Extreme long-lifetime self-assembled monolayer for air-stable molecular junctions

The molecular electronic devices based on self-assembled monolayer (SAM) on metal surfaces demonstrate novel electronic functions for device minimization yet are unable to realize in practical applications, due to their instability against oxidation of the sulfur-metal bond. This paper describes an alternative to the thiolate anchoring group to form stable SAMs on gold by selenides anchoring group. Because of the formation of strong selenium-gold bonds, these stable SAMs allow us to incorporate them in molecular tunnel junctions to yield extremely stable junctions for over 200 days. A detailed structural characterization supported by spectroscopy and first-principles modeling shows that the oxidation process is much slower with the selenium-gold bond than the sulfur-gold bond, and the selenium-gold bond is strong enough to avoid bond breaking even when it is eventually oxidized. This proof of concept demonstrates that the extraordinarily stable SAMs derived from sel-enides are useful for long-lived molecular electronic devices and can possibly become important in many air-stable applications involving SAMs.</p

Sex-Specific Diurnal Immobility Induced by Forced Swim Test in Wild Type and Clock Gene Deficient Mice

Objective: The link between alterations in circadian rhythms and depression are well established, but the underlying mechanisms are far less elucidated. We investigated the circadian characteristics of immobility behavior in wild type (WT) mice and mice with mutations in core Clock genes. Methods: All mice were tested with forced swim test (FST) at 4 h intervals. Results: These experiments revealed significant diurnal rhythms associated with immobility behavior in both male and female WT mice with sex-different circadian properties. In addition, male mice showed significantly less immobility during the night phase in comparison to female mice. Female Per1Brdm1 mice also showed significant rhythmicity. However, the timing of rhythmicity was very different from that observed in female wild type mice. Male Per1Brdm1 mice showed a pattern of rhythmicity similar to that of wild type mice. Furthermore, female Per1Brdm1 mice showed higher duration of immobility in comparison to male Per1Brdm1 mice in both daytime and early night phases. Neither Per2Brdm1 nor ClockΔ19 mice showed significant rhythmicity, but both female Per2Brdm1 and ClockΔ19 mice had lower levels of immobility, compared to males. Conclusions: This study highlights the differences in the circadian characteristics of immobility induced by FST in WT, ClockΔ19, Per1, and Per2 deficient mice

The Trend in the Risk of Flash Flood Hazards with Regional Development in the Guanshan River Basin, China

The economic development of China&rsquo;s mountainous areas has been rapid, but the impact of flash floods is often ignored during regional development planning. Therefore, a method needed to be developed to simulate flash flood disasters and analyze the trends in flash flood disasters with regional development. Taking Guanshan River Basin as the research area, we combined the digital elevation model (DEM) with the inflow hydrograph, using the topography-based hydrological model (TOPMODEL). Verified by historical flash flood disasters, the watershed model was built based on the finite volume conservation flood routing model (FLO-2D). Then, we simulated the hazard distribution of flash flood disasters, developed a risk status assessment factor (RSAF) for flash flood disasters and calculated the increased ratio from 2003 to 2018. The results show that in 2003, the total hazard area of flash flood disasters affecting human settlements was 61,121 m2, which increased to 118,404 m2 in 2018. Since 2003, with the development of the regional economy, more residents moved to risk and extreme risk zones; thus, the risk of flash flood disasters also increased. Due to the significant damage caused by the flash flood on 5 August 2012, some of the local residents moved away from the high risk and extreme risk zones, indicating that the risk trend of flash flood hazard was consistent with the regional development of Guanshan River. We provide suggestions for regional economic development planning; the risk assessment for flash flood disasters must be considered to ensure the stable development of the regional economy, and using the RSAF would be efficient

Study of the Three Gorges Dam&rsquo;s Impact on the Discharge of Yangtze River during Flood Season after Its Full Operation in 2009

