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The progress and challenges of tin-lead alloyed perovskites: Toward the development of large-scale all-perovskite tandem solar cells 锡铅合金钙钛矿的进展与挑战：面向大规模全钙钛矿串联太阳能电池的发展

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.12.002

Xiao Jia , Dan Yang , Dexu Zheng , Zhen Chang , Jishuang Liu , Lu Liu , Lei Peng , Yao Tong , Kai Wang , Shengzhong Liu

The lead-based single-junction perovskite solar cells have achieved impressive efficiencies of up to 26.8%, highlighting their remarkable application potential and driving rapid advancements in large-area modules. However, as efficiencies approach the Shockley-Queisser limit for single-junction cells, further advancements are becoming increasingly challenging. Consequently, researchers have shifted their focus toward tin-lead alloyed perovskite (TLP) materials, aiming to construct multi-junction tandems. Recent advancements in both single-junction and multi-junction perovskite solar cells underscore the vast potential of TLPs, and their continued development promises a novel avenue for the industrialization of perovskite technology. This review provides a comprehensive overview of recent advancements in TLPs for photovoltaic applications, covering ionic compositions, crystallization engineering, modifications of extrinsic substances, and contact layers. It also discusses progress in multi-junction tandems and large-scale modules, providing valuable insights for commercial production. The review concludes by summarizing the overall progress in TLPs and providing a perspective on future research.

铅基单结钙钛矿太阳能电池的效率达到了令人印象深刻的26.8%，突出了其显著的应用潜力，并推动了大面积组件的快速发展。然而，随着效率接近单结电池的Shockley-Queisser极限，进一步的进步变得越来越具有挑战性。因此，研究人员将重点转向锡铅合金钙钛矿（TLP）材料，旨在构建多结串联。单结和多结钙钛矿太阳能电池的最新进展强调了TLPs的巨大潜力，它们的持续发展为钙钛矿技术的工业化提供了一条新的途径。本文综述了光电TLPs的最新进展，包括离子组成、结晶工程、外部物质修饰和接触层。它还讨论了多结串联和大规模模块的进展，为商业生产提供了有价值的见解。本文总结了TLPs的研究进展，并对今后的研究进行了展望。

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引用次数: 0

Virtual screening for an ultra-small NIR emitter with only two isolated hexatomic rings

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.08.022

Zuping Xiong , Jianyu Zhang , Lei Wang , Xiong Liu , Jing Zhi Sun , Haoke Zhang , Ben Zhong Tang

Unlocking the potential of weak interactions to govern the electronic structure of organic molecules remains a significant challenge. This study constructs a quantitative relationship between conformations and strength of electronic through-space interactions (TSIs) for tetraarylethanes (TAEs). To identify long-wavelength emitters, a sophisticated virtual screening is executed for TAEs by constructing a TSI-based database. Consequently, an ultra-small emitter (o-2Md), distinguished by a highly concentrated n-electron configuration, is synthesized and shows a remarkable near-infrared (NIR) emission with a luminescence quantum yield of 25% and an emission wavelength extending beyond 800 nm. Notably, the o-2Md stands out as one of the smallest known organic NIR emitters, showcasing the robustness of n-n TSI in designing efficient emitters. This work not only systematically reveals the important role of weak interactions in manipulating the electronic structure at the single-molecule level but also provides a new platform, the TSI database, for designing advanced optoelectronic materials.

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引用次数: 0

Supramolecular boosted superexchange 超分子增强的超交换

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.102397

Pall Thordarson , Dong Jun Kim

In this issue of Chem, Zhao et al. present a supramolecular strategy for controlling symmetry-breaking charge separation (SB-CS) through guest-mediated superexchange pathways. In a cyclophane host, guest molecules accelerate or suppress SB-CS by enhancing electron-transfer efficiency. This dynamic system enables tunable charge separation and demonstrates potential for photocatalysis, light energy conversion, and applications in organic photovoltaics.

