Chinese Chemical Letters最新文献_第10页

Adsorption, transformation, biodegradation and potential ecological toxicity of iron-based nanoparticles in the aqueous environment 铁基纳米颗粒在水环境中的吸附、转化、生物降解和潜在的生态毒性

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-07-16 DOI: 10.1016/j.cclet.2025.111600

Yang Gao , Xiaocheng Wei , Jing Sun , Shaohu Ouyang

Iron-based nanoparticles (Fe-NPs) have wide environmental applications in various areas due to their excellent physicochemical properties, and these processes also increase their release into the water environment. However, the existing literature on environmental behavior fate (e.g., sorption and transformation) and potential ecotoxicity of Fe-NPs remains limited, which is vital for understanding the Fe-NPs environmental behavior and application as a multifunctional product. In this review, the green synthesis, characterization, and environmental application of Fe-NPs are summarized. We systematically examined the impacts of Fe-NPs physicochemical properties on its adsorption, transformation (e.g., aggregation dispersion, dissolution, oxidation), and biodegradation behavior in aqueous ecosystems. Moreover, we highlight the potential ecological toxicity of Fe-NPs to aquatic organisms. Upon exposure in water environments, Fe-NPs have potential ecological toxicity on aquatic organisms (e.g., microorganisms, plants, zooplankton, and fish). The common mechanisms of Fe-NPs ecotoxicity (e.g., bioaccumulation, oxidation stress, and DNA damage) at the cellular level are presented and the remaining unclear points on nano-toxic mechanisms (e.g., metabolic disturbance, genotoxicity) are discussed. Given the unresolved issues, the substantial gaps and the environmental risk assessment of Fe-NPs require further attention in the future. This paper will provide useful information for assessing the fate and potential ecological risks associated with Fe-NPs in aquatic environments.

铁基纳米颗粒（Fe-NPs）由于其优异的物理化学性质，在各个环境领域有着广泛的应用，这些过程也增加了它们在水环境中的释放。然而，关于Fe-NPs的环境行为命运（如吸附和转化）和潜在生态毒性的现有文献仍然有限，这对于了解Fe-NPs作为多功能产品的环境行为和应用至关重要。本文综述了Fe-NPs的绿色合成、表征及其在环境中的应用。我们系统地研究了Fe-NPs的物理化学性质对其在水生态系统中的吸附、转化（如聚集、分散、溶解、氧化）和生物降解行为的影响。此外，我们强调了铁- nps对水生生物的潜在生态毒性。Fe-NPs暴露于水环境后，对水生生物（如微生物、植物、浮游动物和鱼类）具有潜在的生态毒性。本文介绍了Fe-NPs在细胞水平上的常见生态毒性机制（如生物积累、氧化应激和DNA损伤），并讨论了纳米毒性机制（如代谢紊乱、遗传毒性）的其他不明确点。鉴于尚未解决的问题，未来需要进一步关注铁- nps的巨大差距和环境风险评估。本文将为评价水体环境中Fe-NPs的命运和潜在生态风险提供有用的信息。

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引用次数: 0

Harnessing chirality: A new dawn in inorganic nanomaterial synthesis and biomedical applications 利用手性：无机纳米材料合成和生物医学应用的新曙光

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2024-12-23 DOI: 10.1016/j.cclet.2024.110791

Yue Pan , Jing Ren , Yifan Sun , Luying Lu , Jia Gao , Liping Chen , Shancheng Yan , Zhiyang Li

Chirality, a fundamental property of biological systems, is widely present at the molecular, cellular, and tissue levels. Current studies have shown that chiral inorganic nanomaterials, have good chiral optical activity as well as high enantioselectivity. When interacting with biological systems, the enantioselective behavior of chiral inorganic nanomaterials towards biomolecules can distinguish between different isomers of biomarkers, which, combined with the excellent optical activity of chiral inorganic nanomaterials, allows for the rapid and sensitive detection of biomarkers. Moreover, chiral inorganic nanomaterials exhibit stronger internalization and retention capabilities in cells, and by specifically targeting specific biomarkers can regulate cellular activity and catalyze related reactions, thereby achieving synergistic treatment of various diseases. In addition, chiral inorganic nanomaterials also have good biocompatibility and do not cause cell damage in living organisms. Moreover, chiral inorganic nanomaterials have programmable surfaces that can be tailored to suit specific biological functions. Due to the important role of chiral inorganic nanomaterials in the biomedical field, this paper summarizes and discusses the synthesis and biomedical applications of chiral inorganic nanomaterials. It further looks forward to its future development prospects to provide a reference for promoting relevant research on chiral inorganic nanomaterials in biomedical fields.

