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Enhancing backbone organization and photovoltaic performance of M-series acceptors by using partially fluorinated side chains 通过使用部分氟化侧链增强 M 系列受体的骨架组织和光伏性能

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.06.005

Side-chain fluorination of nonfullerene acceptors (NFAs) has been rarely reported to enhance their photovoltaic performance, although it may improve their backbone organization and carrier mobilities. Here, we design new partially fluorinated side chains and incorporate them into M-series NFAs, which are featured with a ladder-type heteroheptacene-cored skeleton without sp³-hybridized carbons. Compared with the traditional M-series acceptor with non-fluorinated side chains (MC7F0), the NFA with partially fluorinated side chains (MC7F3) shows down-shifted energy levels, reduced miscibility, and more importantly, improved backbone organization, thereby leading to the formation of a 3D network packing structure with enhanced carrier transport. Consequently, the MC7F3-based device exhibits a power conversion efficiency of 17.61% and an excellent fill factor of 79.48%, both of which are among the best values for all A-D-A-type NFAs reported so far. The results highlight that side-chain fluorination can efficiently enhance π-conjugated backbone organization, improve intermolecular interaction, increase electron mobilities, and boost photovoltaic performance of NFAs.

非富勒烯受体（NFAs）的侧链氟化可改善其骨架组织和载流子迁移率，但很少有报道称氟化可提高其光伏性能。在这里，我们设计了新的部分氟化侧链，并将其加入到 M 系列非富勒烯受体中，这种受体具有梯形杂七烯芯骨架，没有 sp3 杂化碳。与传统的带有非氟化侧链的 M 系列受体（MC7F0）相比，带有部分氟化侧链的 NFA（MC7F3）能级下移，混溶性降低，更重要的是骨架组织得到改善，从而形成了三维网络堆积结构，载流子传输能力增强。因此，基于 MC7F3 的器件显示出 17.61% 的功率转换效率和 79.48% 的出色填充因子，这两项指标都是迄今所报道的所有 A-D-A 型 NFA 的最佳值之一。研究结果表明，侧链氟化可有效增强π-共轭骨架组织，改善分子间相互作用，提高电子迁移率，从而提高 NFA 的光伏性能。

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引用次数: 0

The legacy of Professor Li-Xin Dai: Organometallic and asymmetric catalysis 戴立新教授的遗产：有机金属催化和不对称催化

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.003

Prof. Li-Xin Dai will always be remembered for his development of organometallic chemistry and asymmetric synthesis, especially for the refining and synthesis of aureomycin, organoboron chemistry, and the development of novel chiral ligands for transition-metal-catalyzed asymmetric reactions. In addition to making significant contributions to science, Prof. Dai has also made a profound impact as an esteemed educator and mentor, imparting his knowledge and work ethic to future generations of chemists and fostering fruitful collaborations with his colleagues.

人们将永远铭记戴立新教授在有机金属化学和不对称合成方面的发展，尤其是在金霉素的提纯和合成、有机硼化学以及开发用于过渡金属催化不对称反应的新型手性配体方面。除了对科学做出重大贡献外，戴教授还作为一位受人尊敬的教育家和导师产生了深远的影响，他将自己的知识和职业道德传授给后代化学家，并与同事们建立了富有成效的合作关系。

引用次数: 0

Bioengineering of syrbactin megasynthetases for immunoproteasome inhibitor production 用于生产免疫蛋白酶体抑制剂的西林杆菌巨合成酶生物工程

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.07.013

The natural product (NP) class of syrbactins are potent proteasome inhibitors produced by hybrids of non-ribosomal peptide synthetases (NRPSs) and polyketide synthases (PKSs). Here, we describe the stepwise reassembly of an entire NRPS/PKS hybrid to produce a new syrbactin derivative by utilizing the recently described “eXchange Unit between Thiolation domains” (XUTs) approach. Remarkably, XUT-based engineering allowed the direct assembly of PKS and NRPS modules to introduce an α,β-unsaturated Michael system in a macrolactam moiety, which represents the inhibitory warhead of syrbactins. The novel derivative was produced in E. coli, isolated, and examined for its ability to inhibit yeast (yCP), human constitutive (cCP), and immunoproteasome (iCP). The engineered NP maintained the inhibitory activities of the syrbactin class but, due to rational modifications, inhibited iCP most strongly. Moreover, analysis of the crystal structure of yCP in complex with the derivative revealed further design strategies for even more specific iCP inhibition.

