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Reaction-based small-molecule fluorescent probes for endoplasmic reticulum- and mitochondria-targeted biosensing and bioimaging 用于内质网和线粒体靶向生物传感和生物成像的反应型小分子荧光探针
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-17 DOI: 10.1007/s40843-024-3097-4
Abdul Hadi Mehmood  (, ), Faiz Ullah  (, ), Baoli Dong  (, ), Hong Liu  (, )

Fluorescent probes have revolutionized modern biological research by making it possible to observe and measure an extensive range of cellular and subcellular processes. Among the subcellular compartments, the endoplasmic reticulum (ER) and mitochondria (MT) remain exciting targets owing to the information they reveal about the cellular processes. Consequently, monitoring pH, polarity, viscosity, metal ions, reactive nitrogen species (RNS), reactive sulfur species (RSS) and reactive oxygen species (ROS) in ER and MT with fluorescent probes is of great importance to understand the cellar and subcellular process. Recent years, redox-sensitive probes and ion probes are designed and synthesized for the detection and quantification of RNS/RSS/ROS (collectively as reactive oxygen/nitrogen/sulfur species, RONSS) and metal ions within ER and MT. These probes provide powerful tools for the researchers to learn more about the complex relationship between cellular redox homeostasis and organelle function, and understand the mechanism of disease processes and pathogenesis for developing potential treatments. In this review, the design principles, synthesis methods, targeting mechanism for ER- and MT-targeted RONSS, and metal-ion-specific fluorescent probes are discussed. The recent progress for the synthesis and applications of ER/MT-targeted probes, and their applications for monitoring cellular and subcellular processes are summarized, and the development trends and application prospects of the probes are analyzed.

荧光探针使观察和测量广泛的细胞和亚细胞过程成为可能,从而彻底改变了现代生物学研究。在亚细胞区室中,内质网(ER)和线粒体(MT)仍然是令人兴奋的目标,因为它们揭示了有关细胞过程的信息。因此,利用荧光探针监测内质网和线粒体中的 pH 值、极性、粘度、金属离子、活性氮物种(RNS)、活性硫物种(RSS)和活性氧物种(ROS)对了解细胞和亚细胞过程具有重要意义。近年来,人们设计和合成了氧化还原敏感探针和离子探针,用于检测和定量ER和MT中的RNS/RSS/ROS(统称为活性氧/氮/硫物种,RONSS)和金属离子。这些探针为研究人员了解细胞氧化还原平衡与细胞器功能之间的复杂关系、理解疾病过程和发病机制以开发潜在治疗方法提供了有力工具。本综述讨论了 ER 和 MT 靶向 RONSS 以及金属离子特异性荧光探针的设计原理、合成方法、靶向机制。总结了ER/MT靶向探针的合成和应用的最新进展,以及它们在监测细胞和亚细胞过程中的应用,并分析了探针的发展趋势和应用前景。
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引用次数: 0
Promising graphdiyne-based nanomaterials for environmental pollutant control 用于控制环境污染物的前景看好的石墨二炔基纳米材料
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-16 DOI: 10.1007/s40843-024-3004-5
Chuanqi Pan  (, ), Qianli He  (, ), Chaofan Li  (, )

Environmental pollutants, including gas phase pollutants, liquid organic pollutants, heavy metal ions, and pathogenic bacteria, pose a serious threat to our ecological environment and human health. Effectively addressing these pollutants has become one of the most urgent issues. Graphdiyne (GDY), as an emerging carbon material for environmental remediation, has unique acetylene bonds and abundant pore structures. The unique carbon atomic structure of sp/sp2 hybrid endows it with tunable electronic structure and outstanding physical and chemical properties. This review summarizes the practical applications of GDY-based nanomaterials in the context of environmental pollution control, including carbon monoxide (CO) oxidation, ozone (O3) decomposition, heavy metal ion detection and adsorption, organic pollutant degradation, and bacterial inactivation. Furthermore, the structure-performance relationship of GDY-based nanomaterials is analyzed, and the issues and challenges in the field of environmental remediation of GDY-based materials are indicated.

