Article
Multidisciplinary Sciences
Xue-Xin Li, Cai-Hong Li, Ming-Jun Hou, Bo Zhu, Wei-Chao Chen, Chun-Yi Sun, Ye Yuan, Wei Guan, Chao Qin, Kui-Zhan Shao, Xin-Long Wang, Zhong-Min Su
Summary: In this study, the authors present a method for the precise synthesis of polyoxometalates (POMs) through Ce-mediated molecular tailoring, resulting in the transformation of gigantic {Mo-132} into a half-closed {Ce11Mo96}, which exhibits significantly enhanced proton conductivity compared to {Mo-132}.
NATURE COMMUNICATIONS
(2023)
Article
Engineering, Environmental
Qiaoling Kang, Dawei Lai, Mengfei Su, Boru Xiong, Wenyin Tang, Qingyi Lu, Feng Gao
Summary: A crystal morphological evolution mechanism was proposed for the synthesis of hollow nanoframes with unique yolk-shell structure and multiheteroatoms doping, which showed excellent electrochemical catalytic activities for oxygen evolution reaction. The study not only provided novel nanostructures, but also offered a facile strategy for encapsulating active components inside porous substrates, opening up new possibilities for the utilization of nanomaterials as potential catalysts for energy storage and conversion.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Sarah Al Gharib, Abdel Karim El Omar, Adnan Naja, Ariane Deniset-Besseau, Sergey A. Denisov, Pascal Pernot, Mehran Mostafavi, Jacqueline Belloni
Summary: The study investigates the nucleation and growth of crystallites in highly supersaturated solutions of potassium nitrate induced by a single laser nanosecond pulse. It is found that the turbidity increases proportionally with time during the early growth stage, with an accretion rate constant of 4.7 x 10(7) L mol(-1) s(-1).
CRYSTAL GROWTH & DESIGN
(2021)
Article
Chemistry, Multidisciplinary
Kun Chen, Shengqiu Liu, Wei Zhu, Panchao Yin
Summary: The study finds that surface engineering of polyoxovanadate (POV) clusters can improve their bioavailability and pharmacokinetic properties, mitigating the adverse effects of vanadium compounds. Surface-engineered POVs have shorter elimination half-life and higher elimination rates, which favor the elimination of possible side effects. In addition, surface engineering significantly increases the oral bioavailability of POVs. These findings suggest that surface engineering is an effective approach to optimize the therapeutic efficacy of POVs and reduce their adverse effects.
Article
Energy & Fuels
Xiaojing Yu, Shifa Ullah Khan, Zhongxin Jin, Qiong Wu, Haijun Pang, Huiyuan Ma, Xinming Wang, Lichao Tan, Guixin Yang
Summary: Water cluster encapsulated polyoxometalate (POM)-based hydrogen-bonded supramolecular frameworks (PHSFs) are novel advanced high-capacity electrode materials for supercapacitors. In this study, four new PHSFs were synthesized and their electrochemical properties were evaluated.
JOURNAL OF ENERGY STORAGE
(2022)
Article
Materials Science, Ceramics
S. K. Evstropiev, D. A. Yurchenko, V. L. Stolyarova, N. B. Knyazyan, G. G. Manukyan, A. V. Shashkin
Summary: This study investigates the influence of Ag diffusion on the crystallization and luminescence properties of MgO-Al2O3-TiO2-SiO2 glass. It is found that Ag diffusion significantly improves the microhardness of the glass and leads to the formation of various luminescent molecular clusters. The Ag-diffused glass and glass ceramics can effectively convert UV and blue light into radiation in the red and NIR spectral range.
CERAMICS INTERNATIONAL
(2022)
Article
Chemistry, Multidisciplinary
Daishi Fujita, Ryoto Suzuki, Yuya Fujii, Mayu Yamada, Takahiro Nakama, Akimasa Matsugami, Fumiaki Hayashi, Jing-Ke Weng, Maho Yagi-Utsumi, Makoto Fujita
Summary: Encapsulation of a protein in a molecular cage with an open framework stabilizes its tertiary structure and enhances its enzymatic activity, particularly in organic solvents. The key to this stability lies in the isolated space, reminiscent of chaperonins. This new protein-based nanobiotechnology accelerates molecular biology research and industrial applications.