The impact of the Three Gorges Dam (TGD) on the discharge after its first operation in 2003 has drawn much attention. Most of the existing research focuses on the TGD&rsquo;s impact after its initial operation in 2003. However, the water level first reached the TGD&rsquo;s maximum water level, 175 m, in September 2009. In this paper, to quantify the TGD&rsquo;s impact during flood season after its full operation in 2009, we created a hydrological model to reconstruct the daily discharge unregulated by the TGD from 2003 to 2018 at the five stations downstream from the TGD. The TGD had an impact on the maximum 1-day discharge and maximum 30-day runoff and the coefficient of variation of the daily discharge, but it had less impact on the flood season runoff and the coefficient of skewness of the daily discharge. Additionally, the TGD was only responsible for 18.3% of the change in the maximum 1-day discharge at the Datong station, which is 1123 km downstream from the TGD. Moreover, the TGD had limited impact on the discharge after its initial operation in 2003, but the impact of the TGD on discharge increased after its full operation in 2009. This study helps to show the TGD&rsquo;s impact on the discharge of the Yangtze River from the Yichang station (43 km downstream from the TGD) to the Datong station

Effect of Continuous Renal Replacement Therapy with the oXiris Hemofilter on Critically Ill Patients: A Narrative Review

Critically ill patients with sepsis and severe COVID-19 are commonly characterized by a dysregulated immune response and an acute kidney injury. Continuous renal replacement therapy (CRRT) is now proposed as a promising adjuvant therapy to treat these critically ill patients by removing cytokines, pathogen-associated molecular patterns, and damage-associated molecular patterns from the blood. Although multiple hemofilters, including high-cutoff membranes, the oXiris hemofilter, the CytoSorb hemoadsorption device, and the Toraymyxin hemoperfusion cartridge, have been used in current clinical practice, the use of the oXiris hemofilter in critically ill patients is of particular interest because it is the only kind of hemofilter that can provide renal replacement therapy, remove endotoxins, and adsorb cytokines simultaneously. During the past five years, a growing body of literature has shown that CRRT with the oXiris hemofilter can improve hemodynamics and organ function and can decrease cytokines and endotoxins in both septic and COVID-19 patients. Here, we performed a narrative review to describe the development history of the oXiris hemofilter and to discuss the therapeutic effect of oXiris-CRRT on critically ill patients by searching the PubMed, Web of Science, and clinicaltrials.gov databases for articles published from inception to 8 September 2022 (updated on 1 November) with an English language restriction. We also summarized the current knowledge on anticoagulation techniques and safety concerns when delivering oXiris-CRRT sessions

High performance mechano-optoelectronic molecular switch

Abstract Highly-efficient molecular photoswitching occurs ex-situ but not to-date inside electronic devices due to quenching of excited states by background interactions. Here we achieve fully reversible in-situ mechano-optoelectronic switching in self-assembled monolayers (SAMs) of tetraphenylethylene molecules by bending their supporting electrodes to maximize aggregation-induced emission (AIE). We obtain stable, reversible switching across >1600 on/off cycles with large on/off ratio of (3.8 ± 0.1) × 103 and 140 ± 10 ms switching time which is 10-100× faster than other approaches. Multimodal characterization shows mechanically-controlled emission with UV-light enhancing the Coulomb interaction between the electrons and holes resulting in giant enhancement of molecular conductance. The best mechano-optoelectronic switching occurs in the most concave architecture that reduces ambient single-molecule conformational entropy creating artificially-tightened supramolecular assemblies. The performance can be further improved to achieve ultra-high switching ratio on the order of 105 using tetraphenylethylene derivatives with more AIE-active sites. Our results promise new applications from optimized interplay between mechanical force and optics in soft electronics

Direct synthesis of the organic and Ge free Al containing BOG zeolite (ITQ-47) and its application for transformation of biomass derived molecules

