结构化学最新文献

英文中文

2D zirconium-based metal-organic framework/bismuth(III) oxide nanorods composite for electrocatalytic CO2-to-formate reduction 二维锆基金属有机框架/氧化铋(III)纳米棒复合材料用于电催化二氧化碳到甲酸盐的还原反应

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-07-01 DOI: 10.1016/j.cjsc.2024.100301

Electrocatalytic carbon dioxide reduction reaction (eCO₂RR) represents one of the most promising technologies for sustainable conversion of CO₂ to value-added products. Although metal-organic frameworks (MOFs) can be vastly functionalized to create active sites for CO₂RR, low intrinsic electrical conductivity always makes MOFs unfavorable candidates for eCO₂RR. Besides, studies on how to regulate eCO₂RR activity of MOFs from linkers' functionalities viewpoint lag far behind when compared with the assembly of multinuclear metal-centered clusters. In this work, non-toxic bismuth(III) oxide (Bi₂O₃) was incorporated into a series of two-dimensional (2D) MOFs (ZrLX) established from Zr-oxo clusters and triazine-centered 3-c linkers with different functionalities (LX = 1–5) to give composites ZrLX/Bi₂O₃. To investigate how functionalities on linkers distantly tune the eCO₂RR performance of MOFs, electron-donating/withdrawing groups were installed at triazine core or benzoate terminals. It is found that ZrL2/Bi₂O₃ (‒F functionalized on triazine core) exhibits the best eCO₂RR performance with the highest Faradaic efficiency (FE) of 96.73% at −1.07 V vs. RHE, the largest electroactive surface (C_dl = 4.23 mF cm⁻²) and the highest electrical conductivity (5.54 × 10⁻⁷ S cm⁻¹), highlighting tuning linker functionalities and hence electronic structure as an alternative way to regulate eCO₂RR.

电催化二氧化碳还原反应（eCORR）是将二氧化碳持续转化为高附加值产品的最有前途的技术之一。尽管金属有机框架（MOFs）可以进行大量功能化处理，为二氧化碳还原反应创造活性位点，但其内在导电性较低，始终是 eCORR 的不利候选材料。此外，与多核金属中心簇的组装相比，如何从连接体的功能性角度调节 MOFs 的 eCORR 活性的研究还远远落后。在这项工作中，将无毒的氧化铋（III）（BiO）加入到一系列二维 MOFs（Zr）中，这些二维 MOFs 是由 Zr-oxo 簇和具有不同功能性（= 1-5）的以三嗪为中心的 3-连接体建立的，从而得到 Zr/BiO 复合材料。为了研究连接体上的官能团如何远距离调节 MOF 的 eCORR 性能，在三嗪核心或苯甲酸酯末端安装了电子捐赠/撤回基团。研究发现，Zr/BiO（三嗪核心上的-F官能化）表现出最佳的 eCORR 性能，在 -1.07 V RHE 时法拉第效率最高，达 96.73%，电活性表面最大（= 4.23 mF cm），电导率最高（5.54 × 10 S cm）。

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引用次数: 0

Tandem catalysis for photoreduction of CO2 into multi-carbon fuels on atomically thin dual-metal phosphochalcogenides 在原子级双金属磷钙钛矿薄膜上串联催化二氧化碳光还原成多碳燃料

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-07-01 DOI: 10.1016/j.cjsc.2024.100320

引用次数: 0

Lithium-ion rapid transport mechanism and channel design in solid electrolytes 固体电解质中的锂离子快速传输机制和通道设计

IF 2.2 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-25 DOI: 10.1016/j.cjsc.2024.100381

Jia-hui Li, Jinkai Qiu, Cheng Lian

引用次数: 0

Design of two-dimensional porous covalent organic framework semiconductors for visible-light-driven overall water splitting: A theoretical perspective 设计用于可见光驱动整体水分离的二维多孔共价有机框架半导体：理论视角

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-25 DOI: 10.1016/j.cjsc.2024.100375

Utilizing sunlight to split water into H₂ and O₂ is a highly promising approach in renewable energy production approaches. Recently, significant efforts have been devoted to developing innovative photocatalysts for splitting water. Metal-free two-dimensional (2D) covalent organic frameworks (COFs) are emerging as ideal catalytic platforms for this purpose. However, the rational design of these materials requires appropriate band alignment and active sites capable of catalyzing both hydrogen and oxygen evolution reactions (OERs), which depends on the judicious selection of molecular precursors. To address these requirements, first-principles calculations have proven to be an efficient method for designing and screening potential photocatalysts. Here, we provide a concise overview of recent advancements in the development of 2D COFs photocatalysts for overall water splitting (OWS), examining it from a theoretical perspective. This includes outlining the design principles, exploring the data-driven discovery of potential candidates using a COFs database, and applying machine learning (ML) techniques to predict the electronic structure of COFs based on the molecular orbitals of their precursors. Furthermore, we discuss the accuracy of current computational methods and address future challenges and potential of 2D COFs in practical applications for OWS.

