Article
Engineering, Environmental
Chao Liu, Wenliang Li, Ying Liu, Hailong Wang, Baoqiu Yu, Zongbi Bao, Jianzhuang Jiang
Summary: The enantiomeric porous organic cages, (R)/(S)-BTPOC, prepared via dynamic covalent chemistry, exhibit high CO2 and I-2 adsorption capacities, excellent recyclability, and adsorption ability closely associated with porosity, pi-conjugated network structure, and imine bonds content. This study demonstrates the great application potential of these microporous POCs.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Inorganic & Nuclear
Michael R. Dworzak, Meaghan M. Deegan, Glenn P. A. Yap, Eric D. Bloch
Summary: The influence of ligand functionalization on two series of isoreticular Ni(II)- and Co(II)-based calixarene-capped cages was investigated. The highly soluble cages can still have access to high surface areas for many of the isolated phases.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Mingming Hua, Shuping Wang, Yanjun Gong, Jingjing Wei, Zhijie Yang, Jian-Ke Sun
Summary: The researchers successfully engineered mesopores into microporous organic cages through host-guest interactions with long chain ionic surfactants, equipping the resulting hierarchically porous cage soft materials with charge-selective uptake and release abilities in solution. Interestingly, trapping enzymes within the cage turns it into a nanoreactor, leading to a 5-fold enhancement in enzymatic catalysis activity compared to free enzymes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Eva Martinez-Ahumada, Donglin He, Victoria Berryman, Alfredo Lopez-Olvera, Magali Hernandez, Vojtech Jancik, Vladimir Martis, Marco A. Vera, Enrique Lima, Douglas J. Parker, Andrew I. Cooper, Ilich A. Ibarra, Ming Liu
Summary: This study conducted the first experimental investigation on porous organic cages (POCs) for capturing SO2. It was found that a tertiary amine POC (6FT-RCC3) exhibited high and reversible SO2 capture, demonstrating excellent performance for at least 50 adsorption-desorption cycles. The adsorption behavior was analyzed using FTIR spectroscopy, C-13 CP-MAS NMR experiments, and computational calculations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Ke Tian, Sven M. Elbert, Xin-Yue Hu, Tobias Kirschbaum, Wen-Shan Zhang, Frank Rominger, Rasmus R. Schroeder, Michael Mastalerz
Summary: Anthropogenic greenhouse gases, including perfluorocarbons (PFCs), contribute significantly to global warming. PFCs are thousands to tens of thousands of times more harmful to the environment than carbon dioxide. This study presents a series of porous organic cage compounds with different alkyl chains, allowing the investigation of the relationship between the degree of fluorination and the gas sorption properties. One compound with superior selectivities for PFCs versus N-2 or CO2 under ambient conditions is identified.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Physical
Zezhong John Li, Simcha Srebnik
Summary: Research on cage-based porous materials for carbon capture has shown that external adsorption sites on a 15-crown-5 ether-substituted imine-linked POC can enhance CO2 adsorption capacity, with higher adsorption capacity and greater sensitivity to temperature and pressure changes compared to sites within the cage cavity, making them suitable for pressure- and temperature-swing separation applications.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Takahiro Ami, Kouki Oka, Keiho Tsuchiya, Norimitsu Tohnai
Summary: Porous organic salts (POSs) are porous organic materials formed by self-assembly of aromatic sulfonic acids and amines through hydrogen bonding. They have high solubility and recyclability. By introducing substituents, the void structure and environment of POSs can be controlled, significantly affecting their gas adsorption behavior.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Hailong Wang, Yinghua Jin, Nana Sun, Wei Zhang, Jianzhuang Jiang
Summary: Porous organic cages (POCs) are a class of organic materials with intrinsic porosity. Post-synthetic modification (PSM) has emerged as a highly viable strategy for broadening the functions and applications of POCs, leading to improved stability, tunable porosity, and selective guest binding. This approach allows for the realization of intricate structures and unique gas adsorption selectivity that cannot be achieved through traditional predesign methods.
