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Efficient propane dehydrogenation catalyzed by Ru nanoparticles anchored on a porous nitrogen-doped carbon matrix 锚定在多孔掺氮碳基体上的 Ru 纳米粒子催化的高效丙烷脱氢反应
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-11 DOI: 10.1016/j.cclet.2024.110444
Tianyi Yang , Fangxi Su , Dehuan Shi , Shenghong Zhong , Yalin Guo , Zhaohui Liu , Jianfeng Huang
Propane dehydrogenation (PDH) is a vital industrial process for producing propene, utilizing primarily Cr-based or Pt-based catalysts. These catalysts often suffer from challenges such as the toxicity of Cr, the high costs of noble metals like Pt, and deactivation issues due to sintering or coke formation at elevated temperatures. We introduce an exceptional Ru-based catalyst, Ru nanoparticles anchored on a nitrogen-doped carbon matrix (Ru@NC), which achieves a propane conversion rate of 32.2 % and a propene selectivity of 93.1 % at 550 °C, with minimal coke deposition and a low deactivation rate of 0.0065 h−1. Characterizations using techniques like TEM and XPS, along with carefully-designed controlled experiments, reveal that the notable performance of Ru@NC stems from the modified electronic state of Ru by nitrogen dopant and the microporous nature of the matrix, positioning it as a top contender among state-of-the-art PDH catalysts.
丙烷脱氢(PDH)是生产丙烯的重要工业工艺,主要使用铬基或铂基催化剂。这些催化剂经常面临各种挑战,例如铬的毒性、铂等贵金属的高成本以及在高温下烧结或形成焦炭导致的失活问题。我们介绍了一种特殊的 Ru 基催化剂--锚定在掺氮碳基体上的 Ru 纳米颗粒(Ru@NC),它在 550 °C 时的丙烷转化率达到 32.2%,丙烯选择性达到 93.1%,同时焦炭沉积极少,失活率低至 0.0065 h-1。利用 TEM 和 XPS 等技术进行的表征以及精心设计的对照实验表明,Ru@NC 的显著性能源于氮掺杂改变了 Ru 的电子状态以及基质的微孔性质,使其成为最先进的 PDH 催化剂中的佼佼者。
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引用次数: 0
Additive regulating Li+ solvation structure to construct dual LiF−rich electrode electrolyte interphases for sustaining 4.6 V Li||LiCoO2 batteries 通过添加剂调节 Li+ 溶解结构,构建富含 LiF 的双电极电解质相间层,用于维持 4.6 V Li||LiCoO2 电池的电压
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-11 DOI: 10.1016/j.cclet.2024.110014
Xi Tang , Chunlei Zhu , Yulu Yang , Shihan Qi , Mengqiu Cai , Abdullah N. Alodhayb , Jianmin Ma

The battery energy density can be improved by raising the operating voltage, however, which may lead to rapid capacity decay due to the continuous electrolyte decomposition and the thickening of electrode electrolyte interphases. To address these challenges, we proposed tripropyl phosphate (TPP) as an additive−regulating Li+ solvation structure to construct a stable LiF–rich electrode carbonate−based electrolyte interphases for sustaining 4.6 V Li||LiCoO2 batteries. This optimized interphases could help reduce the resistance and achieve better rate performance and cycling stability. As expected, the Li||LiCoO2 battery retained 79.4 % capacity after 100 cycles at 0.5 C, while the Li||Li symmetric cell also kept a stable plating/stripping process over 450 h at the current density of 1.0 mA/cm2 with a deposited amount of 0.5 mAh/cm2.

然而,通过提高工作电压可以提高电池的能量密度,但由于电解质的持续分解和电极电解质相间层的增厚,这可能会导致容量的快速衰减。为了应对这些挑战,我们提出了磷酸三丙酯(TPP)作为添加剂来调节 Li+ 溶解结构,以构建稳定的富含 LiF 的电极碳酸盐电解质相间层,用于维持 4.6 V 锂||钴酸锂电池。这种优化的中间相有助于降低电阻,实现更好的速率性能和循环稳定性。正如预期的那样,在 0.5 摄氏度条件下循环 100 次后,钴酸锂电池的容量保持在 79.4%,而在电流密度为 1.0 mA/cm2 且沉积量为 0.5 mAh/cm2 的条件下,锂离子对称电池也能在 450 小时内保持稳定的电镀/剥离过程。
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引用次数: 0
Elucidating oxygen evolution and reduction mechanisms in nitrogen-doped carbon-based photocatalysts 阐明掺氮碳基光催化剂中的氧进化和还原机制
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1016/j.cclet.2024.110439
Yan Wang , Jiaqi Zhang , Xiaofeng Wu , Sibo Wang , Masakazu Anpo , Yuanxing Fang
Solar-induced water oxidation reaction (WOR) for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages. WOR is also associated with important reduction reactions, such as oxygen reduction reaction (ORR), which leads to the production of hydrogen peroxide (H2O2). These transitions are instrumental in the emergence and evolution of life. In this study, transition metals were loaded onto nitrogen-doped carbon (NDC) prepared under the primitive Earth's atmospheric conditions. These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination. The chemical pathways initiated by the pristine and metal-loaded NDC were investigated. This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.