手性是生物系统的基本性质，广泛存在于分子、细胞和组织水平。目前的研究表明，手性无机纳米材料具有良好的手性光学活性和对映体选择性。在与生物系统相互作用时，手性无机纳米材料对生物分子的对映选择性行为可以区分生物标志物的不同异构体，结合手性无机纳米材料优异的光学活性，可以快速、灵敏地检测生物标志物。此外，手性无机纳米材料在细胞内表现出更强的内化和滞留能力，并通过特异性靶向特定生物标志物调节细胞活性，催化相关反应，从而实现多种疾病的协同治疗。此外，手性无机纳米材料还具有良好的生物相容性，在生物体中不会造成细胞损伤。此外，手性无机纳米材料具有可编程的表面，可以定制以适应特定的生物功能。鉴于手性无机纳米材料在生物医学领域的重要作用，本文对手性无机纳米材料的合成及其在生物医学领域的应用进行了综述和讨论。进一步展望其未来发展前景，为推动手性无机纳米材料在生物医学领域的相关研究提供参考。

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引用次数: 0

Achieving enhancing endosome escape of Tat47-57-derived stapled peptides through decafluorobiphenyl bridge 通过十氟联苯桥增强tat47 -57衍生的钉接肽的核内体逃逸

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-05-01 DOI: 10.1016/j.cclet.2025.111278

Shu Li , Yuanyuan Tang , Xiaojing Liu , Shibo Song , Baokang Zhu , Min Chang , Yali Peng

Cell-penetrating peptides (CPPs) hold great potential as a tool using non-invasive delivery of therapeutic or diagnostic molecules into mammalian cells, but their broad application has been limited by poor endosomal escape. Thus, the rational design and selection of CPPs remains a challenge and calls for deeper mechanistic understandings. Here, we developed novel stapled cell-penetrating peptides based on the highly positively charged HIV Tat47-57 peptide using decafluorobiphenyl-cysteine S_NAr chemistry which selectively disrupt endosomal membranes. A series of stapled peptides with a cross-linked structure were synthesized and investigated their cellular uptake, endosomal escape and intracellular delivery of cargoes. Among these peptides, analogues P3 and P6 demonstrated the highest cellular uptake and endosomal escape activities with efficiencies 3.5−9-fold higher than that of Tat47-57. Notably, the results demonstrated that the decafluorobiphenyl bridge of stapled peptides exhibited significant ability for cellular uptake and endosomal escape. Moreover, we found that fluorine atoms of decafluorobiphenyl bridge played a key role for disrupting endosomal membranes. Finally, the utility of this strategy has been demonstrated by the intracellular delivery of biomacromolecules (avidin and negatively charged phosphopeptides). Together, these results suggest that the decafluorobiphenyl-cysteine S_NAr chemistry may be an efficient strategy for the development of novel stapled CPPs.

细胞穿透肽（CPPs）作为一种将治疗或诊断分子无创递送到哺乳动物细胞中的工具具有巨大的潜力，但其广泛应用受到内体逃逸能力差的限制。因此，cps的合理设计和选择仍然是一个挑战，需要更深入的机理理解。在这里，我们利用十氟联苯半胱氨酸SNAr化学开发了基于高正电荷HIV Tat47-57肽的新型钉接细胞穿透肽，该肽选择性地破坏了内体膜。合成了一系列具有交联结构的钉接肽，并研究了它们的细胞摄取、内体逃逸和细胞内转运。在这些多肽中，类似物P3和P6表现出最高的细胞摄取和内体逃逸活性，效率比Tat47-57高3.5 - 9倍。值得注意的是，结果表明，钉接肽的十氟联苯桥具有显著的细胞摄取和内体逃逸能力。此外，我们发现十氟联苯桥的氟原子在破坏内体膜方面发挥了关键作用。最后，生物大分子（亲和素和带负电荷的磷酸肽）的细胞内递送证明了这种策略的效用。总之，这些结果表明，十氟联苯-半胱氨酸SNAr化学可能是开发新型钉接CPPs的有效策略。