在这一期的Chem中，Zhao等人提出了一种通过客体介导的超交换途径控制对称破缺电荷分离（SB-CS）的超分子策略。在环双亲体中，客体分子通过提高电子转移效率来加速或抑制SB-CS。该动态系统实现了可调电荷分离，并展示了光催化、光能转换和有机光伏应用的潜力。

引用次数: 0

Overcoming key challenges: Next-generation synthetic anion transporters 克服关键挑战：下一代合成阴离子转运体

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.102394

Jennifer Ruth Hiscock

In this issue of Chem, Gale and co-workers bring together multiple fundamental supramolecular and medicinal chemistry principles to overcome the limitations associated with synthetic anion transporter technologies. These researchers report systems that are more active than those found in nature, alonside systems that can selectively target organelle membranes.

在本期的《化学》杂志上，Gale及其同事将多种基本的超分子和药物化学原理结合在一起，克服了与合成阴离子转运体技术相关的局限性。这些研究人员报告了比自然界中发现的更活跃的系统，以及可以选择性地靶向细胞器膜的系统。

引用次数: 0

Identifying the lithium bond and lithium ionic bond in electrolytes 识别电解质中的锂键和锂离子键

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.07.016

Nan Yao , Xiang Chen , Shu-Yu Sun , Yu-Chen Gao , Legeng Yu , Yan-Bin Gao , Wei-Lin Li , Qiang Zhang

Lithium (Li) chemistry has been a significant branch of modern chemistry due to its wide and critical applications, such as Li batteries. Similar to the hydrogen (H) bond, the Li bond is the central topic of Li chemistry, but its nature is far from clear. Herein, the fundamental chemistry of the Li bond is systematically investigated, taking Li battery electrolytes as an example. Specifically, the Li bond and Li ionic bond can be differentiated according to nuclear magnetic resonance spectroscopy as ⁷Li chemical shifts exhibit a downfield and upfield shift, respectively. The downfield shift indicates an electron localization effect of the Li bond beyond electrostatic interactions, which mainly dominate the ionic bond. Bond and electronic structure analyses further verify the difference between these two bonds. This work establishes principles to identify the Li bond and Li ionic bond, which contribute to Li chemistry and related applications, such as Li batteries.

锂（Li）化学因其广泛而关键的应用（如锂电池）而成为现代化学的一个重要分支。与氢（H）键类似，锂键也是锂化学的核心课题，但其本质却远未明晰。本文以锂电池电解质为例，系统研究了锂键的基本化学性质。具体来说，根据核磁共振波谱可以区分锂键和锂离子键，因为 7Li 化学位移分别表现为下场位移和上场位移。下场偏移表明锂键的电子定位效应超出了静电相互作用，而静电相互作用主要主导离子键。键和电子结构分析进一步验证了这两种键之间的差异。这项研究确立了识别锂键和锂离子键的原则，有助于锂化学和锂电池等相关应用。

引用次数: 0

Manipulating symmetry-breaking charge separation employing molecular recognition 利用分子识别操纵对称性破坏电荷分离

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.07.010

Xueze Zhao , Ryan M. Young , Chun Tang , Guangcheng Wu , Kathryn R. Peinkofer , Yaoyao Han , Shuliang Yang , Yi-Kang Xing , Han Han , Huang Wu , Xuesong Li , Yuanning Feng , Ruihua Zhang , Charlotte L. Stern , Michael R. Wasielewski , J. Fraser Stoddart

The exploration of symmetry-breaking charge separation (SB-CS) is imperative when designing functional light-harvesting materials. Past explorations, however, have been confined to covalent systems, more often than not requiring complicated/demanding syntheses and facing inconvenient regulation of charge transfer processes. Here, we present a concept that regulates the efficiency of SB-CS through molecular recognition utilizing a pyridinium-based cyclophane as a host. This host undergoes photo-driven excited-state SB-CS. By employing different guests with distinct frontier molecular orbital energy levels, we have achieved comprehensive control of electron transfer pathways in the cyclophane, modulating between accelerated (>10-fold) intramolecular SB-CS involving superexchange and direct intermolecular electron transfer between the host and guest. The improvement in SB-CS efficiency results in catalytic activity for the photo-oxidation of a sulfur-mustard simulant. This research offers an opportunity for tuning SB-CS by utilizing molecular recognition, which holds the potential for achieving precise regulation without complicated organic syntheses.