环境污染物,包括气相污染物、液态有机污染物、重金属离子和致病细菌,对我们的生态环境和人类健康构成了严重威胁。有效解决这些污染物已成为最紧迫的问题之一。Graphdiyne(GDY)作为一种新兴的环境修复碳材料,具有独特的乙炔键和丰富的孔隙结构。sp/sp2杂化的独特碳原子结构使其具有可调的电子结构和出色的物理化学性能。本综述总结了基于 GDY 的纳米材料在环境污染控制方面的实际应用,包括一氧化碳(CO)氧化、臭氧(O3)分解、重金属离子检测和吸附、有机污染物降解和细菌灭活。此外,还分析了 GDY 基纳米材料的结构性能关系,并指出了 GDY 基材料在环境修复领域面临的问题和挑战。
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引用次数: 0
Hydrogen embrittlement of retrogression-reaged 7xxx-series aluminum alloys—a comprehensive review 逆行时效 7xxx 系列铝合金的氢脆--综合评述
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-12 DOI: 10.1007/s40843-024-3096-0
Mohamed Qassem, Amir Ershad Fanaei, Mousa Javidani

Hydrogen embrittlement remains a crucial concern in industries that rely on high-strength materials. Exposure to hydrogen poses a significant threat to the mechanical integrity of such materials. This review article briefly discusses the fundamentals of hydrogen embrittlement, including its mechanisms and the effects of various factors, such as chemical composition and environmental conditions. Several heat treatments have been developed to eliminate the risk of hydrogen embrittlement. Among various suggested heat treatments, the retrogression-reaging (RRA) treatment has proven effective in optimizing the balance between mechanical properties and resistance to hydrogen embrittlement. This review highlights the role of RRA treatment in modifying the microstructure of Al-Zn-Mg alloys to enhance their ability to resist hydrogen embrittlement, building on existing literature. An interesting aspect explored in this article is the intricate relationship between pre-deformation and subsequent RRA treatment. Additionally, the review discusses the use of RRA as a post-weld heat treatment to mitigate the susceptibility of weldments to hydrogen embrittlement. A comprehensive exploration of these topics is beneficial for a thorough understanding of the multifaceted functions of RRA treatment. However, despite its advantages, the widespread adoption of RRA treatment in the industry is hindered by certain challenges. This review addresses these challenges, offering insights into the latest strategies to overcome them.

在依赖高强度材料的行业中,氢脆仍然是一个重要问题。暴露在氢气中会对此类材料的机械完整性造成严重威胁。这篇综述文章简要讨论了氢脆的基本原理,包括其机理以及化学成分和环境条件等各种因素的影响。为消除氢脆风险,已开发出几种热处理方法。在各种建议的热处理方法中,逆行-时效(RRA)处理已被证明能有效优化机械性能和抗氢脆性能之间的平衡。本综述以现有文献为基础,重点介绍了 RRA 处理在改变铝-锌-镁合金微观结构以增强其抗氢脆能力方面的作用。本文探讨的一个有趣方面是预变形与后续 RRA 处理之间的复杂关系。此外,综述还讨论了使用 RRA 作为焊后热处理来减轻焊接件对氢脆的敏感性。对这些主题的全面探讨有助于深入了解 RRA 处理的多方面功能。然而,尽管 RRA 处理具有诸多优势,但其在行业中的广泛应用却受到某些挑战的阻碍。本综述探讨了这些挑战,并就克服这些挑战的最新战略提出了见解。
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引用次数: 0
Supramolecular glass: a new platform for ultralong phosphorescence 超分子玻璃:超长磷光新平台
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-11 DOI: 10.1007/s40843-024-3119-5
Fei Nie, Dongpeng Yan
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引用次数: 0
Simultaneously achieving high sensitivity, low dark current and low detection limits in anti-perovskites towards X-ray detection 同时实现高灵敏度、低暗电流和低探测极限的反超视蛋白,用于 X 射线探测
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-29 DOI: 10.1007/s40843-024-3125-y
Haixing Meng, Ying Li
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引用次数: 0
Stabilizing oxygen redox reaction in phase-transition-free P2-type Co/Ni-free cathode via Cu doping for sodium-ion batteries 通过掺杂铜稳定钠离子电池中无相变 P2- 型 Co/Ni 无正极中的氧氧化还原反应
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-26 DOI: 10.1007/s40843-024-3081-9
Hai-Xia Zhang  (, ), Lin-Rong Wu  (, ), Hao-Rui Wang  (, ), Dong-Zheng Wu  (, ), Shao-Hui Guo  (, ), Ding Zhang  (, ), Xiao-Chuan Duan  (, ), Xian-Ming Zhang  (, )