CHEMICAL SOCIETY REVIEWS
(2021)
Review
Chemistry, Multidisciplinary
Wenjing Wang, Kongzhao Su, Daqiang Yuan
Summary: Gases are crucial in various industries, and the separation of pure gases is essential. Porous organic cages (POCs) are a promising class of materials with tailor-made cavities, low energy consumption, and simplified operational procedures. Similar to established porous framework materials, POCs have shown potential for gas separation applications. This review focuses on the progress and future prospects of POCs in selective gas separation, along with existing challenges.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Miao Yang, Fenglei Qiu, El-Sayed M. El-Sayed, Wenjing Wang, Shunfu Du, Kongzhao Su, Daqiang Yuan
Summary: This study synthesized seven water-stable hydrazone-linked POCs with diverse structures, tunable window diameters, and cavity volumes, which can effectively remove various pollutants from water.
Article
Chemistry, Multidisciplinary
Dayton J. Vogel, Tina M. Nenoff, Jessica M. Rimsza
Summary: This study investigates the mechanisms of hydrogen isotope separation in barely porous organic cages (POCs) using ab initio molecular dynamics simulations. The results reveal that temperature and pore size have an impact on the separation process, and highly functionalized materials exhibit unique escape mechanisms for D-2 and H-2. Calculations of isotope velocities suggest that effective pore sizes may extend beyond the pore openings, and a restricted molecular behavior is observed in the barely nanoporous pore openings of highly functionalized POCs.
Article
Nanoscience & Nanotechnology
Isaiah Borne, Donglin He, Stephen J. A. DeWitt, Ming Liu, Andrew Cooper, Christopher W. Jones, Ryan P. Lively
Summary: The preparation and characterization of fiber sorbents with POCs embedded in a cellulose acetate polymer matrix showed stable and adsorptive properties for model separations. Spun fibers retained high adsorbent loading and outperformed pelletized counterparts in adsorption tests, demonstrating the potential of fiber sorbents embedded with POCs for effective gas separations.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Chemistry, Multidisciplinary
Nishesh Kumar Gupta, Alfredo Lopez-Olvera, Eduardo Gonzalez-Zamora, Eva Martinez-Ahumada, Ilich A. Ibarra
Summary: This article focuses on the adsorption characteristics of sulfur dioxide (SO2) in porous materials such as metal-organic frameworks, metal-organic cages, and porous organic cages under reversible conditions. The preferential binding sites in these materials are highlighted, providing valuable information on the progress made towards improving SO2 capture by hybrid systems.
Article
Chemistry, Inorganic & Nuclear
Meaghan M. Deegan, Eric D. Bloch
Summary: This study successfully isolated metal node-terminated, capped paddlewheel-based cage structures using chelating dicarboxylate ligand derivates (esp) to form Mo-12(btc)(4)(esp)(6) cages and demonstrated that pillaring the isolated cage with DABCO generated an amorphous polymer with exceptional thermal stability and enhanced porosity, which is promising for potential applications in gas storage and separation.
DALTON TRANSACTIONS
(2021)
Review
Chemistry, Multidisciplinary
Xinchun Yang, Zakir Ullah, J. Fraser Stoddart, Cafer T. Yavuz
Summary: Porous organic cages (POCs) are a new class of low-density crystalline materials that have wide applications in molecular recognition, gas storage and separation, and proton conduction. Compared to other porous structures like MOFs, COFs, and POPs, POCs have the advantages of specific surface areas, porosities, open pore channels, tunable structures, and solubilities in common solvents. This review summarizes recent progress in POCs, including their design, synthesis, characterization, and applications, and discusses future challenges and opportunities in the field.
