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Photovoltaic potential of nitro-functionalized non-fullerene acceptors depends on its bonding site 硝基功能化非富勒烯受体的光伏电势取决于其成键位置
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2025-10-10 DOI: 10.1016/j.chempr.2025.102756
Mingpeng Li , Waqar Ali Memon , Zihao Deng , Huan Wang , Shilong Xiong , Heng Li , Top Archie Dela Peña , Cuifen Zhang , Yunpeng Wang , Jiaying Wu , Zaifei Ma , Nan Zheng , Leilei Tian , Feng He
Nitration is rarely employed to optimize non-fullerene acceptors (NFAs) owing to the pronounced steric hindrance and strong electron-withdrawing inductive effects of nitro groups. This study presents a site-specific nitration strategy to systematically modulate NFA properties and photovoltaic performance. A series of nitrated and non-nitrated NFAs were synthesized, exhibiting distinct energy levels, molecular configurations, and packing modes. Notably, the quasi-planar heterojunction (Q-PHJ) device based on NO2Q-2F, which incorporates a central nitration site, achieved a champion efficiency of 19.14% and an extended T80 lifetime of 6,450 h under dark storage conditions, attributed to its tighter three-dimensional network stacking. In contrast, the HQ-NO2-based device, which features terminal nitration, yielded a lower efficiency of 12.45%. This work underscores the critical role of nitration positioning in unlocking the potential of NFAs. It also provides new opportunities to further explore the impact of nitration on photovoltaic performance for developing advanced organic semiconductors.
由于硝基明显的空间位阻和强的吸电子诱导效应,很少采用硝化法来优化非富勒烯受体。本研究提出了一种特定地点的硝化策略来系统地调节NFA特性和光伏性能。合成了一系列硝化和非硝化nfa,表现出不同的能级、分子构型和包装模式。值得注意的是,基于NO2Q-2F的准平面异质结(Q-PHJ)器件,包含一个中心硝化位点,由于其更紧密的三维网络堆叠,在暗存储条件下实现了19.14%的champion效率和6450 h的T80寿命延长。相比之下,基于红旗no2的装置具有终端硝化功能,其效率较低,为12.45%。这项工作强调了硝化定位在释放nfa潜力方面的关键作用。这也为进一步探索硝化对光伏性能的影响为开发先进的有机半导体提供了新的机会。
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引用次数: 0
Exciton delocalization suppresses polariton scattering 激子离域抑制极化子散射
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2025-10-10 DOI: 10.1016/j.chempr.2025.102759
Yongseok Hong , Ding Xu , Milan Delor
Exciton-polaritons (EPs) are hybrid light-matter quasiparticles that combine exciton-mediated nonlinearities with long-range coherence, ideal for energy harvesting and nonlinear optics. Optimizing EPs is predicated on a still-elusive understanding of how disorder affects their propagation and dephasing times. Here, using cutting-edge femtosecond spatiotemporal microscopy, we image EP propagation in two-dimensional semiconductors, molecular crystals, and amorphous molecular films with systematically varied exciton-phonon coupling, exciton delocalization, and static disorder. Despite possessing similar EP dispersions, we observe dramatically different transport velocities and scattering times across systems. We establish a robust scaling law linking EP scattering to exciton transfer integral, demonstrating that polaritons based on materials with large exciton bandwidths are protected against disorder even for highly excitonic EPs. This observation cannot be deduced from the systems’ linear optical properties. Our work highlights the critical role of the matter component in dictating polariton properties and provides precise guidelines for simultaneously optimizing EP propagation and nonlinearities.