Due to their high capacity, the P2-type layered oxide cathodes containing oxygen redox reaction processes have attracted wide attention for sodium-ion batteries. However, these materials usually exhibit poor electro- chemical properties, resulting from irreversible oxygen redox reactions and phase transition processes at high voltages, and thus hinder their large-scale application. This work reveals the mechanism for the significantly improved cycle stability and rate performance of Co/Ni-free Na0.75Li0.25−2/3xCuxMn0.75−1/3x O2 via Cu doping. Ex-situ XPS demonstrates that Cu doping reduces the amount of Mn3+ that triggers the Jahn-Teller effect during the cycling. In addition, the electron enrichment of oxygen around Cu can alleviate the irreversible oxidation of oxygen, and thus suppressing the phase transition originates from the rapid weakening of the electrostatic repulsion between O-O. Meanwhile, in-situ XRD results verify that the Na0.75Li0.19Cu0.09Mn0.72O2 maintains the P2 phase structure during charging and discharging, resulting in a near-zero strain characteristic of 1.9%. Therefore, the optimized cathode delivers a high reversible capacity of 194.9 mAh g−1 at 0.1 C and excellent capacity retention of 88.6% after 100 cycles at 5 C. The full cell paired with commercial hard carbon anode delivers energy density of 240 Wh kg−1. Our research provides an idea for designing a new type of intercalated cathode for sodium-ion batteries with low cost and high energy density.

由于具有高容量,含有氧氧化还原反应过程的 P2- 型层状氧化物阴极在钠离子电池中受到广泛关注。然而,由于高电压下不可逆的氧氧化还原反应和相变过程,这些材料通常表现出较差的电化学性能,从而阻碍了它们的大规模应用。这项研究揭示了通过掺杂铜使无钴/无镍 Na0.75Li0.25-2/3xCuxMn0.75-1/3x O2 的循环稳定性和速率性能显著提高的机理。原位 XPS 显示,掺入 Cu 可减少循环过程中引发 Jahn-Teller 效应的 Mn3+ 量。此外,Cu 周围氧的电子富集可以减轻氧的不可逆氧化,从而抑制了源自 O-O 之间静电排斥力迅速减弱的相变。同时,原位 XRD 结果证实,Na0.75Li0.19Cu0.09Mn0.72O2 在充放电过程中保持了 P2 相结构,从而产生了 1.9% 的近零应变特性。因此,优化后的阴极在 0.1 C 时的可逆容量高达 194.9 mAh g-1,在 5 C 下循环 100 次后的容量保持率为 88.6%。我们的研究为设计低成本、高能量密度的新型钠离子电池插层阴极提供了思路。
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引用次数: 0
Adenosine triphosphate-responsive carbon dots nanoreactors for T1-weighted magnetic resonance imaging-guided tumor chemodynamic therapy 用于 T1 加权磁共振成像引导的肿瘤化学动力疗法的三磷酸腺苷响应型碳点纳米反应器
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-25 DOI: 10.1007/s40843-024-3038-8
Fuchun Nan  (, ), Xiaokuang Xue  (, ), Jian Li  (, ), Ke Liang  (, ), Jian Wang  (, ), William W. Yu  (, ), Jiechao Ge  (, ), Pengfei Wang  (, )