在设计功能性光收集材料时，探索对称破缺电荷分离（SB-CS）势在必行。然而，过去的探索仅限于共价系统，往往需要复杂/苛刻的合成，而且电荷转移过程的调节也不方便。在这里，我们提出了一个概念，利用基于吡啶的环烷作为宿主，通过分子识别来调节 SB-CS 的效率。这种宿主会发生光驱动激发态 SB-CS。通过采用具有不同前沿分子轨道能级的不同客体，我们实现了对环烷中电子传递途径的全面控制，在涉及超交换的加速（10 倍）分子内 SB-CS 与宿主和客体之间的直接分子间电子传递之间进行调节。SB-CS 效率的提高使得硫-芥末模拟物的光氧化反应具有催化活性。这项研究为利用分子识别技术调节 SB-CS 提供了一个机会，从而有可能在不进行复杂有机合成的情况下实现精确调节。

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引用次数: 0

Stay creative 保持创造性

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.11.010

Brigitte A.K. Kriebisch , Christine M.E. Kriebisch

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Brigitte and Christine Kriebisch completed their MSc in chemistry at the Technical University of Munich before joining Prof. Job Boekhoven for their doctoral studies. Their fascination with biological nanomachinery that harvests chemical energy to achieve directional motion and directional pumping drives them to develop synthetic analogs that hold future potential in medical applications. For example, they can imagine nanorobots that swim through blood vessels for cargo transport or to detect tumor cells.

下载：下载高分辨率图片（331KB）下载：下载全尺寸图片下载：下载全尺寸图片下载：下载全尺寸图片下载：下载全尺寸图片brigitte和Christine Kriebisch在慕尼黑工业大学完成了化学硕士学位，然后加入Job Boekhoven教授进行博士研究。他们对生物纳米机械的痴迷驱使他们开发具有未来医学应用潜力的合成类似物，这种机械可以收集化学能来实现定向运动和定向泵送。例如，他们可以想象纳米机器人在血管中游动，用于货物运输或检测肿瘤细胞。

引用次数: 0

The key of Zn2+ transfer kinetics in zinc metal batteries 锌金属电池中Zn2+转移动力学的关键

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.12.001

Wenxuan Sun , Zengguang Li , Wei Guo , Yongzhu Fu

Interface chemistry inevitably affects Zn dendrite formation and interfacial kinetics, which pose serious challenges in zinc metal batteries (ZMBs). In the December issue of Chem, Guo et al. identified that Zn²⁺ transport in the solid electrolyte interphases (SEIs) is the rate-limiting step of Zn²⁺ transfer kinetics in typical ZMBs and designed a SEI comprising Zn₃N₂ species, thereby overcoming the above-mentioned issues.

界面化学不可避免地影响Zn枝晶的形成和界面动力学，这对锌金属电池（zmb）的研究提出了严峻的挑战。在12月的Chem杂志上，Guo等人发现Zn2+在固体电解质界面（SEIs）中的转移是典型zmb中Zn2+转移动力学的限速步骤，并设计了一个包含Zn3N2物种的SEI，从而克服了上述问题。

引用次数: 0

Fluorinating electrophilic interception in the oxidation or protonation of alkynyl tetracoordinate borons 炔基四配位硼氧化或质子化过程中的氟化亲电截流作用

