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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
Huimin Liu , Lichen Bai , Arno Bergmann , Beatriz Roldan Cuenya , Jingshan Luo
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 (NOx−) and gases (NOx), into the environment, causing a considerable burden on the natural denitrification processes. Electrocatalytic reduction of NOx− and NOx 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 NOx− and NOx 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。
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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
Leonard Präve , Wolfgang Kuttenlochner , Werner W.A. Tabak , Chiara Langer , Markus Kaiser , Michael Groll , Helge B. Bode
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。
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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。
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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
Shu-Yi Li, Shu-Cong Fan, Peng Zhang, Wen-Yu Yuan, Ying Wang, Quan-Guo Zhai
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引用次数: 0
Post-synthetic tuning of metal coordination on entangled scaffolds 缠结支架上金属配位的合成后调整
IF 19.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Chem
Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.08.023
Yuya Domoto
Entangled structures have fascinated scientists for both their artistic beauty and functional properties. Zhang and co-workers have recently reported, in the Journal of the American Chemical Society, the synthesis of a cinquefoil knot in which metal coordination sites can be tuned using post-synthetic protocols, providing a way to edit the skeletons of topological molecules in order to endow them with otherwise inaccessible functions.
纠缠结构的艺术美感和功能特性令科学家们着迷。Zhang 及其合作者最近在《美国化学学会杂志》（Journal of the American Chemical Society）上报告了一种五叶结的合成，其中的金属配位位点可通过后合成协议进行调整，从而提供了一种编辑拓扑分子骨架的方法，以赋予它们其他无法获得的功能。
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引用次数: 0
Camphor the polymerization; stay for the depolymerization 樟树聚合；留下解聚
IF 19.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Chem
Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.023
Inbar Zaltsman , Moshe Kol
The environmental accumulation of oil-based plastics calls for the introduction of alternatives emerging from renewable resources that are chemically recycled back to monomer. In this issue of Chem, Miyake and coworkers describe camphor-derived monomers that give polymers of varying stereo-regularities and desired properties that may be depolymerized back to monomer.
油基塑料在环境中的累积效应要求引入可从可再生资源中提取的替代品，这种替代品可以通过化学反应回收单体。在本期《化学》杂志上，Miyake 及其同事介绍了樟脑衍生单体，这些单体可生成具有不同立体规则性和理想特性的聚合物，并可解聚回单体。
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引用次数: 0
Battery detectives: Uncovering cathode impact on anode-free Li cell performance by operando NMR 电池侦探：通过操作型核磁共振发现阴极对无阳极锂电池性能的影响
IF 19.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Chem
Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.009
J. David Bazak , Karl T. Mueller , Vijayakumar Murugesan
Anode-free Li-ion batteries could attain new levels of energy density, but challenges remain in controlling deposition and managing degradation. In this issue of Chem, Kwon et al. probe Li metal growth using operando NMR to unravel how cathode materials impact performance and establish criteria for the high-energy/low-cost design tradeoff.
无阳极锂离子电池可以达到新的能量密度水平，但在控制沉积和管理降解方面仍然存在挑战。在本期的《化学》杂志上，Kwon 等人利用操作数核磁共振技术探究了锂金属的生长，从而揭示了阴极材料对性能的影响，并为高能量/低成本设计权衡建立了标准。
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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。
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引用次数: 0
Fine-tuning of proteasome inhibitors through rational pathway engineering 通过合理的途径工程微调蛋白酶体抑制剂
IF 19.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Chem
Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.019
Martin Baunach
The production of tailored biological drugs by genetic engineering represents a significant challenge in the field of natural product chemistry. In this issue of Chem, Bode and co-workers have successfully developed a biosynthetic production platform for novel syrbactin-class proteasome inhibitors by assembling an NRPS/PKS hybrid from four different natural megasynthetases.
通过基因工程生产定制生物药物是天然产物化学领域的一项重大挑战。在本期《化学》杂志上，Bode 及其合作者通过从四种不同的天然巨合成酶中组装出一种 NRPS/PKS 混合物，成功开发出了一种新型 syrbactin 类蛋白酶体抑制剂的生物合成生产平台。
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引用次数: 0
Simple physical organic model to predict mechanochemical bond-breaking 预测机械化学键断裂的简单物理有机模型
IF 19.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Chem
Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.010
Manabu Abe
Mechanochemical force can pull apart specific bonds, an action that is crucial for efficient and selective chemical transformations. Predicting chemical reactivity under tension force unlocks the selective bond cleavage reaction using ultrasonic irradiation. In this issue of Chem, Craig, Kulik, Moore, and colleagues developed an intuitive physical organic model to understand and predict the chemical reactivity of carbon-carbon bonds under tension.
机械化学力可以拉开特定的化学键，这种作用对于高效和选择性的化学转化至关重要。通过预测拉力作用下的化学反应性，可以利用超声波辐照解开选择性键裂反应。在本期《化学》杂志中，克雷格、库利克、摩尔及其同事开发了一种直观的物理有机模型，用于理解和预测碳-碳键在拉力作用下的化学反应性。
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引用次数: 0
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