Search

Polymer products typically present as mixtures with a range of molecular weights, which notably influence the expression of their properties. In this study, a technique is proposed to separate polyethylene glycol (PEG) mixtures of varying molecular weights using metal–organic frameworks (MOFs), thereby narrowing down their molecular weight distribution. Due to the hydrogen bond interactions between PEG and ‐OH groups in the pores of NU‐1000, NU‐1000 can selectively adsorb PEG with larger molecular weights from PEG mixture. This separation method consistently yields with narrower molecular weight distribution across multiple cycles. This is the first application of MOFs in regulating the dispersity (Ð) of polymers in solution, providing a novel approach for separating and purifying mixed molecular weight polymers. [ABSTRACT FROM AUTHOR]

In this study, we propose a mechanochemical approach that combines mesoporous ZnO (m-ZnO) as a mechanoredox catalyst and silane-mediated atom transfer chemistry to achieve efficient hydrodehalogenation of organic halides. The reaction can be conducted under mild conditions without the use of a large amount of organic solvent. Substrates ranging from activated alkyl halides to unactivated aryl halides were converted to the corresponding debrominated hydrogenation products in moderate to excellent isolated yields (50–95%). In addition, m-ZnO can be recycled and reused without appreciable loss of catalytic activity. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Mechanoredox chemistry that uses highly polarized piezoelectric materials as mechanoredox catalysts to promote redox reactions has emerged recently. It provides an alternative approach alongside the existing polymerization methods. Despite recent accomplishments, determining the quantitative relationship between the structure of ZnO and its catalytic performance for polymerization is still challenging. Herein, we prepared various ZnO crystals with different polar facets ratios to achieve efficient mechanically induced reversible addition‐fragmentation chain transfer polymerization (mechano‐RAFT). ZnO prepared from Zn(NO3)2 showed a high polar facet ratio of 1.66 and offered the highest catalytic activity among all ZnO samples. A near‐quantitative initiator efficiency of 99.5% and narrow molecular weight distribution were achieved for the polymerization of n‐butyl acrylate. Furthermore, the high chain‐end fidelity and chain extension capability were also evidenced by MALDI‐TOF MS and GPC analysis. This work highlighted the significant contribution of polar facets in ZnO to its catalytic activity and will guide the design of mechanoredox catalysis with superior catalytic performance in the future. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Mechanoredox chemistry that uses highly polarized piezoelectric materials as mechanoredox catalysts to promote redox reactions has emerged recently. It provides an alternative approach alongside the existing polymerization methods. Despite recent accomplishments, determining the quantitative relationship between the structure of ZnO and its catalytic performance for polymerization is still challenging. Herein, we prepared various ZnO crystals with different polar facets ratios to achieve efficient mechanically induced reversible addition‐fragmentation chain transfer polymerization (mechano‐RAFT). ZnO prepared from Zn(NO3)2 showed a high polar facet ratio of 1.66 and offered the highest catalytic activity among all ZnO samples. A near‐quantitative initiator efficiency of 99.5% and narrow molecular weight distribution were achieved for the polymerization of n‐butyl acrylate. Furthermore, the high chain‐end fidelity and chain extension capability were also evidenced by MALDI‐TOF MS and GPC analysis. This work highlighted the significant contribution of polar facets in ZnO to its catalytic activity and will guide the design of mechanoredox catalysis with superior catalytic performance in the future. [ABSTRACT FROM AUTHOR]