太阳诱导的氧进化水氧化反应(WOR)是地球大气在原始阶段从还原型向氧化型转变的关键步骤。水氧化反应还与重要的还原反应有关,如氧还原反应(ORR),它导致产生过氧化氢(H2O2)。这些转变对生命的出现和进化至关重要。在这项研究中,过渡金属被负载到在原始地球大气条件下制备的掺氮碳 (NDC) 上。研究发现,这些负载金属的 NDC 样品在光照下可催化 WOR 和 ORR。研究了原始 NDC 和金属负载 NDC 引发的化学途径。这项研究为了解与我们星球早期演化相关的潜在机制提供了宝贵的见解。
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引用次数: 0
Application of titanium-based advanced oxidation processes in pesticide-contaminated water purification: Emerging opportunities and challenges
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1016/j.cclet.2024.110438
Chu Wu , Zhichao Dong , Jinfang Hou , Jian Peng , Shuangyu Wu , Xiaofang Wang , Xiangwei Kong , Yue Jiang
Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants (ECs) from water, surpassing the limitations of traditional methods. Environmental functional materials (EFMs), particularly high-end oxidation systems using eco-friendly nanomaterials, show promise for absorbing and degrading ECs. This literature review presents a comprehensive analysis of diverse traditional restoration techniques-biological, physical, and chemical-assessing their respective applications and limitations in pesticide-contaminated water purification. Through meticulous comparison, we unequivocally advocate for the imperative integration of environmentally benign nanomaterials, notably titanium-based variants, in forthcoming methodologies. Our in-depth exploration scrutinizes the catalytic efficacy, underlying mechanisms, and adaptability of pioneering titanium-based nanomaterials across a spectrum of environmental contexts. Additionally, strategic recommendations are furnished to surmount challenges and propel the frontiers of implementing eco-friendly nanomaterials in practical water treatment scenarios.
{"title":"Application of titanium-based advanced oxidation processes in pesticide-contaminated water purification: Emerging opportunities and challenges","authors":"Chu Wu ,&nbsp;Zhichao Dong ,&nbsp;Jinfang Hou ,&nbsp;Jian Peng ,&nbsp;Shuangyu Wu ,&nbsp;Xiaofang Wang ,&nbsp;Xiangwei Kong ,&nbsp;Yue Jiang","doi":"10.1016/j.cclet.2024.110438","DOIUrl":"10.1016/j.cclet.2024.110438","url":null,"abstract":"<div><div>Efficient and innovative nano-catalytic oxidation technologies offer a breakthrough in removing emerging contaminants (ECs) from water, surpassing the limitations of traditional methods. Environmental functional materials (EFMs), particularly high-end oxidation systems using eco-friendly nanomaterials, show promise for absorbing and degrading ECs. This literature review presents a comprehensive analysis of diverse traditional restoration techniques-biological, physical, and chemical-assessing their respective applications and limitations in pesticide-contaminated water purification. Through meticulous comparison, we unequivocally advocate for the imperative integration of environmentally benign nanomaterials, notably titanium-based variants, in forthcoming methodologies. Our in-depth exploration scrutinizes the catalytic efficacy, underlying mechanisms, and adaptability of pioneering titanium-based nanomaterials across a spectrum of environmental contexts. Additionally, strategic recommendations are furnished to surmount challenges and propel the frontiers of implementing eco-friendly nanomaterials in practical water treatment scenarios.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 3","pages":"Article 110438"},"PeriodicalIF":9.4,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143318381","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fe3+ ion quantification with reusable bioinspired nanopores 利用可重复使用的生物启发纳米孔量化 Fe3+ 离子
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1016/j.cclet.2024.110428
Yanqiong Wang , Yaqi Hou , Fengwei Huo , Xu Hou
Excessive Fe3+ ion concentrations in wastewater pose a long-standing threat to human health. Achieving low-cost, high-efficiency quantification of Fe3+ ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment processes. In this study, by leveraging the rapid, real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe3+, a linear relationship between the ion current and Fe3+ ion concentration was established. Utilizing this linear relationship, quantification of Fe3+ ion concentration in unknown solutions was achieved. Furthermore, ethylenediaminetetraacetic acid disodium salt was employed to displace Fe3+ from the nanopores, allowing them to be restored to their initial conditions and reused for Fe3+ ion quantification. The reusable bioinspired nanopores remain functional over 330 days of storage. This recycling capability and the long-term stability of the nanopores contribute to a significant reduction in costs. This study provides a strategy for the quantification of unknown Fe3+ concentration using nanopores, with potential applications in environmental assessment, health monitoring, and so forth.