激子-极化子(EPs)是混合光-物质准粒子,结合了激子介导的非线性和远程相干性,是能量收集和非线性光学的理想选择。优化EPs是基于对无序如何影响其传播和减相时间的理解。在这里,我们使用尖端的飞秒时空显微镜,对二维半导体、分子晶体和非晶分子膜中具有系统变化的激子-声子耦合、激子离域和静态无序的EP传播进行了成像。尽管具有相似的EP色散,但我们观察到系统之间的输运速度和散射时间显着不同。我们建立了一个强大的标度律,将EP散射与激子转移积分联系起来,证明了基于具有大激子带宽的材料的极化子即使对于高激子EPs也可以防止无序。这一观察结果不能从系统的线性光学性质中推断出来。我们的工作强调了物质成分在决定极化子性质方面的关键作用,并为同时优化EP传播和非线性提供了精确的指导。
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引用次数: 0
Single-atom-enhanced membrane for simultaneous bacteria and heavy metal on-site water treatment 同时处理细菌和重金属的单原子增强膜
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2025-10-15 DOI: 10.1016/j.chempr.2025.102785
David Panáček , Renata Večeřová , Zdeněk Baďura , Vítězslav Hrubý , Lukáš Zdražil , Milan Kolář , Thamraa Alshahrani , Aleš Panáček , Aristides Bakandritsos , Radek Zbořil
Access to clean water remains a major global challenge, especially in remote and disaster-affected areas, where centralized water treatment is often unavailable. This study introduces a single-atom engineering approach to designing a filtration system capable of simultaneously purifying water from bacteria and heavy metals on site, thus providing a sustainable and user-friendly method for water purification. The system demonstrates exceptional efficiency in removing bacterial and heavy metal contaminants from various water sources. Our findings show remarkable filtration efficiency (>99.999%) against a broad spectrum of microorganisms in distilled, tap, and river water. Moreover, the membrane demonstrates a high adsorption capacity for heavy metals, specifically 661 and 248 mg g−1 for Pb2+ and Cd2+, respectively. The simple operation and high membrane permeability, requiring only a hand-powered vacuum, ensure applicability in off-grid settings. In addition, the membrane material maintains more than 90% efficiency after 20 regeneration cycles, addressing both cost and sustainability issues.
获得清洁水仍然是一项重大的全球挑战,特别是在往往无法进行集中水处理的偏远和受灾地区。本研究采用单原子工程方法设计了一种能够同时在现场净化水中细菌和重金属的过滤系统,从而为水的净化提供了一种可持续的、用户友好的方法。该系统在去除各种水源中的细菌和重金属污染物方面表现出卓越的效率。我们的研究结果表明,在蒸馏水、自来水和河水中,对广谱微生物的过滤效率显著(99.999%)。此外,该膜对重金属的吸附能力较高,对Pb2+和Cd2+的吸附量分别为661和248 mg g−1。操作简单,膜渗透性高,只需要手动真空,确保在离网设置的适用性。此外,膜材料在20次再生循环后保持90%以上的效率,解决了成本和可持续性问题。
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引用次数: 0
Reducing polysulfide hydrodynamic radius toward low-temperature lithium–sulfur batteries 降低低温锂硫电池的多硫化物流体动力半径
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2026-02-06 DOI: 10.1016/j.chempr.2025.102881
Tian Jin , Meng Zhao , Xi-Yao Li , Zi-Xian Chen , Bo-Quan Li , Jia-Qi Huang , Qiang Zhang
Lithium–sulfur (Li–S) batteries are promising in realizing high energy density. Employing weakly solvating electrolytes (WSEs) further improves the anode stability. However, the lithium polysulfide (LiPS) redox kinetics is hindered in WSEs, and the underlying mechanism remains unclear. Herein, the LiPS kinetics in WSEs is quantitatively deciphered using rotating disk electrode analysis. The electron transfer number during oxidation is reduced in WSEs, evidencing intrinsically suppressed oxidation extent. Meanwhile, the diffusion coefficient and the electrolyte viscosity concurrently increase, implying a reduced LiPS hydrodynamic radius in WSEs based on the Stokes–Einstein relation and corresponding to inhibited LiPS molecular aggregation. Attributed to the reduced aggregation, WSE-based Li–S batteries exhibit record-low-temperature performances, delivering 8.0 mAh cm−2 and 303 Wh kg−1 at 0°C in 6 Ah-level pouch cells. This work establishes a new kinetic analysis methodology to guide rational electrolyte design and highlights the promise of WSEs to enable low-temperature Li–S batteries.