There are various strategies to conduct tumor microenvironment (TME) stimulus-responsive (e.g., acid, H2O2 or glutathione) nanoreactors for increasing the efficiency of chemodynamic therapy (CDT). Among these, the exploitation of adenosine triphosphate (ATP, another over-expressed biomarker in TME)-responsive nanoreactors for tumor CDT is still challenging. Herein, the ATP-responsive iron-doped CDs (FeCDs) were firstly prepared and then co-assembled with glucose oxidase (GOx) to obtain FeCDs/GOx liposomes as ATP-responsive nanoreactors. Under TME conditions, the nanoreactors initially released FeCDs and GOx. Subsequently, with the existence of ATP, iron ions were rapidly released from the FeCDs to trigger Fenton/Fenton-like reactions for generating ·OH. Meanwhile, the T1-weighted magnetic resonance imaging (MRI) was achieved due to the released iron ions. Moreover, the GOx converted endogenous glucose in tumor to gluconic acid and H2O2 to satisfy the requirement of ·OH generation. In vitro as well as in vivo experiments illustrated that the obtained ATP-responsive CD nanoreactors could be used as a versatile nanotheranostics for simultaneously T1-weighted MRI-guided tumor CDT. This work presents a new ATP-responsive nanoreactor with self-supplied H2O2 for multifunctional nanotheranostic applications.

为提高化学动力疗法(CDT)的效率,有多种策略来开发肿瘤微环境(TME)刺激响应型(如酸、H2O2 或谷胱甘肽)纳米反应器。其中,利用三磷酸腺苷(ATP,TME中另一种过度表达的生物标志物)响应型纳米反应器进行肿瘤化学动力学治疗仍具有挑战性。本文首先制备了ATP响应的掺铁CDs(FeCDs),然后与葡萄糖氧化酶(GOx)共同组装得到FeCDs/GOx脂质体作为ATP响应的纳米反应器。在 TME 条件下,纳米反应器最初释放出 FeCDs 和 GOx。随后,随着 ATP 的存在,铁离子迅速从 FeCDs 中释放出来,引发 Fenton/Fenton 类反应,生成 -OH。同时,由于铁离子的释放,T1 加权磁共振成像(MRI)得以实现。此外,GOx 还能将肿瘤中的内源性葡萄糖转化为葡萄糖酸和 H2O2,从而满足产生 -OH 的要求。体外和体内实验表明,所获得的 ATP 响应型 CD 纳米反应器可作为一种多功能纳米otheranostics,同时用于 T1 加权磁共振成像引导的肿瘤 CDT。这项工作提出了一种新的 ATP 响应型纳米反应器,它具有自我供应 H2O2 的功能,可用于多功能纳米otheranostic 应用。
{"title":"Adenosine triphosphate-responsive carbon dots nanoreactors for T1-weighted magnetic resonance imaging-guided tumor chemodynamic therapy","authors":"Fuchun Nan \u0000 (,&nbsp;),&nbsp;Xiaokuang Xue \u0000 (,&nbsp;),&nbsp;Jian Li \u0000 (,&nbsp;),&nbsp;Ke Liang \u0000 (,&nbsp;),&nbsp;Jian Wang \u0000 (,&nbsp;),&nbsp;William W. Yu \u0000 (,&nbsp;),&nbsp;Jiechao Ge \u0000 (,&nbsp;),&nbsp;Pengfei Wang \u0000 (,&nbsp;)","doi":"10.1007/s40843-024-3038-8","DOIUrl":"10.1007/s40843-024-3038-8","url":null,"abstract":"<div><p>There are various strategies to conduct tumor microenvironment (TME) stimulus-responsive (e.g., acid, H<sub>2</sub>O<sub>2</sub> or glutathione) nanoreactors for increasing the efficiency of chemodynamic therapy (CDT). Among these, the exploitation of adenosine triphosphate (ATP, another over-expressed biomarker in TME)-responsive nanoreactors for tumor CDT is still challenging. Herein, the ATP-responsive iron-doped CDs (FeCDs) were firstly prepared and then co-assembled with glucose oxidase (GOx) to obtain FeCDs/GOx liposomes as ATP-responsive nanoreactors. Under TME conditions, the nanoreactors initially released FeCDs and GOx. Subsequently, with the existence of ATP, iron ions were rapidly released from the FeCDs to trigger Fenton/Fenton-like reactions for generating ·OH. Meanwhile, the <i>T</i><sub>1</sub>-weighted magnetic resonance imaging (MRI) was achieved due to the released iron ions. Moreover, the GOx converted endogenous glucose in tumor to gluconic acid and H<sub>2</sub>O<sub>2</sub> to satisfy the requirement of ·OH generation. <i>In vitro</i> as well as <i>in vivo</i> experiments illustrated that the obtained ATP-responsive CD nanoreactors could be used as a versatile nanotheranostics for simultaneously <i>T</i><sub>1</sub>-weighted MRI-guided tumor CDT. This work presents a new ATP-responsive nanoreactor with self-supplied H<sub>2</sub>O<sub>2</sub> for multifunctional nanotheranostic applications.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3742 - 3752"},"PeriodicalIF":6.8,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A portable and washable solar steam evaporator based on graphene and recycled gold for efficient point-of-use water purification 基于石墨烯和回收金的便携式可清洗太阳能蒸汽蒸发器,用于高效的使用点水净化
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-24 DOI: 10.1007/s40843-024-3089-2
Fei Li  (, ), Jiongpeng Huang  (, ), Dingxin Xu  (, ), Chengjin Wang  (, ), Liang Zhao  (, ), Xinyu Gong  (, ), Hang Li  (, ), Can Yang Zhang  (, ), Qinghua Song  (, ), Yang Su  (, ), Hui-Ming Cheng  (, )

