Chinese Chemical Letters最新文献

英文中文

Structuring MoO3-polyoxometalate hybrid superstructures to boost electrocatalytic hydrogen evolution reaction 构建 MoO3-聚氧化金属酸盐混合超结构，促进电催化氢气进化反应

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-15 DOI: 10.1016/j.cclet.2024.110467

Bowen Li, Ting Wang, Ming Xu, Yuqi Wang, Zhaoxing Li, Mei Liu, Wenjing Zhang, Ming Feng

Improving the surface atoms utilization efficiency of catalysts is extremely important for large-scale H₂ production by electrochemical water splitting, but it remains a great challenge. Herein, we reported two kinds of MoO₃-polyoxometalate hybrid nanobelt superstructures (MoO₃-POM HNSs, POM = PW₁₂O₄₀ and SiW₁₂O₄₀) using a simple hydrothermal method. Such superstructure with highly uniform nanoparticles as building blocks can expose more surface atoms and emanate increased specific surface area. The incorporated POMs generated abundant oxygen vacancies, improved the electronic mobility, and modulated the surface electronic structure of MoO₃, allowing to optimize the H* adsorption/desorption and dehydrogenation kinetics of catalyst. Notably, the as-prepared MoO₃-PW₁₂O₄₀ HNSs electrodes not only displayed the low overpotentials of 108 mV at 10 mA/cm² current density in 0.5 mol/L H₂SO₄ electrolyte but also displayed excellent long-term stability. The hydrogen evolution reaction (HER) performance of MoO₃-POM superstructures is significantly better than that of corresponding bulk materials MoO₃@PW₁₂O₄₀ and MoO₃@SiW₁₂O₄₀, and the overpotentials are about 8.3 and 4.9 times lower than that of single MoO₃. This work opens an avenue for designing highly surface-exposed catalysts for electrocatalytic H₂ production and other electrochemical applications.

提高催化剂的表面原子利用效率对于电化学水分离大规模生产 H2 极其重要，但这仍然是一个巨大的挑战。在此，我们采用简单的水热法报道了两种 MoO3 聚氧化铝杂化纳米带上层结构（MoO3-POM HNSs，POM = PW12O40 和 SiW12O40）。这种以高度均匀的纳米颗粒为构件的超结构可以暴露出更多的表面原子，并增加比表面积。加入的 POM 产生了大量的氧空位，提高了电子迁移率，并调节了 MoO3 的表面电子结构，从而优化了催化剂的 H* 吸附/解吸和脱氢动力学。值得注意的是，制备的 MoO3-PW12O40 HNSs 电极不仅在 0.5 mol/L H2SO4 电解液中以 10 mA/cm2 的电流密度显示出 108 mV 的低过电位，而且显示出优异的长期稳定性。MoO3-POM 超结构的氢进化反应（HER）性能明显优于相应的块体材料 MoO3@PW12O40 和 MoO3@SiW12O40，其过电位分别是单一 MoO3 的 8.3 倍和 4.9 倍。这项工作为设计用于电催化制取 H2 及其他电化学应用的高表面暴露催化剂开辟了一条途径。

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引用次数: 0

EDA-complexes-enabled photochemical synthesis of α-amino acids with imines and tetrabutylammonium oxalate 用亚胺和草酸四丁基铵光化学合成α-氨基酸的 EDA 复合物

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-14 DOI: 10.1016/j.cclet.2024.110446

Min-Hang Zhou, Jun Jiang, Wei-Min He

引用次数: 0

Recent progress on non-metallic carbon nitride for the photosynthesis of H2O2: Mechanism, modification and in-situ applications 用于 H2O2 光合作用的非金属氮化碳的最新进展：机理、改性和原位应用

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-14 DOI: 10.1016/j.cclet.2024.110457