Article
Materials Science, Multidisciplinary
Maxim Vreeswijk, Alexandre Kot, Finn Giuliani, Samuel Humphry-Baker
Summary: The growth mechanism of large WC crystals from a liquid Co-based flux has been identified, where abnormal grains nucleate on the (W,Co)(6)C eta phase and consume it through a carburisation reaction. By adopting the eutectic composition, the size of abnormal grains is enhanced. This growth mechanism could be applied to various metal carbides with similar diffusion rates.
INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Sharad S. Amin, Kieran D. Jones, Alexander J. Kibler, Heather A. Damian, Jamie M. Cameron, Kevin S. Butler, Stephen P. Argent, Max Winslow, David Robinson, Nicholas J. Mitchell, Hon Wai Lam, Graham N. Newton
Summary: Here, we report the synthesis and characterization of a new class of hybrid Wells-Dawson polyoxometalate (POM) with a diphosphoryl group (P2O6X). Modifying the bridging unit X impacts the redox potentials of the POM. The easy preparation of a range of alpha-functionalized diphosphonic acids (X=(CRR2)-R-1) provides possibilities for diverse functionalized hybrid POMs. Compared to existing phosphonate hybrid Wells-Dawson POMs, diphosphoryl-substituted POMs offer a wider tunable redox window and enhanced hydrolytic stability. This study provides a basis for the rational design and synthesis of next-generation hybrid Wells-Dawson POMs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Analytical
Jinmei Tian, Bin Jiang, Hong Shao, Yuting Wang, Tianqi Wang, Feng Li, Dan Li, Ying Yang, Xiangting Dong
Summary: In this study, one-dimensional tandem heterojunctions of SnO2 @POMs@WO3 nanofibers were prepared using coaxial electrospinning, and the gas sensing performance was significantly improved compared to SnO2 @WO3 nanofibers. The optimized response to 100 ppm ethanol reached 8.8, providing a new strategy for developing high-performance gas sensors through synthesizing one-dimensional tandem heterojunctions and introducing POMs.
SENSORS AND ACTUATORS B-CHEMICAL
(2023)
Article
Polymer Science
Shuwen Chen, Hao Zheng, Xiaofeng Liu, Juan Peng
Summary: In contrast to coil-coil block copolymers, the investigation into conjugated rod-rod block copolymers is limited. In this study, the researchers controlled the co-crystalline and microphase-separated structures in a family of rod-rod block copolymers with different molecular weights and explored their correlation with charge transport properties. The findings are important for the development of organic optoelectronic materials and devices.
Article
Chemistry, Inorganic & Nuclear
Firasat Hussain, Imran Khan, Vivek Das
Summary: The catalytic activity of tetrameric lanthanide-substituted phospho, germano, and silicotungstate compounds was investigated for the oxidation of alcohol derivatives. The study found that the lanthanide-substituted phosphotungstates exhibited better catalytic activity compared to the silico and germanotungstate analogues. The reaction was carried out in an environmentally friendly solvent (water) in the presence of a green oxidant (H2O2). The recovered catalysts were characterized using FT-IR spectroscopy and powder X-ray diffraction. The catalysts showed stability and could be reused with only a slight decrease in catalytic activity after five consecutive cycles.
INORGANICA CHIMICA ACTA
(2022)
Article
Chemistry, Physical
Anda Ioana Gratiela Petrehele, Narcis Duteanu, Mona Claudia Morgovan, Sanda Monica Filip, Stefania Ciocan, Eleonora Marian
Summary: Five new complexes with metal cations (Mn2+, Fe3+, Co2+, Ni2+, and Cu2+) of monolacunary Keggin monovanado-deca-tungstophosphate, K-8[PVW10O39]center dot 15H(2)O, have been successfully synthesized. The molar ratio of the combination between metal cations and K-8[PVW10O39]center dot 15H(2)O was determined to be 1:1, and their general molecular formulas were found to be K-n[MPVW10O39(H2O)]center dot xH(2)O (n = 5 for M = Fe3+ and n = 6 for M = Mn2+, Co2+, Ni2+, and Cu2+). The optimal conditions for the synthesis of these complexes have been determined, and various characterization methods have been used to confirm their compositions, structures, and properties.