天然产物 (NP) 类西布曲明是由非核糖体肽合成酶 (NRPS) 和多肽合成酶 (PKS) 杂交产生的强效蛋白酶体抑制剂。在这里，我们描述了利用最近描述的 "硫化结构域之间的交换单元"（XUTs）方法，逐步重新组装整个 NRPS/PKS 杂交体，从而产生一种新的 syrbactin 衍生物。值得注意的是，基于 XUT 的工程学方法可以直接组装 PKS 和 NRPS 模块，从而在大内酰胺分子中引入一个 α、β-不饱和迈克尔系统，该系统代表了 syrbactins 的抑制性弹头。这种新型衍生物在大肠杆菌中产生、分离并检测了其抑制酵母（yCP）、人组成型（cCP）和免疫蛋白酶体（iCP）的能力。改造后的 NP 保持了 syrbactin 类的抑制活性，但由于进行了合理的修饰，对 iCP 的抑制作用最强。此外，通过分析 yCP 与衍生物复合物的晶体结构，还发现了进一步的设计策略，以实现更特异的 iCP 抑制作用。

引用次数: 0

Electroreduction of alkaline/natural seawater: Self-cleaning Pt/carbon cathode and on-site co-synthesis of H2 and Mg hydroxide nanoflakes 碱性/天然海水的电还原：自清洁铂/碳阴极和 H2 与氢氧化镁纳米片的现场共合成

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.05.018

Distributed coastal/offshore seawater splitting plants can facilitate H₂-based economy’s global deployment. Increasingly, studies emerge mostly focusing on inhibiting anodic oxidation of halide ions. Equally tricky cathodic precipitation in natural seawater reduction (NSR) is neglected due to the use of alkaline seawater in most studies. Herein, we explore possible strategies (introducing a proton sponge to change cathodic microenvironments, breaking local OH⁻ gradients, employing self-cleaning cathodes) to alleviate surface precipitation. We introduce a famous H₂ evolution-active metal, Pt, onto a self-cleaning carbon support with H₂ gas evacuation capability. Our proposed binder-free Pt/carbon cathode is more robust than many previous Pt/C cathodes for NSR. Moreover, we highlight possibilities of co-electrosynthesizing nano-sized Mg hydroxides and H₂ from natural seawater. This work suggests that designs of local environments, pH gradient disruption, and/or cathode architecture-based gas/liquid flows may suppress surface precipitation. We demonstrate in detail the various issues in NSR and possible solutions.

分布式沿海/近海海水分离厂可促进基于 H2 的经济在全球范围内的应用。越来越多的研究主要集中于抑制卤化离子的阳极氧化。同样，由于大多数研究都使用碱性海水，自然海水还原（NSR）中棘手的阴极沉淀问题也被忽视了。在此，我们探讨了减轻表面沉淀的可能策略（引入质子海绵以改变阴极微环境、打破局部 OH- 梯度、采用自清洁阴极）。我们将一种著名的具有 H2 演化活性的金属--铂--引入到具有 H2 气体排空能力的自清洁碳支持物中。我们提出的无粘结剂铂/碳阴极比以前许多用于 NSR 的铂/碳阴极更坚固。此外，我们还强调了从天然海水中共同电合成纳米级氢氧化镁和 H2 的可能性。这项工作表明，局部环境设计、pH 梯度破坏和/或基于阴极结构的气体/液体流动可以抑制表面沉淀。我们详细展示了 NSR 中的各种问题和可能的解决方案。

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引用次数: 0

Operando electrochemical NMR spectroscopy reveals a water-assisted formate formation mechanism 操作电化学核磁共振光谱揭示了水辅助甲酸盐形成机制

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.06.001

The affinity of oxygen (O)-bound species is a key factor in CO₂ reduction (CO₂R) reactions (including C₁ and C₂₊ products), although existing experimental methods cannot quantitatively track the O atoms active within CO₂R reactions in real time. Among the diversified products from CO₂R reactions, the formate (HCOO⁻) possesses the highest profit per mole of electrons. Here, we report an operando electrochemical nuclear magnetic resonance (NMR) method, which allows to quantitatively describe the complex species containing O atoms during the electrochemical CO₂R reactions. Based on Cu and bimetallic Cu-based materials (Bi₂CuO₄ and In₂Cu₂O₅) systems, we found that by introducing Bi and In metal adsorption sites, the O atoms of adsorbed H₂O can directly involve in the formation of HCOO⁻ through a water-assisted mechanism (∗COOH⁻ regeneration), thereby improving the selectivity of liquid HCOO⁻ product mostly from 34.2% to 98%. This strategy gives valuable insights into the design of HCOO⁻-favored catalysts.