Hao Lv , Zhi Li , Peng Yin , Ping Wan , Mingshan Zhu

Photocatalytic hydrogen peroxide (H₂O₂) production has been considered as a promising strategy for H₂O₂ synthesis due to its environmentally friendly. Among various photocatalysts, carbon nitride-based materials are excellent candidates for H₂O₂ production because of their excellent visible-light response, low cost and high stability. In this review, we summarize in detail the research progress on the photocatalytic production of H₂O₂ by carbon nitride. First, we summarize the basic principles of photocatalysis and photocatalytic H₂O₂ production. Second, the classification and modification methods of carbon-nitride-based materials are discussed, including morphology modulation, noble metal loading, defect control, heterojunction regulation, molecular structure engineering and elemental doping. Finally, the different in-situ applications of H₂O₂ via photosynthesis were discussed, including disinfection and antibiotic resistant genes degradation, organic pollutants degradation, medical applications and fine chemical synthesis. This review brings great promise for in-situ H₂O₂ photosynthesis, which is expected to serve as a key component in future applications.

光催化过氧化氢（H2O2）生产因其对环境友好而被认为是一种有前途的 H2O2 合成策略。在各种光催化剂中，氮化碳基材料因其卓越的可见光响应、低成本和高稳定性而成为生产 H2O2 的最佳候选材料。在本综述中，我们将详细总结氮化碳光催化生产 H2O2 的研究进展。首先，我们总结了光催化和光催化产生 H2O2 的基本原理。其次，讨论了氮化碳基材料的分类和改性方法，包括形貌调控、贵金属负载、缺陷控制、异质结调控、分子结构工程和元素掺杂。最后，讨论了 H2O2 通过光合作用的不同原位应用，包括消毒和抗生素耐药基因降解、有机污染物降解、医疗应用和精细化学品合成。本综述为原位 H2O2 光合作用带来了巨大前景，有望成为未来应用的关键组成部分。

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引用次数: 0

Modular miniaturized synthesis and in situ biological evaluation facilitate rapid discovery of potent MraY inhibitors as antibacterial agents 模块化微型合成和原位生物评估有助于快速发现作为抗菌剂的强效 MraY 抑制剂

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-12 DOI: 10.1016/j.cclet.2024.110455

Mianling Yang , Meehyein Kim , Peng Zhan

引用次数: 0

A composite hydrogel with porous and homogeneous structure for efficient osmotic energy conversion 一种具有多孔均匀结构的复合水凝胶，可实现高效渗透能量转换

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-12 DOI: 10.1016/j.cclet.2024.110449

Guilong Li, Wenbo Ma, Jialing Zhou, Caiqin Wu, Chenling Yao, Huan Zeng, Jian Wang

With the impact of energy crisis and environmental problems, it is urgent to develop green sustainable energy. Osmotic energy stored in the salinity difference between seawater and river water is one of the sustainable, abundant, and renewable energy. However, the membranes used to capture osmotic energy by reverse electrodialysis (RED) always suffer from low ion selectivity, low stability and low power. Hydrogels with three-dimensional (3D) networks have shown great potential for ion transportation and energy conversion. In this work, based on the homogeneity and porosity characteristics of acrylamide (AM) hydrogel, as well as the remarkable stability and abundant negative charge of 3-sulfopropyl acrylate potassium salt (SPAK), a high-performance AM/SPAK cation-selective hydrogel membrane was successfully developed for harvesting osmotic energy. Compared to AM hydrogels, utilizing AM/SPAK as a monomer mixture greatly facilitated the preparation of homogeneous polymers, exhibiting a porous structure, exceptional ion selectivity, and remarkable stability. A maximum output power density of 13.73 W/m² was achieved at a 50-fold NaCl concentration gradient, exceeding the commercial requirement of 5 W/m². This work broadens the idea for the construction and application of composite hydrogel in high efficiency osmotic energy conversion.