[EN] Aluminosilicate boggsite (Si/Al-BOG) has been hydrothermally synthesized without adding org. structure-directing agents (OSDAs) in the synthesis gel using the borosilicogermanium ITQ-47 (Si/B-ITQ-47) zeolite as seeds. The introduction of the costly and environmentally less benign phosphazene org. structure-directing agent is not required to grow the zeolite. Physicochem. characterization expts. show that Si/Al-BOG has good crystallinity, high surface area, tetrahedral Al3+ species, and acid sites. In order to test the catalytic performance of the zeolite, the synthesis of L,L-lactide from L-lactic acid was performed. Si/Al-BOG exhibits 88.2% conversion of L-lactic acid and 83.8% L,L-lactide selectivity, which are better than those of other zeolites studied up to now.This work was supported by the National Natural Science Foundation of China 21971259 and 91645112, The Natural Science Foundation of Hubei Province of China (2014CFA043), and the Key Research Program of Frontier Sciences, CAS (No. QYZDB-SSW-SLH026). The European Union is also acknowledged by ERC-AdG-2014-671093 SynCatMatch, and the Spanish Government through "Severo Ochoa" (SEV-2016-0683, MINECO). Q. H. acknowledges the International Program Fund for doctoral students, Sun Yat-sen University, for scholarships in Spain.Huang, Q.; Chen, N.; Liu, L.; Arias-Carrascal, KS.; Iborra Chornet, S.; Yi, X.; Ma, C.... (2020). Direct synthesis of the organic and Ge free Al containing BOG zeolite (ITQ-47) and its application for transformation of biomass derived molecules. 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Journal of the American Chemical Society, 133(50), 20604-20610. doi:10.1021/ja209220aStrohmaier, K. G., & Vaughan, D. E. W. (2003). Structure of the First Silicate Molecular Sieve with 18-Ring Pore Openings, ECR-34. Journal of the American Chemical Society, 125(51), 16035-16039. doi:10.1021/ja0371653Freyhardt, C. C., Lobo, R. F., Khodabandeh, S., Lewis,, J. E., Tsapatsis, M., Yoshikawa, M., … Davis, M. E. (1996). VPI-8:  A High-Silica Molecular Sieve with a Novel «Pinwheel» Building Unit and Its Implications for the Synthesis of Extra-Large Pore Molecular Sieves. Journal of the American Chemical Society, 118(31), 7299-7310. doi:10.1021/ja954337qMcKeen, J. C., & Davis, M. E. (2009). Conductivity of Mono- and Divalent Cations in the Microporous Zincosilicate VPI-9. The Journal of Physical Chemistry C, 113(22), 9870-9877. doi:10.1021/jp902235zJiang, J., Yu, J., & Corma, A. (2010). Extra-Large-Pore Zeolites: Bridging the Gap between Micro and Mesoporous Structures. Angewandte Chemie International Edition, 49(18), 3120-3145. doi:10.1002/anie.200904016Jiang, J., Jorda, J. L., Diaz-Cabanas, M. J., Yu, J., & Corma, A. (2010). The Synthesis of an Extra-Large-Pore Zeolite with Double Three-Ring Building Units and a Low Framework Density. Angewandte Chemie International Edition, 49(29), 4986-4988. doi:10.1002/anie.201001506Jiang, J., Jorda, J. L., Yu, J., Baumes, L. A., Mugnaioli, E., Diaz-Cabanas, M. J., … Corma, A. (2011). Synthesis and Structure Determination of the Hierarchical Meso-Microporous Zeolite ITQ-43. Science, 333(6046), 1131-1134. doi:10.1126/science.1208652Jiang, J., Yun, Y., Zou, X., Jorda, J. L., & Corma, A. (2015). ITQ-54: a multi-dimensional extra-large pore zeolite with 20 × 14 × 12-ring channels. Chemical Science, 6(1), 480-485. doi:10.1039/c4sc02577fZhang, C., Kapaca, E., Li, J., Liu, Y., Yi, X., Zheng, A., … Yu, J. (2018). An Extra‐Large‐Pore Zeolite with 24×8×8‐Ring Channels Using a Structure‐Directing Agent Derived from Traditional Chinese Medicine. Angewandte Chemie International Edition, 57(22), 