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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
Precisely modulating Li2CO3 coverage on Ni-rich cathode boosts sulfide solid-state lithium battery performance 精确调节富镍阴极上Li2CO3的覆盖范围可提高硫化物固态锂电池的性能
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2025-10-14 DOI: 10.1016/j.chempr.2025.102775
Yiman Feng (冯依曼) , Zhixing Wang , Hongling Yi , Yucen Yan , Gui Luo , Duo Deng , Wenjie Peng , Xiaoping Zhou , Wenchao Zhang , Hui Duan , Feixiang Wu , Jiexi Wang (王接喜)
All-solid-state lithium batteries (ASSLBs) equipped with Ni-rich layered oxide cathodes (NRLOs, Ni content ≥ 80%) exhibit promising electrochemical performance. However, there is significant controversy regarding the role of carbonate species on the surface of NRLOs. This study explores the impact of surface lithium carbonate (Li2CO3) on NRLOs in sulfide ASSLBs using carbon dioxide (CO2) atmosphere treatment to precisely control the amount of Li2CO3. As an electronic insulator, Li2CO3 suppresses space-charge effects and interfacial side reactions with the sulfide solid electrolyte, enhancing cycling stability. Surprisingly, the ASSLB with the NRLO exposed to CO2 for 20 min demonstrates a capacity of 144 mAh g−1 at 2 C and maintains the capacity retention of 95.8% after 200 cycles at 0.5 C. However, excessive Li2CO3 impedes ion kinetics, reduces capacity, and promotes CO2 release that degrades electrolyte integrity, leading to rapid failure. The results highlight the critical balance required in surface carbonate regulation for achieving high-energy-density sulfide ASSLBs.
配备富镍层状氧化物阴极(NRLOs, Ni含量≥80%)的全固态锂电池(ASSLBs)具有良好的电化学性能。然而,碳酸盐物种在NRLOs表面的作用存在很大争议。本研究采用二氧化碳(CO2)气氛处理精确控制Li2CO3的量,探讨了表面碳酸锂(Li2CO3)对硫化物ASSLBs中NRLOs的影响。作为电子绝缘体,Li2CO3抑制了空间电荷效应和与硫化物固体电解质的界面副反应,提高了循环稳定性。令人惊讶的是,将NRLO暴露在CO2中20分钟,ASSLB在2℃下的容量为144 mAh g - 1,在0.5 C下循环200次后容量保持率为95.8%。然而,过量的Li2CO3阻碍了离子动力学,降低了容量,促进了二氧化碳的释放,降低了电解质的完整性,导致快速失效。结果强调了实现高能量密度硫化物asslb所需的表面碳酸盐调节的临界平衡。
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引用次数: 0
Stereoselective hydroarylation of secondary allylic alcohols via a “transient shielding” mechanism 通过“瞬态屏蔽”机制的仲烯丙醇立体选择性氢化芳基化
IF 19.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-12 Epub Date: 2025-10-24 DOI: 10.1016/j.chempr.2025.102791
Peng-Bo Bai , Liwei Wang , Chun-Yuan Bai , Jia-Yi Li , Xin-Xin Yang , Chen Yang , Xianglu Peng , Xiaotian Qi , Gang-Wei Wang
The hydroarylation of alkenes is a powerful approach for introducing aryl functionality into chemical feedstocks. However, its application to alkenes bearing a pre-existing C(sp³) stereocenter remains challenging because of the need for simultaneous control over regio- and stereoselectivity. Herein, we report a Ni-catalyzed, redox-neutral hydroarylation (and hydroalkenylation) of diverse secondary allylic alcohols using aryl (and alkenyl) boronic acids. This method, enabled by a unique “transient shielding” mechanism, affords branched products with excellent chemo-, regio-, and diastereoselectivity. Notably, when readily available enantioenriched allylic alcohols are employed, the reaction furnishes enantiopure β-phenethyl alcohols featuring vicinal tertiary-tertiary or tertiary-quaternary stereocenters. Moreover, when combined with a simple redox sequence, this method allows for the enantiodivergent synthesis of all four possible stereoisomers of the product. Experimental studies and detailed density functional theory (DFT) calculations support the proposed mechanism.
烯烃的氢化芳基化是将芳基官能团引入化工原料的有力途径。然而,由于需要同时控制区域选择性和立体选择性,将其应用于具有预先存在的C(sp³)立体中心的烯烃仍然具有挑战性。在这里,我们报道了镍催化的,氧化还原中性的,用芳基(和烯基)硼酸对不同的仲烯丙醇进行氢化芳基化(和氢化烯基化)。这种方法通过一种独特的“瞬态屏蔽”机制,提供了具有优异的化学选择性、区域选择性和非对映选择性的分支产物。值得注意的是,当使用容易获得的富集对映异构的烯丙醇时,反应会得到具有邻近叔-叔或叔-季立体中心的对映纯β-苯乙基醇。此外,当与简单的氧化还原序列相结合时,该方法允许对映发散合成产品的所有四种可能的立体异构体。实验研究和详细的密度泛函理论(DFT)计算支持提出的机制。
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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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Chem
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