锂硫电池是实现高能量密度的理想电池。采用弱溶剂化电解质(wse)进一步提高了阳极的稳定性。然而,锂多硫化物(LiPS)在wse中的氧化还原动力学受到阻碍,其潜在机制尚不清楚。在这里,利用旋转圆盘电极分析定量地破译了WSEs中的LiPS动力学。氧化过程中的电子转移数在wse中减少,表明氧化程度受到内在抑制。同时,扩散系数和电解质粘度同时增加,表明基于Stokes-Einstein关系的wse中LiPS流体动力半径减小,对应于LiPS分子聚集受到抑制。由于减少了聚集,基于wse的Li-S电池表现出创纪录的低温性能,在6 ah级别的袋状电池中,在0°C下提供8.0 mAh cm - 2和303 Wh kg - 1。这项工作建立了一种新的动力学分析方法来指导合理的电解质设计,并突出了wse在低温锂硫电池中的应用前景。
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引用次数: 0
ElectroChemputer with integrated monitoring for programmable electrochemistry ElectroChemputer与集成监控可编程的电化学
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2026-02-23 DOI: 10.1016/j.chempr.2025.102907
Melanie Guillén Soler , Robert Rauschen , Kristine Laws , Abhishek Sharma , Niclas Grocholski , Mark McNulty , Leroy Cronin
Electrochemical synthesis offers a sustainable and atom-economical alternative to conventional methods. Although recent advances have enabled electrochemical discovery, the integration of real-time control with analysis promises to allow electrochemical “fly by wire.” Herein, we present the ElectroChemputer, a programmable, modular standard platform enabling fully automated execution of electrochemical workflows. It integrates nuclear magnetic resonance (NMR) spectroscopy and electroanalytical reaction monitoring to provide structural and quantitative insight into reaction progression. Across 170 h of runtime, the system accumulated >1,500 coordinated unit operations and acquired >600 cyclic voltammograms. The ElectroChemputer enabled real-time stopped-flow NMR monitoring and data analysis of complex processes, such as decarboxylation via alternating polarity. Furthermore, we explored its flexibility for diverse transformations, including nucleophilic substitutions, oxidative couplings, and electrodepositions. By using queues and blueprints, it could run multiple protocols in parallel, demonstrating its adaptability across reaction classes, electrode materials, and configurations. Through its modular architecture, the ElectroChemputer sets the stage for programmable, autonomous, and democratized electrochemical synthesis.
电化学合成为传统方法提供了一种可持续和原子经济的替代方法。虽然最近的进展使电化学发现成为可能,但实时控制与分析的集成有望使电化学“通过导线飞行”。在此,我们提出了ElectroChemputer,这是一个可编程的模块化标准平台,可以完全自动化地执行电化学工作流程。它集成了核磁共振(NMR)光谱和电分析反应监测,以提供结构和定量的洞察反应进程。在170小时的运行过程中,系统累计进行了1500次协调单元操作,获得了600次循环伏安图。ElectroChemputer实现了实时停流核磁共振监测和复杂过程的数据分析,例如通过交替极性脱羧。此外,我们还探索了它在各种转化中的灵活性,包括亲核取代、氧化偶联和电沉积。通过使用队列和蓝图,它可以并行运行多个协议,展示了它在反应类别、电极材料和配置之间的适应性。通过其模块化架构,ElectroChemputer为可编程、自主和民主化的电化学合成奠定了基础。
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引用次数: 0
Direct access to chiral nitrogen-rich (semi-)saturated heterocycles 直接获得手性富氮(半)饱和杂环
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2025-11-07 DOI: 10.1016/j.chempr.2025.102817
Marco Pierau , Mathis J. Karrasch , Paulina Hartmann , Constantin G. Daniliuc , Andrea Hamza , Frank Glorius
Nitrogen-enriched (partially) saturated fused heterocycles have emerged as highly relevant scaffolds for improved pharmaceuticals. Increased solubility, along with fine-tuneable target affinity and specificity, differentiate them from their nitrogen-poor aromatic counterparts. Contrary to their growing demand, applications are severely limited by arduous bottom-up synthesis routes and the lack of a general solution for facile access. Herein, we report an efficient method for the synthesis of chiral (semi-)saturated pyridine-fused heterocycles and their respective N-permutations by enantioselective arene hydrogenation with a newly developed ruthenium catalyst. We obtained versatile and highly valuable product motifs, including pyridine- and piperidine-fused scaffolds with up to four newly formed stereocenters, of which several have not been previously reported. We conducted extensive in silico studies to elucidate a rare inverse-pressure-dependent enantioselectivity and to develop a rational model for predicting the stereochemical outcome. This contribution is expected to accelerate the exploration of new frameworks in drug discovery.