6486-6490. doi:10.1002/anie.201801386Li, J., Corma, A., & Yu, J. (2015). Synthesis of new zeolite structures. Chemical Society Reviews, 44(20), 7112-7127. doi:10.1039/c5cs00023hLi, Y., & Yu, J. (2014). New Stories of Zeolite Structures: Their Descriptions, Determinations, Predictions, and Evaluations. Chemical Reviews, 114(14), 7268-7316. doi:10.1021/cr500010rC. Y. Chen and S. I.Zones , in Zeolite and Catalysis: Synthesis, Reaction and Application , ed. A. C. Jiri Cejka and S. Zones , Wiley-VCH Verlag GmbH & Co. KGaA , Weinheim , 2010 , ch. 6, vol. 1 , pp. 155–164Valtchev, V., Majano, G., Mintova, S., & Pérez-Ramírez, J. (2013). Tailored crystalline microporous materials by post-synthesis modification. Chem. Soc. Rev., 42(1), 263-290. doi:10.1039/c2cs35196jZones, S. I., Benin, A., Hwang, S.-J., Xie, D., Elomari, S., & Hsieh, M.-F. (2014). Studies of Aluminum Reinsertion into Borosilicate Zeolites with Intersecting Channels of 10- and 12-Ring Channel Systems. Journal of the American Chemical Society, 136(4), 1462-1471. doi:10.1021/ja4100194Gao, F., Jaber, M., Bozhilov, K., Vicente, A., Fernandez, C., & Valtchev, V. (2009). Framework Stabilization of Ge-Rich Zeolites via Postsynthesis Alumination. Journal of the American Chemical Society, 131(45), 16580-16586. doi:10.1021/ja904458yMeng, X., & Xiao, F.-S. (2013). Green Routes for Synthesis of Zeolites. Chemical Reviews, 114(2), 1521-1543. doi:10.1021/cr4001513Iyoki, K., Itabashi, K., & Okubo, T. (2014). Progress in seed-assisted synthesis of zeolites without using organic structure-directing agents. Microporous and Mesoporous Materials, 189, 22-30. doi:10.1016/j.micromeso.2013.08.008Xie, B., Song, J., Ren, L., Ji, Y., Li, J., & Xiao, F.-S. (2008). Organotemplate-Free and Fast Route for Synthesizing Beta Zeolite. Chemistry of Materials, 20(14), 4533-4535. doi:10.1021/cm801167eZhang, H., Xie, B., Meng, X., Müller, U., Yilmaz, B., Feyen, M., … Xiao, F.-S. (2013). Rational synthesis of Beta zeolite with improved quality by decreasing crystallization temperature in organotemplate-free route. Microporous and Mesoporous Materials, 180, 123-129. doi:10.1016/j.micromeso.2013.06.031Liao, Y., Pan, S., Bian, C., Meng, X., & Xiao, F.-S. (2015). Improved catalytic activity in methanol electro-oxidation over the nickel form of aluminum-rich beta-SDS zeolite modified electrode. Journal of Materials Chemistry A, 3(11), 5811-5814. doi:10.1039/c4ta06699eYokoi, T., Yoshioka, M., Imai, H., & Tatsumi, T. (2009). Diversification of RTH-Type Zeolite and Its Catalytic Application. Angewandte Chemie International Edition, 48(52), 9884-9887. doi:10.1002/anie.200905214Song, J., Dai, L., Ji, Y., & Xiao, F.-S. (2006). Organic Template Free Synthesis of Aluminosilicate Zeolite ECR-1. Chemistry of Materials, 18(12), 2775-2777. doi:10.1021/cm052593oZhang, H., Yang, C., Zhu, L., Meng, X., Yilmaz, B., Müller, U., … Xiao, F.-S. (2012). Organotemplate-free and seed-directed synthesis of levyne zeolite. Microporous and Mesoporous Materials, 155, 1-7. doi:10.1016/j.micromeso.2011.12.051Xie, B., Zhang, H., Yang, C., Liu, S., Ren, L., Zhang, L., … Xiao, F.-S. (2011). Seed-directed synthesis of zeolites with enhanced performance in the absence of organic templates. Chemical Communications, 47(13), 3945. doi:10.1039/c0cc05414cZhang, H., Guo, Q., Ren, L., Yang, C., Zhu, L., Meng, X., … Xiao, F.-S. (2011). Organotemplate-free synthesis of high-silica ferrierite zeolite induced by CDO-structure zeolite building units. Journal of Materials Chemistry, 21(26), 9494. doi:10.1039/c1jm11786fWang, Y., Wang, X., Wu, Q., Meng, X., Jin, Y., Zhou, X., & Xiao, F.