022

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