Article
Chemistry, Inorganic & Nuclear
Xiaoqin Cui, Fu-Qiang Zhang, Xin Li, Juan-Juan Hou, Huan Li, Xian-Ming Zhang
Summary: The research describes a new type of inorganic host material, titanium-oxide or polyoxotitanate clusters, which can encapsulate inorganic molecules or ions. A specific molecular cage, Ti-18, was found to encapsulate an entire organic ethylenediamine ion and demonstrate exceptional versatility in balancing charges and facilitating reactions. Ti-18 exhibits strong light absorption due to ethylenediamine coordination and shows superior photocatalytic activity compared to anatase TiO2.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Laurens Vandebroek, Hiroki Noguchi, Alexander Anyushin, Luc Van Meervelt, Arnout R. D. Voet, Tatjana N. Parac-Vogt
Summary: This study reports the hierarchical self-assembly of hybrid bioinorganic structures through specific and tailored interactions. A supramolecular assembly was formed between the designer protein Pizza6-S (Pizza6) and the polyoxometalate (POM) {K3Cu3(NO3)[A-alpha-PW9O34](2)}. The crystal structure revealed the dissociation and reassembly of Cu3 with the protein to form a novel POM-protein cage. Spectroscopic characterization of the Pizza6/Cu3 solution suggests that the dissociation of Cu3 is facilitated by the synergistic effect of six histidine residues, resulting in the formation of the hierarchical supramolecular assembly.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Chemistry, Physical
Zhifeng Xiao, Hannah F. Drake, Yohannes H. Rezenom, Peiyu Cai, Hong-Cai Zhou
Summary: The study demonstrates the structural flexibility and stimulus-responsive features of zirconocene-based PCCs. Two interconvertible PCCs, PCC-20c and PCC-20t, are constructed from the same cluster and ligand but exhibit different shapes and properties. The conversion from PCC-20t into PCC-20c is found to be an entropically driven process influenced by solvent environment, counter anions, and light irradiation.
Article
Chemistry, Inorganic & Nuclear
Edward Britton, Richard J. Ansell, Mark J. Howard, Michaele J. Hardie
Summary: New photoswitchable pyridyl-azo-phenyl-decorated tripodal host ligands (L-az) have been synthesized, showing a remarkable 7-fold Borromean-weave entanglement and forming metallo-cryptophanes cages with less robust photoswitching behavior.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Andre P. Birve, Harshal D. Patel, Jason R. Price, Witold M. Bloch, Thomas Fallon
Summary: A fluxional bis-monodentate ligand, based on the bullvalene molecule, self-assembles with M2+ to produce complex coordination cages. Guest-exchange simplifies the system, leading to a mixture of 38 diastereoisomers. NMR spectroscopy and DFT calculations elucidate the isomerization pathway.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Julius Gemen, Michal J. Bialek, Miri Kazes, Linda J. W. Shimon, Moran Feller, Sergey N. Semenov, Yael Diskin-Posner, Dan Oron, Rafal Klajn
Summary: Combining confinement effects with fast guest exchange kinetics allows for the development of stimuli-responsive supramolecular systems that can rapidly and reversibly tailor material properties.
Article
Chemistry, Inorganic & Nuclear
Yang Cheng, Qingqing Yang, Jiang He, Wenjie Zou, Keyu Liao, Xiaoyong Chang, Chao Zou, Wei Lu
Summary: This article introduces a series of substituted anionic ligands containing Cr(iii) complexes, which exhibit phosphorescent properties in degassed fluid solutions.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Eugenia Peresypkina, Kevin Grill, Barbara Hiltl, Alexander V. Virovets, Werner Kremer, Jan Hilgert, Wolfgang Tremel, Manfred Scheer
Summary: One-pot self-assembly reactions involving a polyphosphorus complex, a coinage metal salt, and flexible aliphatic dinitriles produced coordination polymers of various dimensions. Different lengths of dinitriles at x=7 led to the formation of unprecedented 3D networks in the self-assembly system.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Rebecca L. Spicer, Helen M. O'Connor, Yael Ben-Tal, Hang Zhou, Patrick J. Boaler, Fraser C. Milne, Euan K. Brechin, Guy. C. Lloyd-Jones, Paul J. Lusby
Summary: Coordination cage catalysis is a strategy that utilizes a cage as an exogenous catalyst, rather than relying on the endogenous binding of substrates. The cage alters the properties of a cofactor guest, which then transfers reactivity to the bulk-phase to catalyze reactions.
