Article
Chemistry, Multidisciplinary
Ze-Xing Cai, Yanjie Xia, Yoshikazu Ito, Masataka Ohtani, Hikaru Sakamoto, Akitaka Ito, Yijia Bai, Zhong-Li Wang, Yusuke Yamauchi, Takeshi Fujita
Summary: The application scope of metal-organic frameworks (MOFs) can be expanded by rationally designing the structure and components of MOFs. A versatile templated strategy is proposed in this study, where organic ligands are weaved into hydrogen-bonded organic frameworks (HOFs) to synthesize MOF nanotubes controllably. Hybrid nanotubes containing nanometal crystals and N-doped graphene show excellent electrocatalytic HER activity and durability.
Article
Chemistry, Physical
Benjamin W. J. Chen, Saurabh Bhandari, Manos Mavrikakis
Summary: Hydrogen bonding interactions play a crucial role in influencing the reaction mechanisms of formic acid decomposition on Cu(111) surface, with bimolecular FA-HCOO complexes being identified as dominant intermediates. The study predicts that 40-80% of the reaction flux may go through pathways involving these complexes under specific reaction conditions. Additionally, the hydrogen-bonded complexes stabilize intermediates and transition states, providing important insights for the development of novel catalysts in industrial chemistries involving hydrogen bonding intermediates.
Article
Chemistry, Multidisciplinary
Sumra Idrees, Zhikai Li, Fang Fang, Huowang He, Irfan Majeed, Yihuan Zhang, Atsuhiro Osuka, Yan Cao, Zhuo Zeng, Xiaopeng Li, Hua-Wei Jiang
Summary: This report demonstrated the synthesis of a one-dimensional tubular assembly comprising porphyrin nanoring subunits. The nanotubes were formed through hydrogen bonding and exhibited well-defined arrays of nanotube bundles. The ordered 1D tubular nanoscale structure was observed using high-resolution transmission electron microscopy.
Article
Chemistry, Physical
Congyan Liu, Fei Ye, Zhiling Xiang, Yan Wang, Tian Zhang, Bo Liu
Summary: This study reports the first example of an elastic hydrogen-bonded ionic framework (HIF), which exhibits remarkable elasticity and two-dimensional elasticity at liquid nitrogen temperature. The crystallographic analyses reveal that hydrogen bonds and electrostatic interactions between anionic and cationic chains play a crucial role in maintaining the elastic properties.
Article
Chemistry, Multidisciplinary
Lucia Trevisan, Andrew D. Bond, Christopher A. Hunter
Summary: This study investigated the cooperative H-bonding interactions in supramolecular networks involving alcohols using phenol oligomers. It was found that intramolecular H-bonding interactions in the chain can increase the strength of intermolecular H-bonds, with pairwise interactions between nearest neighbors playing a dominant role. A simple model was developed to quantify the sensitivity of H-bond properties to polarization, with a measured kappa value of 0.33 indicating a 33% increase in polarity after formation of the first H-bond in the chain. The cumulative cooperative effect in longer H-bonded chains reaches an asymptotic value, leading to a maximum increase in polarity of the terminal H-bond donor of 50%.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Yanqiang Li, Xu Zhang, Jieyu Zheng, Yang Zhou, Weiqi Huang, Yipeng Song, Han Wang, Xianyu Song, Junhua Luo, Sangen Zhao
Summary: A new hydrogen bonded supramolecular framework, Cd(H2C6N7O3) (2)center dot 8H(2)O, exhibits an exceptionally large birefringence of 0.60, which is significantly larger than any commercial birefringent crystals and the largest among hydrogen bonded supramolecular framework crystals. The exceptional birefringence is mainly attributed to strong covalent interactions within (H2C6N7O3) organic ligands and their coplanarity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Brian J. Eckstein, Loren C. Brown, Bruce C. Noll, Michael P. Moghadasnia, Gary J. Balaich, C. Michael McGuirk
Summary: The manner of bonding between constituent atoms or molecules affects the properties of materials. Porous frameworks exemplify this, with their connectivity modes giving rise to subclasses with unique properties. Chalcogen bonding, a subclass of s-hole bonding, is shown to be a viable mode of connectivity in low-density porous frameworks, expanding the diversity of porous framework materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Organic
Zejiang Liu, Kang Kang, Yidan Zhou, Rui Liu, Yimin Cai, Wen Feng, Lihua Yuan
Summary: A novel supramolecular strategy utilizing H-bonded macrocycles for controlling the binding process in response to external stimulus has been reported in this study, showing significant progress in the field of catalysis. The switchable macrocycle ensemble, achieved by adjusting intermolecular interactions, enables the opening of the anion binding site and enhances the yield of catalytic reactions.