Article
Multidisciplinary Sciences
Chengxi Zhao, Linjiang Chen, Yu Che, Zhongfu Pang, Xiaofeng Wu, Yunxiang Lu, Honglai Liu, Graeme M. Day, Andrew Cooper
Summary: Energy-structure-function (ESF) maps can facilitate the discovery of functional materials by predicting stable crystalline arrangements and functions of interest. The authors demonstrate a digital navigation protocol for ESF maps in the context of hydrogen-bonded organic frameworks constructed from triptycene- and spiro-biphenyl-based molecular building blocks.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Donglin He, Chengxi Zhao, Linjiang Chen, Marc A. Little, Samantha Y. Chong, Rob Clowes, Katherine McKie, Mark G. Roper, Graeme M. Day, Ming Liu, Andrew Cooper
Summary: A trianglimine macrocycle (TAMC) was reported to selectively adsorb ethyl acetate by forming a solvate, with crystal structure prediction showing it to be the lowest energy solvate structure. This solvate leaves a metastable, templated cavity after solvent removal. Adsorption and breakthrough experiments confirmed TAMC's adequate adsorption kinetics for separating ethyl acetate from azeotropic mixtures with ethanol.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Yuting Shen, Shi Su, Wen Zhao, Shaobo Cheng, Tao Xu, Kuibo Yin, Linjiang Chen, Longbing He, Yilong Zhou, Hengchang Bi, Shu Wan, Qiubo Zhang, Liang Wang, Zhenhua Ni, Florian Banhart, Gianluigi A. Botton, Feng Ding, Rodney S. Ruoff, Litao Sun
Summary: Nanodiamonds were successfully synthesized using a hydrothermal method with graphene-oxide or nitrated polycyclic aromatic hydrocarbons as starting materials, resulting in nanodiamonds with diameters in the 2-3 nm range. Theoretical calculations suggest that sub-4 nm nanodiamonds may have a more stable structure than graphene-oxide and nitrated polycyclic aromatic hydrocarbons at the nanoscale.
Article
Chemistry, Multidisciplinary
Xue Wang, Mounib Bahri, Zhiwei Fu, Marc A. Little, Lunjie Liu, Hongjun Niu, Nigel D. Browning, Samantha Y. Chong, Linjiang Chen, John W. Ward, Andrew Cooper
Summary: By using tetrahedral spiroborate linkages, square-planar cobalt(II) phthalocyanine units are assembled into a 3D COF with noninterpenetrated nbo topology, exhibiting high crystallinity and long-range order. The COF has cubic pores and permanent porosity, with a BET surface area of 1726 m(2) g(-1).
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Edward O. Pyzer-Knapp, Linjiang Chen, Graeme M. Day, Andrew I. Cooper
Summary: The study introduces a new method using parallel Bayesian optimization to acquire ESF data, providing the same level of insight at a lower computational cost and paving the way for high-throughput virtual screening. By greatly reducing the opportunity risk associated with the choice of system, this approach achieved a significant computational speedup in a specific research scenario.
Article
Chemistry, Multidisciplinary
Xiaoyu Wu, Linjiang Chen, Eric Jean Amigues, Ruiyao Wang, Zhongfu Pang, Lifeng Ding
Summary: This study investigated the use of Aluminum-based metal-organic frameworks (MOFs) for capturing radioactive organic iodide (ROI) from a gas composition resembling the off-gas from reprocessing used nuclear fuel. Functionalizing the top-performing CAU-11 with -SO3H groups showed promising results in enhancing ROI adsorption and separation capabilities.
