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231.
Tao Song Dr. Da Wang Prof. Hongxia Wang Dr. Jia Yu Prof. Siqi Shi 《Angewandte Chemie (International ed. in English)》2023,62(31):e202305004
Integrating the advantages of both inorganic ceramic and organic polymer solid-state electrolytes, small-molecule solid-state electrolytes represented by LiI-3-hydroxypropionitrile (LiI-HPN) inorganic–organic hybrid systems possess good interfacial compatibility and high modulus. However, their lack of intrinsic Li+ conduction ability hinders potential application in lithium metal batteries until now, despite containing LiI phase composition. Herein, inspired by evolution tendency of ionic conduction behaviors together with first-principles molecular dynamics simulations, we propose a stepped-amorphization strategy to break the Li+ conduction bottleneck of LiI-HPN. It involves three progressive steps of composition (LiI-content increasing), time (long-time standing), and temperature (high-temperature melting) regulations, to essentially construct a small-molecule-based composite solid-state electrolyte with intensified amorphous degree, which realizes efficient conversion from an I− to Li+ conductor and improved conductivity. As a proof, the stepped-optimized LiI-HPN is successfully operated in lithium metal batteries cooperated with Li4Ti5O12 cathode to deliver considerable compatibility and stability over 250 cycles. This work not only clarifies the ionic conduction mechanisms of LiI-HPN inorganic–organic hybrid systems, but also provides a reasonable strategy to broaden the application scenarios of highly compatible small-molecule solid-state electrolytes. 相似文献
232.
Caitlin E. Shields Dr. Xue Wang Dr. Thomas Fellowes Rob Clowes Dr. Linjiang Chen Prof. Graeme M. Day Prof. Anna G. Slater Dr. John W. Ward Dr. Marc A. Little Prof. Andrew I. Cooper 《Angewandte Chemie (International ed. in English)》2023,62(34):e202303167
Hydrogen-bonded organic frameworks (HOFs) with low densities and high porosities are rare and challenging to design because most molecules have a strong energetic preference for close packing. Crystal structure prediction (CSP) can rank the crystal packings available to an organic molecule based on their relative lattice energies. This has become a powerful tool for the a priori design of porous molecular crystals. Previously, we combined CSP with structure-property predictions to generate energy-structure-function (ESF) maps for a series of triptycene-based molecules with quinoxaline groups. From these ESF maps, triptycene trisquinoxalinedione (TH5) was predicted to form a previously unknown low-energy HOF (TH5-A) with a remarkably low density of 0.374 g cm−3 and three-dimensional (3D) pores. Here, we demonstrate the reliability of those ESF maps by discovering this TH5-A polymorph experimentally. This material has a high accessible surface area of 3,284 m2 g−1, as measured by nitrogen adsorption, making it one of the most porous HOFs reported to date. 相似文献
233.
Jiahui Xian Suisheng Li Hui Su Peisen Liao Shihan Wang Runan Xiang Yawei Zhang Prof. Qinghua Liu Prof. Guangqin Li 《Angewandte Chemie (International ed. in English)》2023,62(30):e202306726
The conversion of industrial exhaust gases of nitrogen oxides into high-value products is significantly meaningful for global environment and human health. And green synthesis of amino acids is vital for biomedical research and sustainable development of mankind. Herein, we demonstrate an innovative approach for converting nitric oxide (NO) to a series of α-amino acids (over 13 kinds) through electrosynthesis with α-keto acids over self-standing carbon fiber membrane with CoFe alloy. The essential leucine exhibits a high yield of 115.4 μmol h−1 corresponding a Faradaic efficiency of 32.4 %, and gram yield of products can be obtained within 24 hours in lab as well as an ultra-long stability (>240 h) of the membrane catalyst, which could convert NO into NH2OH rapidly attacking α-keto acid and subsequent hydrogenation to form amino acid. In addition, this method is also suitable for other nitrogen sources including gaseous NO2 or liquidus NO3− and NO2−. Therefore, this work not only presents promising prospects for converting nitrogen oxides from exhaust gas and nitrate-laden waste water into high-value products, but also has significant implications for synthetizing amino acids in biomedical and catalytic science. 相似文献
234.