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.07.034

Xingxing Ma , Zihao Zhong , Qiuling Song

Introduction of fluorine atoms or fluorine-containing moieties into organic molecules can dramatically influence their properties, thereby increasing their applicability as drugs or building blocks for organic materials. Herein, we report intriguing fluorinating electrophilic interception achieving the synthesis of various fluorine-containing compounds where oxidation or protodeboronation of alkenyl boron species from 1,2-migration of alkynyl tetracoordinate borons were involved. Obviously, α,α-difluoroketones are readily accessible within 30 min, which might provide an alternative approach to [¹⁸F]α,α-difluoroketones. Meanwhile, versatile monofluoroalkenes, α-SCF₃ ketones, and (highly deuterated) SCF₃-containing alkenes can be assembled in good yields via this strategy. This protocol features tunable synthesis, high stereoselectivity and efficiency, applicability to late-stage modifications of bioactive molecules, and modular introduction of fluorine atoms/fluorinated groups. Additionally, these transformations can perfectly suppress the Zweifel pathway and keep the fluorine atoms/fluorinated groups intact without elimination, and the difluoropiperidine scaffolds could also be forged efficiently via this protocol.

在有机分子中引入氟原子或含氟分子可以极大地影响它们的性质，从而提高它们作为药物或有机材料构件的适用性。在此，我们报告了通过引人入胜的氟化亲电截取技术合成各种含氟化合物的过程，其中涉及到炔基四配位硼的 1,2 迁移产生的烯基硼氧化或原硼化反应。很明显，α,α-二氟酮类化合物在 30 分钟内就可以获得，这可能为[18F]α,α-二氟酮类化合物提供了一种替代方法。同时，通过这种方法还能以良好的产率组装出多功能的单氟烯、α-SCF3 酮和含 SCF3 的（高氚代）烯烃。该方案具有可调合成、高立体选择性和高效率、适用于生物活性分子的后期修饰以及氟原子/氟化基团的模块化引入等特点。此外，这些转化可以完美地抑制 Zweifel 通路，并保持氟原子/氟化基团的完整而不被消除，二氟哌啶支架也可以通过该方案高效地锻造出来。

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引用次数: 0

Tetralactam-based anion transporters 基于四内酰胺的阴离子转运体

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2025-01-09 DOI: 10.1016/j.chempr.2024.09.028

Alexander M. Gilchrist , Daniel A. McNaughton , Mohamed Fares , Xin Wu , Bryson A. Hawkins , Stephen J. Butler , David E. Hibbs , Philip A. Gale

Synthetic anion transporters provide a promising avenue to treat diseases such as cystic fibrosis and cancer. Anion binding site preorganization is one aspect of transporter design that can be manipulated to enhance binding. Macrocycles possess preorganized binding cavities, enabling more selective and efficient anion binding and transport. In this study, we build on a macrocyclic tetralactam scaffold by preparing a series of fluorinated and non-fluorinated tetralactam anion transporters. Anion binding and transport assays were used to analyze the substituent effects on scaffold lipophilicity, selectivity, solubility, binding strength, and transport rates. The series was analyzed for the ability to bind and transport Cl⁻ and F⁻ anions across lipid bilayers. Some highly fluorinated tetralactams display extremely high levels of Cl⁻ and F⁻ transport activity, showing record activities in 8-hydroxypyrene-1,3,6-trisulfonic acid (HPTS) assays and a Eu(III) probe-based F⁻ transport assay.

合成阴离子转运体为治疗囊性纤维化和癌症等疾病提供了一条前景广阔的途径。阴离子结合位点预组织是转运体设计的一个方面，可以通过操作来增强结合。大环具有预组织的结合空腔，可实现更有选择性和更高效的阴离子结合和转运。在本研究中，我们以大环四内酰胺为支架，制备了一系列含氟和不含氟的四内酰胺阴离子转运体。阴离子结合和转运试验用于分析取代基对支架亲油性、选择性、溶解性、结合强度和转运率的影响。分析了该系列化合物与 Cl- 和 F- 阴离子结合并通过脂质双分子层转运的能力。在 8-羟基芘-1,3,6-三磺酸 (HPTS) 试验和基于 Eu(III) 探针的 F- 运输试验中，一些高氟化四内酰胺显示出极高的 Cl- 和 F- 运输活性。

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