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引用次数: 0

Facet engineering of NH2-MIL-125(Ti) for enhanced synergistic adsorption and photocatalysis reduction of U(VI) under visible light NH2-MIL-125（Ti）在可见光下增强协同吸附和光催化还原U（VI）的Facet工程

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2024-12-06 DOI: 10.1016/j.cclet.2024.110733

Wenting Li , Nina Wu , Chengze Li , Jin Guo , Guangxun Zhang , Huan Pang

Modulating the exposed facets of metal-organic frameworks (MOFs) is an effective strategy to enhance the synergistic effects between adsorption and photocatalytic reduction of U(VI). Herein, we successfully synthesized four morphologically distinct types of NH₂-MIL-125(Ti), offering insights into the impact of facet engineering on the combined adsorption and photoreduction of U(VI). An elevated exposure ratio of the {001} facet endows NH₂-MIL-125(Ti) with a larger surface area, enhanced light absorption, and efficient separation of photogenerated charge carriers. Among the four photocatalysts (W, D, S and T), T with a high proportion of {001} facets, demonstrated outstanding adsorption-photocatalytic synergy, achieving over 97 % of U(VI) within 20 min of visible light irradiation across a broad concentrations and pH range, without requiring a hole-trapping agent. The uranium extraction mechanism involves U(VI) coordination and chelation with active sites during adsorption, followed by reduction to U(IV) via photogenerated electrons during photocatalysis. This study highlights the use of facet engineering to enhance adsorption and photocatalytic efficiency in MOF-based photocatalysts.

调节金属有机骨架（mof）的暴露面是增强吸附和光催化还原U（VI）之间协同效应的有效策略。在此，我们成功地合成了四种形态不同的NH2-MIL-125(Ti)，为facet工程对U（VI）的联合吸附和光还原的影响提供了见解。{001}面曝光率的提高使NH2-MIL-125（Ti）具有更大的表面积，增强的光吸收，并有效地分离光生电荷载流子。在四种光催化剂（W、D、S和T）中，{001}晶片比例较高的T表现出出色的吸附-光催化协同作用，在较宽的浓度和pH范围内，在可见光照射20 min内，不需要空穴捕获剂，就能达到97% %以上的U（VI）。铀的萃取机理是吸附过程中U（VI）与活性位点的配位和螯合，光催化过程中通过光生电子还原为U（IV）。本研究强调了利用facet工程来提高mof基光催化剂的吸附和光催化效率。

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引用次数: 0

Ferrate(VI) combined with sulfur(IV) as an effective process for aromatic organoarsenic degradation: Essential role of Fe(III) flocs 高铁酸盐（VI）与硫（IV）联合降解芳香族有机砷的有效过程：铁（III）絮凝体的重要作用

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-07-03 DOI: 10.1016/j.cclet.2025.111538

Chang Xu , Mengfan Luo , Jia Zhao , Jialong Yin , Can Feng , Heng Zhang , Peng Zhou , Zhaokun Xiong , Bo Lai