与氧（O）结合的物种的亲和力是二氧化碳还原（CO2R）反应（包括 C1 和 C2+ 产物）中的一个关键因素，尽管现有的实验方法无法实时定量跟踪在 CO2R 反应中活跃的 O 原子。在 CO2R 反应的多种产物中，甲酸盐（HCOO-）每摩尔电子的利润最高。在此，我们报告了一种操作电化学核磁共振（NMR）方法，该方法可定量描述电化学 CO2R 反应过程中含有 O 原子的复杂物种。基于铜和双金属铜基材料（Bi2CuO4 和 In2Cu2O5）体系，我们发现通过引入 Bi 和 In 金属吸附位点，吸附 H2O 的 O 原子可通过水辅助机制（∗COOH- 再生）直接参与 HCOO- 的形成，从而将液态 HCOO- 产物的选择性从 34.2% 提高到 98%。这一策略为设计 HCOO 偏好催化剂提供了宝贵的启示。

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引用次数: 0

Elucidating the role of cathode identity: Voltage-dependent reversibility of anode-free batteries 阐明阴极特性的作用：无阳极电池的电压可逆性

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.06.008

The cathode material in a lithium (Li) battery determines the system cost, energy density, and thermal stability. In anode-free batteries, the cathode also serves as the source of Li for electrodeposition, thus impacting the reversibility of plating and stripping. Here, we show that the reason LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) cathodes deliver lower Coulombic efficiencies than LiFePO₄ (LFP) is the formation of tortuous Li deposits, acidic species in the electrolyte, and accumulation of “dead” Li⁰. Batteries containing an LFP cathode generate dense Li deposits that can be reversibly stripped, but Li is lost to the solid electrolyte interphase (SEI) and corrosion according to operando ⁷Li NMR, which seemingly “revives” dead Li⁰. X-ray photoelectron spectroscopy (XPS) and in situ ¹⁹F/¹H NMR indicate that these differences arise because upper cutoff voltage alters electrolyte decomposition, where low-voltage LFP cells prevent anodic decomposition, ultimately mitigating the formation of protic species that proliferate upon charging NMC811.

锂（Li）电池中的阴极材料决定了系统成本、能量密度和热稳定性。在无阳极电池中，阴极也是电沉积锂的来源，从而影响电镀和剥离的可逆性。在这里，我们发现 LiNi0.8Mn0.1Co0.1O2 (NMC811) 阴极的库仑效率低于 LiFePO4 (LFP)的原因是畸形锂沉积的形成、电解质中的酸性物质以及 "死 "锂的积累。含有 LFP 阴极的电池会产生可逆剥离的致密锂沉积物，但根据操作性 7Li NMR，锂会流失到固体电解质相间层（SEI）和腐蚀中，这似乎会 "复活 "死亡的 Li0。X 射线光电子能谱 (XPS) 和原位 19F/1H NMR 显示，出现这些差异的原因是上限截止电压改变了电解质分解，低电压 LFP 电池阻止了阳极分解，最终减轻了 NMC811 充电时增殖的原生物种的形成。

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引用次数: 0

Electrocatalytic reduction of nitrogen oxide species to ammonia 电催化氧化氮还原成氨

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.07.006

The nitrogen cycle is one of the most important biochemical cycles. However, the development of human society has led to a substantial release of nitrogen oxide species, both as ions (NO_x⁻) and gases (NO_x), into the environment, causing a considerable burden on the natural denitrification processes. Electrocatalytic reduction of NO_x⁻ and NO_x emerges as a promising approach to transform these waste products into valuable ammonia, thereby contributing to the restoration of the nitrogen cycle. This review provides a concise overview of recent advances in electrocatalytic NO_x⁻ and NO_x reduction to ammonia, including detailed reaction mechanisms, catalyst development strategies based on both theoretical and experimental results, and the design and selection of electrolytic cells. Furthermore, it highlights key challenges associated with scaling up the reaction from laboratory-scale to practical industrial-scale application and explores potential opportunities to upgrade this reaction.