废水中过量的 Fe3+ 离子浓度长期以来一直威胁着人类健康。对未知溶液中的 Fe3+ 离子浓度进行低成本、高效率的定量分析,可以为环境管理决策和优化水处理工艺提供指导。在本研究中,利用纳米孔的快速、实时检测能力以及单宁酸与 Fe3+ 的特异性化学结合亲和力,建立了离子电流与 Fe3+ 离子浓度之间的线性关系。利用这种线性关系,实现了对未知溶液中 Fe3+ 离子浓度的定量。此外,还利用乙二胺四乙酸二钠盐将 Fe3+ 从纳米孔中置换出来,使其恢复到初始状态并重新用于 Fe3+ 离子定量。可重复使用的生物启发纳米孔在储存 330 天后仍能保持功能。这种回收能力和纳米孔的长期稳定性大大降低了成本。这项研究提供了一种利用纳米孔量化未知 Fe3+ 浓度的策略,有望应用于环境评估、健康监测等领域。
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引用次数: 0
N-doped carbon confined ternary Pt2NiCo intermetallics for efficient oxygen reduction reaction
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1016/j.cclet.2024.110429
Chenhao Zhang , Qian Zhang , Yezhou Hu , Hanyu Hu , Junhao Yang , Chang Yang , Ye Zhu , Zhengkai Tu , Deli Wang
Developing high performance electrocatalysts for the cathodic oxygen reduction reaction (ORR) is essential for the widespread application of fuel cells. Herein, a promising Pt2NiCo atomic ordered ternary intermetallic compound with N-doped carbon layer coating (o-Pt2NiCo@NC) has been synthesized via a facile method and applied in acidic ORR. The confinement effect provided by the carbon layer not only inhibits the agglomeration and sintering of intermetallic nanoparticles during high temperature process but also provides adequate protection for the nanoparticles, mitigating the aggregation, detachment and poisoning of nanoparticles during the electrochemical process. As a result, the o-Pt2NiCo@NC demonstrates a mass activity (MA) and specific activity (SA) of 0.65 A/mgPt and 1.41 mA/cmPt2 in 0.1 mol/L HClO4, respectively. In addition, after 30,000 potential cycles from 0.6 V to 1.0 V, the MA of o-Pt2NiCo@NC shows much lower decrease than the disordered Pt2NiCo alloy and Pt/C. Even cycling at high potential cycles of 1.5 V for 10,000 cycles, the MA still retains ∼70 %, demonstrating superior long-term durability. Furthermore, the o-Pt2NiCo@NC also exhibits strong tolerance to CO, SOx, and POx molecules in toxicity tolerance tests. The strategy in this work provides a novel insight for the development of ORR catalysts with high catalytic activity, durability and toxicity tolerance.
{"title":"N-doped carbon confined ternary Pt2NiCo intermetallics for efficient oxygen reduction reaction","authors":"Chenhao Zhang ,&nbsp;Qian Zhang ,&nbsp;Yezhou Hu ,&nbsp;Hanyu Hu ,&nbsp;Junhao Yang ,&nbsp;Chang Yang ,&nbsp;Ye Zhu ,&nbsp;Zhengkai Tu ,&nbsp;Deli Wang","doi":"10.1016/j.cclet.2024.110429","DOIUrl":"10.1016/j.cclet.2024.110429","url":null,"abstract":"<div><div>Developing high performance electrocatalysts for the cathodic oxygen reduction reaction (ORR) is essential for the widespread application of fuel cells. Herein, a promising Pt<sub>2</sub>NiCo atomic ordered ternary intermetallic compound with N-doped carbon layer coating (<em>o</em>-Pt<sub>2</sub>NiCo@NC) has been synthesized <em>via</em> a facile method and applied in acidic ORR. The confinement effect provided by the carbon layer not only inhibits the agglomeration and sintering of intermetallic nanoparticles during high temperature process but also provides adequate protection for the nanoparticles, mitigating the aggregation, detachment and poisoning of nanoparticles during the electrochemical process. As a result, the <em>o</em>-Pt<sub>2</sub>NiCo@NC demonstrates a mass activity (MA) and specific activity (SA) of 0.65 A/mg<sub>Pt</sub> and 1.41 mA/cm<sub>Pt</sub><sup>2</sup> in 0.1 mol/L HClO<sub>4</sub>, respectively. In addition, after 30,000 potential cycles from 0.6 V to 1.0 V, the MA of <em>o</em>-Pt<sub>2</sub>NiCo@NC shows much lower decrease than the disordered Pt<sub>2</sub>NiCo alloy and Pt/C. Even cycling at high potential cycles of 1.5 V for 10,000 cycles, the MA still retains ∼70 %, demonstrating superior long-term durability. Furthermore, the <em>o</em>-Pt<sub>2</sub>NiCo@NC also exhibits strong tolerance to CO, SO<sub>x</sub>, and PO<sub>x</sub> molecules in toxicity tolerance tests. The strategy in this work provides a novel insight for the development of ORR catalysts with high catalytic activity, durability and toxicity tolerance.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 3","pages":"Article 110429"},"PeriodicalIF":9.4,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143318377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Coating colloidal particles with a well-defined polymer layer by surface-initiated photoinduced polymerization-induced self-assembly and the subsequent seeded polymerization 通过表面引发的光诱导聚合自组装和随后的种子聚合,为胶体颗粒涂上一层定义明确的聚合物层