A solar steam evaporator provides a sustainable and efficient alternative water purification solution to address the global freshwater shortage. Previous efforts have made significant advances in maximizing its water evaporation rate, but no single evaporator has all the properties necessary for practical point-of-use application, including a high efficiency for generation of drinkable water, an excellent portability critical for on-site water purification, good washability for mitigating evaporator fouling, and good reusability. We report a strategy to produce a high-performance photothermal material for point-of-use water purification. By simultaneously incorporating graphene and gold particles grown from recycled electronic waste in a mechanically strong sponge, we achieved highly efficient water purification under realistic conditions. In addition to a high evaporation rate (3.55 kg/m2/h under one-sun irradiation) attributed to a control of atomic structure of graphene and the size-dependent surface plasmon resonance of gold nanoparticles, it is portable which can be folded, vacuum compacted, dried and rehydrated without compromising performance. It also allows repeated washing to remove contaminant fouling so that it can be reused. The evaporator transforms various types of contaminated water into drinkable clean water, and can be mounted at any angle to optimize the incident solar irradiation. Furthermore, the assembled steam evaporator device could gain purified water meeting the World Health Organization drinking water standards with a high evaporation rate of 9.36 kg/m2/h under outdoor sunlight.

太阳能蒸汽蒸发器为解决全球淡水短缺问题提供了一种可持续的高效替代水净化解决方案。以往的研究在最大限度地提高水蒸发率方面取得了重大进展,但没有一种蒸发器具备实际使用点应用所需的所有特性,包括生成饮用水的高效率、对现场水净化至关重要的出色便携性、减轻蒸发器结垢的良好可清洗性以及良好的可重复使用性。我们报告了一种生产用于使用点水净化的高性能光热材料的策略。通过将石墨烯和从回收的电子废料中生长出来的金颗粒同时加入机械强度高的海绵中,我们在现实条件下实现了高效的水净化。除了石墨烯原子结构的控制和金纳米粒子尺寸相关的表面等离子体共振所带来的高蒸发率(一太阳照射下为 3.55 kg/m2/h)之外,它还具有便携性,可以折叠、真空压缩、干燥和再水化,而不会影响其性能。它还可以反复清洗,清除污染物污垢,以便重复使用。蒸发器可将各种受污染的水转化为可饮用的清洁水,并可安装在任何角度,以优化入射太阳辐照。此外,组装好的蒸汽蒸发器装置在室外阳光照射下可获得符合世界卫生组织饮用水标准的纯净水,蒸发率高达 9.36 公斤/平方米/小时。
{"title":"A portable and washable solar steam evaporator based on graphene and recycled gold for efficient point-of-use water purification","authors":"Fei Li \u0000 (,&nbsp;),&nbsp;Jiongpeng Huang \u0000 (,&nbsp;),&nbsp;Dingxin Xu \u0000 (,&nbsp;),&nbsp;Chengjin Wang \u0000 (,&nbsp;),&nbsp;Liang Zhao \u0000 (,&nbsp;),&nbsp;Xinyu Gong \u0000 (,&nbsp;),&nbsp;Hang Li \u0000 (,&nbsp;),&nbsp;Can Yang Zhang \u0000 (,&nbsp;),&nbsp;Qinghua Song \u0000 (,&nbsp;),&nbsp;Yang Su \u0000 (,&nbsp;),&nbsp;Hui-Ming Cheng \u0000 (,&nbsp;)","doi":"10.1007/s40843-024-3089-2","DOIUrl":"10.1007/s40843-024-3089-2","url":null,"abstract":"<div><p>A solar steam evaporator provides a sustainable and efficient alternative water purification solution to address the global freshwater shortage. Previous efforts have made significant advances in maximizing its water evaporation rate, but no single evaporator has all the properties necessary for practical point-of-use application, including a high efficiency for generation of drinkable water, an excellent portability critical for on-site water purification, good washability for mitigating