氮循环是最重要的生化循环之一。然而，人类社会的发展导致大量氮氧化物以离子（NOx-）和气体（NOx）的形式释放到环境中，给自然脱氮过程造成了相当大的负担。电催化还原氮氧化物和氮氧化物是一种很有前景的方法，可将这些废物转化为有价值的氨，从而促进氮循环的恢复。本综述简要概述了电催化一氧化氮和氮氧化物还原成氨的最新进展，包括详细的反应机理、基于理论和实验结果的催化剂开发策略，以及电解槽的设计和选择。此外，该书还强调了将该反应从实验室规模扩大到实际工业规模应用所面临的关键挑战，并探讨了升级该反应的潜在机会。

引用次数: 0

Promoting stimuli-responsive motion in soft matter by host-guest interactions 通过主客体相互作用促进软物质的刺激响应运动

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.06.016

Soft actuators capable of performing complex mechanical motions are highly sought after for the development of next-generation smart materials. Nevertheless, none of the soft actuators reported to date have achieved multiple actuation modes using a single material. To overcome this limitation, we present a responsive composite film that displays distinct actuation modes when exposed to organic vapors. This material is readily prepared and scaled up by incorporating novel urea-cage compounds into a polymer matrix. Through a comprehensive investigation into the actuation mechanism, we demonstrate that the exceptional actuation behavior arises from the polymorphic transformations of the crystalline urea cages, which are triggered by selective host-guest interactions between the cages and solvent guests. It is worth emphasizing that, for the first time, the tool of host-guest chemistry has been harnessed to achieve complex mechanical motion in a soft actuator.

能够执行复杂机械运动的软致动器在下一代智能材料的开发中备受追捧。然而，迄今为止所报道的软致动器中，还没有一种能利用单一材料实现多种致动模式。为了克服这一局限性，我们提出了一种反应性复合薄膜，它在暴露于有机蒸汽时能显示出不同的致动模式。通过在聚合物基体中加入新型脲笼化合物，这种材料很容易制备和放大。通过对致动机理的全面研究，我们证明这种特殊的致动行为源于结晶脲笼的多态转变，这种转变是由脲笼和溶剂客体之间的选择性主客体相互作用引发的。值得强调的是，我们首次利用主客体化学工具在软致动器中实现了复杂的机械运动。

引用次数: 0

Bridging gaps between lab- and fab-oriented anode design for proton exchange membrane water electrolyzers 弥合质子交换膜水电解槽实验室阳极设计与工厂阳极设计之间的差距

IF 23.5 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.004

Jun Xu, Yuting Yang, Huanyu Jin, Yao Zheng, Shi-Zhang Qiao

Rationally designing anode electrocatalysts is crucial for advancing next-generation proton exchange membrane water electrolyzers (PEMWEs). However, the most developed oxygen evolution catalysts in labs often cannot be directly applied to commercial PEMWEs due to differences in durability, performance, and cost. In this perspective, we review these gaps between fundamental lab research and practical device requirements and propose solutions to bridge them. We cover degradation mechanisms and durability evaluations in lab-scale aqueous model systems (AMSs) and PEMWEs. The need for performance benchmarking for anode screening and assessment is addressed, emphasizing reliable test protocols in AMSs and PEMWEs. Additionally, we discuss the importance of cost reduction in anodic catalyst design for future PEMWEs systems. Finally, we highlight major challenges and propose outlooks for anode design in fab-oriented applications to achieve the ultimate green hydrogen goal of “1 kg H₂ produced by 1 USD in 1 decade” (“111” goal).

合理设计阳极电催化剂对于推动下一代质子交换膜水电解器（PEMWEs）的发展至关重要。然而，由于耐久性、性能和成本方面的差异，实验室中最先进的氧进化催化剂往往不能直接应用于商用 PEMWE。在本文中，我们回顾了实验室基础研究与实际设备要求之间的差距，并提出了弥合这些差距的解决方案。我们将对实验室规模的水模型系统（AMS）和 PEMWE 的降解机制和耐用性进行评估。我们讨论了阳极筛选和评估对性能基准的需求，强调了 AMS 和 PEMWEs 中可靠的测试协议。此外，我们还讨论了为未来的 PEMWEs 系统降低阳极催化剂设计成本的重要性。最后，我们强调了在面向晶圆厂的应用中阳极设计所面临的主要挑战并提出了展望，以实现 "十年内用 1 美元生产 1 千克 H2"（"111 "目标）的绿色氢气终极目标。

引用次数: 0

Metal-cluster-powered ultramicropore alliance in pore-space-partitioned metal-organic frameworks for benchmark one-step ethylene purification 孔隙空间分区金属有机框架中的金属簇驱动超微孔联盟，实现基准一步法乙烯纯化

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem

Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.011

引用次数: 0

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