Article
Chemistry, Multidisciplinary
Johannes W. M. Osterrieth, Jarnes Rampersad, David Madden, Nakul Rampal, Luka Skoric, Bethany Connolly, Mark D. Allendorf, Vitalie Stavila, Jonathan L. Snider, Rob Ameloot, Joao Marreiros, Conchi Ania, Diana Azevedo, Enrique Vilarrasa-Garcia, Bianca F. Santos, Xian-He Bu, Ze Chang, Hana Bunzen, Neil R. Champness, Sarah L. Griffin, Banglin Chen, Rui-Biao Lin, Benoit Coasne, Seth Cohen, Jessica C. Moreton, Yamil J. Colon, Linjiang Chen, Rob Clowes, Francois-Xavier Coudert, Yong Cui, Bang Hou, Deanna M. D'Alessandro, Patrick W. Doheny, Mircea Dinca, Chenyue Sun, Christian Doonan, Michael Thomas Huxley, Jack D. Evans, Paolo Falcaro, Raffaele Ricco, Omar Farha, Karam B. Idrees, Timur Islamoglu, Pingyun Feng, Huajun Yang, Ross S. Forgan, Dominic Bara, Shuhei Furukawa, Eli Sanchez, Jorge Gascon, Selvedin Telalovic, Sujit K. Ghosh, Soumya Mukherjee, Matthew R. Hill, Muhammed Munir Sadiq, Patricia Horcajada, Pablo Salcedo-Abraira, Katsumi Kaneko, Radovan Kukobat, Jeff Kenvin, Seda Keskin, Susumu Kitagawa, Ken-ichi Otake, Ryan P. Lively, Stephen J. A. DeWitt, Phillip Llewellyn, Bettina Lotsch, Sebastian T. Emmerling, Alexander M. Putz, Carlos Marti-Gastaldo, Natalia M. Padial, Javier Garcia-Martinez, Noemi Linares, Daniel Maspoch, Jose A. Suarez del Pino, Peyman Moghadam, Rama Oktavian, Russel E. Morris, Paul S. Wheatley, Jorge Navarro, Camille Petit, David Danaci, Matthew J. Rosseinsky, Alexandros P. Katsoulidis, Martin Schroder, Xue Han, Sihai Yang, Christian Serre, Georges Mouchaham, David S. Sholl, Raghuram Thyagarajan, Daniel Siderius, Randall Q. Snurr, Rebecca B. Goncalves, Shane Telfer, Seok J. Lee, Valeska P. Ting, Jemma L. Rowlandson, Takashi Uemura, Tomoya Liyuka, Monique A. van derVeen, Davide Rega, Veronique Van Speybroeck, Sven M. J. Rogge, Aran Lamaire, Krista S. Walton, Lukas W. Bingel, Stefan Wuttke, Jacopo Andreo, Omar Yaghi, Bing Zhang, Cafer T. Yavuz, Thien S. Nguyen, Felix Zamora, Carmen Montoro, Hongcai Zhou, Angelo Kirchon, David Fairen-Jimenez
Summary: Porosity and surface area analysis are important in modern materials science. However, there is a lack of attention to the reproducibility issue in calculating BET surface areas from identical isotherms, raising concerns over the reliability of reported BET areas. To address this, a new computational approach called BET surface identification (BETSI) has been developed for accurately and systematically determining the BET area of nanoporous materials.
ADVANCED MATERIALS
(2022)
Article
Multidisciplinary Sciences
Weiwei Zhang, Linjiang Chen, Sheng Dai, Chengxi Zhao, Cheng Ma, Lei Wei, Minghui Zhu, Samantha Y. Chong, Haofan Yang, Lunjie Liu, Yang Bai, Miaojie Yu, Yongjie Xu, Xiao-Wei Zhu, Qiang Zhu, Shuhao An, Reiner Sebastian Sprick, Marc A. Little, Xiaofeng Wu, Shan Jiang, Yongzhen Wu, Yue-Biao Zhang, He Tian, Wei-Hong Zhu, Andrew Cooper
Summary: This study presents a general and scalable method to prepare robust, highly crystalline imine COFs, which greatly enhances crystallinity and porosity through a reconstruction route. This nanoconfinement-assisted reconstruction strategy is a step towards programming function in organic materials through atomistic structural control.