evaporator fouling, and good reusability. We report a strategy to produce a high-performance photothermal material for point-of-use water purification. By simultaneously incorporating graphene and gold particles grown from recycled electronic waste in a mechanically strong sponge, we achieved highly efficient water purification under realistic conditions. In addition to a high evaporation rate (3.55 kg/m<sup>2</sup>/h under one-sun irradiation) attributed to a control of atomic structure of graphene and the size-dependent surface plasmon resonance of gold nanoparticles, it is portable which can be folded, vacuum compacted, dried and rehydrated without compromising performance. It also allows repeated washing to remove contaminant fouling so that it can be reused. The evaporator transforms various types of contaminated water into drinkable clean water, and can be mounted at any angle to optimize the incident solar irradiation. Furthermore, the assembled steam evaporator device could gain purified water meeting the World Health Organization drinking water standards with a high evaporation rate of 9.36 kg/m<sup>2</sup>/h under outdoor sunlight.</p></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"67 11","pages":"3700 - 3709"},"PeriodicalIF":6.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrocatalytic conversion of CO2 to CH4 over Cu-based cluster via atomically precise local environment modulation 通过原子级精确局部环境调制,在铜基团簇上实现二氧化碳到甲烷的电催化转化
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-24 DOI: 10.1007/s40843-024-3088-5
Li Shi  (, ), Hanbo Wu  (, ), Wendi Xu  (, ), Wei Fu  (, ), Xiaobing Wang  (, ), Zhengyu Gu  (, ), Xiuyun Zhang  (, ), Jianyu Chen  (, ), Yanwen Ma  (, ), Jin Zhao  (, )

The development of low-cost, high-performance catalysts at the atomic scale has become a challenging issue for the large-scale applications of renewable clean energy technologies. Herein, on the basis of density functional theory calculation, we systematically investigate the effect of the local environment on the activity and selectivity of electrochemical carbon dioxide reduction reaction over single/multi-atom alloy clusters formed by the transition metal (Fe, Co, and Ni)-doped Cu13/55 clusters. Our findings reveal that the catalytic performance of multi-atom alloy clusters far exceeds that of Cu (211) surface. Notably, the Co666 configuration exhibits exceptional performance with a remarkably low free energy barrier of just 0.33 eV. Furthermore, our investigations demonstrate that catalytic performance is predominantly determined by the relative proportion of modifying metallic dopant species that generate a coordination number of 6. This ratio principally influences the adsorption strength of key intermediates (HCOO* and H2COO*). Bader charge analyses and free energy calculations elucidate a new mechanistic pathway, wherein the hydrogenation of CO2 at C-sites catalyzes the reduction of CO2 to CH4. This theoretical research provides valuable insights into the fundamental processes and energy landscapes involved in converting CO2 to CH4 on the studied catalytic structure, potentially paving the way for more efficient and sustainable carbon dioxide utilization strategies.