-S. (2014). Seed-directed and organotemplate-free synthesis of TON zeolite. Catalysis Today, 226, 103-108. doi:10.1016/j.cattod.2013.08.002Wu, Q., Wang, X., Meng, X., Yang, C., Liu, Y., Jin, Y., … Xiao, F.-S. (2014). Organotemplate-free, seed-directed, and rapid synthesis of Al-rich zeolite MTT with improved catalytic performance in isomerization of m-xylene. Microporous and Mesoporous Materials, 186, 106-112. doi:10.1016/j.micromeso.2013.11.043Zhang, L., Yang, C., Meng, X., Xie, B., Wang, L., Ren, L., … Xiao, F.-S. (2010). Organotemplate-Free Syntheses of ZSM-34 Zeolite and Its Heteroatom-Substituted Analogues with Good Catalytic Performance. Chemistry of Materials, 22(10), 3099-3107. doi:10.1021/cm100030xYang, C., Ren, L., Zhang, H., Zhu, L., Wang, L., Meng, X., & Xiao, F.-S. (2012). Organotemplate-free and seed-directed synthesis of ZSM-34 zeolite with good performance in methanol-to-olefins. Journal of Materials Chemistry, 22(24), 12238. doi:10.1039/c2jm31479gIyoki, K., Kamimura, Y., Itabashi, K., Shimojima, A., & Okubo, T. (2010). Synthesis of MTW-type Zeolites in the Absence of Organic Structure-directing Agent. Chemistry Letters, 39(7), 730-731. doi:10.1246/cl.2010.730Kamimura, Y., Iyoki, K., Elangovan, S. P., Itabashi, K., Shimojima, A., & Okubo, T. (2012). OSDA-free synthesis of MTW-type zeolite from sodium aluminosilicate gels with zeolite beta seeds. Microporous and Mesoporous Materials, 163, 282-290. doi:10.1016/j.micromeso.2012.07.014Moteki, T., & Okubo, T. (2013). From Charge Density Mismatch to a Simplified, More Efficient Seed-Assisted Synthesis of UZM-4. Chemistry of Materials, 25(13), 2603-2609. doi:10.1021/cm400727rOgawa, A., Iyoki, K., Kamimura, Y., Elangovan, S. P., Itabashi, K., & Okubo, T. (2014). Seed-directed, rapid synthesis of MAZ-type zeolites without using organic structure-directing agent. Microporous and Mesoporous Materials, 186, 21-28. doi:10.1016/j.micromeso.2013.11.026Kubota, Y., Itabashi, K., Inagaki, S., Nishita, Y., Komatsu, R., Tsuboi, Y., … Okubo, T. (2014). Effective Fabrication of Catalysts from Large-Pore, Multidimensional Zeolites Synthesized without Using Organic Structure-Directing Agents. Chemistry of Materials, 26(2), 1250-1259. doi:10.1021/cm403797jKamimura, Y., Itabashi, K., Kon, Y., Endo, A., & Okubo, T. (2017). Seed-Assisted Synthesis of MWW-Type Zeolite with Organic Structure-Directing Agent-Free Na-Aluminosilicate Gel System. Chemistry - An Asian Journal, 12(5), 530-542. doi:10.1002/asia.201601569Iyoki, K., Takase, M., Itabashi, K., Muraoka, K., Chaikittisilp, W., & Okubo, T. (2015). Organic structure-directing agent-free synthesis of NES-type zeolites using EU-1 seed crystals. Microporous and Mesoporous Materials, 215, 191-198. doi:10.1016/j.micromeso.2015.05.042ZHOU, H., WU, Y., ZHANG, W., & WANG, J. (2014). Organotemplate-free Hydrothermal Synthesis of SUZ-4 Zeolite: Influence of Synthesis Conditions. Chinese Journal of Chemical Engineering, 22(1), 120-126. doi:10.1016/s1004-9541(14)60019-7Sogukkanli, S., Iyoki, K., Elangovan, S. P., Itabashi, K., & Okubo, T. (2017). Seed-directed Synthesis of CON-type Zeolite Using Tetraethylammonium Hydroxide as a Simple Organic Structure-directing Agent. Chemistry Letters, 46(9), 1419-1421. doi:10.1246/cl.170602Luo, Y., Wang, Z., Sun, J., Wang, Y., Jin, S., Zhang, B., … Yang, W. (2017). A Facile and Green Method for the Synthesis of SFE Borosilicate Zeolite and Its Heteroatom-Substituted Analogues with Promising Catalytic Performances. Chemistry - A European Journal, 24(2), 306-311. doi:10.1002/chem.201704668Iyoki, K., Itabashi, K., Chaikittisilp, W., Elangovan, S. P., Wakihara, T., Kohara, S., & Okubo, T. (2014). Broadening the Applicable Scope of Seed-Directed, Organic Structure-Directing Agent-Free Synthesis of Zeolite to Zincosilicate Components: A Case of VET-Type Zincosilicate Zeolites. Chemistry of Materials, 26(5), 1957-1966. doi:10.1021/cm500229fNg, E.