Article
Materials Science, Multidisciplinary
Yingzhao He, Zhangcan Yang
Summary: Molecular dynamics simulations were used to study the growth of helium bubbles in tungsten nanotendrils, focusing on the effects of grain boundaries. The presence of grain boundaries in tendrils led to distinct features in helium bubble growth compared to bulk or planar surfaces without grain boundaries. The resulting surface morphology was influenced by the type of dislocation lines punched out by the bubbles in different grain boundary models. These findings provide insights into the formation of branch structures in fuzz tendrils observed in experiments.
JOURNAL OF NUCLEAR MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jia-Qi Lv, Bo Li, Qianqian Liu, Zhixin Gao, Zhong-Ling Lang, Song Liang, Yingqi Li, Hong-Ying Zang
Summary: Three novel redox-active tetranuclear iron-oxo clusters were synthesized and used as anode materials for Li-ion batteries. Among them, cluster H-6[Fe4O2(H2O)(2)(SO4)(7)]·H2O exhibited a specific discharge capacity of 1784 mAhg(-1) and good cycle performance. This is the first application of inorganic iron-oxo clusters for Li-ion storage.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Zoe L. Sinclair, Nicola L. Bell, Jessica. R. R. Bame, De-Liang Long, Leroy Cronin
Summary: Polyoxopalladates (POPs) are a class of self-assembling palladium-oxide clusters that have different sizes, shapes, and compositions. The largest compound in this family, {Pd-84}(Ac), is an ideal molecule for exploring supramolecular behavior in aqueous media. Through molecular visualization and nuclear magnetic resonance studies, it has been found that {Pd-84}(Ac) forms a 1:7 host-guest complex with benzyl viologen (BV2+) in aqueous solution.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Daniel J. Kowalski, Catriona M. MacGregor, De-Liang Long, Nicola L. Bell, Leroy Cronin
Summary: Library generation experiments are important in chemistry for discovering new materials, methods, and models, but generating high quality libraries is challenging. This study demonstrates the automation of library generation workflows using coordination chemistry and automated hardware. Directed exploration and diversity analysis of a process space was achieved, leading to unexpected discoveries of new complexes. The engineering of serendipity through the appearance of unexpected ligands highlights the potential of this approach.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Zhan-Guo Jiang, Hui-Min Zeng, Xiangyu Zhang, Yuan Tan, You-Zhao Lan, Yu Wang, De-Liang Long, Leroy Cronin, Cai-Hong Zhan
Summary: By replacing the H2O ligands with polyoxometalate (POM) [H2W12O40](6-) {W12O40} pro-ligands, a novel nano porous 2D network {[Cu-2(OAc)(4)](2)(W12O40)}(n) was synthesized. The compound exhibited high efficiency as a homogeneous catalyst in the homo-coupling of terminal alkynes under mild conditions and low amounts. In situ DRIFTS results revealed the changes of alkyne substances during the catalytic process, while XPS results showed electron transfer from {W12O40} to Cu(ii) to promote the C-H activation step. A synergistic Cu(ii)-POM catalytic mechanism was proposed.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
Yujie Ren, Yinghan Zhang, Qi Zheng, Lianjun Wang, Wan Jiang
Summary: Porous carbon-based composites with large surface area derived from MOF show great potential as high-efficiency electromagnetic wave absorbers.
Article
Behavioral Sciences
Vanessa Bowden, Dale Long, Shayne Loft
Summary: This study investigated the impact of a voluntary-use range and bearing line (RBL) tool on the performance of manually supervising high-degree conflict detection automation in simulated air traffic control. The results showed that providing RBLs improved automation failure detection, but the cost of high-degree automation still remained.
Article
Chemistry, Inorganic & Nuclear
Jake A. Thompson, Rebeca Gonzalez-Cabaleiro, Laia Vila-Nadal
Summary: Density functional theory calculations were used to evaluate the accuracy of various exchange-correlation functionals in reproducing the experimental redox potentials, U(0)(Red), for [PW11M(H2O)O-39](q-) M = Mn(III/II), Fe(III/II), Co(III/II), and Ru(III/II). The effect of K+ counterions on the calculated U(0)(Red) values was also assessed.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Daniel Malcolm, Laia Vila-Nadal
Summary: Porous metal oxide materials were synthesized using a ring-shaped macrocyclic polyoxometalate (POM) structural building unit. The POMs, known as POMzites, were assembled by connecting the building blocks with transition metal linkers. Through benchmarking, it was found that 8 potassium cations located within the pore provided the most accurate model. In addition, two similar POMs were analyzed and deemed suitable as POMzite building blocks. Another experiment demonstrated that substituting different cations into the pore affected the dimensions and reactivity of the structures.