Dr. Qing-Yun Guo Zitong Wang Dr. Xuanyu Feng Yingjie Fan Prof. Dr. Wenbin Lin 《Angewandte Chemie (International ed. in English)》2023,62(35):e202306905
Although many monometallic active sites have been installed in metal–organic frameworks (MOFs) for catalytic reactions, there are no effective strategies to generate bimetallic catalysts in MOFs. Here we report the synthesis of a robust, efficient, and reusable MOF catalyst, MOF-NiH, by adaptively generating and stabilizing dinickel active sites using the bipyridine groups in MOF-253 with the formula of Al(OH)(2,2′-bipyridine-5,5′-dicarboxylate) for Z-selective semihydrogenation of alkynes and selective hydrogenation of C=C bonds in α,β-unsaturated aldehydes and ketones. Spectroscopic studies established the dinickel complex (bpy⋅−)NiII(μ2-H)2NiII(bpy⋅−) as the active catalyst. MOF-NiH efficiently catalyzed selective hydrogenation reactions with turnover numbers of up to 192 and could be used in five cycles of hydrogenation reactions without catalyst leaching or significant decrease of catalytic activities. The present work uncovers a synthetic strategy toward solution-inaccessible Earth-abundant bimetallic MOF catalysts for sustainable catalysis. 相似文献
235.
Éadaoin McCourt Dr. Kane Esien Li Zhenyu Dr. Solveig Felton Dr. Peter Nockemann 《Angewandte Chemie (International ed. in English)》2023,62(7):e201809334
Herein, we report on the preparation of liquid dimeric lanthanide(III)-containing compounds. Starting from the design of dimeric solids, we demonstrate that by tuning of anion and cation structures we can lower the melting points below room temperature, whilst maintaining the dimeric structure. Magnetic measurements could establish the spin-spin interactions of the neighboring lanthanide(III) ions in the liquid state at low temperatures, and matched the interactions of the analogous crystalline solid compounds. 相似文献
236.
Jiahui Zeng Yu Fu Yue Wu Shanshan Wang Wenxiang Zhang Prof. Heping Ma 《Angewandte Chemie (International ed. in English)》2023,62(42):e202310235
Xe is an ideal anesthetic gas, but it has not been widely used in practice due to its high cost and low output. Closed-circuit Xe recovery and recycling is an economically viable method to ensure adequate supply in medical use. Herein, we design an innovative way to recover Xe by using a stable fluorinated metal-organic framework (MOF) NbOFFIVE-1-Ni to eliminate CO2 from moist exhaled anesthetic gases. Unlike other Xe recovery MOFs with low Xe/CO2 selectivity (less than 10), NbOFFIVE-1-Ni could achieve absolute molecular sieve separation of CO2/Xe with excellent CO2 selectivity (825). Mixed-gas breakthrough experiments assert the potential of NbOFFIVE-1-Ni as a molecular sieve adsorbent for the effective and energy-efficient removal of carbon dioxide with 99.16 % Xe recovery. Absolute CO2/Xe separation in NbOFFIVE-1-Ni makes closed-circuit Xe recovery and recycling can be easily realized, demonstrating the potential of NbOFFIVE-1-Ni for important anesthetic gas regeneration under ambient conditions. 相似文献
237.
Basem Moosa Lukman O. Alimi Weibin Lin Aliyah Fakim Prashant M. Bhatt Mohamed Eddaoudi Niveen M. Khashab 《Angewandte Chemie (International ed. in English)》2023,62(46):e202311555
Porous molecular sorbents have excellent selectivity towards hydrocarbon separation with energy saving techniques. However, to realize commercialization, molecular sieving processes should be faster and more efficient compared to extended frameworks. In this work, we show that utilizing fluorine to improve the hydrophobic profile of leaning pillararenes affords a substantial kinetic selective adsorption of benzene over cyclohexane (20 : 1 for benzene). The crystal structure shows a porous macrocycle that acts as a perfect match for benzene in both the intrinsic and extrinsic cavities with strong interactions in the solid state. The fluorinated leaning pillararene surpasses all reported organic molecular sieves and is comparable to the extended metal–organic frameworks that were previously employed for this separation such as UIO-66. Most importantly, this sieving system outperformed the well-known zeolitic imidazolate frameworks under low pressure, which opens the door to new generations of molecular sieves that can compete with extended frameworks for more sustainable hydrocarbon separation. 相似文献
238.