This study employed the ferrate(VI)/sulfur(IV) (Fe(VI)/S(IV)) system to degrade aromatic organoarsenic compounds, with a focus on elucidating the role of in situ-formed Fe(III) flocs. The introduction of S(IV) significantly enhanced oxidative degradation efficiency compared to Fe(VI) alone, achieving 94.8 % p-arsanilic acid (p-ASA) degradation within 3 min. The evolution of active species under varying S(IV) dosages was systematically investigated via radical quenching experiments and probe compound analysis. SO₄^•−, ^•OH and Fe(IV)/Fe(V) were identified as the dominant reactive species in the Fe(VI)/S(IV) system, with Fe(IV)/Fe(V) serving as the primary driver of p-ASA degradation. Characterization revealed that Fe(III) flocs contributed to arsenic (As) adsorption. While S(IV) addition altered the morphology and structure of Fe(III) flocs, these changes exerted negligible effects on As adsorption capacity. A plausible degradation pathway for p-ASA was proposed, supported by density functional theory (DFT) calculations and degradation product analysis. The system demonstrated robust resistance to common interfering ions, while the low toxicity of degradation byproducts highlighted its potential as a sustainable technology for AOCs elimination. This work elucidated structural modifications in Fe(III) flocs induced by S(IV) and underscored the pivotal role of Fe(IV)/Fe(V), positioning the Fe(VI)/S(IV) system as a promising strategy for AOCs degradation.

本研究采用高铁酸盐(VI)/硫（IV） (Fe（VI)/S(IV)）体系降解芳香族有机砷化合物，重点阐明了原位形成的Fe（III）絮凝体的作用。与单独使用Fe（VI）相比，S（IV）的引入显著提高了氧化降解效率，在3 min内实现了94.8 %对氨基苯甲酸（p-ASA）的降解。通过自由基猝灭实验和探针化合物分析，系统地研究了不同S（IV）剂量下活性物质的演化。在Fe(VI)/S（IV）体系中，SO4•−、•OH和Fe(IV)/Fe(V)是主要的活性物质，其中Fe(IV)/Fe(V)是p-ASA降解的主要驱动力。表征表明，Fe（III）絮凝体有助于砷（As）的吸附。虽然S（IV）的加入改变了Fe（III）絮凝体的形态和结构，但这些变化对As吸附能力的影响可以忽略不计。在密度泛函理论（DFT）计算和降解产物分析的支持下，提出了p-ASA的合理降解途径。该系统显示出对常见干扰离子的强大抗性，而降解副产物的低毒性突出了其作为消除AOCs的可持续技术的潜力。本研究阐明了S（IV）诱导Fe（III）絮凝体的结构修饰，并强调了Fe(IV)/Fe(V)的关键作用，将Fe(VI)/S（IV）体系定位为AOCs降解的一种有前景的策略。

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引用次数: 0

Orthogonal configurative dye 2-anthryl asymmetric aza-BODIPY enhancing SOCT-ISC for phototherapy 正交构型染料2-蒽基不对称氮杂体吡啶增强SOCT-ISC光疗

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-04-02 DOI: 10.1016/j.cclet.2025.111171

Shu Lv , Xiuyan Gong , Yunsheng Xue , Gaowu Qin , Xin-Dong Jiang , Guiling Wang

Orthogonal molecular orbitals (MOs) of donor-acceptor (D-A) pairs favor the spin-orbit charge transfer intersystem crossing (SOCT-ISC) transition, and herein 2-anthryl asymmetric aza-boradiazaindacene (aza-BODIPY) (AH-BDP) was designed and prepared. According to the X-ray crystallography, the steric hindrance in orthogonal molecule AH-BDP results in a large dihedral angle between the two MO planes. Since low ΔE_st prefers to undertake ISC and efficiently produce reactive oxygen species (ROS), the calculated ΔE_st for AH-BDP is 0.757 eV, significantly smaller than that of the aza-BDOPY without anthryl group DH-BDP (1.052 eV). AH-BDP as a heavy-atom-free photosensitizer not only produced the singlet oxygen, but also possessed photothermal conversion efficiency. Self-assembly AH-BDP nanoparticles (NPs) could efficiently induce HCT116 cells elimination in nude mice through ROS/heat-mediated pathways.