Herein, we designed and synthesized a series of rare earth doped BiOF/Bi2MoO6 heterojunctions. The doping locations of rare earth ions were altered to determine the influence on the visible and near-infrared photocatalytic activity of heterojunctions. It is experimentally and theoretically confirmed that doping with Tm3+/Yb3+ in one semiconductor of the heterojunction produces superior photocatalytic efficiency than doping in both semiconductors. In addition, the near infrared photocatalytic efficiency strongly relied on upconversion luminescence from the Re3+ doped semiconductor in the heterojunction. By further modifying with CQDs, the CQDs/BiOF:Tm3+,Yb3+/Bi2MoO6 sample shows excellent visible and near-infrared photocatalytic performance, with 90% degradation of RhB occurring in the first 20 min under visible irradiation. This can be attributed to the large BET area, efficient photoinduced carrier separation and the upconversion process of the composite. This research will provide a systematic solution for realizing full-spectrum responsive and highly efficient photocatalysis by combination of rare earth ion doping, quantum dot modification and Z-scheme heterojunctions. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Recently, piezocatalysis has attracted considerable attention as a new type of renewable mechanical energy conversion technology, which relies on the strain induced polarization of the piezoelectric material. This new technology has been extensively applied in the applications of water splitting, water remediation, gas purification and tumor therapy. Despite the rapid development in the piezocatalysis, the utilization of piezoelectric materials for synthetic purpose is still under exploration. Piezoelectric means to promote organic reactions expand the scope of piezoelectrically mediated reactions and show successes in both organic and polymer synthesis. Herein, we provide a comprehensive review on recent progress of piezoelectrically mediated reactions, catalytic mechanisms and applications in the last few years. The limitations and future directions of this area are also discussed. We believe this review will provide new insights into the underlying mechanism of piezoelectric mediated electron transfer process and guide the design of new chemistry. [ABSTRACT FROM AUTHOR]

Systemic inflammation with alterations in inflammatory markers is involved in aging and Alzheimer's disease. However, few studies have investigated the longitudinal trajectories of systemic inflammatory markers during aging and Alzheimer's disease, and specific markers contributing to Alzheimer's disease remain undetermined. In this study, a longitudinal cohort (cohort 1: n = 290; controls, 136; preclinical Alzheimer's disease, 154) and a cross-sectional cohort (cohort 2: n = 351; controls, 62; Alzheimer's disease, 63; vascular dementia, 58; Parkinson's disease dementia, 56; behavioural variant frontotemporal dementia, 57; dementia with Lewy bodies, 55) were included. Plasma levels of inflammatory markers were measured every 2 years during a 10-year follow-up in the longitudinal cohort and once in the cross-sectional cohort. The study demonstrated that the inflammatory markers significantly altered during both aging and the development of Alzheimer's disease. However, only complement C3, interleukin-1β, and interleukin-6 exhibited significant changes in participants with preclinical Alzheimer's disease, and their longitudinal changes were significantly associated with the development of Alzheimer's disease compared to controls over the 10-year follow-up. In the cross-sectional cohort, complement C3 demonstrates specificity to Alzheimer's disease, while interleukin-1β and interleukin-6 were also altered in other dementias. The study provides a new perspective on the involvement of inflammatory markers in the aging process and the development of Alzheimer's disease, implying that regulating inflammation may have a pivotal role in promoting successful aging and in the prevention and treatment of Alzheimer's disease., (© The Author(s) 2024. Published by Oxford University Press on behalf of the Guarantors of Brain. All rights reserved. For commercial re-use, please contact reprints@oup.com for reprints and translation rights for reprints. All other permissions can be obtained through our RightsLink service via the Permissions link on the article page on our site—for further information please contact journals.permissions@oup.com.)

Herein, we designed and synthesized a series of rare earth doped BiOF/Bi 2 MoO 6 heterojunctions. The doping locations of rare earth ions were altered to determine the influence on the visible and near-infrared photocatalytic activity of heterojunctions. It is experimentally and theoretically confirmed that doping with Tm 3+ /Yb 3+ in one semiconductor of the heterojunction produces superior photocatalytic efficiency than doping in both semiconductors. In addition, the near infrared photocatalytic efficiency strongly relied on upconversion luminescence from the Re 3+ doped semiconductor in the heterojunction. By further modifying with CQDs, the CQDs/BiOF:Tm 3+ ,Yb 3+ /Bi 2 MoO 6 sample shows excellent visible and near-infrared photocatalytic performance, with 90% degradation of RhB occurring in the first 20 min under visible irradiation. This can be attributed to the large BET area, efficient photoinduced carrier separation and the upconversion process of the composite. This research will provide a systematic solution for realizing full-spectrum responsive and highly efficient photocatalysis by combination of rare earth ion doping, quantum dot modification and Z-scheme heterojunctions.