ACS ORGANIC & INORGANIC AU
(2023)
Article
Materials Science, Multidisciplinary
Hsin Wang, J. Sebastian Manzano, Philip J. Kitson, Margaret Mullin, Chang-Gen Lin, Igor I. Slowing, Leroy Cronin
Summary: Nanomaterials exhibit unique properties that can be tailored based on their morphology and composition. To overcome the limitations of existing synthesis methods, a digital synthesis method is developed to capture and document the entire synthesis process, making it more accessible and reproducible. This method utilizes chemical description language and three single reactors to automate the synthesis of various nanomaterials, enabling researchers from different fields to easily access and reproduce these materials.
Article
Chemistry, Multidisciplinary
Min Meng, Lingrong Liao, Qi Zheng, Weimin Xuan
Summary: By tuning the geometry and size of the ligand and using phosphite as a bridging linker, {Ti-3(mu(3)-O)} can be assembled into a discrete {Ti-6} cluster, coordination capsule {Ti18Cu3} and one-dimensional coordination polymer {Ti-6}(n).
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Tingting Zhao, Nicola L. Bell, Greig Chisholm, Balamurugan Kandasamy, De-Liang Long, Leroy Cronin
Summary: In order to meet the increasing energy density demands of battery technology, the development of electrolytes with high electron storage capacity is crucial. Polyoxometalate (POM) clusters have the potential to act as electron storage electrolytes for flow batteries. However, little is known about the factors influencing the storage ability of these clusters, hindering their rational design. This study investigates large POM clusters and identifies key structural and speciation factors influencing their improved storage ability over previously reported clusters.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Daniel J. Kowalski, Catriona M. MacGregor, De-Liang Long, Nicola L. Bell, Leroy Cronin
Summary: Library generation experiments are crucial in chemistry for discovering new materials, methods, and models. This study demonstrates the automation of workflows using coordination chemistry for library generation. Validation of key synthetic operations, generation of focused libraries in chemical and process space, and development of a new workflow for prospecting library formation were conducted. The study showcases the directed exploration of process space and the engineering of serendipity for discovering unexpected compounds.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Jake A. Thompson, Laia Vila-Nadal
Summary: In this study, the accuracy of various exchange-correlation functionals in reproducing experimental P-31 NMR chemical shifts was systematically investigated using Density Functional Theory (DFT) calculations. The results showed that neutralizing the charge can reduce discrepancies between the calculated and experimental results, but uncertainties still exist for the [B-PW9O34](9-) anion.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Przemyslaw Frei, Philip J. Kitson, Alexander X. Jones, Leroy Cronin
Summary: Performing chemical transformations in a standard way is important for accessibility to high value reagents. This study presents a new concept in reactionware design using 3D printing, allowing the generation of high value compounds. By treating integrated reactor sequences as modular, different synthetic pathways can be selected.
Article
Chemistry, Inorganic & Nuclear
Hong-Ru Tan, Xiang Zhou, Hanqi You, Qi Zheng, Sheng-Yin Zhao, Weimin Xuan
Summary: Incorporating catalytic units into a crystalline porous matrix is an efficient way to build heterogeneous catalysts with high efficiency. By designing the porous skeleton and utilizing appropriate building blocks, the catalytic performance for organic transformations can be greatly enhanced due to the synergistic effect from the multicomponent and confined porous microenvironment around catalytically active sites. In this study, a porous polyoxometalate-based metal-organic framework (POMOF-1) was designed and synthesized, which exhibited excellent catalytic activity for selective oxidative coupling of amines to produce N-containing compounds. The POMOF-1 framework featured microporous channels with catalytically active sites arranged orderly, and it showed improved activity and selectivity compared to homogeneous catalysts. The POMOF-1 framework also demonstrated robustness and recyclability, making it a promising platform for multifunctional catalysis.
DALTON TRANSACTIONS
(2023)
Article
Electrochemistry
Kristine Laws, Marcus Tze-Kiat Ng, Abhishek Sharma, Yibin Jiang, Alexander J. S. Hammer, Leroy Cronin
Summary: This study developed a closed-loop robotic platform driven by a probabilistic algorithm for synthesis and electrochemical characterization. It successfully explored the redox behavior of different polyoxometalates (POMs) precursors and identified 24 complex solutions with significantly different redox activity.