ORGANIC CHEMISTRY FRONTIERS
(2021)
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
Biochemistry & Molecular Biology
Steven van Terwingen, Daniel Brux, Ruimin Wang, Ulli Englert
Summary: In a hydrochloride of a pyrazolyl-substituted acetylacetone, the chloride anion is hydrogen-bonded to the protonated pyrazolyl moiety. Co-crystallization with tetrafluorodiiodobenzene (TFDIB) leads to a supramolecular aggregate with TFDIB centrally located. The interaction between the iodine atom in TFDIB and the chloride acceptor forms an almost linear halogen bond, orthogonal to the N-H center dot center dot center dot Cl hydrogen bond. Bond critical points were confirmed for both short contacts through an analysis of electron density distribution.
Article
Chemistry, Inorganic & Nuclear
Adam W. Augustyniak, Anna M. Trzeciak
Summary: The palladium azolate/carboxylate network, Pd-dmpzc, catalyzes the selective hydrogenation of phenyl-acetylene to styrene in water. Under optimized conditions, Pd-dmpzc provided better results than other palladium catalysts, with analysis showing the presence of different Pd2+ species and Pd-0 NPs contributing to the catalytic reaction.
INORGANICA CHIMICA ACTA
(2021)
Review
Polymer Science
Emmanouil Vereroudakis, Dimitris Vlassopoulos
Summary: Supramolecular polymers are important in both scientific and technological aspects due to their dynamic nature and responsiveness to environmental parameters, showing diverse self-assembly structures and potential applications. However, there are still significant challenges in understanding the basic knowledge and unresolved issues, requiring further systematic categorization and analysis of experimental evidence.
PROGRESS IN POLYMER SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Rui Pei, Jing Liu, Chuanyong Jing, Min Zhang
Summary: In this study, an in vitro multi-enzyme cascade pathway for the conversion of CO2 into dihydroxyacetone (DHA) is constructed and immobilized within a hydrogen-bonded organic framework (HOF-101). The immobilized pathway shows a significant increase in DHA yield and high stability, offering innovative ideas for the efficient conversion of carbon dioxide and the synthesis of fine compounds.
Article
Chemistry, Multidisciplinary
Jiali Huang, Yunbin Li, Hao Zhang, Zhen Yuan, Shengchang Xiang, Banglin Chen, Zhangjing Zhang
Summary: This article reports the structure of a new type of microporous material, hydrogen-bonded organic frameworks (HOFs), with a 4-fold interpenetrated diamond network structure, which exhibits excellent chemical and thermal stability. The activated HOF-FJU-46 shows the highest xenon uptake and xenon/krypton selectivity among the reported HOFs to date.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Sergi Bujosa, Azahara Doncel-Gimenez, Nils Baeumer, Gustavo Fernandez, Enrique Orti, Antonio Costa, Carmen Rotger, Juan Arago, Bartolome Soberats
Summary: Hydrogen-bonded squaramide (SQ) supramolecular polymers exhibit uncommon thermoreversible polymorph transitions between particle- and fiber-like nanostructures. The transitions are triggered by the molecular reorganization of the SQ units changing from slipped to head-to-tail hydrogen bonding patterns. These transitions have concentration-dependent and kinetic characteristics, and are of interest in developing stimuli-responsive systems.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Multidisciplinary Sciences
Nicholas Pearce, Katherine E. A. Reynolds, Surajit Kayal, Xue Z. Sun, E. Stephen Davies, Ferdinando Malagreca, Christian J. Schuermann, Sho Ito, Akihito Yamano, Stephen P. Argent, Michael W. George, Neil R. Champness
Summary: This study demonstrates the ability to control photoinduced charge transfer within homo- and hetero-rotaxanes through the organization of the components of mechanically interlocked molecules, introducing alternative pathways for electron donation.
NATURE COMMUNICATIONS
(2022)
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
Physics, Multidisciplinary
G. Cassabois, G. Fugallo, C. Elias, P. Valvin, A. Rousseau, B. Gil, A. Summerfield, C. J. Mellor, T. S. Cheng, L. Eaves, C. T. Foxon, P. H. Beton, M. Lazzeri, A. Segura, S. Novikov
Summary: In this study, parallel investigation of exciton and phonon radiative linewidths in atomically thin layers of hexagonal boron nitride (h-BN) was conducted, revealing a significant radiative broadening in the two-dimensional material and indicating the existence of radiative states for optical phonons in 2D. This finding has important implications for fundamental physics and optoelectronic applications.