本文设计并制备了2-蒽基不对称氮杂-硼二氮杂二烯（aza-BODIPY）（AH-BDP）分子轨道的正交给体-受体（D-A）对有利于自旋-轨道电荷转移系统间交叉（SOCT-ISC）转变。x射线晶体学表明，正交分子AH-BDP中的位阻导致两个MO平面之间存在较大的二面角。由于低ΔEst更倾向于进行ISC并高效产生活性氧（ROS），因此AH-BDP的计算ΔEst为0.757 eV，明显小于不含蒽基DH-BDP的aza-BDOPY （1.052 eV）。AH-BDP作为一种无重原子光敏剂，不仅产生单线态氧，而且具有光热转换效率。自组装AH-BDP纳米颗粒（NPs）可以通过ROS/热介导途径有效诱导裸鼠HCT116细胞清除。

引用次数: 0

Boosting photocatalytic overall water splitting efficiency and stability with adjacent cobalt-based dual cocatalysts 与相邻的钴基双助催化剂提高光催化整体水分解效率和稳定性

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-07-11 DOI: 10.1016/j.cclet.2025.111581

Li Tian , Xiangjiu Guan , Jingkuo Qu , Anna Dai , Jiaye Cai , Zheng Zhang , Shichao Zong , Liejin Guo

Cocatalysts are pivotal in realizing photocatalytic overall water splitting (POWS) by mitigating carrier recombination and expediting reaction kinetics. Nevertheless, conventional cocatalysts still faces with challenges in balancing high efficiency and low cost. Herein, adjacent CoP and CoOOH, as noble-metal-free dual cocatalysts for hydrogen/oxygen evolution, are introduced onto the surface of Al-doped SrTiO₃ (Al:STO), achieving stable and efficient POWS, with a hydrogen and oxygen evolution rate of 4.86 and 2.30 mmol h^-1 g^-1, respectively, and an apparent quantum yield of 12.7 % at 350 ± 10 nm. The superior performance is attributed to the unique adjacent structure of CoP and CoOOH dual cocatalysts. Functioning as critical reactive sites for hydrogen and oxygen evolution, respectively, co-modification of CoP and CoOOH effectively promotes the surface redox reaction. Notably, due to the Schottky junction form between CoP and CoOOH, the uniformly distributed and tightly attached adjacent CoP-CoOOH dual cocatalysts shortened the distance of both charge-carrier migration from bulk to the surface of photocatalyst and proton transfer from oxidation sites to reduction sites, thereby enhancing the charge-separation efficiency and protecting CoP against oxidation during photocatalytic overall water splitting process. This work offers innovative insights for designing efficient, noble-metal-free cocatalysts for POWS.

助催化剂是实现光催化全水分解（POWS）的关键，它能减轻载体重组，加快反应动力学。然而，传统的助催化剂在平衡高效和低成本方面仍然面临着挑战。本文将邻近的CoP和CoOOH作为无重金属的析氢/析氧双助催化剂引入到Al掺杂SrTiO3 （Al:STO）表面，实现了稳定高效的POWS，在350 ± 10 nm处，析氢和析氧速率分别为4.86和2.30 mmol h-1 g-1，表观量子产率为12.7 %。这种优异的性能归功于CoP和CoOOH双助催化剂独特的相邻结构。CoP和CoOOH的共修饰分别作为析氢和析氧的关键反应位点，有效地促进了表面氧化还原反应。值得注意的是，由于CoP与CoOOH之间存在Schottky结，相邻的CoP-CoOOH双助催化剂分布均匀且附着紧密，缩短了电荷载流子从本体到光催化剂表面的迁移距离和质子从氧化位点到还原位点的转移距离，从而提高了电荷分离效率，保护CoP在光催化整体水分解过程中不被氧化。这项工作为设计高效、无贵金属的战俘共催化剂提供了创新的见解。

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引用次数: 0

Metal diborides as robust and highly stable electrodes for efficient electrocatalytic reduction of CO2 to CO in ionic liquid-based electrolytes 金属二硼化物是离子液体电解质中有效的电催化将CO2还原为CO的强大且高度稳定的电极

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-08-06 DOI: 10.1016/j.cclet.2025.111675

Yidan Mao , Bingyu Li , Shuailing Ma , Siwen Cui , Zihan Zhang , Pinwen Zhu , Kongsheng Qi , Xiaodong Li , Weiwei Dong , Wei Luo , Rajeev Ahuja , Dexin Yang , Tian Cui