在能源危机和环境问题的影响下，开发绿色可持续能源迫在眉睫。海水与河水的盐度差所储存的渗透能是一种可持续、丰富和可再生的能源。然而，利用反向电渗析（RED）捕获渗透能的膜总是存在离子选择性低、稳定性差和功率低的问题。具有三维（3D）网络的水凝胶在离子传输和能量转换方面显示出巨大的潜力。本研究基于丙烯酰胺（AM）水凝胶的均匀性和多孔性特点，以及丙烯酸 3-磺丙基钾盐（SPAK）的显著稳定性和丰富的负电荷，成功开发了一种用于收集渗透能的高性能 AM/SPAK 阳离子选择性水凝胶膜。与 AM 水凝胶相比，使用 AM/SPAK 作为单体混合物极大地促进了均质聚合物的制备，这种聚合物具有多孔结构、优异的离子选择性和出色的稳定性。在 NaCl 浓度梯度为 50 倍时，最大输出功率密度达到 13.73 W/m2，超过了 5 W/m2 的商业要求。这项研究拓宽了复合水凝胶在高效渗透能量转换中的构建和应用思路。

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引用次数: 0

Boron/phosphorus co-doped nitrogen-rich carbon nanofiber with flexible anode for robust sodium-ion battery 具有柔性阳极的硼/磷共掺富氮碳纳米纤维，可用于制造坚固耐用的钠离子电池

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-12 DOI: 10.1016/j.cclet.2024.110452

Jiaojiao Liang , Youming Peng , Zhichao Xu , Yufei Wang , Menglong Liu , Xin Liu , Di Huang , Yuehua Wei , Zengxi Wei

Flexible energy storage devices have been paid much attention and adapts to apply in various fields. Benefiting from the active sites of boron (B) and phosphorus (P) doping materials, co-doped carbon materials are widely used in energy storage devices for the enhanced electrochemical performance. Herein, B and P co-doped flexible carbon nanofibers with nitrogen-rich (B-P/NC) are investigated with electrospinning for sodium-ion battery. The flexible of binderless B-P/NC with annealing of 600 °C (B-P/NC-600) exhibits the remarkable performance for the robust capacity of 200 mAh/g at 0.1 A/g after 500 cycles and a durable reversible capacity of 160 mAh/g even at 1 A/g after 12,000 cycles, exhibiting the equally commendable stability of flexible B-P/NC-600. In addition, B-P/NC-600 delivers the reversible capacity of 265 mAh/g with the test temperature of 60 °C. More importantly, the flexible B-P/NC-600 is fabricated as anode for the whole battery, delivering the capacity of 90 mAh/g at 1 A/g after 200 cycles. Meanwhile, theoretical calculation further verified that boron and phosphorus co-doping can improve the adsorption capacity of nitrogen carbon materials. The favorable performance of flexible B-P/NC-600 can be ascribed to the nitrogen-rich carbon nanofibers with three-dimensional network matrix for the more active site of boron and phosphorus co-doping. Our work paves the way for the improvement of flexible anodes and wide-operating temperature of sodium-ion batteries by doping approach of much heteroatom.

柔性储能装置已被广泛关注并应用于各个领域。得益于硼（B）和磷（P）掺杂材料的活性位点，共掺杂碳材料被广泛应用于储能器件，以增强其电化学性能。本文利用电纺丝技术研究了富氮（B-P/NC）的硼和磷共掺杂柔性碳纳米纤维在钠离子电池中的应用。退火温度为 600 °C 的无粘合剂 B-P/NC 柔性纳米碳纤维（B-P/NC-600）性能卓越，循环 500 次后，在 0.1 A/g 下可达到 200 mAh/g 的稳健容量，循环 12,000 次后，在 1 A/g 下仍可达到 160 mAh/g 的持久可逆容量，显示出柔性 B-P/NC-600 同样值得称道的稳定性。此外，B-P/NC-600 还能在 60 °C 测试温度下提供 265 mAh/g 的可逆容量。更重要的是，柔性 B-P/NC-600 可用作整个电池的阳极，在 1 A/g 循环 200 次后，可提供 90 mAh/g 的容量。同时，理论计算进一步验证了硼磷共掺杂能提高氮碳材料的吸附能力。柔性 B-P/NC-600 的良好性能可归因于富氮碳纳米纤维的三维网络基质为硼磷共掺杂提供了更多的活性位点。我们的工作为通过掺杂更多杂质原子来提高钠离子电池的柔性阳极和宽工作温度铺平了道路。