Article
Chemistry, Multidisciplinary
David Gerard Madden, Daniel O'Nolan, Nakul Rampal, Robin Babu, Ceren Camur, Ali N. Al Shakhs, Shi-Yuan Zhang, Graham A. Rance, Javier Perez, Nicola Pietro Maria Casati, Carlos Cuadrado-Collados, Denis O'Sullivan, Nicholas P. Rice, Thomas Gennett, Philip Parilla, Sarah Shulda, Katherine E. Hurst, Vitalie Stavila, Mark D. Allendorf, Joaquin Silvestre-Albero, Alexander C. Forse, Neil R. Champness, Karena W. Chapman, David Fairen-Jimenez
Summary: We are witnessing the dawn of hydrogen economy, where hydrogen is becoming a primary fuel for heating, transportation, and energy storage. Metal-organic frameworks (MOFs) have emerged as promising adsorbent materials for hydrogen storage, but their use has been limited by a lack of densification methods. In this study, researchers screened and analyzed a database of MOFs to find an optimal material for hydrogen storage, and successfully synthesized and evaluated a monolithic MOF with high storage performance at lower operating pressures.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
James Felton, Elena Blundo, Zakhar Kudrynskyi, Sanliang Ling, Jonathan Bradford, Giorgio Pettinari, Timothy Cooper, Matthew Wadge, Zakhar Kovalyuk, Antonio Polimeni, Peter Beton, David Grant, Gavin Walker, Amalia Patane
Summary: This study investigates the interaction between the vdW semiconductor SnS2 and hydrogen, demonstrating a controlled chemical conversion to semiconducting-SnS or beta-Sn. It successfully creates SnS2/SnS heterostructures with uniform layers, atomically flat interfaces, and well-aligned crystallographic axes. This scalable approach provides a promising route for engineering nanoscale semiconductor technologies based on the abundant elements Sn and S.
Article
Nanoscience & Nanotechnology
Letizia Liiro-Peluso, James Wrigley, David B. Amabilino, Peter H. Beton
Summary: The efficiency of organic bulk-heterojunction (BHJ) solar cells depends on the bulk and surface structure of the active layer, which can be resolved at the nanoscale using high-resolution atomic force microscopy (AFM). In this study, poly(3-hexylthiophene):[6,6]-phenyl C-61 butyric acid methyl ester (P3HT:PCBM) active layer mixtures with different stoichiometries were investigated using AC-mode AFM. The nanoscale organization of P3HT and the P3HT:PCBM mixtures at the surface-air interface of the BHJ architecture were observed, and the effect of different ratios of PCBM on the morphology was analyzed. When exposed to ambient light, the morphologies of the samples were significantly different and submolecular resolution was not achieved.
ACS APPLIED NANO MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Stefania Moro, Nicholas Siemons, Oscar Drury, Daniel A. Warr, Thomas A. Moriarty, Luis M. A. Perdigao, Drew Pearce, Maximilian Moser, Rawad K. . Hallani, Joseph Parker, Iain McCulloch, Jarvist M. Frost, Jenny Nelson, Giovanni Costantini
Summary: Conjugated polymers with glycol-based chains have promising applications in bioelectronics and thermoelectrics. In this study, we determined the microstructure of these polymers with submonomer resolution and found that the side chains play a crucial role in polymer assembly. The conformation of the side chains is influenced by their free analogues, rather than the backbone torsional potential energy. These findings can be extended to other conjugated polymers for microstructure characterization.
Article
Biochemistry & Molecular Biology
Samuel Quinn, E. Stephen Davies, Nicholas Pearce, Callum Rosenberg, Constance R. R. Pfeiffer, Georgia R. F. Orton, Neil R. R. Champness
Summary: This study describes donor-acceptor dyads and triads composed of core-substituted naphthalene diimide (NDI) chromophores and either phenothiazine or phenoxazine donors. Synthesis, electrochemical, and spectroelectrochemical investigations are used to characterize the different redox states of these molecules, confirming their ability to combine electron donating and accepting moieties while retaining the individual redox properties.
Article
Chemistry, Multidisciplinary
Jonathan S. S. Austin, Nathan D. D. Cottam, Chengxi Zhang, Feiran Wang, Jonathan H. H. Gosling, Oliver Nelson-Dummet, Tyler S. S. James, Peter H. H. Beton, Gustavo F. F. Trindade, Yundong Zhou, Christopher J. J. Tuck, Richard Hague, Oleg Makarovsky, Lyudmila Turyanska
Summary: We report on the formulation of all-inorganic perovskite nanocrystals inks and their application in graphene photodetectors. By controlling the device structure and fabricating process, we achieved high photoresponsivity and controlled spectral response. Inkjet printing of perovskite, graphene, and gold nanoparticle inks enabled the realization of fully printed photodetectors with the highest reported photoresponsivity value. The developed perovskite ink offers opportunities for stable and sensitive graphene-based photon detectors.