-P., Chateigner, D., Bein, T., Valtchev, V., & Mintova, S. (2012). Capturing Ultrasmall EMT Zeolite from Template-Free Systems. Science, 335(6064), 70-73. doi:10.1126/science.1214798Kamimura, Y., Itabashi, K., & Okubo, T. (2012). Seed-assisted, OSDA-free synthesis of MTW-type zeolite and «Green MTW» from sodium aluminosilicate gel systems. Microporous and Mesoporous Materials, 147(1), 149-156. doi:10.1016/j.micromeso.2011.05.038Simancas, R., Dari, D., Velamazán, N., Navarro, M. T., Cantín, A., Jordá, J. L., … Rey, F. (2010). Modular Organic Structure-Directing Agents for the Synthesis of Zeolites. Science, 330(6008), 1219-1222. doi:10.1126/science.1196240Ghorbanpour, A., Gumidyala, A., Grabow, L. C., Crossley, S. P., & Rimer, J. D. (2015). Epitaxial Growth of ZSM-5@Silicalite-1: A Core–Shell Zeolite Designed with Passivated Surface Acidity. ACS Nano, 9(4), 4006-4016. doi:10.1021/acsnano.5b01308Bouizi, Y., Rouleau, L., & Valtchev, V. P. (2006). Bi-phase MOR/MFI-type zeolite core–shell composite. Microporous and Mesoporous Materials, 91(1-3), 70-77. doi:10.1016/j.micromeso.2005.11.016PEREZPARIENTE, J. (1990). 29Si and 27Al MAS NMR study of zeolite $beta; with different Si/Al Ratios. Journal of Catalysis, 124(1), 217-223. doi:10.1016/0021-9517(90)90116-2Lentz, P., Nagy, J. ., Delevoye, L., Dumazy, Y., Fernandez, C., Amoureux, J.-P., … Nastro, A. (1999). 2D multiple quantum 27Al NMR and 29Si NMR characterization of levyne. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 158(1-2), 13-20. doi:10.1016/s0927-7757(99)00125-9Boronat, M., & Corma, A. (2019). What Is Measured When Measuring Acidity in Zeolites with Probe Molecules? ACS Catalysis, 9(2), 1539-1548. doi:10.1021/acscatal.8b04317Maity, A., Chaudhari, S., Titman, J. J., & Polshettiwar, V. (2020). Catalytic nanosponges of acidic aluminosilicates for plastic degradation and CO2 to fuel conversion. Nature Communications, 11(1). doi:10.1038/s41467-020-17711-6Dusselier, M., Van Wouwe, P., Dewaele, A., Jacobs, P. A., & Sels, B. F. (2015). Shape-selective zeolite catalysis for bioplastics production. Science, 349(6243), 78-80. doi:10.1126/science.aaa716

High performance mechano-optoelectronic molecular switch

Highly-efficient molecular photoswitching occurs ex-situ but not to-date inside electronic devices due to quenching of excited states by background interactions. Here we achieve fully reversible in-situ mechano-optoelectronic switching in self-assembled monolayers (SAMs) of tetraphenylethylene molecules by bending their supporting electrodes to maximize aggregation-induced emission (AIE). We obtain stable, reversible switching across >1600 on/off cycles with large on/off ratio of (3.8 ± 0.1) × 103 and 140 ± 10 ms switching time which is 10-100× faster than other approaches. Multimodal characterization shows mechanically-controlled emission with UV-light enhancing the Coulomb interaction between the electrons and holes resulting in giant enhancement of molecular conductance. The best mechano-optoelectronic switching occurs in the most concave architecture that reduces ambient single-molecule conformational entropy creating artificially-tightened supramolecular assemblies. The performance can be further improved to achieve ultra-high switching ratio on the order of 105 using tetraphenylethylene derivatives with more AIE-active sites. Our results promise new applications from optimized interplay between mechanical force and optics in soft electronics.</p