富氮(部分)饱和的熔融杂环已成为改进药物的高度相关的支架。增加的溶解度,以及可微调的靶标亲和力和特异性,使它们与氮贫乏的芳香对应物区分开来。与日益增长的需求相反,应用程序受到自下而上合成路线的严格限制,并且缺乏易于访问的通用解决方案。本文报道了一种新开发的钌催化剂,通过对映选择性芳烃加氢合成手性(半)饱和吡啶融合杂环及其n -排列的有效方法。我们获得了多功能和高价值的产品基序,包括吡啶和哌啶融合的支架,最多有四个新形成的立体中心,其中一些以前没有报道过。我们进行了大量的硅研究,以阐明一种罕见的逆压力依赖性对映体选择性,并建立一个合理的模型来预测立体化学结果。预计这一贡献将加速探索药物发现的新框架。
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引用次数: 0
Unstructured protein mimics have enzymatic activity 非结构蛋白质模拟物具有酶活性
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2026-02-26 DOI: 10.1016/j.chempr.2026.102996
Felipe Jiménez-Ángeles , Monica Olvera de la Cruz
Random copolymers containing charged, polar, and hydrophobic monomers protect enzymes so they can function in non-biological environments. These heteropolymers imitate unstructured proteins in coacervates that mimic membraneless organelles. Reporting in a recent issue of Nature, a team led by Xu and Alexander-Katz has designed heteropolymers with enzymatic activity by selecting monomers that modulate their chemical microenvironment to replicate enzymatic functionalities.
含有带电、极性和疏水单体的随机共聚物保护酶,使其在非生物环境中也能发挥作用。这些异聚物模仿凝聚体中的非结构化蛋白质,模仿无膜细胞器。在最近一期的《自然》杂志上,徐和亚历山大-卡茨领导的一个团队通过选择调节其化学微环境的单体来复制酶的功能,设计了具有酶活性的异聚聚合物。
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引用次数: 0
A redesigned aldehyde dehydrogenase enables intermolecular biocatalytic amide formation from aldehydes and amines 重新设计的醛脱氢酶使分子间的生物催化酰胺形成从醛和胺
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2026-02-25 DOI: 10.1016/j.chempr.2026.102994
Francesco Mascia , Magdalena Abramiuk , Aneta Swárovská , Wolfgang Kroutil
Amide formation represents a key reaction in pharmaceutical synthesis, for which more environmentally friendly methods are sought. In Science, Gao et al. report a biocatalytic oxidative strategy exploiting a redesigned aldehyde dehydrogenase that allows the coupling of aldehydes with amines at the expense of an oxidant [NAD(P)+, molecular oxygen].