Article
Nanoscience & Nanotechnology
Xiaoyu Wu, Yu Che, Linjiang Chen, Eric Jean Amigues, Ruiyao Wang, Jinghui He, Huilong Dong, Lifeng Ding
Summary: Large-scale computational screening is a crucial tool for discovering functional materials, but effectively analyzing the generated data remains a challenge. In this study, the researchers computationally screened 1087 metal-organic frameworks (MOFs) to capture trace amounts of methyl iodide (CH3I), a difficult radioactive contaminant to separate. They also developed a simple and general approach to map and analyze the high-dimensional structure-function data obtained through high-throughput screening. The resulting maps are human-interpretable and reveal top-performing MOFs as well as complex structure-function correlations that are hidden when examining individual MOF features.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Jinhong Jia, Jingjiang Liu, Zhi-Qiang Wang, Tao Liu, Peiyao Yan, Xue-Qing Gong, Chengxi Zhao, Linjiang Chen, Congcong Miao, Wei Zhao, Shanshan (Diana) Cai, Xi-Cun Wang, Andrew Cooper, Xiaofeng Wu, Tom Hasell, Zheng-Jun Quan
Summary: Inverse vulcanization (IV) is a technique that converts elemental sulfur into sulfur-rich functional polymers. Previous methods required harsh reaction conditions, limiting the range of feasible crosslinkers. This study introduces a new photoinduced IV method that allows reaction at ambient temperatures, significantly expanding the range of substrates and products, and providing sustainable alternatives for environmentally harmful plastics.
Article
Chemistry, Physical
Tao Liu, Linjiang Chen, Xiaobo Li, Andrew I. I. Cooper
Summary: This study investigates the photocatalytic hydrogen evolution activity of three molecular photocatalysts (1-3) by theoretical investigations. The results reveal that slow exciton recombination, fast relaxation to the lowest-energy excited state, and a shorter charge transfer distance between the photocatalyst and the metal cocatalyst are important factors influencing the photocatalytic activity.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Caitlin E. Shields, Xue Wang, Thomas Fellowes, Rob Clowes, Linjiang Chen, Graeme M. Day, Anna G. Slater, John W. Ward, Marc A. Little, Andrew I. Cooper
Summary: Designing hydrogen-bonded organic frameworks (HOFs) with low densities and high porosities is challenging due to the preference for close packing in most molecules. Crystal structure prediction (CSP) can rank alternative crystal packings for organic molecules based on their lattice energies. By combining CSP with structure-property predictions, a previously unknown low-energy HOF (TH5-A) with remarkably low density and three-dimensional pores was discovered for triptycene trisquinoxalinedione (TH5). This TH5-A polymorph demonstrates high porosity with a surface area of 3,284 m(2) g(-1), making it one of the most porous HOFs reported.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Haofan Yang, Yu Che, Andrew I. Cooper, Linjiang Chen, Xiaobo Li
Summary: Using a combination of machine learning and high-throughput experimental screening, the exploration of ternary organic heterojunction photocatalysts was accelerated, resulting in the discovery of highly active photocatalysts with high sacrificial hydrogen production rates.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xiaobo Li, Phillip M. Maffettone, Yu Che, Tao Liu, Linjiang Chen, Andrew I. Cooper
Summary: Organic molecules play a crucial role in photocatalysts, but reliable structure-property design rules are difficult to formulate. By integrating experiment, computation, and machine learning, researchers were able to identify common structural features in molecules with high catalytic activity. The study marks a step towards the machine-learning assisted discovery of molecular organic photocatalysts, with potential applications beyond photocatalytic hydrogen evolution.
Article
Chemistry, Physical
Linjiang Chen, Yu Che, Andrew I. Cooper, Samantha Y. Chong
Summary: This study utilizes PXRD experiments and molecular dynamics simulations to reveal the adsorption mechanism of SF6 in the alpha-CC2 cage crystal, illustrating the dynamic flexibility and cooperative porosity of the system.
FARADAY DISCUSSIONS
(2021)