The electrocatalytic reduction of carbon dioxide (CO₂) into fuels holds significant promise for addressing energy and environmental challenges, albeit hindered by constraints in conversion efficiency, production rates, and electrode stability. Metal diborides are considered as promising electrocatalysts that may demonstrate superior CO₂ electroreduction performance due to their distinctive electronic properties. Herein, a series of novel bulk metal diborides, encompassing transition metals from group IVB to group VIIB elements, were fabricated using a high pressure-high temperature technique, which were directly utilized as self-supporting electrodes for electrocatalytic reduction of CO₂. The zirconium diboride (ZrB₂) electrode stood out in metal diborides with superior electrocatalytic activity in generating carbon monoxide (CO), achieving a Faradaic efficiency of 92.2% at −2.2 V vs. Ag/Ag⁺ in ionic liquid-based electrolytes. Impressively, the ZrB₂ electrode demonstrated stable catalysis of CO₂ reduction to CO over a nearly 60-h electrolysis period. Furthermore, the ZrB₂ electrode and ionic liquid-based electrolytes could synergistically catalyze the reduction of CO₂ to CO. Experimental results and density functional theory calculations support the notion that exposed metal sites on the ZrB₂ (001) surface could enhance *CO desorption and restrain the hydrogen evolution reaction, thereby facilitating the conversion of CO₂ into CO.

电催化将二氧化碳（CO2）还原为燃料对于解决能源和环境挑战具有重要的前景，尽管受到转换效率、生产率和电极稳定性的限制。金属二硼化物由于其独特的电子特性，被认为是一种很有前途的电催化剂，可能表现出优越的CO2电还原性能。本文采用高压-高温技术制备了一系列包含从IVB族到VIIB族过渡金属的新型块状金属二硼化物，并将其直接用作电催化还原CO2的自支撑电极。二硼化锆（ZrB2）电极在生成一氧化碳（CO）方面表现出优异的电催化活性，在−2.2 V下，相对于离子液体电解质中Ag/Ag+的法拉第效率达到92.2%。令人印象深刻的是，ZrB2电极在近60小时的电解时间内表现出稳定的CO2还原成CO的催化作用。此外，ZrB2电极和离子液体电解质可以协同催化CO2还原为CO。实验结果和密度泛函理论计算支持这样的观点，即ZrB2（001）表面暴露的金属位点可以增强*CO的解吸，抑制析氢反应，从而促进CO2转化为CO。

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引用次数: 0

Triply stabilized NH4V4O10 via glycine pillaring enables universal cathode for outstanding rate aqueous zinc-ion batteries and stable aqueous ammonium-ion batteries 通过甘氨酸柱状结构，三重稳定的NH4V4O10可用于高倍率的水锌离子电池和稳定的水铵离子电池

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-08-16 DOI: 10.1016/j.cclet.2025.111729

Zihan Wang , Meizhen Dai , Pengcheng Song , Wenxuan Liu , Junhua You , Fang Hu , Yusheng Wu , Kai Zhu

NH₄V₄O₁₀ has attracted significant attention as a cathode material for aqueous zinc-ion batteries (AZIBs) due to its adjustable interlayer spacing (∼9.5 Å) and high theoretical specific capacity (∼400 mAh/g). However, its development is hindered by sluggish Zn²⁺ kinetics and structural instability. In this work, a glycine (Gly) intercalation strategy is demonstrated, which establishes three stabilization mechanisms in the Gly-NVO cathode: (1) Gly pillars are shown to expand the interlayer spacing to 1.21 nm; (2) Hydrogen-bonding networks are formed between layers; (3) Reversible NH₄⁺ (de)intercalation behavior is observed. The Gly-NVO cathode delivers a capacity of 520 mAh/g at 0.2 A/g (393 Wh/kg energy density), along with outstanding rate capability (400 and 150 mAh/g at 10 and 50 A/g, corresponding to power densities of 5688 and 24.3 kW/kg, respectively). A capacity retention of 88.2 % is maintained after 10,000 cycles at 50 A/g. DFT calculations confirm that the introduction of Gly significantly enhances the electrical conductivity of NVO while effectively weakening electrostatic interactions, and energy barrier for Zn²⁺ intercalation and vanadium dissolution are reduced by Gly. Additionally, due to the reversible NH₄⁺ (de)intercalation behavior in Gly-NVO, the assembled aqueous ammonium-ion batteries (AAIBs) exhibit stable cycling ability. This work highlights organic molecule pre-intercalation as a viable strategy for optimizing the durability of ammonium vanadate cathodes.