Article
Chemistry, Multidisciplinary
Alexandre Walther, Irene Regeni, Julian J. Holstein, Guido H. Clever
Summary: Azulene is introduced as the backbone for a new family of Pd(II)-based self-assemblies, and these self-assemblies can be modulated by changing the organic ligands equipped with different donor groups. The addition of organic disulfonate guests to the smallest cage leads to a rapid transformation to a distorted-tetrahedral species, while cages formed from ligands with isoquinoline donors either encapsulate the guests or show no interaction. The tetrahedral species can be reverted back to its original topology by capturing the guest using another, stronger binding cage.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Tobias Dwyer, Timothy C. Moore, Joshua A. Anderson, Sharon C. Glotzer
Summary: Entropy compartmentalization provides new self-assembly routes to colloidal host-guest structures. By modifying the shape of guest particles, a variety of crystal structures and pore motifs can be formed when mixed with star-shaped host particles. The assembly is driven by entropy compartmentalization, with different contributions from the host and guest particles to the free energy of the system.
Article
Chemistry, Physical
Tobias Dwyer, Timothy C. Moore, Joshua A. Anderson, Sharon C. Glotzer
Summary: Entropy compartmentalization provides a new self-assembly route for colloidal host-guest (HG) structures. Leveraging host particle shape has been recently proposed and demonstrated for the assembly of HG structures. However, the influence of guest particles on the porous network structure of host particles has not been explored.
Article
Chemistry, Inorganic & Nuclear
Miao Li, Yu-Qi Shi, Xinye Gan, Longbin Su, Jialin Liang, Huiqi Wu, Yiting You, Meizi Che, Peiyang Su, Tun Wu, Zhe Zhang, Wei Zhang, Liao-Yuan Yao, Pingshan Wang, Ting-Zheng Xie
Summary: A new type of coordination-driven host combining porphyrin and terpyridine moieties with a long cavity was designed and synthesized in this study. The host can encapsulate bisite or monosite guests through axial coordination binding of porphyrin and aromatic pi interactions of terpyridine. Characterization of the ligands and prismatic complexes was conducted using ESI-MS, TWIM-MS, NMR spectrometry, and single-crystal X-ray diffraction analysis. The encapsulation mechanism of guests was investigated through ESI-MS, NMR spectrometry, and transient absorption spectroscopy analysis. The binding constant and stability were determined by UV-Vis spectrometry and gMS2 techniques. A selectively confined condensation reaction was performed and detected by NMR spectrometry based on the prism. This study provides a new type of host that could be used for the detection of pyridyl- and amine-contained molecules and confined catalysis.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Organic
Sudhakar Ganta, Jan-Hendrik Borter, Christoph Drechsler, Julian J. Holstein, Dirk Schwarzer, Guido H. Clever
Summary: A [Pd2L4] coordination cage, consisting of electron-rich phenothiazine-based ligands and encapsulating an electron-deficient anthraquinone-based disulfonate guest, has been reported. Transient absorption spectroscopy reveals photoinduced electron transfer from the host's chromophores to the guest, as indicated by characteristic spectral features. The host-guest complex was characterized using various techniques, and spectroelectrochemical experiments and DFT calculations support the proposed light-induced charge separation.
ORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Multidisciplinary
Daniel L. Stares, Cristina Mozaceanu, Michael D. Ward, Christoph A. Schalley
Summary: We show that ESI-MS can be used to determine the different modes of guest binding with a Co8L12 cubic cage. High stoichiometry guest binding was observed, with the guests predominantly binding externally, but internal guest inclusion was also observed at higher guest loading.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Yayong Sun, Jing Wei, Zhihua Fu, Minyi Zhang, Sangen Zhao, Gang Xu, Chunsen Li, Jian Zhang, Tianhua Zhou
Summary: A series of hydrogen-bonded organic frameworks (HOFs) with high stability and proton conductivity have been successfully developed based on the self-assembly of lipid bilayer membranes.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Xiao-Xue Liu, Zi-Rui Wang, Guang-Hui Chen, Qiao-Hong Li, Jun Tao, Lei Zhang
Summary: Here, a twisted cubic Cu(I)(4)Ti(IV)(4)-oxo cluster stabilized by in situ-formed 2,2'-biphenolate ligands from the oxidative coupling of phenols is reported. The 2,2'-biphenolate-functionalized Cu(I)(4)Ti(IV)(4)O-4 cluster exhibits shorter Cu-M contacts and smaller HOMO-LUMO gaps than those of reported Ti(IV)(4)O-4.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Guo-Bin Xiao, Xijiao Mu, Shuyu Zhou, Liu Zhu, Yong Peng, Qing Liang, Xiaoxin Zou, Jian Zhang, Lei Zhang, Jing Cao
Summary: Researchers introduce a lead-doped titanium-oxo cluster protected by S-containing ligands at the perovskite-SnO2 interface, which is subsequently transformed into a PbSO4-PbTi3O7 heterostructure through in situ heating. The heterostructure boosts interfacial electron extraction and reduces charge recombination by connecting the oxygen atoms from sulfate ions with iodine from the perovskite, while the metallic interface between PbSO4 and PbTi3O7 promotes electron transport across the interface. This strategy achieves an efficiency as high as 24.2% for the modified perovskite solar cells and greatly improves device stability by stabilizing the interface. This work provides a novel approach for preparing wide-band gap cathode interlayers using directional transformation of heterometallic oxo clusters.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Jiajin Xia, Baolong Zhu, Qiuling Wan, Yinghua Yu, Shenlin Huang, Jian Zhang, Xueliang Huang
Summary: Transition metal-catalyzed divergent synthesis through alternation of the catalyst is demonstrated, providing an operationally simple way to access different valuable products from the same reactants. A gold-catalyzed cascade reaction of conjugated diynamides with allylic alcohols is described, giving selectively substituted allenes and furans by varying the catalysts. Mechanistic studies reveal a [3,3]-sigmatropic rearrangement and an intramolecular Himbert arene/allene Diels-Alder cycloaddition as additional reaction sequences to access dearomatized products with bicyclo[2,2,2]octadiene core.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Fang -Fang Liu, Di Wang, Guang-Hui Chen, Jian Zhang, Lei Zhang
Summary: Two isostructural Sn5-oxo clusters, (nBuSn)5(mu 3-O)2(EG4)L3 (H2EG = ethylene glycol, L = 4-tert-butylbenzoate or 4-hydroxybenzoate), were successfully prepared using (nBuSn)OH2Cl as tin source pre-cursor. Comparative studies on contact angle test and electrocatalytic carbon dioxide reduction reveal that the 4-tert-butylbenzoate decorated Sn5 with a more hydrophobic surface shows higher catalytic activity.
JOURNAL OF SOLID STATE CHEMISTRY
(2023)
Article
Materials Science, Multidisciplinary
Zhi-Run Wang, Jun-Qiang Chen, Qiao-Hong Li, Hai-Xia Zhang, Jian Zhang
Summary: This study reports 2D lead-MOFs that generate white light through the combined effect of free excitons and self-trapped excitons. The synthesized BIF-142-Cl exhibits outstanding white-light emission with color coordinates close to pure white light, excellent color rendering index, and gentle correlation color temperature. Additionally, the emission can be adjusted from blue to white light by changing the excitation wavelength. This synthetic strategy not only offers potential for solid-state lighting materials but also expands possibilities in anticounterfeiting, display media, and information identification fields.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Multidisciplinary Sciences
Haoyue Guo, Matthew R. Carbone, Chuntian Cao, Jianzhou Qu, Yonghua Du, Seong-Min Bak, Conan Weiland, Feng Wang, Shinjae Yoo, Nongnuch Artrith, Alexander Urban, Deyu Lu
Summary: X-ray absorption spectroscopy (XAS) database of sulfur K-edge XAS spectra of lithium thiophosphate materials is developed based on atomic structures. The database contains 2681 spectra for 66 crystalline and glassy structure models, making it the largest collection of computational XAS spectra for lithium thiophosphates. It can be used to correlate spectral features with local coordination and short-range ordering in sulfide-based solid electrolytes.