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引用次数: 0

Corrigendum to ‘How ligand coordination and superatomic-states accommodate the structure and property of a metal cluster: Cu4 (dppy)4 Cl2 vs. Cu21 (dppy)10 with altered photoluminescence’ Chin. Chem. Lett. 2024, 35, 108340 配体配位和超原子态如何影响金属簇的结构和性质？Cu4 (dppy)4 Cl2 vs. Cu21 (dppy)10 with altered photoluminescence' Chin.Chem.2024, 35, 108340

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-12 DOI: 10.1016/j.cclet.2024.109912

Haiming Wu , Gaya N. Andrew , Rajini Anumula , Zhixun Luo

引用次数: 0

Dual atom-bridge effect promoting interfacial charge transfer in 2D/2D Cs3Bi2Br9/BiOBr epitaxial heterojunction for efficient photocatalysis 促进二维/二维 Cs3Bi2Br9/BiOBr 外延异质结中界面电荷转移的双原子桥效应，实现高效光催化

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-09-11 DOI: 10.1016/j.cclet.2024.110430

Yuan Teng , Zichun Zhou , Jinghua Chen , Siying Huang , Hongyan Chen , Daibin Kuang

Optimizing the interfacial quality of halide perovskites heterojunction to promote the photogenerated charge separation is of great significance in photocatalytic reactions. However, the delicately regulation of interfacial structure and properties of halide perovskites hybrid is still a big challenge owing to the growth uncontrollability and incompatibility between different constituents. Here we use BiOBr nanosheets as the start-template to in situ epitaxially grow Cs₃Bi₂Br₉ nanosheets by “cosharing” Bi and Br atoms strategy for designing a 2D/2D Cs₃Bi₂Br₉/BiOBr heterojunction. Systematic studies show that the epitaxial heterojunction can optimize the synergistic effect of BiOBr and Cs₃Bi₂Br₉ via the formation of tight-contact interfaces, strong interfacial electronic coupling and charge redistribution, which can not only drive the Z-scheme charge transfer mechanism to greatly promote the spatial separation of electron-hole pairs, but also modulate the interfacial electronic structure to facilitate the adsorption and activation of toluene molecules. The heterojunction exhibited 62.3 and 2.4-fold photoactivity improvement for toluene oxidation to benzaldehyde than parental BiOBr and Cs₃Bi₂Br₉, respectively. This study not only proposed a novel dual atom-bridge protocol to engineer high-quality perovskite heterojunctions, but also uncovered the potential of heterojunction in promoting electron-hole separation as well as the application in photocatalytic organic synthesis.

优化卤化物过氧化物异质结的界面质量以促进光生电荷分离在光催化反应中具有重要意义。然而，由于生长的不可控性和不同成分之间的不相容性，如何微妙地调节卤化物过氧化物杂质的界面结构和性能仍然是一个巨大的挑战。在此，我们以 BiOBr 纳米片为起始模板，通过 Bi 原子和 Br 原子 "共用 "策略原位外延生长 Cs3Bi2Br9 纳米片，从而设计出二维/二维 Cs3Bi2Br9/BiOBr 异质结。系统研究表明，外延异质结可以通过形成紧密接触界面、强界面电子耦合和电荷再分布优化 BiOBr 和 Cs3Bi2Br9 的协同效应，不仅可以驱动 Z 型电荷转移机制，极大地促进电子-空穴对的空间分离，还可以调控界面电子结构，促进甲苯分子的吸附和活化。与亲代 BiOBr 和 Cs3Bi2Br9 相比，异质结在甲苯氧化成苯甲醛时的光活性分别提高了 62.3 倍和 2.4 倍。这项研究不仅提出了一种新颖的双原子桥方案来设计高质量的包晶异质结，而且揭示了异质结在促进电子-空穴分离方面的潜力以及在光催化有机合成中的应用。

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引用次数: 0

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

Chinese Chemical Letters

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。

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

Chinese Chemical Letters

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。

引用次数: 0

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