NH4V4O10作为水性锌离子电池（azib）的正极材料，由于其可调节的层间距（~ 9.5 Å）和高理论比容量（~ 400 mAh/g）而引起了极大的关注。然而，由于Zn2+动力学迟缓和结构不稳定，阻碍了它的发展。在这项工作中，展示了甘氨酸（Gly）插入策略，该策略在Gly- nvo阴极中建立了三种稳定机制：(1)甘氨酸柱将层间距扩大到1.21 nm；(2)层间形成氢键网络；(3)观察到可逆的NH4+ (de)插层行为。gy - nvo阴极在0.2 a /g（393 Wh/kg能量密度）时提供520 mAh/g的容量，以及出色的速率能力（在10和50 a /g时400和150 mAh/g，对应的功率密度分别为5688和24.3 kW/kg）。在50 A/g下进行10,000次循环后，容量保持率为88.2 %。DFT计算证实，Gly的引入显著提高了NVO的电导率，同时有效地减弱了静电相互作用，并且Gly降低了Zn2+嵌入和钒溶解的能垒。此外，由于Gly-NVO中可逆的NH4+ (de)嵌入行为，组装的水铵离子电池（AAIBs）表现出稳定的循环能力。这项工作强调有机分子预插层是优化钒酸铵阴极耐久性的可行策略。

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引用次数: 0

Three-component alkenylcarboxylation of two distinct alkenes with CO2 via photoinduced palladium catalysis 光诱导钯催化下两种不同烯烃与CO2的三组分烯基羧化反应

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2026-04-01 Epub Date: 2025-05-12 DOI: 10.1016/j.cclet.2025.111304

Jie Zhou , Luping Hu , Rui Wang , Ruijie Wang , Jun Xu , Huajian Xu

Alkene cross-coupling provides a simple and efficient approach for constructing CC bonds using readily accessible alkene feedstocks. Despite significant progress in CC bonds formation through the difunctionalization of alkenes, analogous reaction involving two distinct alkenes remains extremely limited. Herein, we report the excited-state palladium(0) catalyzed alkenylcarboxylation of two distinct alkenes with CO₂, delivering a variety of carboxylic acids in moderate to excellent yields. This reaction features high regio- & chemoselectivity, broad substrate scope (>70 examples), and facile derivatization of products. Mechanistic studies indicate that the key step for this new strategy lies in the reductive activation of electron-deficient alkenes with the excited-state palladium complex to generate alkene radical anions. The current single-electron reduction strategy for alkenes catalyzed by photoexcited palladium(0) not only broadens the scope of excited palladium chemistry but also provides a mild approach for alkenes activation. Furthermore, this method serves as an efficient tool for the rapid construction of multiple CC bonds in a one-pot operation using two distinct alkenes.

烯烃交叉偶联提供了一个简单而有效的方法来构建CC键使用容易获得的烯烃原料。尽管通过烯烃的双官能化形成CC键取得了重大进展，但涉及两种不同烯烃的类似反应仍然非常有限。在此，我们报告了激发态钯(0)催化两种不同的烯烃与CO2的烯基羧化反应，以中等到优异的收率提供各种羧酸。该反应具有高区域化学选择性，底物范围广（70个例子）和产物易于衍生化的特点。机理研究表明，这一新策略的关键在于用激发态钯配合物还原激活缺电子烯烃，生成烯烃自由基阴离子。目前光激发钯(0)催化烯烃的单电子还原策略不仅拓宽了激发钯化学的范围，而且为烯烃的活化提供了一种温和的途径。此外，该方法是一种高效的工具，可以在一锅操作中使用两种不同的烯烃快速构建多个CC键。

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引用次数: 0