Article
Biology
Maud Dumoux, Thomas Glen, Jake L. R. Smith, Elaine M. L. Ho, Luis M. A. Perdigao, Avery Pennington, Sven Klumpe, Neville B. Y. Yee, David Andrew Farmer, Pui Y. A. Lai, William Bowles, Ron Kelley, Juergen M. Plitzko, Liang Wu, Mark Basham, Daniel K. Clare, C. Alistair Siebert, Michele C. Darrow, James H. Naismith, Michael Grange, Giulia Zanetti
Summary: Cryogenic plasma FIB/SEM overcomes challenges in imaging non-stained biological samples, producing high-quality images with automated workflows. This technique allows for three-dimensional imaging of bacteria, human cells, and tissue with resolutions typically ranging from 20-50 nm.
Article
Chemistry, Multidisciplinary
Mustaqeem Shiffa, Benjamin T. Dewes, Jonathan Bradford, Nathan D. Cottam, Tin S. Cheng, Christopher J. Mellor, Oleg Makarovskiy, Kazi Rahman, James N. O'Shea, Peter H. Beton, Sergei V. Novikov, Teresa Ben, David Gonzalez, Jiahao Xie, Lijun Zhang, Amalia Patane
Summary: 2D semiconductors show great potential in various fields, but current fabrication methods have limitations. This study demonstrates a bottom-up approach for high-quality, wafer-scale 2SEM based on the wide band gap gallium selenide compound. The optical properties of the layers are utilized for photon sensing in the UV spectrum, offering a scalable route to deep-UV optoelectronics.
Article
Chemistry, Multidisciplinary
Rosemary J. J. Young, Michael T. T. Huxley, Lingjun Wu, Jack Hart, James O'Shea, Christian J. J. Doonan, Neil R. R. Champness, Christopher J. J. Sumby
Summary: We investigated the photochemical and chemical processes of Mn(diimine)(CO)(3)X (X = halide) complexes in permanently porous metal-organic frameworks (MOFs). We observed the photo-liberation of CO from the metal and its escape from the MOF crystals. Crystallographic snapshots of the photolysis products were obtained due to the high crystallinity and structural flexibility of the MOF. Time resolved experiments revealed complementary spectroscopic studies and characterized the final photolysis product as a possible Mn(ii) entity. These findings provide insights into the chemistry of MOF-based photoCORMs and catalysts.
Article
Chemistry, Multidisciplinary
Josephine F. Smernik, Pol Gimeno-Fonquernie, Jorge Albalad, Tyla S. Jones, Rosemary J. Young, Neil R. Champness, Christian J. Doonan, Jack D. Evans, Christopher J. Sumby
Summary: This study investigates the synthesis of Mn-based metal-organic frameworks (MOFs), finding that MnMOF-1 is a kinetic or metastable phase, while a newly identified 2D layered material, MnMOF-2D, is the thermodynamically favored product. It is also shown that using longer linkers can help to form more stable structures. In addition, two new porous 3D Mn-based MOFs were successfully synthesized, highlighting the viability of using tetratopic hinged linkers to form 3D MOFs.
Article
Chemistry, Multidisciplinary
Matthew Edmondson, Eleanor S. Frampton, Chris J. Judd, Neil R. Champness, Robert G. Jones, Alex Saywell
Summary: A thermally induced order-disorder transition of 2H-TPP on Au(111) was investigated using scanning probe microscopy and X-ray photoelectron spectroscopy. The transition from an ordered close-packed phase to a disordered diffuse phase was found to be correlated with an on-surface cyclodehydrogenation reaction, and further heating of the diffuse phase resulted in the formation of a distinct nitrogen environment indicative of the Au-TPP species.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Nicholas Pearce, Marysia Tarnowska, Nathan J. Andersen, Alexander Wahrhaftig-Lewis, Ben S. Pilgrim, Neil R. Champness
Summary: This paper reviews the field of mechanically interlocked molecules that utilize a handcuff component. The different structures of rotaxanes and catenanes that interlock different components using the handcuff motif are discussed, and a new nomenclature is proposed to unify terminology. By interpreting this class of molecules in a unified manner, new opportunities for employing this structural unit for new architectures are identified.