Article
Chemistry, Multidisciplinary
Yi-Hong Xiao, Zhi-Zhou Ma, Xue-Xian Yang, Dong-Sheng Li, Zhi-Gang Gu, Jian Zhang
Summary: This study demonstrates the synthesis of ordered chiral carbon nanodot arrays in a porous material, which enables efficient circularly polarized luminescence. By confining chiral amino acids in the porous material and carbonizing them into chiral carbon nanodots, the transfer of chirality on the excited state is achieved, resulting in strong CPL performance.
Article
Chemistry, Physical
Xiaohui Sun, Xiaofeng Yi, Jian Zhang, Lei Zhang
Summary: This study demonstrates the controllable formulation and regulation of variety and connection modes of cuboidal {M4X4} building units (M=In, Ni; X= O, Cl) by exploiting solvent effect and organic-ligand-induced effect. The formation of the In10Ni8-oxo cluster with a wheel-shaped architecture is achieved with the assistance of aromatic carboxylates, presenting the largest size record in the realm of InOCs. The In10Ni8-oxo cluster shows high reverse saturable absorption, making it suitable as an optical limiting material.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Kalpana Chintakrinda, Nagaraju Narayanam, Guang-Hui Chen, Jian Zhang, Lei Zhang
Summary: Two titanium-oxo clusters with similar nuclearity but different surface-decorated ligands were synthesized using an ionothermal reaction. These clusters exhibited varying activities for photocatalytic degradation and distinct photocurrent responses, providing valuable insights into the design of Ti-oxo molecular clusters.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Kerry Sun, Chuntian Cao, Dingyi Zhao, Xiao Tong, Seong-Min Bak, Yonghua Du, Feng Wang, Daniel A. Steingart
Summary: The superionic solid-state argyrodite electrolyte Li6PS5Br can enhance the safety and energy density of lithium and lithium-ion batteries. However, this electrolyte still suffers from electrode degradation, and the stability of LFP against Li6PS5Br is not inherently guaranteed.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Ping Shao, Yu-Mei Wan, Luocai Yi, Shumei Chen, Hai-Xia Zhang, Jian Zhang
Summary: In this study, a Cu@BIF-144(Zn) composite is synthesized and shown to exhibit a synergistic effect in CO2RR, enhancing selectivity and activity for the production of multi-electron-transfer products.
Article
Materials Science, Multidisciplinary
Dong-Fei Lu, Shangda Li, Ming-Xue Guan, Yu-Peng Han, Yayong Sun, Xin Wu, Fei Wang, Jian Zhang
Summary: In this study, the first visible-light-active titanium sulfonate metal-organic framework (FIR-138) with 2-fold interpenetrated srs topology was successfully synthesized. FIR-138 exhibited good stability and excellent visible-light absorption performance, and demonstrated outstanding visible-light photocatalytic performance in organic reactions.
ACS MATERIALS LETTERS
(2023)
Article
Chemistry, Inorganic & Nuclear
Jun-Qiang Chen, Hai-Xia Zhang, Zhi-Run Wang, Qin-Long Hong, Jian Zhang
Summary: In this study, a new MOC cage with a unique trigonal bipyramidal configuration was reported, which was constructed by the combination effects of coordination bonds and π-π interactions. The cage structure could be modulated by the metal centers, leading to diverse coordination environments and optical properties.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Engineering, Environmental
Xueyan Lin, Wenyue Li, Vy Nguyen, Shu Wang, Shize Yang, Lu Ma, Yonghua Du, Bin Wang, Zhaoyang Fan
Summary: In this study, Fe single metal atom catalyst was incorporated into the sulfur cathode design, which improved the sulfide reaction kinetics and reduced the shuttle effects of lithium polysulfides, leading to enhanced performance and cycling stability of Li-S batteries.
CHEMICAL ENGINEERING JOURNAL
(2023)