Dr. Xuelin Yao Dr. Heng Zhang Fanmiao Kong Dr. Antoine Hinaut Dr. Rémy Pawlak Prof. Dr. Masanari Okuno Dr. Robert Graf Dr. Peter N. Horton Prof. Dr. Simon J. Coles Prof. Dr. Ernst Meyer Prof. Dr. Lapo Bogani Prof. Dr. Mischa Bonn Prof. Dr. Hai I. Wang Prof. Dr. Klaus Müllen Prof. Dr. Akimitsu Narita 《Angewandte Chemie (International ed. in English)》2023,62(46):e202312610
Structurally defined graphene nanoribbons (GNRs) have emerged as promising candidates for nanoelectronic devices. Low band gap (<1 eV) GNRs are particularly important when considering the Schottky barrier in device performance. Here, we demonstrate the first solution synthesis of 8-AGNRs through a carefully designed arylated polynaphthalene precursor. The efficiency of the oxidative cyclodehydrogenation of the tailor-made polymer precursor into 8-AGNRs was validated by FT-IR, Raman, and UV/Vis-near-infrared (NIR) absorption spectroscopy, and further supported by the synthesis of naphtho[1,2,3,4-ghi]perylene derivatives ( 1 and 2 ) as subunits of 8-AGNR , with a width of 0.86 nm as suggested by the X-ray single crystal analysis. Low-temperature scanning tunneling microscopy (STM) and solid-state NMR analyses provided further structural support for 8-AGNR . The resulting 8-AGNR exhibited a remarkable NIR absorption extending up to ∼2400 nm, corresponding to an optical band gap as low as ∼0.52 eV. Moreover, optical-pump TeraHertz-probe spectroscopy revealed charge-carrier mobility in the dc limit of ∼270 cm2 V−1 s−1 for the 8-AGNR . 相似文献
239.
Miharu Eguchi Minsu Han Yusuke Asakura Jonathan P. Hill Joel Henzie Katsuhiko Ariga Alan E. Rowan Watcharop Chaikittisilp Yusuke Yamauchi 《Angewandte Chemie (International ed. in English)》2023,62(46):e202307615
Reactions occurring at surfaces and interfaces necessitate the creation of well-designed surface and interfacial structures. To achieve a combination of bulk material (i.e., framework) and void spaces, a meticulous process of “nano-architecting” of the available space is necessary. Conventional porous materials such as mesoporous silica, zeolites, and metal–organic frameworks lack advanced cooperative functionalities owing to their largely monotonous pore geometries and limited conductivities. To overcome these limitations and develop functional structures with surface-specific functions, the novel materials space-tectonics methodology has been proposed for future materials synthesis. This review summarizes recent examples of materials synthesis based on designing building blocks (i.e., tectons) and their hybridization, along with practical guidelines for implementing materials syntheses and state-of-the-art examples of practical applications. Lastly, the potential integration of materials space-tectonics with emerging technologies, such as materials informatics, is discussed. 相似文献
240.
A novel membrane-based sensor device for upstream membrane integrity monitoring has been developed and evaluated in this study. The sensor is based on relative trans-membrane pressures created by two membranes in series inside the sensor device that detects deposition from the sample stream onto the first of the sensor membranes. The sensor pressure signals can distinguish between intact or damaged membranes in the upstream membrane filtration process. Studies were conducted to evaluate both stabilities and sensitivities of the relative trans-membrane pressure monitoring technique. Sensitivity, based on the response times of the membrane sensor for particle detection, was determined for a range of operating conditions, membrane sandwich configurations, and particle concentrations in both simulated membrane failures and for actual pin-hole defects on a submerged MF membrane. The results showed that both sensitivities and stability strongly depended on membrane sandwich configurations (membrane characteristics) in the sensor, and mode of operation (pressurized or vacuum). The membrane sensor detected bentonite particles with a concentration of 0.3 mg/L (turbidity ∼0.3 NTU) in approximately 35 min in the vacuum mode. The sensor is reliable, sensitive and low cost. It has potential applications in decentralized systems or in multichannel monitoring of local conditions in a large plant. Possible applications of the membrane sensor for fouling monitoring are also discussed. 相似文献