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1016/j.cclet.2024.110431
Bing Niu , Honggao Huang , Liwei Luo , Li Zhang , Jianbo Tan
Core-shell colloidal particles with a polymer layer have broad applications in different areas. Herein, we developed a two-step method combining aqueous surface-initiated photoinduced polymerization-induced self-assembly and photoinduced seeded reversible addition-fragmentation chain transfer (RAFT) polymerization to prepare a diverse set of core-shell colloidal particles with a well-defined polymer layer. Chemical compositions, structures, and thicknesses of polymer layers could be conveniently regulated by using different types of monomers and feed [monomer]/[chain transfer agent] ratios during seeded RAFT polymerization.
带有聚合物层的核壳胶体粒子在不同领域有着广泛的应用。在此,我们开发了一种两步法,结合水表面诱导的光诱导聚合自组装和光诱导的种子可逆加成-碎片链转移(RAFT)聚合,制备出多种具有明确聚合物层的核壳胶体粒子。在种子可逆加成-链转移聚合过程中,通过使用不同类型的单体和进料[单体]/[链转移剂]比例,可以方便地调节聚合物层的化学成分、结构和厚度。
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引用次数: 0
Understanding excitonic behavior and electroluminescence light emitting diode application of carbon dots 了解碳点的激子行为和电致发光发光二极管的应用
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1016/j.cclet.2024.110426
Yuan Liu , Boyang Wang , Yaxin Li , Weidong Li , Siyu Lu
Carbon dots (CDs), due to their low cost, high stability, and high luminous efficiency, have emerged as an excellent material for the emissive layer in next-generation electroluminescent light-emitting diodes (ELEDs). However, improving the efficiency of fluorescent CDs-based ELEDs remains challenging, primarily because it is difficult to utilize triplet excitons in the electroluminescence process. Therefore, enhancing the exciton utilization efficiency of CDs during electroluminescence is crucial. Based on this, we exploited the characteristic large exciton binding energy commonly found in CDs to develop exciton-emitting CDs. These CDs facilitate the radiative recombination of excitons during electroluminescence, thereby improving the electroluminescent efficiency. By rationally selecting precursors, we developed high quantum efficiency CDs and subsequently constructed CDs-based ELEDs. The blue-light device exhibited an external quantum efficiency of over 4 %. This study introduces a novel design concept for CDs, providing a new strategy for developing high-performance blue ELEDs based on CDs.
碳点(CD)因其低成本、高稳定性和高发光效率,已成为下一代电致发光二极管(ELED)发光层的绝佳材料。然而,提高基于荧光光盘的电致发光二极管的效率仍然具有挑战性,这主要是因为在电致发光过程中很难利用三重激子。因此,提高 CD 在电致发光过程中的激子利用效率至关重要。在此基础上,我们利用光盘中常见的大激子结合能特性,开发出了激子发光光盘。这些光盘有助于激子在电致发光过程中进行辐射重组,从而提高电致发光效率。通过合理选择前驱体,我们开发出了高量子效率的光盘,并随后构建了基于光盘的电致发光器件。该蓝光器件的外部量子效率超过 4%。这项研究引入了一种新颖的光盘设计理念,为开发基于光盘的高性能蓝光发光二极管提供了一种新策略。
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引用次数: 0
Constriction-susceptible lithium support for fast cycling of solid-state lithium metal battery 用于固态锂金属电池快速循环的易收缩锂支持物
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-06 DOI: 10.1016/j.cclet.2024.110417
Dong Sui, Jiayi Liu
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引用次数: 0
Corrigendum to “Morphology controllable conjugated network polymers based on AIE-active building block for TNP detection” 基于 AIE 活性结构单元的形态可控共轭网络聚合物用于 TNP 检测 "的更正
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-05 DOI: 10.1016/j.cclet.2023.108998
Shan Jiang , Lingchen Meng , Wenyue Ma , Qingkai Qi , Wei Zhang , Bin Xu , Leijing Liu , Wenjing Tian
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引用次数: 0
期刊
Chinese Chemical Letters
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