利用太阳光将水分离成 H2 和 O2 是一种极具前景的可再生能源生产方法。最近，人们致力于开发创新的光催化剂来分离水。无金属二维（2D）共价有机框架（COFs）正在成为实现这一目的的理想催化平台。然而，这些材料的合理设计需要适当的能带排列和能够同时催化氢和氧进化反应（OER）的活性位点，这取决于对分子前体的明智选择。为了满足这些要求，第一原理计算已被证明是设计和筛选潜在光催化剂的有效方法。在此，我们简要概述了用于整体水分离（OWS）的二维 COFs 光催化剂开发的最新进展，并从理论角度对其进行了研究。这包括概述设计原则、探索使用 COFs 数据库以数据驱动发现潜在候选物质，以及应用机器学习 (ML) 技术根据 COFs 前体的分子轨道预测其电子结构。此外，我们还讨论了当前计算方法的准确性，并探讨了二维 COFs 在 OWS 实际应用中的未来挑战和潜力。保留所有权利。

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引用次数: 0

Rigid-flexible-ligand-ornamented lanthanide-incorporated selenotungstates and photoluminescence properties 刚性柔性配体饰有镧系元素的硒钨酸盐和光致发光特性

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-22 DOI: 10.1016/j.cjsc.2024.100370

Currently, organic-inorganic hybrid lanthanide-incorporated polyoxometalates (POMs) have emerged as a prominent research area. Herein, we employ a simple raw material assembly method to synthesize two neoteric mixed-organic-ligand-ornamented lanthanide (Ln) incorporated selenotungstates [H₂N(CH₃)₂]₁₆Na₂[Ln₄(H₂O)₆(HPZDA)₂(HFMA)₂W₈O₂₁][B-α-SeW₉O₃₃]₄·29H₂O (Ln = Sm³⁺ (1), La³⁺ (2); H₂PZDA = 2,3-pyrazine dicarboxylic acid, H₂FMA = fumaric acid). 1 and 2 are isomorphic with the polyanions constructed from four trivacant Keggin [B-α-SeW₉O₃₃]^8– ({SeW₉}) segments and a rigid-flexible-ligand-ornamented dodeca-nuclear W–Ln heterometallic [Ln₄(H₂O)₆(HPZDA)₂(HFMA)₂W₈O₂₁]¹⁴⁺ cluster. Moreover, the solid-state fluorescence spectrum of 1 at room temperature mainly exhibits the characteristic emission peak of Sm³⁺ cations. Additionally, energy transfer from {SeW₉} to Sm³⁺ ions in 1 has been demonstrated by time-resolved spectroscopy. This work presents a feasible dual-ligand synergistic strategy for constructing novel POM derivatives and POM-based fluorescent materials.

目前，有机-无机混合镧系元素掺杂聚氧化金属盐（POMs）已成为一个突出的研究领域。在此，我们采用简单的原料组装方法合成了两种新有机混合配体镧系元素（Ln）掺杂硒钨酸盐[HN(CH)]Na [Ln(HO)(HPZDA)(HFMA)WO][B--SeWO]-29HO （Ln = Sm（），La（）；HPZDA = 2,3-吡嗪二羧酸，HFMA = 富马酸）。并与由四个三价凯金[B--SeWO]（{SeW}）段和刚-柔-配体-饰十二核 W-Ln 异金属[Ln(HO)(HPZDA)(HFMA)WO]簇构建的多阴离子同构。此外，室温下的固态荧光光谱主要呈现出 Sm 阳离子的特征发射峰。此外，时间分辨光谱也证明了{SeW}向 Sm 离子的能量转移。这项工作为构建新型 POM 衍生物和基于 POM 的荧光材料提供了一种可行的双配体协同策略。

引用次数: 0

Structure and assembly mechanism of high-nuclear lanthanide-oxo clusters 高核镧系氧化物团簇的结构和组装机制

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-19 DOI: 10.1016/j.cjsc.2024.100372

引用次数: 0

Atomically precise superatomic silver nanoclusters stabilized by O-donor ligands 由 O-供体配体稳定的原子精度超原子银纳米团簇

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-19 DOI: 10.1016/j.cjsc.2024.100371

引用次数: 0

Anion-pillared MOFs for challenging hydrocarbon separations 用于高难度碳氢化合物分离的阴离子柱状 MOFs

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-19 DOI: 10.1016/j.cjsc.2024.100374

引用次数: 0

Harnessing d-f transition rare earth complexes for single layer white organic light emitting diodes 利用 d-f 过渡稀土络合物制造单层白色有机发光二极管

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-11 DOI: 10.1016/j.cjsc.2024.100369

引用次数: 0

A flexible-robust MOF for efficient purification of perfluoropropane 用于高效提纯全氟丙烷的灵活稳健的 MOF

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2024-06-09 DOI: 10.1016/j.cjsc.2024.100368

引用次数: 0

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