开发低成本、高性能的原子尺度催化剂已成为可再生清洁能源技术大规模应用的挑战性课题。在此,我们在密度泛函理论计算的基础上,系统研究了局部环境对过渡金属(Fe、Co 和 Ni)掺杂 Cu13/55 簇形成的单/多原子合金簇电化学二氧化碳还原反应活性和选择性的影响。我们的研究结果表明,多原子合金团簇的催化性能远远超过了 Cu (211) 表面。值得注意的是,Co666 构型表现出卓越的性能,其自由能垒非常低,仅为 0.33 eV。此外,我们的研究还表明,催化性能主要取决于产生 6 配位数的改性金属掺杂物的相对比例,这一比例主要影响关键中间产物(HCOO* 和 H2COO*)的吸附强度。巴德尔电荷分析和自由能计算阐明了一种新的机理途径,即 C 位上的 CO2 加氢催化 CO2 还原成 CH4。这项理论研究为了解在所研究的催化结构上将 CO2 转化为 CH4 所涉及的基本过程和能量景观提供了宝贵的见解,有可能为制定更高效、更可持续的二氧化碳利用战略铺平道路。
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引用次数: 0
Effective exciplex system with high emission efficiency via intramolecular hydrogen bonding for efficient solution processable OLEDs 通过分子内氢键实现高发射效率的有效赋形剂系统,可用于高效溶液加工型有机发光二极管
IF 6.8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-20 DOI: 10.1007/s40843-024-3067-x
Xiaoyi Lai  (, ), Junqing Wang  (, ), Xiaolong Liu  (, ), Lei Hua  (, ), Bin Li  (, ), Weiguo Zhu  (, ), Jun Yeob Lee, Yafei Wang  (, )

Exciplex system is a charming candidate for thermally activated delayed fluorescence (TADF) due to its intrinsic small energy difference between the lowest singlet state and triplet excited state (ΔEST). However, high emission efficiency and fast radiative decay rate are still a formidable task for the exciplex emission. Herein two novel tri(triazolo) triazine-based TADF emitters, named TTT-HPh-Ac and TTT-MePh-Ac, are synthesized and characterized. Using such TADF emitters as the donor molecule and (1,3,5-triazine-2,4,6-triyl)tris(benzene-3,1-dial)tris(diphenylphosphine oxide) (PO-T2T) as the acceptor molecule, the exciplex system of TTT-HPh-Ac:PO-T2T and TTT-MePh-Ac:PO-T2T are prepared, which show a tiny ΔEST of 40 ± 20 meV and fast reverse intersystem crossing rate. As a result, very high emission efficiency (97%) and a small non-radiative decay rate are detected for the exciplex TADF system. The solution processable organic light-emitting diode using the exciplex system as the emitter achieves a maximum external quantum efficiency (EQEmax) of 17.0%. When using the exciplex as the host matrix, the TTT-MePh-Ac:PO-T2T based solution processable device shows a better performance with an EQEmax of 20% with a very small efficiency roll-off of 6% at 1000 cd m−2. This work proves that the molecule with both intramolecular hydrogen bonding and proper twisted molecular geometry in exciplex is more favorable to enhance its emission efficiency and suppress the non-radiative transition, which provides a new way to develop efficient and stable exciplex emitters.

由于最低单态和三重激发态之间的固有能差(ΔEST)较小,赋形剂系统是热激活延迟荧光(TADF)的迷人候选者。然而,高发射效率和快速辐射衰减率仍然是复合物发射的艰巨任务。本文合成并表征了两种新型三(三唑并)三嗪基 TADF 发射器,分别命名为 TTT-HPh-Ac 和 TTT-MePh-Ac。以这种 TADF 发射体为供体分子,以(1,3,5-三嗪-2,4,6-三基)三(苯-3,1-二)三(二苯基氧化膦)(PO-T2T)为受体分子,制备了 TTT-HPh-Ac:PO-T2T 和 TTT-MePh-Ac:PO-T2T 的复合物体系。因此,检测到该复合物 TADF 系统具有极高的发射效率(97%)和较小的非辐射衰减率。使用该赋形剂系统作为发射器的可溶液加工有机发光二极管的最大外部量子效率(EQEmax)为 17.0%。当使用赋形剂作为主基质时,基于 TTT-MePh-Ac:PO-T2T 的可溶液加工器件显示出更好的性能,在 1000 cd m-2 时,EQEmax 为 20%,效率衰减非常小,仅为 6%。这项工作证明,在赋形剂中同时具有分子内氢键和适当扭曲分子几何形状的分子更有利于提高其发射效率和抑制非辐射转变,这为开发高效稳定的赋形剂发射器提供了一条新途径。
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引用次数: 0
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