酰胺形成是药物合成中的一个关键反应,因此需要寻找更环保的方法。在《科学》杂志上,Gao等人报道了一种利用重新设计的醛脱氢酶的生物催化氧化策略,该策略允许醛与胺的偶联,而牺牲氧化剂[NAD(P)+,分子氧]。
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引用次数: 0
Vacancy-interface coupling in nanomaterials for photocatalytic energy and environmental applications 纳米材料在光催化能源和环境方面的应用
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2026-02-19 DOI: 10.1016/j.chempr.2025.102913
Meijun Guo , Shuai Zhang , Jingrun Ran , Shi-Zhang Qiao
Vacancy-interface coupling has emerged as a powerful strategy for boosting photocatalytic performance through the synergistic regulation of charge dynamics, interfacial structure, and surface pathways. Engineering vacancies at interfaces allow photogenerated carriers to be trapped, separated, and directed to reactive sites, enhancing activity and selectivity. This perspective highlights recent advances in vacancy-mediated interfacial engineering for solar-driven transformations through representative cases in plastics and biomass photoreforming, H2O2 evolution, water splitting, and CO2 reduction. Particular emphasis is placed on in situ spectroscopic evidence for the dynamic evolution of vacancies and their real-time interactions with reactive sites. By integrating experimental insights with theoretical modeling, we demonstrate how vacancy-interface coupling results in robust, tunable, and efficient photocatalysts. Finally, we outline key challenges and opportunities for developing robust and application-oriented systems that fully exploit defect-interface synergy for sustainable energy and environmental applications.
空位-界面耦合已经成为通过电荷动力学、界面结构和表面途径的协同调节来提高光催化性能的一种强有力的策略。界面上的工程空缺允许光生成的载流子被捕获、分离并定向到反应位点,从而提高活性和选择性。这一观点强调了空缺介导的界面工程在太阳能驱动转化中的最新进展,通过塑料和生物质光重整、H2O2演化、水裂解和CO2还原的代表性案例。特别强调的是放置在原位光谱证据的动态演变的空缺和他们的实时相互作用与反应位点。通过将实验见解与理论建模相结合,我们展示了空位界面耦合如何产生鲁棒、可调和高效的光催化剂。最后,我们概述了开发健壮和面向应用的系统的关键挑战和机遇,这些系统充分利用了可持续能源和环境应用的缺陷接口协同作用。
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引用次数: 0
Understanding and mitigating degradation in amine-based sorbents for CO2 direct air capture 了解和减轻胺基吸附剂对二氧化碳直接空气捕获的降解
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2026-02-26 DOI: 10.1016/j.chempr.2026.102958
Anthony J. Varni , Wade A. Braunecker , Marcos F. Calegari Andrade , G. Michael Carroll , Yoseph A. Guta , Elwin Hunter-Sellars , Christopher W. Jones , Noemi Leick , Sichi Li , Amitesh Maiti , Maxwell A.T. Marple , Hyun June Moon , Miles A. Sakwa-Novak , Carsten Sievers , Nicholas A. Strange , Simon H. Pang
The success of direct air capture (DAC) of CO2 depends on sorbents that combine high capacity, low energy requirements, and long-term durability. Amine-based sorbents—including solid-supported aminopolymers, grafted amines, and amine-functionalized resins—remain the leading candidates, but their limited lifetimes drive up costs and constrain deployment. In this review, we outline the current understanding of amine-based sorbent degradation with an emphasis on clearly identifying what is known about structure-property-performance relationships, as well as important knowledge gaps. More specifically, we discuss how polymer chemistry, sorbent design variables, and environmental and process conditions contribute to performance loss. In parallel, we outline how advances in spectroscopy, modeling, and accelerated testing are beginning to illuminate chemical and physical degradation mechanisms. Looking forward, we identify future research directions that will be critical for gaining a deeper understanding of degradation, as well as opportunities for developing innovative mitigation strategies for improving the lifetime of amine-based sorbents.
二氧化碳的直接空气捕获(DAC)的成功取决于吸附剂的高容量,低能源需求和长期耐用性。胺基吸附剂(包括固载氨基聚合物、接枝胺和胺功能化树脂)仍然是主要的候选材料,但它们有限的使用寿命提高了成本,限制了部署。在这篇综述中,我们概述了目前对胺基吸附剂降解的理解,重点是清楚地识别已知的结构-性能-性能关系,以及重要的知识空白。更具体地说,我们讨论了聚合物化学、吸附剂设计变量、环境和工艺条件如何导致性能损失。同时,我们概述了光谱学、建模和加速测试的进展如何开始阐明化学和物理降解机制。展望未来,我们确定了未来的研究方向,这些方向对于深入了解降解至关重要,也有助于开发创新的缓解策略,以改善胺基吸附剂的使用寿命。
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引用次数: 0
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